JP3790809B2 - Method and apparatus for producing thin film by Raman shift pulse laser deposition - Google Patents

Description

[0001]
BACKGROUND OF THE INVENTION
The present invention relates to a method and apparatus for producing a high-quality crystal thin film and laminated thin film having a smoothness of nanometer dimension by suppressing generation of surface particles by Raman shift pulse laser deposition, and more particularly, a semiconductor. Thin films of various materials such as metal oxides such as dielectrics, superconductors, magnetics, conductors, insulators, metals, and inorganic and organic compounds, for example, epitaxial (single crystal of electronic and magnetic materials) The present invention relates to a method and an apparatus for producing a thin film, a crystalline thin film, an amorphous thin film, a laminated thin film thereof, an artificial lattice, and a thin film for an electronic / magnetic element.
[0002]
[Prior art]
As methods for forming thin films of various materials, there are a pulse laser deposition method, a sputtering method, a heating deposition method using a K cell or an electron beam, a plasma CVD method, and the like. Among them, the pulse laser deposition method is applicable to both inorganic and organic materials, can be formed even under oxygen pressure, and can easily control the composition ratio of constituent elements in the film. Have.
Therefore, the pulse laser deposition method is used to fabricate elements such as metal oxides and compounds such as copper oxide-based high-temperature superconductors and manganese-based giant magnetoresistive materials with complex elemental composition ratios. It is suitable as a film forming method.
However, the laser vapor deposition method has a drawback that surface particles are easily generated, and this is the biggest problem to be solved.
[0003]
In order to develop next-generation electronic and magnetic thin film devices such as superconductor three-terminal devices, Josephson coupling devices, giant magnetoresistive magnetic heads and tunnel transistors, nanometer-scale smoothness and thickness It is necessary to achieve the production of high-quality crystalline thin films and the lamination of thin films. However, since none of the conventional methods has produced such a high-quality crystalline thin film and laminated thin film due to precipitation of surface particles, none of the conventional methods has been used in industry.
[0004]
In the pulsed laser deposition method, it is expected that a better quality film can be produced as the laser light with a shorter wavelength is used. Is mainly used and studied, but it has not yet completely suppressed surface particles. The solid-state laser such as Nd: YAG can change the wavelength by using a fundamental wave (1064 nm), a second harmonic (532 nm), a third harmonic (355 nm), a fourth harmonic (266 nm) and a harmonic generation crystal. it can. When up to the third harmonic of the prior art was used, a high quality crystal thin film was not produced because of many surface particles.
[0005]
[Problems to be solved by the invention]
Under such circumstances, the present inventors conducted research on the preparation of a Ba ₂ Cu ₃ O _y (YBCO) high-temperature superconductor thin film by a laser vapor deposition method using Nd: YAG fourth harmonics. Succeeded in significantly suppressing particle formation. This is because the laser light is changed from the third to the fourth harmonic to the short wavelength light, and the YAG solid laser has a narrower pulse width (1/3 to 1/5) than the excimer gas laser. The present inventors have succeeded in reducing the number of surface particles, and from this fact, the inventors have recognized that the generation of surface particles can be further reduced if the wavelength is further reduced.
[0006]
For the development of electronic and magnetic elements, it is possible to produce high-quality crystalline thin films and laminated thin films with smoothness of nanometer dimensions by suppressing the generation of surface particles. Is required.
Further, in order to evaporate an inorganic material by the pulse laser method to form a thin film, output energy of several tens mJ / pulse and continuous and stable oscillation of the pulse laser beam are required. However, since there is no light source having a wavelength shorter than the oscillation frequency of 193 nm of the ArF excimer laser, high output and stable oscillation, a pulse laser light source in the vacuum ultraviolet region having sufficient output and stability and a laser using the same It is necessary to develop a method and apparatus for producing thin films and laminated thin films by vapor deposition.
[0007]
The present invention has been made to solve the above-described problems. The Raman effect is used to shorten the wavelength of laser light, and the Raman energy has sufficient output energy and stability including vacuum ultraviolet rays for vapor deposition. An object of the present invention is to provide a method for producing a high-quality crystal thin film and a laminated thin film in which a shifted pulsed laser beam is generated and generation of surface particles by pulse laser deposition using the pulsed laser beam is suppressed, and an apparatus capable of embodying the method. To do.
In addition, the present invention provides a method and apparatus for producing a thin film by Raman shift pulse laser deposition that suppresses the generation of surface particles and makes it possible to produce a high-quality crystalline thin film and a laminated thin film having nanometer-dimensional smoothness. For the purpose.
