CN112466738A - Multi-nozzle gas cluster ion beam processing system and operation method - Google Patents

Abstract

A multi-nozzle gas cluster ion beam processing system and method of operation, a method of irradiating a substrate with a Gas Cluster Ion Beam (GCIB), based on a GCIB processing system, said system comprising a set of at least two nozzles for forming and emitting gas cluster beams; loading a substrate to be processed into a GCIB processing system; irradiating at least one region on the substrate with a first GCIB formed by at least two nozzle groups; irradiating at least one region on the substrate with a second GCIB formed by at least first and second two nozzle groups, wherein the first GCIB and the second GCIB are directed along an ion beam axis common to the first GCIB and the second GCIB; wherein the GCIB processing system further comprises a gas separator and at least one gas supply in communication with a first nozzle group and with a second nozzle group different from the first nozzle.

Description

Multi-nozzle gas cluster ion beam processing system and operation method

Technical Field

The present invention relates to a system having a plurality of nozzles for irradiating a substrate using a Gas Cluster Ion Beam (GCIB), and a method of irradiating a substrate using the multi-nozzle GCIB processing system.

Background

Gas cluster ion beams (GCIB's) are used for doping, etching, cleaning, smoothing and growing or depositing layers on substrates. For ease of discussion, a gas-cluster is an aggregate of nanomaterials that are in a gaseous state under standard temperature and pressure conditions. Such gas clusters may consist of aggregates that are aggregated together, including several to thousands of molecules or more. The gas-clusters may be ionized by electron bombardment, thereby causing the gas-clusters to form a directed beam of controllable energy. These cluster ions typically each carry a positive charge given by the product of the magnitude of the charge and an integer representing the charge state of the cluster ion or an integer greater than 1. Larger sized cluster ions are generally most useful because they can carry a large amount of energy per cluster ion, while only modest energy per molecule. The ion clusters disintegrate upon collision with the substrate. Each molecule in a particular dissociated ion cluster carries only a small fraction of the total cluster energy. Thus, the impact effect of large ion clusters is large, but limited to very shallow surface areas. This allows the gas cluster ions to be effective for a variety of surface modification processes without the deeper subsurface damage typical of conventional ion beam processing.

Conventional cluster ion sources produce cluster ions having a broad size distribution, which reaches thousands of molecules in proportion to the number of molecules in each cluster. During the adiabatic expansion of the high pressure gas from the nozzle to the vacuum, condensation of individual gas atoms (or molecules) can form clusters of atoms. A gas separator with small holes will strip the diverging gas stream from the center of this expanding gas stream to produce a collimated cluster beam. Neutral clusters of various sizes are created and maintained by weak interatomic forces known as van der waals forces. This method has been used to generate clusters from a variety of gases (e.g., helium, neon, argon, krypton, xenon, nitrogen, oxygen, carbon dioxide, sulfur hexafluoride, nitric oxide, nitrous oxide, and mixtures of these gases). Some emerging applications for GCIB processing of substrates on an industrial scale are in the semiconductor field. Although GCIB processing of substrates is performed using a variety of gas cluster source gases, many of which are inert gases, many semiconductor processing applications still use reactive gases, sometimes combined or mixed with inert or noble gases, to form GCIBs. The compositions of certain gases or gas mixtures are incompatible due to their reactivity, and there is a need for a GCIB system that overcomes the incompatibility problem.

Disclosure of Invention

It is an object of the present invention to provide an assembly and system having a plurality of nozzles for irradiating a substrate with a Gas Cluster Ion Beam (GCIB), and an associated method involving irradiating a substrate using a multi-nozzle GCIB processing system to process a layer on the substrate. Furthermore, the present invention relates to an assembly and system having a plurality of nozzles for irradiating a substrate with GCIB and to an associated method of sequentially irradiating a substrate to treat layers on the substrate using a multiple nozzle GCIB processing system.

The technical scheme of the invention is as follows: a multi-nozzle gas cluster ion beam processing system and method of operation, a method of irradiating a substrate with a Gas Cluster Ion Beam (GCIB), based on a GCIB processing system, said system comprising a set of at least two nozzles for forming and emitting gas cluster beams; loading a substrate to be processed into a GCIB processing system; irradiating at least one region on the substrate with a first GCIB formed by at least two nozzle groups; irradiating at least one region on the substrate with a second GCIB formed by at least first and second two nozzle groups, wherein the first GCIB and the second GCIB are directed along an ion beam axis common to the first GCIB and the second GCIB;

wherein the GCIB processing system further comprises a gas separator, and at least one gas supply in communication with a first nozzle group and with a second nozzle group different from the first nozzle, the first and second nozzle groups comprising at least one nozzle, and wherein each nozzle of the at least two nozzle groups is configured to form and emit a gas cluster beam, and the two nozzles of the at least one nozzle group are arranged in close proximity to each other and are capable of at least partially focusing each gas beam of the ion gas cluster beams emitted from the at least two nozzle groups into the gas separator along an ion beam axis; the at least one gas supply comprises: a first gas supply in communication with the first nozzle group; the second gas supply source is communicated with the second nozzle group; the first GCIB irradiating at least one region on the substrate comprises: flowing a first gas mixture from at least one gas supply through at least a first nozzle group to form a first ion gas cluster beam, directing the first ion gas cluster beam through a gas separator along a beam axis, then ionizing the first ion gas cluster beam to form a first GCIB, and accelerating the first GCIB toward a substrate; the second GCIB illuminating at least one region on the substrate, comprising: flowing a second gas mixture from at least one gas supply through at least a second nozzle group to form a second ion gas cluster beam, directing the second ion gas cluster beam through the gas separator along the ion beam axis, and then ionizing the second ion gas cluster beam to form a second GCIB and accelerating the second GCIB toward the substrate.

Wherein the first GCIB and the second GCIB have the same atomic and/or molecular composition; or the first GCIB and the second GCIB have different atomic and/or molecular compositions.

Wherein the first and second GCIBs comprise one or more elements selected from the group consisting of H, B, C, Si, Ge, N, P, As, O, S, F, C1, Br, He, Ne, Ar, Kr, or Xe.

Wherein one or more gas supply parameters selected from stagnation pressure and stagnation temperature are the same or different for the first and second GCIBs. Wherein one or more process parameters selected from beam energy, beam energy distribution, beam focus, and beam dose are the same or different for the first GCIB and the second GCIB.

The first GCIB irradiating a layer on the substrate over which the at least one region on the substrate is to perform one or more processes on the substrate selected from the group of doping, growing, depositing, etching, smoothing, amorphizing, or modifying; and irradiating at least one region on the substrate with the second GCIB to perform one or more processes selected from the group of doping, growing, depositing, etching, smoothing, amorphizing or modifying the substrate one layer above it; while at least a portion of the substrate is irradiated with a first GCIB and at least a portion of the substrate is irradiated with a second GCIB.

Sequentially performing a partial overlap comprising between irradiating at least a portion of the substrate with the first GCIB and irradiating at least a portion of the substrate with the second GCIB; the sequential second illumination partially overlaps the sequential first illumination.

At least a portion of the substrate is irradiated with a first GCIB and at least a portion of the substrate is irradiated with a second GCIB alternately and sequentially.

The GCIB processing system also includes a gas separator, and at least one gas supply in fluid communication with a first nozzle group and with a second nozzle group different from the first nozzle group, the first and second nozzle groups each comprising at least one nozzle of at least two nozzle groups, and wherein each nozzle of at least two nozzle groups is configured to form and emit an ion gas cluster beam having an ion gas cluster beam axis, the at least two nozzles being grouped at an angle such that each ion gas cluster beam axis converges toward a single intersection point, and one or more ion gas cluster beams are directed into the gas separator along the beam axis.

Providing a GCIB processing system having at least two nozzles for forming and emitting gas cluster beams; loading a substrate to be processed into the GCIB processing system; sequentially, first, at least one region on the substrate is irradiated with a first GCIB formed by a first nozzle group of the at least two nozzle groups; then, in turn, irradiating at least one region on the substrate with a second GCIB formed on the substrate; or a second nozzle group of the at least two nozzle groups is different from the first nozzle group.

According to one embodiment, a method of irradiating a substrate with a GCIB is provided. The method includes providing a GCIB processing system that includes a set of at least two nozzles for forming and emitting a gas cluster beam. The method further comprises the following steps: loading a substrate to be processed into a GCIB processing system; irradiating at least one region on the substrate with a first GCIB formed from a set of at least two nozzles; and irradiating at least one region on the substrate with the second radiation. GCIBs formed using a set of at least two nozzles, wherein a first GCIB and a second GCIB are directed along an ion beam axis common to the first GCIB and the second GCIB. Further comprising providing a GCIB processing system having a set of at least two nozzles for forming and emitting gas cluster beams, and loading a substrate to be processed into the GCIB processing system. The method further comprises the following steps: at least one region on the substrate is first sequentially irradiated with a first GCIB formed using a first nozzle group in a set of at least two nozzles, and then sequentially irradiated with a second GCIB. A second set of nozzles different from the first set of nozzles is used in the set of at least two nozzles.

Has the advantages that: GCIB systems that address the incompatibility problem of compositions of certain gases or gas mixtures that are incompatible due to their reactivity. The plurality of nozzles are used in an associated method of irradiating a substrate with GCIB and sequentially irradiating the substrate with a plurality of nozzle GCIB processing systems to process layers on the substrate.

Drawings

Figure 1 is a schematic diagram of a multi-nozzle GCIB processing system according to an embodiment of the present invention.

Figure 2 is a schematic diagram of a multi-nozzle GCIB processing system according to another embodiment of the invention.

Figure 3 is a schematic diagram of a multi-nozzle GCIB processing system according to yet another embodiment of the invention.

Figure 4 is a schematic diagram of an embodiment of an ionizer for use in a GCIB processing system.

Fig. 5-9 are schematic diagrams of various embodiments of various multi-nozzle assemblies including multiple nozzles, single or multiple gas supplies, and various gas flow interconnections disposed therebetween, respectively.