[0008]
[Means for Solving the Problems]
In order to solve the above problems, the present invention irradiates a substance having a high reference molecular frequency with an ultraviolet pulse laser beam to shorten the wavelength of the laser beam, and includes a vacuum ultraviolet ray and sufficient output energy and stability for vapor deposition. This is a method for producing a thin film of a material on a substrate by generating a Raman-shifted pulsed laser beam having a temperature and evaporating a target material by pulsed laser deposition including the Raman-shifted vacuum ultraviolet light.
The present invention also includes the following steps:
(1) A gas having a high reference molecular frequency ν _f , such as hydrogen or deuterium molecules, is preliminarily set to a predetermined pressure of several to several tens of atmospheres in a high-pressure gas sealing tube having optical windows that can transmit light at both ends. The ultraviolet pulse laser beam having the frequency ν ₀ is condensed into the sealed gas using a lens or the like from one window and irradiated to ν ₀ ± n ν _f (where n is an integer). The first step of efficiently generating Raman-shifted light including vacuum ultraviolet rays toward the other window,
(2) A substrate holder with a heater capable of setting a substrate such as an inorganic single crystal substrate or a glass substrate and controlling its temperature, and a target holder capable of setting a target of an inorganic or organic material to be used to produce a thin film. A target is set in advance in a vacuum chamber that can be evacuated to low pressure or vacuum, and the pulsed target material is pulsed by condensing and irradiating the Raman-shifted pulsed laser beam or light splitting it onto the target using a lens. A second step of automatically decomposing and evaporating and colliding with the substrate,
Is performed for a predetermined number of pulses to produce a crystalline or amorphous thin film of the substance.
[0009]
In the present invention, a plurality of targets are set in advance in a vacuum chamber having a target holder capable of setting a plurality of targets and a substrate holder.
The process of performing the first process and the second process for the predetermined number of pulses is sequentially performed for each target, and a thin film (laminated thin film) is formed by sequentially laminating thin films of these substances on the substrate. It is a method to do.
[0010]
The present invention is an apparatus for producing the thin film,
A Raman shift laser light generating means capable of generating a Raman shift pulsed laser light containing vacuum ultraviolet light having a shorter wavelength by enclosing the high pressure gas and irradiating the pulsed laser light;
A Raman shift light condensing variable irradiation means for irradiating the target with a Raman shift laser light or a light splitting it with a lens or the like that can transmit vacuum ultraviolet rays while changing the degree of condensing, and a substrate are set at a high temperature. Vapor deposition means using a vacuum chamber comprising a substrate holder with a heater capable of temperature control and a target uniform evaporation mechanism such as a target rotation mechanism for uniformly evaporating the target, and a target holder; It is an apparatus which has.
[0011]
Furthermore, the present invention is an apparatus for producing the laminated thin film,
Means for generating the Raman shift pulse laser beam;
Condensation variable irradiation means of Raman shift pulse laser light,
The substrate holder and the target uniform evaporation mechanism, and a target position moving mechanism capable of setting a plurality of targets of various substances and materials and sequentially moving each target to a laser beam focusing position. Vapor deposition means using a vacuum chamber;
It is an apparatus which has.
[0012]
DETAILED DESCRIPTION OF THE INVENTION
Next, the present invention will be described in more detail.
As described above, the present invention irradiates a substance having a high reference molecular frequency with ultraviolet pulse laser light to shorten the wavelength of the laser light, and includes output energy and stability sufficient for vapor deposition including vacuum ultraviolet light. It is characterized in that a pulsed laser beam having a Raman shift is generated and a target material is evaporated by pulsed laser deposition including the Raman shifted vacuum ultraviolet ray to produce a thin film of the material on the substrate.
The Raman effect is defined as ν ₀ + n ν _f (where n is an integer) when a substance having a reference molecular frequency of ν _f is irradiated with light such as high-power pulsed laser light having a ν ₀ frequency. ) Light (anti-Stokes line) and light having a frequency of ν ₀ −n ν _f (Stokes line) are generated.
In order to efficiently generate short-wavelength pulsed vacuum ultraviolet light, use high-frequency ultraviolet pulsed laser light as high frequency as possible, such as the fourth harmonic of an Nd: YAG laser or ArF excimer gas laser as incident light. As a material for Raman shift, it is necessary to use a molecular gas such as hydrogen or deuterium having a point-symmetric molecular structure, which is a necessary condition for the Raman effect, and having a reference frequency as high as possible. In the present invention, the incident light includes the fourth harmonic of an Nd: YAG laser, the third and fourth harmonics of a Ti: sapphire laser, and an ArF excimer gas laser, and hydrogen, deuterium as Raman shift substances. , Methane, deuterated methane, ethane, deuterated ethane and the like are preferably used, but are not limited thereto.
[0013]
The film formation by the pulsed laser deposition method by Raman shift does not depend on the material of the thin film to be produced and the type of substance, but in explaining the present invention, by pulsed laser deposition including the Raman shifted vacuum ultraviolet ray, The fact that the present inventors have learned during the study of the production of a thin film of YBCO superconductor and LaPbMnO-based magnetic material, and a laminated thin film of YBCO and CeO ₂ (cerium oxide), and the method of the present invention, An example of demonstrating that it is possible to produce a crystalline thin film and a laminated thin film with higher quality than the conventional method will be described in detail below.
[0014]
In order to increase the efficiency of conversion to vacuum ultraviolet rays and produce a high-quality crystal thin film, it is necessary to set an optimum gas pressure such as hydrogen gas in the high-pressure gas sealing tube within a range of about 4 to 20 atm. When a crystal thin film is produced by laser vapor deposition using the fourth harmonic of a conventional YAG laser, a laser energy of about 25-40 mJ / pulse is required. On the other hand, in the case of film formation by the pulse laser vapor deposition method using the Raman shift, there is energy loss due to light absorption and scattering by the gas in the sealed tube and absorption by the lens, so that the incident light enters the high pressure gas sealed tube. The 4th harmonic used for this required about twice as much energy as 50-70 mJ / pulse. Therefore, the incident laser needs to be high output and variable, and in order to increase the conversion efficiency into vacuum ultraviolet rays, it needs a variable light collection function for condensing and irradiating the gas sealed tube. .
[0015]
During film formation, irradiation of pulsed laser light breaks the chemical bonds of the target material and momentarily generates constituent elements such as atoms, ions, and various clusters, resulting in a plasma state called an ablation plume (evaporation flame). A flame is generated that strikes the substrate and forms a thin film. In this evaporation flame, particles collide with oxygen and an oxidation reaction takes place. The quality and electromagnetic characteristics of the thin film greatly depend on the energy and degree of oxidation of the particles in the evaporation flame at the time of film formation, and thus the shape, size, and color of the evaporation flame. In addition, in the Raman shift pulse laser deposition method, light of various wavelengths is mixed, and all of these lights have different focal lengths. Therefore, the lens mainly focuses on which wavelength of light, and to what extent the light is on the target. The evaporative flame changes greatly depending on whether the target is decomposed or evaporated by focusing and irradiating. For this purpose, it is necessary to change the position of the lens under a vacuum or the like using a lens that transmits even short-wavelength vacuum ultraviolet rays to make the light condensing variable. Also, for example, in order to produce a crystal laminated thin film of a plurality of materials such as YBCO and CeO ₂ , both targets are placed in a vacuum chamber from the beginning, and vapor deposition is performed by changing the targets sequentially without breaking the vacuum. There is a need.
[0016]
Based on these facts, the Raman shift pulse laser deposition method needs to construct as many production means and optimize the conditions as the incidental to the Raman effect as compared with the conventional method. In other words, it has been demonstrated that it is possible to produce thin films and laminated thin films with reduced surface particles with good reproducibility by means of the Raman shift pulse laser deposition, which can be a technology that can be used in industry. It became.
[0017]
【Example】
Next, an embodiment of a thin film and multilayer thin film manufacturing method and a thin film and multilayer thin film manufacturing apparatus according to the present invention will be described with reference to the accompanying drawings. However, the present invention is not limited to the examples.
[0018]
FIG. 1 is a schematic view showing an example of the configuration of a thin film and laminated thin film manufacturing apparatus 1 that embodies the thin film and laminated thin film manufacturing method according to the present invention. In the embodiment, the thin film and laminated thin film manufacturing apparatus 1 includes a short wavelength ultraviolet pulse laser generator 2,
A high-pressure gas sealing tube 3 capable of sealing a gas such as hydrogen at a high pressure and generating vacuum ultraviolet rays by a Raman shift effect;
A condensing variable lens 4 for condensing and irradiating the light from the ultraviolet pulse laser generator 2 in the high-pressure gas sealing tube 3 and a pulse laser beam including vacuum ultraviolet rays generated by the Raman effect are changed in position. Then, a variable-condensing irradiation means 5 for irradiating the target in the vacuum chamber while changing the degree of condensing, and a substrate holder 6 with a heater capable of setting the substrate such as a crystal or a glass substrate and controlling the temperature of the substrate to a high temperature. And a target holder 7 on which a target can be set, and a vacuum chamber 9 that can be evacuated to a low pressure or a vacuum by a vacuum pump 8.