Fig. 10A-12B are cross-sectional views of various embodiments of various multi-nozzle assemblies, respectively, depicting various arrangements of multiple nozzles and having various gas separator cross-sectional shapes to accommodate the various nozzle arrangements.

Figures 13A-D are schematic diagrams of various embodiments of multiple nozzle assemblies, respectively, having nozzles mounted at inwardly directed angles such that ion gas shower beams intersect at a point along the main GCIB axis.

Figures 14A-14F respectively provide schematic diagrams of methods for operating a GCIB processing system having a plurality of nozzles in accordance with various embodiments.

Detailed Description

In the following description, for purposes of explanation and not limitation, specific details are set forth, such as a particular geometry of the metrology system and descriptions of various components and processes, in order to facilitate a thorough understanding of the present invention. However, it should be understood that the invention may be practiced in other embodiments that depart from these specific details. Referring now to fig. 1, a GCIB processing system 100 for modifying, depositing, growing or doping layers is shown in accordance with an embodiment. GCIB processing system 100 includes vacuum vessel 102, substrate holder 150, and vacuum processing systems 170A, 170B, and 170C, with substrate 152 to be processed secured to substrate holder 150. The substrate 152 may be a semiconductor substrate, a wafer, a Flat Panel Display (FPD), a Liquid Crystal Display (LCD), or any other workpiece. GCIB processing system 100 is configured to generate a GCIB for processing substrate 152.

Still referring to GCIB processing system 100 in fig. 1. As shown in fig. 1, the vacuum vessel 102 includes three communicating chambers, a source chamber 104, an ionization/acceleration chamber 106, and a process chamber 108, to provide a reduced pressure enclosure. The three chambers are evacuated to the appropriate operating pressure by vacuum pumping systems 170A, 170B and 170C, respectively. In the three communicating chambers 104, 106, 108, a gas cluster beam may be formed in the first chamber (source chamber 104) and a GCIB may be formed in the second chamber (ionization/acceleration chamber 106), where the gas cluster beam is ionized and accelerated. The substrate 152 may then be processed with the accelerated GCIB in the third chamber (processing chamber 108).

In the exemplary embodiment of fig. 1, GCIB processing system 100 includes two gas supplies 115, 1015 and two nozzles 116, 1016. Further embodiments will be discussed later, in which the number of nozzles is different from two and the number of gas supplies is different from two, all falling within the scope of the invention. Each of the two gas supplies 115 and 1015 is connected to one of the two stagnation chambers 116 and 1016 and the nozzles 110 and 1010, respectively. The first gas supply source 115 includes a first gas source 111, a second gas source 112, a first gas control valve 113A, a second gas control valve 113B, and a gas metering valve 113. For example, a first gas composition is stored in a first gas source. The gas source 111 enters one or more gas metering valves 113 under pressure through a first gas control valve 113A. In addition, for example, the second gas component stored in the second gas source 112 enters under pressure through the second gas control valve 113B. Further, for example, the first gas component or the second gas component, or both, of the first gas supply 115 may include a condensable inert gas, carrier gas, or diluent gas. For example, the inert gas, carrier gas, or diluent gas may include a noble gas, i.e., He, Ne, Ar, Kr, Xe, or Rn.

Similarly, the second gas supply source 1015 includes a first gas source 1011, a second gas source 1012, a first gas control valve 1013A, a second gas control valve 1013B, and a gas metering valve 1013. For example, a first gas composition is stored at a first gas source 1011 under pressure through a first gas control valve 1013A into one or more gas metering valves 1013. Additionally, for example, a second gas component stored in the second gas source 1012 is admitted at a second pressure via a second gas control. The first gas component or the second gas component, or both, of the second gas supply 1015 may include a condensable inert gas, a carrier gas, or a diluent gas. For example, the inert gas, carrier gas, or diluent gas may include a noble gas, i.e., He, Ne, Ar, Kr, Xe, or Rn.

In addition, first gas sources 111 and 1011 and second gas sources 112 and 1012 are used to generate ionized clusters, respectively. The material composition of the first and second gas sources 111, 1011, 112 and 1012 comprises the main atomic (or molecular) species, i.e. the first and second atomic composition that is desired to be introduced to dope, deposit, modify or grow atoms. And (3) a layer.

High pressure, condensable gases comprising a first gas component and/or a second gas component enter the stagnation chamber 116 from a first gas supply 115 through a gas supply tube 114 and are injected through a suitably shaped nozzle 110 into a vacuum at a lower pressure whereupon the combustible gases expand from the stagnation chamber 116 to a lower pressure region of the source chamber 104 due to the expansion of the high pressure, the gas velocity accelerates to a supersonic velocity and a shower of ion gases is emitted from the nozzle 110.

Similarly, a high pressure condensable gas comprising the first gas component and/or the second gas component is introduced into the stagnation chamber 1016 from the second gas supply 1015 through the gas supply tube 1014 and is discharged by suitable shaping into a substantially low pressure vacuum as the gas velocity accelerates to a supersonic velocity due to the expansion of the high pressure expandable gas from the stagnation chamber 1016 to the low pressure region of the source chamber 104 and the ion gas cluster beam is emitted from the nozzle 1010.

The nozzles 110 and 1010 are mounted in close proximity so that the single ion gas cluster beam generated by the nozzles 110, 1010 substantially coalesces into a single ion gas cluster beam 118 in the vacuum environment of the source chamber 104 before reaching the gas separator 120. The "a" of the gas cluster beam 118 represents a mixture of components provided by the first and second gas supplies 115 and 1015, which are injected through the nozzles 110 and 1010.

The inherent cooling of the jet is exchanged for kinetic energy in static enthalpy, which is caused by the expansion of the jet, thereby condensing a portion of the jet and forming a gas cluster beam 118 having clusters, each cluster consisting of several to several atoms or molecules making up one thousand weak bonds. A gas separator 120 is located downstream of the outlets of the nozzles 110 and 1010 between the source chamber 104 and the ionization/acceleration chamber 106 to partially separate a portion of the gas molecules on the peripheral edge of the gas molecular beam 118, which may not have condensed into clusters formed by the gas molecules in the core of the ion gas cluster beam 118, which may have formed clusters. Among other reasons, such selection of a portion of the ion gas cluster 118 may result in a pressure reduction in the downstream region where higher pressures may be detrimental (e.g., the ionizer 122 and the process chamber 108). In addition, the gas separator 120 defines an initial size for the ion gas cluster beam entering the ionization/acceleration chamber 106.

The first and second gas supplies 115 and 1015 may be configured to independently control stagnation pressures and temperatures of the gas mixture introduced into the stagnation chambers 116 and 1016. Temperature control may be achieved by using a suitable temperature control system. A heater and/or cooler in each air supply (not shown). Additionally, the manipulator 117 may be mechanically coupled to the nozzle 110, for example, via the stagnation chamber 116, the manipulator 117 being configured to position the coupled nozzle 110 relative to the gas separator 120, independent of the nozzle 1010. Similarly, the manipulator 1017 may be mechanically coupled to the nozzle 1010, e.g., via the stagnation chamber 1016, the manipulator 1017 being configured to position the coupled nozzle 1010 relative to the gas separator 120, independent of the nozzle 110. Thus, each nozzle in the multi-nozzle assembly is relative to a single gas separator 120, which can be individually manipulated for proper positioning.

After forming the gas cluster beam 118 in the source chamber 104, the constituent gas clusters in the gas cluster beam 118 are ionized by the ionizer 122 to form the GCIB 128. The ionizer 122 may comprise an electron impact ionizer that generates electrons from one electron. Or more filaments 124 are accelerated and directed to collide with gas clusters in the ion gas cluster beam 118 inside the ionization/acceleration chamber 106. Upon collision with a gas cluster, electrons of sufficient energy release electrons from the molecules in the gas cluster to produce ionization of the ionized molecular gas-cluster can result in a large number of charged gas-cluster ions, typically having a net positive charge.

As shown in fig. 1, beam electronics 130 are used to ionize, extract, accelerate and focus GCIB 128. The beam electronics 130 includes a filament power supply 136 that provides a voltage V_FTo heat the ionizer filament 124.

In addition, beam electronics 130 include a set of suitably biased high voltage electrodes 126 in ionization/acceleration chamber 106 that extract cluster ions from ionizer 122. The high voltage electrode 126 then accelerates the extracted cluster ions to a desired energy and focuses on the GCIB 128. The kinetic energy of the cluster ions in the GCIB128 is typically between about 1000 electron volts (1keV) and tens of keV. For example, the GCIB128 may accelerate to 1 to 100 keV.

As shown in FIG. 1, the beam electronics 130 also includes an anode power supply 134 that provides a voltage V to the anode of the ionizer 122_ATo accelerate electrons emitted from the ionizer filament 124 and cause the electrons to bombard gas clusters in the ion gas cluster beam 118, thereby generating cluster ions. .

In addition, as shown in fig. 1, the beam electronics 130 includes an extraction power supply 138, the extraction power supply 138 providing a voltage VE to bias at least one high voltage electrode 126 to extract ions from the ionization region of the ionizer 122 and form the GCIB 128. For example, the extraction power supply 138 provides a voltage to a first electrode of the high voltage electrodes 126 that is less than or equal to the anode voltage of the ionizer 122.

In addition, the beam electronics 130 may include an accelerator power supply 140, the accelerator power supply 140 providing a voltage V_ACCTo bias one of the high voltage electrodes 126 relative to the ionizer 122, resulting in a total GCIB acceleration energy equal to about V_ACCElectron volts (eV). For example, the accelerator power supply 140 provides a voltage to the second electrode of the high voltage electrodes 126 that is less than or equal to the anode voltage of the ionizer 122 and the extraction voltage of the first electrode.