[0019]
Since the ultraviolet pulse laser generator 2 needs to have a high output as much as possible and the laser beam oscillates stably, the ultraviolet pulse laser beam having a high frequency and a high output, for example, the fourth harmonic of Nd: YAG. A wave pulse laser or an excimer gas laser such as ArF or KrF is used. The high-pressure gas sealing tube 3 preferably has a pressure adjustment function so that the pressure of the sealed gas can be changed from several atmospheres to several tens of atmospheres to optimize the generation efficiency of Raman-shifted vacuum ultraviolet rays and the effect on laser deposition. A hydrogen gas cylinder 3a and a pressure gauge 3b are used. The high-pressure gas sealing tube 3 has an optical window 3c for laser incidence and an optical window for output of Raman shift light. The incident optical window is used to irradiate ultraviolet pulse laser light from the laser generator 2. A fused silica window material that can transmit light is used, and the optical window for output is an optical window made of magnesium fluoride, calcium fluoride, or lithium fluoride so that vacuum ultraviolet rays generated by the Raman effect can be transmitted. Or it can be set as the lens 5a for condensing irradiation also for condensing to a target.
[0020]
Since the substrate holder 6 optimizes the distance between the target and the substrate as one of the conditions when optimizing the film formation conditions, the substrate holder 6 includes a linear introduction mechanism (terminal) 10 for changing the distance. did.
The target holder 7 is not limited to the production of one thin film, but a Raman shift vacuum ultraviolet ray is used so that a plurality of targets (for example, A, B, C3, etc.) can be set and the thin films can be sequentially laminated. A target position moving mechanism 11 by step motor driving or the like for sequentially moving the target to a position where the pulsed laser beam including the laser beam is focused and irradiated, and to prevent the laser beam from being concentrated on one point and causing damage to the target. And a target uniform evaporation mechanism such as a target rotation mechanism 12 driven by a motor. Further, the vacuum pump 8 uses a solenoid valve or the like because it is necessary to optimize the conditions by changing the oxygen pressure while the pressure is low in the case of forming a metal oxide electronic / magnetic material thin film by laser deposition. The pressure control system 8a was provided. The configuration of each mechanism is not limited as long as it has a similar function.
[0021]
Next, the method of the present invention will be specifically described based on an example in which a crystal thin film of YBCO superconductor is produced using the laser vapor deposition thin film production apparatus configured as described above.
[0022]
1) Method A target formed into a disk shape such as YBCO superconductor is set in the target holder 7 in the vacuum chamber 9. The target is rotated by the target rotation mechanism 12 for preventing the laser beam from being concentrated on one point and causing damage to the target. The cleaned SrTiO ₃ (STO) single crystal substrate is set on a substrate holder 6 with a heater, and the vacuum chamber is once evacuated to a high vacuum. After cleaning the substrate surface by raising the substrate temperature to a predetermined temperature (about 650-800 ° C.), a small amount of ultra-high purity oxygen is introduced into the vacuum chamber, and the pressure control system 8a connected to the vacuum pump 8 is adjusted. Then, a predetermined oxygen pressure (about 0.1-1.0 Torr) is set. Hydrogen is introduced into the high-pressure gas sealing tube 3 for Raman shift to a predetermined pressure (about 4-20 atm).
[0023]
After the above operation in advance, the fourth harmonic of the YAG pulse laser is condensed and irradiated into the high-pressure gas sealed tube 3 using the condensing variable lens 4, and the vacuum ultraviolet pulse laser beam is emitted by the Raman effect. generate. The pulsed laser beam containing this vacuum ultraviolet ray is condensed and irradiated onto the target by the condensing variable irradiating means 5, and the target material is pulsed and ablated toward the substrate to produce a YBCO crystal thin film on the substrate. At the time of film formation, in addition to the conditions in the usual laser vapor deposition method, that is, various conditions such as the substrate temperature, oxygen pressure, and laser frequency, conditions associated with the Raman shift laser vapor deposition method, that is, hydrogen gas in the high-pressure gas sealing tube The pressure, the output of the fourth harmonic of the YAG laser, the focusing distance in the high-pressure gas sealed tube, the focusing density of the Raman shift pulsed laser light including vacuum ultraviolet rays on the target were optimized as follows. Substrate temperature: 740 ° C., oxygen pressure: 50 Pa, laser frequency: 1 Hz, hydrogen gas pressure: 5 atm, output of fourth harmonic of YAG laser: 70 mJ / pulse, condensing distance in high-pressure gas sealed tube: 45 cm, Condensation density of the Raman shift pulse laser beam: about ² J / cm ² / pulse.