Further, the beam electronics 130 may include lens power supplies 142, 144, which may be provided with a potential (e.g., V |)_L1And V_L2) Some of the high voltage electrodes 126 are biased to focus the GCIB 128. For example, the lens power supply 142 may provide a voltage less than or equal to the anode voltage of the ionizer 122 to the third electrode of the high voltage electrodes 126, the extraction voltage of the first electrode and the accelerator voltage of the second electrode and the voltage 144 of the lens power supply may provide a voltage less than or equal to the anode voltage of the ionizer 1222, the extraction voltage of the first electrode, the accelerator voltage of the second electrode and the first voltage to the fourth electrode of the high voltage electrodes 126. Lens voltage of the third electrode.

Note that many variations on the ionization and extraction scheme may be used. While the approach described herein is useful for illustration, another extraction approach involves placing the first elements (or extraction optics) of the ionizer and extraction electrodes at V_ACC. This typically requires fiber programming of the control voltage to the ionizer power supply, but creates a simpler overall optical system. The invention described herein is useful regardless of the details of the ionizer and the extraction lens offset. A beam filter 146 in the ionization/acceleration chamber 106 downstream of the high voltage electrode 126 may be used to remove monomers or monomers and light cluster ions from the GCIB128 to define a filtered process GCIB128A into the processing chamber 108. In one embodiment, beam filter 146 substantially reduces the number of clusters having 100 or fewer atoms or molecules or both. The beam filter 146 may include a magnet assembly for application over the GCIB128Magnetic fields to assist the filtering process.

Still referring to fig. 1, a beam gate 148 is disposed in the path of the GCIB128 in the ionization/acceleration chamber 106. The beam gate 148 has an open state in which the GCIB128 is allowed to define a process GCIB128A from the ionization/acceleration chamber 106 through to the processing chamber 108 and is in a closed state in which the GCIB128 is prevented from entering the processing chamber 108. The control cables conduct control signals from the control system 190 to the ion beam gate 148. The control signal controllably switches the ion beam gate 148 between open and closed states.

Substrate 152, which may be a wafer or semiconductor wafer, a Flat Panel Display (FPD), a Liquid Crystal Display (LCD), or other substrate to be processed by GCIB processing, is disposed in the path of processing GCIB 128A. Since most applications desire to process large substrates with spatially uniform results, a scanning system may be required to uniformly scan the process GCIB128A over a large area to produce spatially uniform results.

The X-scan actuator 160 provides linear motion of the substrate support 150 in the direction of X-scan motion (into and out of the plane of the paper). Y-scan actuator 162 provides linear motion of substrate holder 150 in the direction of Y-scan motion 164, which is generally orthogonal to the X-scan motion. The combination of X-scan and Y-scan motions translates substrate 152 held by substrate holder 150 in a raster-like scanning motion by process GCIB128A to cause uniform (or otherwise programmed) illumination of the substrate surface. The processing of the substrate 152 is performed by a process GCIB 128A.

The substrate holder 150 disposes the substrate 152 at an angle relative to the axis of the process GCIB128A such that the process GCIB128A has an ion beam incident angle 166 relative to the substrate 152 surface. The ion beam incident angle 166 may be 90 degrees or other angles, but is typically 90 degrees or near 90 degrees. During the Y scan, the substrate 152 and substrate holder 150 move from the positions shown to alternate positions "a" indicated by indicators 152A and 150A, respectively. Note that substrate 152 will be scanned by process GCIB128A as it is moved between the two positions and moved completely out of the way of process GCIB128A at the two extreme positions (overscan). Although not explicitly shown in fig. 1, similar scanning and overscan are performed in (typically) orthogonal X-scan motion directions (in and out of the page).

A beam current sensor 180 can be disposed above substrate holder 150 in the path of process GCIB128A to intercept a sample of process GCIB128A as the path of process GCIB128A is scanned from substrate holder 150. The beam current sensor 180 is typically a faraday cup or the like, except that the beam entrance opening is closed and typically secured to the walls of the vacuum vessel 102 by an electrically insulating mount 182.

As shown in fig. 1, the control system 190 is connected to the X scan actuator 160 and the Y scan actuator 162 through cables, and controls the X scan actuator 160 and the Y scan actuator 162 so as to put or remove the substrate 152 in or out of the substrate 152. The GCIB128A is processed and the substrate 152 is uniformly scanned relative to the processing GCIB128A to achieve a desired processing of the substrate 152 by the processing GCIB 128A. The control system 190 receives the sampled beam current collected by the beam current sensor 180 through the cable to monitor the GCIB and control the GCIB dose received by the substrate 152 by removing the substrate 152 from the process GCIB 128A. When the predetermined dose has been delivered.

In the embodiment illustrated in fig. 2, GCIB processing system 100' can be similar to the embodiment of fig. 1, and further includes an X-Y positioning stage 253 that is operable to hold and move substrate 252 in two axes to effectively scan substrate 252 relative to process GCIB 128A. For example, the X motion may include motion into and out of the plane of the paper, and the Y motion may include motion in direction 264.

The process GCIB128A impacts the substrate 252 at the protruding impact region 286 on the surface of the substrate 252 and at an angle of ion beam incident angle 266 relative to the surface of the substrate 252. By XY motion, XY positioning stage 253 can position each portion of the surface of substrate 252 in the path of process GCIB128A so that each region of the surface can be brought into registration with projected impact region 286 for processing by process GCIB 128A. An X-Y controller 262 provides electrical signals to the X-Y positioning stage 253 via cables to control position and velocity in the X-axis and Y-axis directions. The X-Y controller 262 receives control signals from the control system 190 via a cable and is operable by the control system 190. The X-Y positioning stage 253 moves in a continuous motion or a stepped motion in accordance with conventional XY stage positioning techniques to position different areas of the substrate 252 within the projected impact region 286. In one embodiment, the XY positioning stage 253 can be operated in a programmable manner by a control device. The system 190 scans any portion of the substrate 252 across the projected impingement region 286 at a programmable speed for GCIB processing by the process GCIB 128A.

The substrate holding surface 254 of the positioning table 253 is electrically conductive and is connected to a dosimetry processor operated by the control system 190. An electrically insulating layer 255 of a positioning table 253 isolates the substrate 252 and the substrate holding surface 254 from the positioned base 260. The charge induced in the substrate 252 by the impinging process GCIB128A is conducted through the substrate 252 and the substrate holding surface 254, and a signal is coupled to the control system 190 through the positioning table 253 for dosimetry. Dosimetry has integration means for integrating GCIB current to determine GCIB treatment dose. In some cases, the GCIB128A process may be neutralized using a source of target neutralizing electrons (not shown), sometimes referred to as electron flood. In this case, faraday cups (not shown, but which may be placed in the housing similar to beam current sensor 180 in fig. 1) may be used to ensure accurate dosimetry despite the addition of a charge source, since typical faraday cups only allow high energy positive ions to enter and be measured.

In operation, the control system 190 signals the opening of the ion beam gate 148 to irradiate the substrate 252 with the process GCIB 128A. The control system 190 monitors measurements of GCIB current collected by the substrate 252 in order to calculate the cumulative dose received by the substrate 252. When the dose received by the substrate 252 reaches a predetermined dose, the control system 190 closes the electron beam gate 148 and processes. The upper surface of the substrate 252 is completed. Based on the measurement of GCIB dose received for a given area of the substrate 252, the control system 190 can adjust the scan speed in order to obtain an appropriate beam dwell time to process different areas of the substrate 252.

Alternatively, the process GCIB may be scanned in a fixed pattern over the surface of the substrate 252 at a constant speed128A; however, GCIB intensity (which may be referred to as Z-axis modulation) is modulated to deliver an intentionally non-uniform dose of sample. GCIB intensity can be adjusted in GCIB processing system 100' by any of a variety of methods, including varying the flow of gas from the GCIB source; by varying the filament voltage V_FOr changing the anode voltage V_ATo condition the ionizer 122; and by varying the filament voltage V_FOr changing the anode voltage V_ATo regulate ionizer 122. By varying the lens voltage V_L1and/V_L2To adjust the lens focus; or with a variable ion beam block, adjustable shutter or iris to mechanically block a portion of the GCIB. The modulation variation may be a continuous analog variation or may be a time modulated switching or gating.

The process chamber 108 may further include an in-situ metrology system. For example, the in-situ metrology system may include an optical diagnostic system having an optical emitter 280 and an optical receiver 282, the optical emitter 280 and the optical receiver 282 configured to illuminate the substrate 252 with an incident optical signal 284 and receive a scattered optical signal 288 from the substrate 252, respectively. The optical diagnostic system includes an optical window to allow the incident light signal 284 and the scattered light signal 288 to enter and exit the process chamber 108. Further, the optical transmitter 280 and the optical receiver 282 may include transmitting and receiving optics, respectively. The optical transmitter 280 receives electrical signals from the control system 190 and responds to control the electrical signals. The optical receiver 282 returns the measurement signal to the control system 190.

The in-situ metrology system may include any instrument configured to monitor the progress of the GCIB processing. According to one embodiment, the in-situ metrology system may constitute an optical scatterometry system. The scatterometry system may include a scatterometer that combines an ion beam profilometer (ellipsometer) and an ion beam profilometer (reflectometer), available from Therma-Wave, Inc. (1250 bearing Way, Fllimmont, Calif. 94539) or Nanometrics, Inc (1550Buckeye Drive, Milpitas, Calif. 95035).

For example, the in-situ metrology system may include an Integrated Optical Digital Profiler (iODP) scatterometer module configured to measure process performance data resulting from the performance of a process in the GCIB processing system 100'. The metrology system may measure or monitor metrology data generated by the process. The metrology data may be used to determine process performance data characterizing a process, such as process rate, relative process rate, feature profile angle, critical dimension, feature thickness or depth, feature shape, and the like. For example, in a process for directionally depositing a material on a substrate, process performance data may include Critical Dimensions (CDs), such as top, middle, or bottom CDs in a feature (i.e., via, line, etc.), feature depth, material thickness, sidewall angle, sidewall shape, deposition rate, relative deposition rate, any parameter spatially distributing it, a parameter characterizing the uniformity of any spatial distribution thereof, and the like. The in-situ metrology system can map one or more feature substrates 252 by operating the XY positioning table 253 via control signals of the control system 190.

In the embodiment illustrated in fig. 3, GCIB processing system 100 "may be similar to the embodiment of fig. 1 and further include a pressure chamber, i.e., pressure sensor chamber 350, for example, located at or near the exit region of ionization/acceleration chamber 106. The pressure sensor chamber 350 includes an inert gas source 352 and a pressure sensor 354, the inert gas source 352 configured to supply an ambient gas to the pressure sensor chamber 350 to increase the pressure in the pressure sensor chamber 350, the pressure sensor 354 configured to measure the increased pressure in the pressure sensor chamber 350. A pressure chamber 350.

The pressure sensor chamber 350 can be configured to modify the beam energy distribution of the GCIB128 to produce a modified processing GCIB 128A'. Such modification of ion beam energy distribution can be achieved by indicating the GCIB128

Along the GCIB path through the increased pressure region within the pressure chamber 350 such that at least a portion of the GCIB traverses the increased pressure region. The degree of change in beam energy distribution can be characterized by a pressure-distance integral along at least a portion of the GCIB path, where the distance (or length of the pressure chamber 350) is represented by the path length (d). The value of the pressure-distance integral increases (by increasing the pressure and/or path length (d)), the ion beam energy distribution widens and the peak energy decreases. As the value of the pressure-distance integral decreases (by decreasing the pressure and/or path length (d)), the beam energy distribution narrows and the peak energy increases. Further details of the pressure sensor design can be found in U.S. patent No.7,060,989 entitled "method and apparatus for improving using a gas cluster ion beam," which is incorporated herein by reference in its entirety.

Control system 190 includes a microprocessor, a memory, and a digital I/O port capable of generating control voltages sufficient to communicate and activate inputs to GCIB processing system 100 (or 100', 100 "), as well as monitoring outputs 100 (or 100', 100") from the GCIB processing system. In addition, the control system 190 may be connected to and exchange information with the vacuum pumping systems 170A, 170B, and 170C, the first gas sources 111 and 1011, the second gas sources 112 and 1012, the first gas control valves 113A and 1013A, and the second gas control valves. 113B and 1013B, electron beam 130, electron beam filter 146, electron beam gate 148, X scan actuator 160, Y scan actuator 162, and beam current sensor 180. For example, a program stored in memory can be used to activate inputs to the aforementioned components of GCIB processing system 100 in accordance with a process recipe in order to perform a GCIB process on substrate 152.

However, the control system 190 can be implemented as a general purpose computer system that performs a portion or all of the microprocessor based processing steps of the invention in response to a processor executing one or more sequences of one or more instructions contained in a memory. Such instructions may be read into the controller memory from another computer-readable medium, such as a hard disk or a removable media drive. One or more processors in a multi-processing arrangement may also be employed as the controller microprocessor to execute the sequences of instructions contained in main memory. In alternative embodiments, hard-wired circuitry may be used in place of or in combination with software instructions. Thus, embodiments are not limited to the specific combination of hardware circuitry and software.

As described above, the control system 190 may be used to configure any number of processing elements, and the control system 190 may collect, provide, process, store, and display data from the processing elements. The control system 190 may include a plurality of applications and a plurality of controllers for controlling one or more processing elements. For example, the control system 190 may include a Graphical User Interface (GUI) component (not shown) that may provide an interface that enables a user to monitor and/or control one or more processing elements.

Control system 190 can be located locally with respect to GCIB processing system 100 (or 100', 100 ") or remotely with respect to GCIB processing system 100 (or 100', 100"). For example, control system 190 can exchange data with GCIB processing system 100 using a direct connection, an intranet, and/or the internet. (the control system 190 may be coupled to an Intranet at, for example, a customer site (i.e., a device manufacturer, etc.), or it may be coupled to an Intranet manufacturer at, for example, a vendor site (i.e., a device)). Alternatively or additionally, the control system 190 may be coupled to the internet. In addition, another computer (i.e., controller, server, etc.) may access the control system 190 to exchange data via a direct connection to an intranet and/or the internet.

The substrate 152 (or 252) may be secured to the substrate holder 150 (or substrate holder 250) by a clamping system (e.g., a mechanical clamping system or an electrical clamping system (e.g., an electrostatic clamping system)) not shown. Accordingly, the substrate holder 150 (or 250) may include a heating system (not shown) or a cooling system (not shown) configured to regulate and/or control the temperature of the substrate holder 150 (or 250) and the substrate 152 (or 252). The vacuum pump systems 170A, 170B, and 170C can include a turbo-molecular vacuum pump (TMP) capable of a pumping speed of about 5000 liters per second (or greater), and a gate valve for throttling the chamber pressure. In conventional vacuum processing equipment, a 1000 to 3000 liter per second TMP can be employed. TMP can be used for low pressure processing, typically less than 50m Torr. Although not shown, it is understood that the pressure sensor chamber 350 may also include a vacuum pump system. Further, the means for monitoring the chamber pressure may be connected to the vacuum vessel 102 or any of the three vacuum chambers 104, 106, 108. The pressure measuring device may be a capacitance manometer or an ionization gauge.

Fig. 2 and 3 also show an alternative embodiment of the nozzle manipulator. Instead of each nozzle 110, 1010 being coupled to an individually operable manipulator 117, 1017 as in fig. 1, each nozzle 110, 1010 is coupled to an operable manipulator 117, 1017. As shown in fig. 1, the nozzles 110, 1010 may be coupled to each other and coupled together to a single manipulator 117A. The position of the nozzles 110, 1010 may then be manipulated as a whole, rather than individually, relative to the gas separator 120.

Referring now to fig. 4, a gas cluster ionizer 122 is shown for ionizing the gas cluster jet (gas cluster beam 118, fig. 1, 2 and 3). The portion 300 is perpendicular to the axis of the GCIB 128. For a typical gas cluster size (2000 to 15000 atoms), the clusters leaving the gas separator aperture (120, fig. 1, 2 and 3) and entering the ionizer (122, fig. 11A, fig. 1, 2 and 3) will travel with kinetic energies of about 130 to 1000 electron volts (eV). At these low energies, any deviation from space charge neutrality within the ionizer 122 will result in rapid dispersion of the jet and significant loss of beam current. Fig. 4 shows a self-neutralizing ionizer. Like other ionizers, gas clusters are also ionized by electron impact. In this design, thermionic electrons (an example of which is indicated at 310) are emitted from a plurality of linear thermionic filaments 302a, 302b and 302c (typically tungsten) and are extracted and focused by the action of an appropriate electric field provided by an electron repeller electrode 306 a. 306b and 306c and beam forming electrodes 304a, 304b and 304 c. The hot electrons 310 pass through the gas-cluster jet and the jet axis and then strike the opposite electron beam forming electrode 304b to generate low-energy secondary electrons (shown, for example, at 312, 314, and 316).

Although (for simplicity) (not shown) the linear thermionic filaments 302b and 302c also generate thermionic electrons, which in turn generate low-energy secondary electrons. All secondary electrons help to ensure that the ionized cluster jet remains space charge neutral by providing low energy electrons that can be attracted to the positively ionized gas cluster jet as needed to maintain space charge neutrality. The beam forming electrodes 304a, 304b and 304c are biased.

Positive with respect to the linear thermionic filaments 302a, 302b, and 302c, and the electron repeller electrodes 306a, 306b, and 306c negative with respect to the linear thermionic filaments 302a, 302b, and 302 c. Insulators 308a, 308b, 308c, 308d, 308e, and 308f electrically insulate and support electrodes 304a, 304b, 304c, 306a, 306b, and 306 c. For example, such self-neutralizing ionizers are effective up to 1000 microamperes or more of argon GCIB.

Alternatively, the ionizer may use extraction of electrons from the plasma to ionize the clusters. The geometry of these ionizers is very different from the three filament ionizers described here, but the working principle and ionizer control are very similar. For example, the design of the ionizer may be similar to the ionizer described in U.S. patent No.5,235,824. U.S. patent No.7,173,252 entitled "ionizer and method for gas cluster ion formation"; the contents of which are incorporated herein by reference in their entirety.

The gas cluster ionizer (122, fig. 13(b), fig. 1, 2, and 3) may be configured to modify the beam energy distribution of the GCIB128 by modifying the charge state of the GCIB 128. For example, the charge state may be altered for electrons used in electron impact induced gas cluster ionization by adjusting the electron flux, electron energy or electron energy distribution.

Referring now to fig. 5-9, various embodiments of the multi-nozzle and gas supply assemblies of GCIB processing systems 100 (or 100', 100 ") of fig. 1, 2, and 3, respectively, are described. Figure 5 shows an embodiment of a multi-nozzle. The gas supply assembly includes a single gas supply 2010 and two nozzles 2110 and 2120, fed by the gas supply 2010. For example, a gas supply arrangement such as first gas supply 115, gas supply 2010 (and all other figures 5-9) of GCIB processing system 100 of figure 1 can include a first gas source, a second gas source, a first gas control valve, a second gas control valve, and a gas metering valve to allow for the formation of a gas mixture comprised of the gases provided. The multi-nozzle and gas supply assembly of figure 5 is suitable for GCIB applications where a single gas requires a large volume of gas or mixture of gases, multiple nozzles need to be used, and therefore the same or similar stagnation conditions (i.e. pressure and temperature can be maintained in the stagnation chamber before the nozzles) and nozzles of the same or similar size as those in prior art single gas supply and single nozzle GCIB systems can be used.