A crystal thin film of YBCO superconductor was produced by the above process.
[0024]
2) Results a) Characteristics of the crystalline thin film of YBCO superconductor produced by the above-mentioned Raman shift pulse laser deposition method experiment, and b) Characteristics of the thin film produced by the conventional laser deposition method using the fourth harmonic of YAG. Comparison with FIG. 2 is shown in FIG. 2, FIG. 3, FIG. 4 and FIG. FIG. 2 shows the temperature dependence of the electrical resistance. Both thin films have a superconducting transition temperature of about 89 K, which is comparable to each other. However, looking at the electrical resistance in the temperature range above the same transition temperature, the sample produced by the Raman shift pulse laser deposition method of a) shows a value less than one third of the sample of b). It turns out that it is a better quality thin film.
[0025]
As shown in the X-ray diffraction spectrum of the thin film in FIG. 3, both the films prepared by the laser vapor deposition methods a) and b) are both (h00) of the STO crystal used for the substrate; Besides the diffraction line, it consists only of the diffraction spectrum of YBCO superconducting crystal (00l); l = 1-11, but the intensity of the diffraction line is generally stronger in the thin film a). This indicates that although c-axis oriented single crystal thin films are both produced, a) is a better quality crystal film.
[0026]
Further, as shown in the scanning electron microscope (SEM) photographs of the thin film of FIGS. 4 and 5 (the inner scale is the upper figure: 1 μm, the lower figure: 10 μm), the Raman shift pulse laser deposition method of FIG. In the produced film, the number of impurity surface particles is greatly reduced and the size thereof is extremely smaller than that of the thin film produced using the conventional YAG fourth harmonic shown in FIG. From the above, it can be seen that the film produced by the Raman shift pulse laser deposition method of a) is improved in surface quality and the film quality is improved.
[0027]
FIG. 6 is an X-ray diffraction spectrum of a two-layer laminated sample in which YBCO and CeO ₂ are sequentially formed by the Raman shift pulse laser deposition method.
(00) of YBCO superconducting crystal; (h00) of CeO ₂ crystal and (h00) of YBCO superconducting crystal, except for (h00) of STO crystal used for the substrate; h = 1-3; Since it consists of only 2 and 4 diffraction spectra, it shows that a good quality YBCO / CeO ₂ crystal laminated thin film is produced.
[0028]
【The invention's effect】
As described above, the thin film and laminated thin film manufacturing method and apparatus according to the present invention change the generation system of Raman shift pulsed laser light including vacuum ultraviolet rays by the Raman effect and the degree of condensing on the target. The condensing variable irradiation system to irradiate and the vacuum chamber system are organically coupled to suppress the generation of impurity surface particles, which could not be produced by conventional YAG fourth harmonics, etc. This makes it possible to produce a crystalline thin film of a quality material such as YBCO.
[0029]
Moreover, the laser vapor deposition method of the present invention does not depend on the type of thin film material or substance to be produced. In other words, as long as the target can be produced, it does not depend on whether it is an inorganic material or an organic material, and is also based on metal oxides such as semiconductors, dielectrics, superconductors, magnetics, conductors, and insulators, metals and compounds The crystal thin film can be produced for any of the above, and a high-quality multilayer laminated thin film can be produced by changing the target position sequentially.
[Brief description of the drawings]
FIG. 1 is a schematic view of an apparatus 1 for producing a thin film and a laminated thin film by a Raman shift pulse laser deposition method.
FIGS. 2a and 2b show the temperature of electrical resistance of a YBCO superconducting crystal thin film prepared by a Raman shift pulse laser deposition method and a pulse laser deposition method using a fourth harmonic of an Nd: YAG pulse laser, respectively. It is a characteristic curve figure which shows dependence.
FIGS. 3A and 3B are X-ray diffraction spectra of a YBCO superconducting crystal thin film prepared by a Raman shift pulse laser deposition method and a pulse laser deposition method using a fourth harmonic of an Nd: YAG pulse laser, respectively. It is.