Figure 6 generally depicts embodiments of the multi-nozzle and gas supply assemblies of the GCIB processing systems 100 (or 100', 100 ") of figures 1, 2, and 3, respectively. The assembly of fig. 6 includes two gas supplies 3010 and 3020 and two gas nozzles 3110 and 3120, making it useful in GCIB applications where it is desirable to form a gas cluster ion beam composed of a mixture of incompatible and/or pyrophoric gases. Such incompatible gas mixtures cannot be readily premixed in a single gas supply (e.g., gas supply 2010 of fig. 5) for injection through a single or multiple nozzles, at least because of adverse chemical reactions that can occur between the components of the single gas supply and the incompatible mixed gas components inside the conduits. Fig. 6 overcomes this problem by providing separate gas supplies 3010, 3020 for incompatible and/or pyrophoric gas mixture components, which are mixed only upon injection from nozzles 3110 and 3120 installed in the nozzle. In close proximity to each other so as to at least partially coalesce and produce a single gas cluster ion beam. Another advantage is that different diluent gases may be used in different gas mixtures, e.g., He may be used as the diluent gas for the first gas mixture and Ar may be used for the second gas mixture. The gas supplies 3010 and 3020 of the multi-nozzle and gas supply system of fig. 6 may also be configured to flow gas mixtures of the same composition to the nozzles 3110 and 3120. Further, the multi-nozzle and gas supply assembly of fig. 6 allows for the injection of the mixture from nozzles 3110 and 3120 at different stagnation pressures and/or temperatures, for example, if the optimal cluster nucleation conditions for the mixture are different, thus requiring different stagnation conditions. Stagnation pressure control is typically achieved by providing a gas metering valve for the gas supply, while stagnation temperature control may be achieved by using a suitable heater or cooling device (not shown).

Fig. 7 depicts a multi-nozzle and gas supply assembly similar to fig. 1 and 2. With reference to fig. 5 and 6, including gas supplies 4010 and 4020 and three nozzles 4110, 4120 and 4130, wherein gas supply 4010 supplies two nozzles 4110 and 4120, respectively, thereby allowing a higher flow rate of one gas mixture, while gas supply 4020 supplies only nozzle 4130 this configuration is suitable for applications requiring high flow rates of one gas mixture component, while retaining the ability to process incompatible and/or pyrophoric gases. Fig. 8 depicts an embodiment similar to that of fig. 6, extended to include three gas supplies 5010, 5020, and 5030, and three nozzles 5110, 5120, and 5130, allowing for the independent introduction of three different gas mixtures into the nozzles. Thus requiring a GCIB flow. Fig. 9 depicts an assembly similar to that of fig. 1-3. The combination of fig. 5 and 8, comprising three gas supplies 6010, 6020, and 6030, and four nozzles 6110, 6120, 6130, and 6140, wherein gas supply 6010 is connected to nozzles 6110 and 6120, allowing high gas mixture flow rates therethrough. The ability to independently provide two other mixed gas components.

Although the embodiments of the figures may be arranged to flow multiple gases or mixtures of gases to each nozzle simultaneously as required by the process conditions, it is also possible to operate multiple gas supplies and nozzles in a sequential manner, wherein at least one step is used in a series of processing steps requiring multiple gases or mixtures of gases to be flowed simultaneously. For example, in the embodiment of fig. 6, a first GCIB processing step may include flowing only a single gas or gas mixture generated by gas supply 3010 and introduced via nozzle 3110, and a second processing step may include first and second gases. Or a gas mixture generated by gas supplies 3010 and 3020 and introduced through nozzles 3110 and 3120, respectively.

It will be apparent that other embodiments of the plurality of nozzles and gas supply assembly are possible, including different numbers of nozzles (e.g., greater than four), and that some of the different numbers of gas supplies (e.g., greater than three) may be connected to the plurality of nozzles to accommodate the high flow rate, all of which fall within the scope of the present invention.

Fig. 10A-12B are cross-sectional schematic diagrams illustrating various spatial arrangements of multiple nozzles and various cross-sectional shapes of a single gas separator to be used with a particular nozzle arrangement. The close proximity of the nozzles within the module ensures that the individual ion gas clusters exiting the nozzles substantially or at least partially coalesce into individual ion gas clusters before reaching the gas separator. The ion gas clusters are bundled into a single ion gas cluster prior to reaching the gas separator, allowing the use of the same GCIB system components as the single gas supply and single nozzle GCIB systems of the prior art downstream of the gas separator. Given that these downstream components may be identical, it is envisioned that existing GCIB systems may be converted to multi-nozzle systems having multiple gas supplies with relatively few modifications and/or parts changes, primarily in GCIB systems.

Fig. 10A depicts a multi-nozzle assembly comprising two nozzles 7010 and 7020, the two nozzles 7010 and 7020 being mounted side-by-side (or alternatively oriented vertically above each other) as viewed in cross-section, forming a cluster beam of ion gas that passes through a gas separator 7000 of substantially circular cross-section. Fig. 10B shows a similar dual nozzle assembly with an elliptical or elliptical gas separator 7100 aligned with nozzles 7110 and 7120. FIG. 10C depicts a dual nozzle assembly with a dual lobe gas separator 7200 aligned with nozzles 7210 and 7220. Fig. 10A-C can be easily extended to assemblies with a large number of nozzles. For example, fig. 11A depicts an assembly with three nozzles 7310, 7320, and 7330, which inject a gas cluster beam through a substantially circular gas separator 7300. Fig. 11B depicts a similar three nozzle assembly, but with a three-lobed gas separator 7400 aligned with nozzles 7410, 7420, and 7430. Likewise, fig. 12A-B extend the concept to an assembly with four nozzles 7510, 7520, 7530, and 7540 and four nozzles 7610, 7620, 7630, and 7640, 7600 respectively, by a generally circular gas splitter 7500 and a four-lobed gas injection ion gas cluster beam splitter, 7600 respectively. Other embodiments are readily contemplated, all of which fall within the scope of the present invention.

Further, as shown in the partial schematic views of fig. 13A-13D, to aid in gas cluster beam coalescence, nozzles (three nozzles 410, 412, 414, although the invention is not limited thereto) may be shown mounted at a small angle. Pointing along the beam axis 119 of the ion gas cluster 118 of fig. 1 and 2 toward a single intersection point 420. As shown in fig. 1, 2 and 3. For example, the gas cluster beam axes 411, 413, 415 of the respective nozzles 410, 412, 414 can intersect at a single intersection point 420 along the beam axis 119 inside the ionizer 122 (e.g., 100 in the GCIB processing system diagram), as shown in fig. 13A. Alternatively, the gas cluster beam axes 411, 413, 415 of the respective nozzles 410, 412, 414 may intersect at a single intersection point 420 along the beam axis 119 downstream of the gas separator 120 but upstream of the ionizer 122. Fig. 13B in another alternative, the ion gas cluster beam axes 411, 413, 415 of the respective nozzles 410, 412, 414 may intersect at a single intersection point 420 along the beam axis 119 between the input and output of the gas separator 120. In fig. 13C, optionally, the gas cluster beam axes 411, 413, 415 of each nozzle 410, 412, 414 may intersect between the exit of the nozzles 410, 412, 414 and the nozzles 410, 412, 414 at a single intersection point 420 along the beam axis 119. The input to the gas separator 120 is shown in FIG. 13D. The inward tilt angle, i.e. the deviation from the parallel direction, may range from 0.5 to 10 degrees, or from 0.5 to 5 degrees, or from 1 to 2 degrees.

A method of irradiating a substrate with a GCIB according to one embodiment. The method includes 1) starting with providing a GCIB processing system having a set of at least two nozzles arranged in close proximity to each other to ensure coalescence of a single ion gas cluster beam before reaching a single gas separator or arranged to have intersecting ion beam axes, and a plurality of nozzles configured to supply at least the entire set of nozzles (e.g., a single nozzle of a mixed gas or a plurality of nozzles of a set). The GCIB processing system can be any of the GCIB processing systems (100, 100' or 100 ") described above in fig. 1, 2 or 3, or any combination thereof, with an arrangement of nozzles and gas supplies as shown in fig. 5, fig. 13D.

In step 2), the substrate is loaded into the GCIB processing system. The substrate may comprise a conductive material, a non-conductive material or a semi-conductive material, or a combination of two or more thereof. In addition, the substrate may include one or more material structures formed thereon, or the substrate may be a blanket substrate without material structures. The substrate can be placed on a substrate holder in a GCIB processing system and can be securely held on the substrate holder. The temperature of the substrate may or may not be controlled. For example, the substrate may be heated or cooled during film formation. The environment around the substrate is kept under reduced pressure.

In step 3), the flow of the first gas mixture is started from the first gas supply. The gas streams of all nozzles or groups of nozzles connected to the first gas supply through the nozzles form gas cluster beams or coalesced and/or intersecting gas cluster beams that enter the ionization chamber GCIB processing system through a single gas separator.

In step 4), an optional second gas mixture is introduced from an optional second gas supply source into the nozzles in all or a group of the remaining nozzles. The nozzles not supplied by the first gas supply of step 8010 and the nozzles supplied with the first gas mixture of step 8030. The optional second gas mixture may be the same or different from the first gas mixture, and if different, these gas mixtures may not be compatible. In addition, one of the gas mixtures may be pyrophoric. The optional second gas mixture also forms one or more ion gas cluster beams that coalesce and/or intersect with one or more beams from the first nozzle or group of nozzles to form a single ion gas cluster beam.

In step 5), the single gas cluster beam is ionized in an ionizer (e.g., ionizer 300 of fig. 4) to form a Gas Cluster Ion Beam (GCIB).

In step 6), the GCIB is accelerated by applying a beam accelerating potential to the GCIB.

In step 7), a GCIB consisting of the first gas mixture and the optional second gas mixture is used to irradiate the substrate loaded in the GCIB processing system.