FIG. 4 is a scanning electron microscope (SEM) photograph of the surface of a YBCO superconducting crystal thin film prepared by a Raman shift pulse laser deposition method.
FIG. 5 is a scanning electron microscope (SEM) photograph of the surface of a YBCO superconducting crystal thin film produced by a pulse laser deposition method using a fourth harmonic of an Nd: YAG pulse laser.
FIG. 6 is an X-ray diffraction spectrum of a YBCO / CeO ₂ two-layer laminated thin film produced by the Raman shift pulse laser deposition method.
[Explanation of symbols]
DESCRIPTION OF SYMBOLS 1 Thin film and laminated thin film production apparatus 2 Ultraviolet pulse laser generator 3 High pressure gas sealed tube 4 for generating Raman shift pulse laser light 4 Condensation variable lens 5 Condensation variable irradiation means 6 Substrate holder 7 with heater 7 Target holder 8 Vacuum Pump 9 Vacuum chamber 10 Straight line introduction mechanism (terminal)
11 Target position movement mechanism 12 Uniform evaporation mechanism such as target rotation mechanism

Claims (5)

It has a point symmetrical molecular structure, and performs a shorter wavelength of the laser beam is irradiated with pulsed ultraviolet laser light high standards frequencies than deuterated ethane molecular gas which can be used as material for Motsura Manshifuto, A Raman-shifted pulsed laser beam including vacuum ultraviolet rays and sufficient output energy and stability for vapor deposition is generated, and the target material is evaporated by pulsed laser vapor deposition including the Raman-shifted vacuum ultraviolet rays to form the material on the substrate. To produce a thin film. The following steps:
(1) hydrogen with reference molecule vibration frequency [nu _f in the high-pressure gas-filled tube having at both ends an optical window that can transmit light, deuterium, from e Tan, or pre-4 atm deuterated ethane gas 20 A high-pressure gas sealing tube sealed at a predetermined gas pressure up to atmospheric pressure is focused and irradiated with ultraviolet pulse laser light having a frequency ν ₀ from one window into the sealed gas, ν ₀ ± a first step of generating Raman-shifted light having a frequency of n ν _f (where n is an integer) and including vacuum ultraviolet rays toward the other window;
(2) A substrate holder with a heater that can set the substrate and control its temperature, and a target holder that can set a target of inorganic material or organic material (target material) for producing a thin film, and even to low pressure and vacuum A target that has been set in advance in a vacuum chamber that can be evacuated is focused on and irradiated with a Raman-shifted pulsed laser beam or light obtained by splitting it, and the target material is decomposed in a pulsed manner. A second step of evaporating and impinging on the substrate,
A method for producing a thin film by laser vapor deposition, characterized in that a crystalline or amorphous thin film of the material is produced by a predetermined number of pulses until the film thickness to be produced is reached. A plurality of targets are set in advance in a vacuum chamber having a target holder that can set a plurality of targets and a substrate holder.
3. The process of performing the first process and the second process for a predetermined number of pulses is sequentially performed for each target, and thin films of these substances are sequentially stacked on the substrate. A method for producing the thin film described. An apparatus used in the method for producing a thin film according to claim 2, wherein a high-pressure gas-sealed tube for Raman shift capable of generating a Raman-shifted pulsed laser beam including vacuum ultraviolet light by irradiating a pulsed laser beam;
Condensation variable irradiation means for Raman-shifted light that irradiates the target with a Raman-shifted pulsed laser beam or light obtained by splitting it, and a heater that can set the substrate and control its temperature up to a high temperature A vacuum chamber comprising a substrate holder with a target and a target uniform evaporation means by a target rotation mechanism for setting the target and evaporating the target uniformly;
An apparatus for producing a thin film by vapor deposition, comprising: A device used in the method for producing a thin film according to claim 3, wherein a high-pressure gas-sealed tube for Raman shift capable of generating a Raman-shifted pulsed laser beam including short-wavelength vacuum ultraviolet rays by irradiation with a pulsed laser beam;
Condensation variable irradiation means for Raman-shifted pulsed light that irradiates the target with a Raman-shifted pulsed laser beam or light obtained by splitting it with a different degree of condensing, and
Target position movement that can set a substrate holder with heater, target uniform evaporation means by target rotation mechanism to uniformly evaporate the target and multiple targets, and can move each target to the laser beam condensing irradiation position sequentially A vacuum chamber comprising a target holder having a mechanism;
An apparatus for producing a thin film characterized by comprising:

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