The beam acceleration potential and beam dose can be selected to achieve the desired properties of the GCIB-irradiated layer on the substrate. For example, the beam acceleration potential and beam dose may be selected to control the desired thickness of the deposited or grown layer, or to achieve a desired surface roughness or other modification of the upper layers on top of the substrate, or to control the concentration and depth of penetration of the dopant into the substrate. Here, the ion beam dose is given in units of the number of clusters per unit area. However, the ion beam dose may also include ion beam current and/or time (e.g., GCIB dwell time). For example, the beam current may be measured and held constant while the time is varied to vary the beam dose. Alternatively, for example, when the time is changed to change the beam dose, the rate at which the clusters irradiate the substrate surface per unit area (i.e., the number of clusters per unit area per unit time) may be kept constant.

In addition, other GCIB attributes may vary, including but not limited to gas flow, stagnation pressure, cluster size or gas nozzle design (e.g., nozzle throat diameter, nozzle length and/or nozzle divergent cross-sectional half angle).

In addition, other GCIB attributes may vary, including but not limited to gas flow, stagnation pressure, cluster size or gas nozzle design (e.g., nozzle throat diameter, nozzle length and/or nozzle divergent cross-sectional half angle).

The choice of the combination of gases for the first and optional second gas mixtures depends on the process to which the substrate is subjected. The deposition or growth of the material layer may comprise depositing or growing SiO on the substrate or on top of an existing layer on the substrate_x，SiN_x，SiC_x，SiC_xO_y，SiC_xN_y，BN_x，BSi_xN_yGe, SiGe (B) or SiC (P) layer. According to embodiments of the present invention, the first or optional second gas mixture may thus comprise a nitrogen-containing gas, a carbon-containing gas, a boron-containing gas, a silicon-containing gas, a phosphorus-containing gas, sulfur. A hydrogen-containing gas, a silicon-containing gas, or a germanium-containing gas, or a combination of two or more thereof. Gases that may be used to form the first and second gas mixtures include: he, Ne, Ar, Kr, Xe, Rn, SiH₄，Si₂H₆，C₄H₁₂Si，C₃H₁₀Si，H₃C-SiH₃，H₃C-SiH₂-CH₃，(CH₃)₃-SiH，(CH₃)₄-Si，SiH₂Cl₂，SiCl₃H，SiCl₄，SiF₄，O₂，CO，CO₂，N₂，NO，NO₂，N₂O，NH₃，NF₃，B₂H₆Alkyl silanes, alkane silanes, alkene silanes, alkyne silanes and CxHy, wherein x.gtoreq.1 and y.gtoreq.24, and combinations of two or more thereof. The first gas mixture and the second gas mixture are formed from a first gas supply and a second gas supply of a GCIB processing system.

When depositing silicon, the substrate may be irradiated by a GCIB formed from a first or optional second gas mixture having a silicon-containing gas. For example, the gas mixture may comprise Silane (SiH)₄). In another example, the gas mixture may include disilane (Si)₂H₆) Ethylchlorosilane (SiH)₂Cl₂) Trichlorosilane (SiCl)₃H) Ethyl silane (C)₄H₁₂Si), trimethylsilane (C)₃H₁₀Si), silicon tetrachloride (SiCl)₄) Silicon tetrafluoride (SiF)₄) Or a combination of two or more thereof.

When depositing or growing materials such as SiO_xThe substrate may be irradiated by a GCIB formed from first and optionally second gas mixtures having a silicon-containing gas and an oxygen-containing gas, respectively. For example, the first gas mixture may comprise Silane (SiH)₄) The second gas mixture may contain O₂. In another example, the second gas mixture may include O₂，CO，CO₂，NO，NO₂Or N₂O, or any combination of two or more thereof.

When depositing or growing materials such as SiC_xThe substrate may be irradiated by a GCIB formed from first and optionally second gas mixtures having a silicon-containing gas and an oxygen-containing gas, respectively. For example, the first gas mixture may comprise Silane (SiH)₄) The second gas mixture may contain O₂. In another example, the second gas mixture may include O₂，CO，CO₂，NO，NO₂Or N₂O, or any combination of two or more thereof.

When depositing or growing, for example, SiN_xOf (2) is a nitrideThe substrate may be irradiated by a GCIB formed from a first and optional second gas mixture having a silicon-containing gas and a nitrogen-containing gas, respectively. For example, the first gas mixture may include Silane (SiH)₄) The second gas mixture may include N₂. In another example, the second gas mixture may include N₂，NO，NO₂，N₂O or NH₃(ii) a Or any combination of two or more thereof.

When depositing materials such as SiC_xThe substrate may be irradiated by a GCIB formed from a pressurized gas mixture having a silicon-containing gas and a carbon-containing gas. For example, the first gas mixture may comprise Silane (SiH)₄) And CH₄. Alternatively, the first gas mixture may contain only Silane (SiH)₄) Optionally, the second gas mixture may comprise CH₄. Additionally, for example, the first gas mixture can include Silane (SiH)₄) And the optional second gas mixture may comprise methylsilane (H)₃C-SiH₃). Further, for example, the first gas mixture may include a silicon-containing gas and CH₄(or more generally, hydrocarbon gas, i.e. C)_xH_y) And the optional second gas mixture may comprise CO or CO₂. Further, any of the first gas mixture and the optional second gas mixture may comprise, for example, an alkylsilane, an alkenylsilane, or an alkynylsilane, or any combination of two or more thereof. Additionally, for example, the first gas mixture can include silane, methylsilane H₃C-SiH3, dimethylsilane H₃C-SiH₂-CH₃) Trimethylsilane ((CH)₃)₃-SiH) or tetramethylsilane ((CH)₃)₄-Si), or any combination of two or more thereof. When growing or depositing materials such as SiC_xN_yThe optional second gas mixture may further comprise a nitrogen-containing gas. For example, the nitrogen-containing gas may include N₂，NH₃，NF₃，NO，N₂O or NO₂Or a combination of two or more thereof. Or addition of a nitrogen-containing gas may allow formation of silicon carbonitrideFilm (SiCN).

When growing or depositing nitrides, such as BN, the substrate may be irradiated by a GCIB formed from a first gas mixture having a boron-containing gas and an optional second gas mixture having a nitrogen-containing gas. For example, the first gas mixture may comprise diborane (B)₂H₆) And the optional second gas mixture may comprise N₂. In another example, the optional second gas mixture may include N₂，NO，NO₂，N₂O or NH₃Or any combination of two or more thereof.

When growing or depositing nitrides (e.g. BSi)_xN_y) The substrate may be irradiated by a GCIB that forms a gas station from a first gas mixture having a silicon-containing gas and an optional second gas mixture having a boron-containing gas and a nitrogen-containing gas. For example, the first gas mixture may comprise Silane (SiH)₄) Optionally, the second gas mixture may comprise diborane (B)₂H₆) And N₂. In another example, the optional second gas mixture may include B₂H₆，N₂，NO，NO₂，N₂O or NH₃Or any combination of two or more thereof.

In addition to layer growth and deposition, other gases may be used to form gas mixtures in the gas source of GCIB processing systems in other processes, such as implantation, doping, and layer surface modification. These gases include gases of germanium, phosphorus and arsenic, e.g. GeH₄，Ge₂H₆，GeH₂Cl₂，GeCl₃H, methyl germane, dimethyl germane, trimethyl germane, tetra-tert-methyl germane, ethyl germane, diethyl germane, triethyl germane, tetraethyl germane, GeCl₄,GeF₄，AsH₃，AsF₅，PH₃，PF₃，PCl₃Or PF₅Or any combination of two or more thereof.

In any of the above examples, the first and/or second gas mixtures may include an optional inert diluent gas. The dilution gas can include a noble gas, e.g., He, Ne, Ar, Kr, Xe, or Rn, which can be different for the first and second gas mixtures.

If the above process is further extended and it may be desirable to introduce an optional third, fourth, etc. gas mixture (not shown) that can be accommodated by the available gas supplies and number of nozzles installed in the GCIB system.

The inventors have found that in SiO₂The multi-nozzle GCIB system was tested during deposition and was used for felt SiO₂Deposition or trench filling, such as Shallow Trench Isolation (STI) structure filling. SiO2₂Similar methods can also be used for film growth. The hardware includes a dual nozzle GCIB system configured with a pressure sensor chamber, as shown in figure 2. With two gas sources. The gas supply configuration for the GCIB system is shown in figure 6. Each gas supply is provided with two gas sources: a first gas source for the process gas and a second gas source for the dilution gas. The nozzle configuration used is that shown in fig. 10A, in which the nozzles are mounted one after the other and the cross-section of the gas skimmer is circular. All other components of the GCIB system are single nozzle, single gas supply GCIB system components.

For depositing SiO on a substrate₂The first gas supply device is configured to supply SiH₄As a Si-containing gas, and then diluted with He to form a first gas mixture that is fed into the first nozzle. The total flow rate through the first nozzle is set in the range of 300 to 700sccm, typically 600sccm, but the flow rate during production can be higher or lower than the above range, for example 200 to 1000 sccm. The percentage of SiH4 in He in the first gas mixture is typically set to 10%, but may be set higher or lower than 10% during production, for example. Between 2% and 20%. The second gas supply device is configured to supply O at a flow rate of 200 to 500sccm₂Flows through the second nozzle as an O-containing gas and is optionally diluted with an additional He flow rate of 800 to 1100 seem to form a second gas mixture. In the actual production process, O₂And the flow rate of the optional diluent gas may be different. Mixing two gasesThe above flow rate range of the substance is converted into O₂/SiH₄The ratio, ranging from 3.3 to 16.7, determines in part the SiO₂Stoichiometry of the membrane.

The deposition process is carried out by using the mixture of the two gases to accelerate the potential V_ACCIs 10 to 50 kV. The gas flow into the pressure chamber was zero (i.e., off), or set at 20sccm, which translates to a pressure-distance integral of about 0.003Torr-cm under these conditions for a GCIB beam current of 15 to 49 μ A.

With O₂/SiH₄Increase in ratio, deposited SiO₂The color of the film ranges from brown to very pale colored or colorless. All films showed evidence of compressive stress in the obtained FTIR spectra, which is a common feature of most as-deposited GCIB films. For example, compressive stress may be reduced or eliminated by a post-deposition annealing process at a temperature range of 600 to 1000 degrees celsius for a duration of 15 to 60 minutes. The annealing process also causes film roughness R_aFrom the moment of deposition

Is reduced to

R_a(the intensity is dependent to a small extent on the GCIB process conditions), the reduction is

R is more than or equal to_a. Gap fill experiments were also performed in which the trenches were successfully filled with SiO2 before the trenches pinched off.

Another process step for forming Shallow Trench Isolation (STI) structures using a GCIB system with multiple nozzles and gas supplies. Methods of forming STI using a conventional single nozzle GCIB processing system are discussed in U.S. provisional patent application No.61/149, 917, entitled "method of forming trench isolation using gas cluster ion beam processing," the entire contents of which are incorporated herein by reference in their entirety.

The method begins at step (1) by providing a GCIB processing system having a set of at least two nozzles arranged in close proximity to one another to ensure that a single ion gas cluster beam converges before reaching a single gas separator, or arranged to have intersecting beam axes, a first gas supply configured to supply the set of all nozzles (e.g., a plurality of nozzles with a single nozzle or sub-set of mixed gases, and a second gas supply to supply the remaining nozzles (i.e., nozzles not supplied by the first gas supply). the GCIB processing system may be any of the GCIB processing systems (100, 100', 100 ") described above in fig. 1, 2 or 3, with any arrangement of nozzles and gas supplies as shown in fig. 5-13D.

In step (2), the substrate is loaded into the GCIB processing system. The substrate may comprise a conductive material, a non-conductive material or a semi-conductive material, or a combination of two or more thereof. In addition, the substrate may include one or more material structures formed thereon, or the substrate may be a blanket substrate without material structures. The substrate can be placed on a substrate holder in a GCIB processing system and can be securely held on the substrate holder. The temperature of the substrate may or may not be controlled. For example, the substrate may be heated or cooled during film formation. The environment around the substrate is kept under reduced pressure.

In step (3), the flow of the first gas mixture is started from the first gas supply. A gas stream passing through a nozzle or group of nozzles connected to a first gas supply forms a cluster beam of ion gas that passes through a single gas separator into an ionization chamber of a GCIB processing system.

In step (4), a second gas mixture is introduced from a second gas supply source into the nozzles in all or a group of the remaining nozzles. Nozzles not supplied by the first gas supply form one or more ion gas cluster beams that coalesce and/or intersect with one or more beams from the first nozzle or group of nozzles to form a single ion gas cluster beam.

In step (5), a single gas cluster beam is ionized in an ionizer, such as ionizer 300 of fig. 4, to form a Gas Cluster Ion Beam (GCIB).

In step (6), the GCIB is accelerated by applying an ion beam acceleration potential to the GCIB.

In step (7), the substrate loaded in the GCIB processing system is irradiated with a GCIB consisting of the first gas mixture and the second gas mixture to form STI structures on the substrate or on a layer on top of the substrate. STI structures may be used, for example, in memory devices.

To form SiO₂STI structures, i.e. using SiO₂Filling the STI trenches, the first gas mixture may include a silicon-containing gas. For example, the first gas mixture may include SiH₄，Si₂H₆，C₄H₁₂Si，C₃H₁₀Si，H₃C-SiH₃，H₃C-SiH₂-CH₃，(CH₃)₃-SiH，(CH₃)₄-Si，SiH₂Cl₂，SiCl₃H, SiCl4, SiF4, alkylsilane, alkenylsilane, alkynylsilane, or any combination of two or more thereof. Optionally, the first gas mixture may further comprise an inert diluent gas. The dilution gas may include a rare gas, for example, He, Ne, Ar, Kr, Xe, or Rn. To form the STI structure, the second gas mixture may include an oxygen-containing gas. For example, the second gas mixture may include O₂，CO，CO₂，NO，NO₂，N₂O or any combination of two or more thereof. Optionally, the second gas mixture may further comprise an inert diluent gas. The dilution gas can include a noble gas, for example, He, Ne, Ar, Kr, Xe, or Rn, or any combination of two or more thereof.

Referring to fig. 14A-14F, a method of irradiating a substrate with a GCIB is provided in accordance with various embodiments. As described above, a GCIB processing system is provided that includes a set of at least two nozzles for forming and emitting gas cluster beams and that loads a substrate to be processed (i.e., a substrate to be irradiated by one or more GCIBs) into the GCIB processing system. At least one region on the substrate is irradiated with a first GCIB formed using at least two nozzle groups and at least one region on the substrate is irradiated with a second GCIB formed using at least two nozzle groups. Also, as described above, the first GCIB and the second GCIB are directed along an ion beam axis that is common to both the first GCIB and the second GCIB. For example, sets of at least two nozzles are arranged in close proximity to each other to ensure that a single ion gas cluster beam coalesces before reaching a single gas separator, or are arranged with intersecting ion gas cluster beam axes.

In one embodiment, as shown in figure 14A, a time series 9100 is provided in which irradiation of at least a portion of the substrate by a first GCIB 9110 and irradiation of at least a portion of the substrate by a second GCIB 9120 is performed. The irradiation occurs at least partially or all at the same time over a period of time. The first GCIB 9110 and the second GCIB 9120 are formed using at least one nozzle of a set of at least two nozzles. For example, a first GCIB 9110 can be formed using a first nozzle of at least two nozzle groups, and a second GCIB 9120 can be formed using a second nozzle of at least two nozzle groups.

In another embodiment, as shown in figure 2, and with reference to figure 14B, a time series 9200 is provided in which the irradiating at least a portion of the substrate with the first GCIB 9210 and the irradiating at least a portion of the substrate with the second GCIB 9220 are performed sequentially. The sequential irradiation of the substrate with the first GCIB 9210 and the second GCIB 9220 may be performed cyclically (as shown) or non-cyclically. The alternation of the first GCIB 9210 and the second GCIB 9220 may be performed for one or more cycles. Sequentially and alternately irradiating the substrate with the first GCIB 9210 can include setting a pulse width 9212 during which the first GCIB 9210 irradiates the substrate and a period (or on/off) period 9214. The substrate with the second GCIB 9220 can include setting a pulse width 9222 during which the second GCIB 9220 illuminates the substrate, and a period (or on/off) 9224. The first GCIB 9210 and the second GCIB 9220 are formed in a set of at least two nozzles using at least one nozzle. For example, a first nozzle of at least two nozzle groups may be used to form the first GCIB 9210, and a second nozzle of at least two nozzle groups may be used to form the second GCIB 9220.

In another embodiment, as shown in figure 2, with reference to figure 14C, a time series 9300 is provided in which the irradiation of at least a portion of the substrate by the first GCIB 9310 and the irradiation of at least a portion of the substrate by the second GCIB9320 are performed sequentially. The sequential irradiation of the substrate with the first GCIB 9310 and the second GCIB9320 can be alternated periodically (as shown) or non-periodically. The alternation of the first GCIB 9310 and the second GCIB9320 may be performed for one or more cycles. Sequentially and alternately irradiating the substrate with the first GCIB 9310 can include setting a pulse width 9312 and a period (or on/off) period 9314 during which the first GCIB 9310 irradiates the substrate. The substrate with the second GCIB9320 can include setting a pulse width 9322 and the second GCIB9320, the pulse width 9322 being such that the second GCIB9320 illuminates the substrate during periods (or on/off) 9324. 9320) The insertion between respective substrate irradiations may be performed with one or more time periods (e.g., initial time delay 9330 and final time delay 9340). The first GCIB 9310 and the second GCIB9320 are formed using at least one nozzle of at least two nozzle groups. For example, a first nozzle of at least two nozzle groups may be used to form a first GCIB 9310, and a second nozzle of at least two nozzle groups may be used to form a second GCIB 9320.

In another embodiment, as shown in figure 2, and with reference to figure 14D, a time series 9400 is provided in which irradiation of at least a portion of the substrate by a first GCIB 9410 and irradiation of at least a portion of the substrate by a second GCIB 9420 are performed sequentially. The sequential irradiation of the substrate with the first GCIB 9410 and the second GCIB 9420 may be alternated periodically (as shown) or aperiodically. The alternation of the first GCIB 9410 and the second GCIB 9420 may be performed for one or more cycles. Further, sequential irradiation of the substrates with the first and second GCIBs (9410, 9420) can be performed with one or more intervening periods of time between each substrate irradiation during which at least one nozzle is purged with at least two nozzle groups. First GCIB 9410 and second GCIB 9420 are formed using at least one nozzle in at least two nozzle groups. For example, a first nozzle of at least two nozzle groups may be used to form first GCIB 9410 and a second nozzle of at least two nozzle groups may be used to form second GCIB 9420.

In another embodiment, as shown in FIG. 2, and with reference to FIG. 14E, a time series 9500 is provided in which the irradiation of at least a portion of the substrate by a first GCIB9510 and the irradiation of at least a portion of the substrate by a second GCIB9520 are performed sequentially. The sequential irradiation of the substrate by the first GCIB9510 and the second GCIB9520 can be performed cyclically (as shown) or non-cyclically. The alternation of the first GCIB9510 and the second GCIB9520 may be performed for one or more cycles. Sequentially and alternately irradiating the substrate with the first GCIB9510 can include setting a pulse width 9512 during which the first GCIB9510 irradiates the substrate and a first period (or on/off) 9514. A substrate with a second GCIB9520 can include a set pulse width 9522 during which the second GCIB9520 irradiates the substrate and a period (or on/off) 9524. Further, the sequential illumination of the substrates with the first and second GCIBs (9510, 9520) can be performed over one or more time periods, e.g., an initial time overlap 9530 and a final time overlap 9540, during which the respective substrate illuminations partially overlap. At least one nozzle of at least two nozzle groups is used to form first GCIB9510 and second GCIB 9520. For example, a first GCIB9510 may be formed using a first nozzle of at least two nozzle groups, and a second GCIB9520 may be formed using a second nozzle of at least two nozzle groups.

In another embodiment, as shown in figure 2, referring to figure 14F, a time series 9600 is provided in which at least a portion of the substrate is simultaneously or sequentially irradiated with a first GCIB 9610 while at least a portion of the substrate is sequentially irradiated with a second GCIB9620 and a third GCIB 9630. The sequential irradiation of the substrate with the second GCIB9620 and third GCIB 9630 can be performed cyclically (as shown) or non-cyclically. The alternation of the second GCIB9620 and the third GCIB 9630 may be performed for one or more cycles. A first nozzle of at least two nozzle groups may be used to form the first GCIB 9610 and a second nozzle of at least two nozzle groups may be used to form the second GCIB9620 and the third GCIB 9630. Alternatively, a first nozzle of at least two nozzle groups may be used to form the first GCIB 9610, a second nozzle of at least two nozzle groups may be used to form the second GCIB9620, and a second nozzle may be used to form the third GCIB 9630. A third nozzle of the at least two nozzle groups.

It will be apparent that other embodiments for simultaneous and/or sequential operation of multiple nozzles and gas supply assemblies are possible, including different numbers of nozzles and different numbers of gas supplies, all of which fall within the scope of the present invention. Any one or more of the embodiments described in fig. 1-3. Fig. 14A to 14F may be combined.

Turning now to another method of irradiating a substrate with a GCIB. The method includes a process flow in which a GCIB processing system is provided having a set of at least two nozzles for forming and emitting a cluster beam of an ion gas. The GCIB processing system may include any of the systems described above.

In 1), a substrate to be processed is loaded into the GCIB processing system.

In 2), at least one region on the substrate is first sequentially irradiated with a first GCIB formed using a first nozzle group in the set of at least two nozzles.

In 3), the at least one region on the substrate is sequentially irradiated with a second GCIB, which is a second nozzle formed using a second nozzle group of the at least two nozzle groups different from the first nozzle group.

The first GCIB and the second GCIB may have the same atomic and/or molecular composition. Alternatively, the first GCIB and the second GCIB have different atomic and/or molecular compositions. The first GCIB and the second GCIB comprise one or more elements selected from the group consisting of: h, B, C, Si, Ge, N, P, As, O, S, F, Cl, Br, He, Ne, Ar, r or Xe.

One or more gas supply parameters selected from the group consisting of stagnation pressure and stagnation temperature may be the same for the first and second GCIBs. Alternatively, one or more gas supply parameters selected from stagnation pressure and stagnation temperature may be different for the first and second GCIBs. Additionally, one or more process parameters selected from the group consisting of beam energy, beam energy distribution, beam focus, and beam dose may be the same for the first GCIB and the second GCIB. Alternatively, one or more process parameters selected from the group consisting of beam energy, beam energy distribution, beam focus and beam dose are different for the first GCIB and the second GCIB.

Irradiating at least one region on the substrate with the first GCIB performs one or more processes on the substrate selected from the group consisting of doping, growth, deposition, etching, smoothing, amorphizing, or modifying of a layer thereon. And, irradiating the at least one region on the substrate with the second GCIB performs one or more processes selected from the substrate consisting of doping, growth, deposition, etching, smoothing, amorphizing or modifying of a layer thereon on the substrate.

In one example, the substrate can be irradiated with a first GCIB to amorphize a surface layer of the substrate. Thereafter, the substrate may be irradiated with a second GCIB to dope or implant a material into the amorphized surface layer. In another example, the substrate can be irradiated with the first GCIB to grow or deposit a layer of material on the substrate. Thereafter, the substrate may be irradiated with a second GCIB to smooth or modify the surface of the deposited material layer.

In another example, the substrate can be irradiated with the first GCIB to dope a surface layer on the substrate. Thereafter, the substrate may be irradiated with a second GCIB to smooth or modify the surface of the layer of doped material.

In another example, the substrate can be irradiated with a first GCIB to deposit a layer of material on the substrate. Thereafter, the substrate may be irradiated with a second GCIB to grow a second material layer in the deposited material layer.

In another example, the substrate can be irradiated with the first GCIB to modify a material layer on the substrate by introducing or removing the first material. Thereafter, the substrate may be irradiated with a second GCIB to further modify the layer of modifying material on the substrate by introducing or removing a second material.

In yet another example, the substrate can be irradiated with the first GCIB to clean or etch a surface layer on the substrate. Thereafter, the substrate may be irradiated with a second GCIB to grow or deposit a material layer on the cleaned or etched surface layer.

Reference throughout this specification to "one embodiment" or "an embodiment" means that a particular feature, structure, material, or characteristic described in connection with the embodiment is included in at least one embodiment of the invention, but does not denote that they are present in every embodiment.

Various operations have been described as multiple discrete operations in turn, in a manner that is most helpful in understanding the present invention. However, the order of description should not be construed as to imply that these operations are necessarily order dependent. In particular, these operations need not be performed in the order of presentation. The operations described may be performed in a different order than the described embodiments. In additional embodiments, various additional operations may be performed and/or described.

One skilled in the relevant art will appreciate that many modifications and variations are possible in light of the above teaching. Those skilled in the art will recognize various equivalent combinations and substitutions for various components illustrated in the figures. It is therefore intended that the scope of the invention be limited not by this detailed description, but rather by the claims appended hereto.

Claims (10)

1. A multi-nozzle gas cluster ion beam processing system and method of operation, wherein, the method of irradiating a substrate with a Gas Cluster Ion Beam (GCIB), is based on a GCIB processing system comprising a set of at least two nozzles for forming and emitting gas cluster beams; loading a substrate to be processed into a GCIB processing system;

irradiating at least one region on the substrate with a first GCIB formed by at least two nozzle groups; irradiating at least one region on the substrate with a second GCIB formed by at least first and second two nozzle groups, wherein the first GCIB and the second GCIB are directed along an ion beam axis common to the first GCIB and the second GCIB;

wherein the GCIB processing system further comprises a gas separator, and at least one gas supply in communication with a first nozzle group and with a second nozzle group different from the first nozzle, the first and second nozzle groups comprising at least one nozzle, and wherein each nozzle of the at least two nozzle groups is configured to form and emit a gas cluster beam, and the two nozzles of the at least one nozzle group are arranged in close proximity to each other and are capable of at least partially focusing each gas beam of the ion gas cluster beams emitted from the at least two nozzle groups into the gas separator along an ion beam axis;

the at least one gas supply comprises: a first gas supply in communication with the first nozzle group; the second gas supply source is communicated with the second nozzle group; the first GCIB irradiating at least one region on the substrate comprises: flowing a first gas mixture from at least one gas supply through at least a first nozzle group to form a first ion gas cluster beam, directing the first ion gas cluster beam through a gas separator along a beam axis, then ionizing the first ion gas cluster beam to form a first GCIB, and accelerating the first GCIB toward a substrate; the second GCIB illuminating at least one region on the substrate, comprising: flowing a second gas mixture from at least one gas supply through at least a second nozzle group to form a second ion gas cluster beam, directing the second ion gas cluster beam through the gas separator along the ion beam axis, and then ionizing the second ion gas cluster beam to form a second GCIB and accelerating the second GCIB toward the substrate.

2. The method of claim 1, wherein the first GCIB and the second GCIB have the same atomic and/or molecular composition; or the first GCIB and the second GCIB have different atomic and/or molecular compositions.

3. The method of claim 1, wherein the first GCIB and the second GCIB comprise one or more elements selected from the group consisting of H, B, C, Si, Ge, N, P, As, O, S, F, C1, Br, He, Ne, Ar, Kr, or Xe.

4. The method of claim 1, wherein one or more gas supply parameters selected from stagnation pressure and stagnation temperature are the same or different for the first GCIB and the second GCIB.

5. The method of claim 1, wherein one or more process parameters selected from beam energy, beam energy distribution, beam focus, and beam dose are the same or different for the first GCIB and the second GCIB.

6. The method of claim 1, wherein irradiating a layer on top of at least one region on said substrate with said first GCIB performs one or more processes selected from the group of doping, growing, depositing, etching, smoothing, amorphizing or modifying on said substrate; and irradiating at least one region on the substrate with the second GCIB to perform one or more processes selected from the group of doping, growing, depositing, etching, smoothing, amorphizing or modifying the substrate one layer above it;

while at least a portion of the substrate is irradiated with a first GCIB and at least a portion of the substrate is irradiated with a second GCIB.

7. The method of claim 6, wherein sequentially performing comprises a partial overlap between irradiating at least a portion of the substrate with the first GCIB and irradiating at least a portion of the substrate with the second GCIB; the sequential second illumination partially overlaps the sequential first illumination.

8. The method of claim 1, further comprising: at least a portion of the substrate is irradiated with a first GCIB and at least a portion of the substrate is irradiated with a second GCIB alternately and sequentially.

9. The method of claim 1, wherein the GCIB processing system further comprises a gas separator and at least one gas supply in fluid communication with a first nozzle group and with a second nozzle group different from the first nozzle group, the first and second nozzle groups each comprising at least one nozzle of at least two nozzle groups, and wherein each nozzle of at least two nozzle groups is configured to form and emit an ion gas cluster beam having an ion gas cluster beam axis, the at least two nozzles grouped at an angle such that each ion gas cluster beam axis converges toward a single intersection point and one or more ion gas cluster beams are directed into the gas separator along the beam axis.

10. A method of irradiating a substrate with a Gas Cluster Ion Beam (GCIB), comprising: providing a GCIB processing system having at least two nozzles for forming and emitting gas cluster beams; loading a substrate to be processed into the GCIB processing system; sequentially, first, at least one region on the substrate is irradiated with a first GCIB formed by a first nozzle group of the at least two nozzle groups; then, in turn, irradiating at least one region on the substrate with a second GCIB formed on the substrate; or a second nozzle group of the at least two nozzle groups is different from the first nozzle group.

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