KR20110063372A - A method for forming an electrical interconnection in an organic opto-electronic device, a method for producing an organic opto-electronic device, and an organic light emitting device - Google Patents

Abstract

PURPOSE: A method for forming an electrical connection unit in an organic optical-electronic device, method for forming an organic optical-electronic device, and organic optical-electronic device are provided to increase the conversion efficiency of serial resistors on the organic optical-electronic device. CONSTITUTION: An insulating layer is formed on a substrate. An organic semiconductor layer(12) is formed on the insulating layer. A structurized metal layer(13) is formed on the organic semiconductor layer. An upper conductive layer(14) is formed on the structurized metal layer. An electrical connection unit(15) is formed on the upper conductive layer.

Description

A method for forming an electrical interconnect in an organic opto-electronic device, a method for forming an organic optoelectronic device, and an organic light emitting device, and a method for forming an organic optoelectronic device. AN ORGANIC OPTO-ELECTRONIC DEVICE, AND AN ORGANIC LIGHT EMITTING DEVICE}

FIELD OF THE INVENTION The present invention relates to new technologies in the field of organic opto-electronic devices, and more particularly to organic light emitting diodes (OLEDs) and organic solar cells.

The field of organic electronic devices has received considerable attention over the past few years mainly due to the rapid development of energy efficiencies in organic photo-electronic devices (OOEDs) and organic photovoltaic devices such as organic light emitting devices.

Organic light emitting diodes have been developed very rapidly in recent years. In particular, efficiencies greater than 100 lumens / W have been successfully achieved for white light emitting diodes. The lifetimes of these systems also increased very quickly, meanwhile, the value of 10,000 hours was significantly exceeded for some material systems. Therefore, organic light emitting diodes are also of interest for applications in lighting systems. The intrinsic advantages of organic light emitting diodes are the high power efficiency and the possibility to implement very thin, large area surface light emitting units.

Conventional structural arrangements of organic light emitting diodes include a transmissive substrate, in most cases glass, which is coated with a transmissive anode often formed of indium tin oxide (ITO). Active organic layers are deposited on the substrate, followed by deposition of a metal cathode for electrical contact. If any bolt is applied between the metal cathode and the transparent anode, the light emitting diode emits light through the substrate (bottom emission). Another variant is the top emitting OLED, in which the top electrode (anode or cathode) is transmissive. The top emitting OLEDs can be constructed under various substrates, for example metal substrates, Si-wafers, display backplanes, printed circuit boards (PCBs), or even transmissive substrates coated with reflective layers, The reflective layer can be the bottom electrode itself. Exemplary documents relating to OLEDs are US 4,539,507, WO 90/13148, US 2004 / 0,062,949, US 2004 / 0,251,816 and US 2007 / 0,051,946.

Large area organic light emitting devices have two problems, uniformity and current distribution, due to the fact that very power efficient organic light emitting devices built on large areas require large current supply. Large area organic light emitting devices require large current handling and distribution. Due to the limited conductivity of the translucent electrode (typically ITO anode), large and position dependent voltage drops occur, which causes non-uniformity of brightness across the organic light emitting device area. These nonuniformities are greater when low voltages (steep IV-curves) are used.

Another large area organic opto-electronic device is an organic photovoltaic (OPV) device. OPV provides great expectations for efficient and large scale conversion of light into electricity. Formation of organic photovoltaic devices requires less material than formation of inorganic crystal photovoltaic devices. The production also consumes significantly less energy than the formation of any other inorganic photovoltaic device.

The efficiency of organic photovoltaic devices has steadily increased. In 2008, a proven power conversion efficiency of 5% was reached, and in 2010, a psychological barrier of 8% was broken, tailoring the efficiency of organic photovoltaic devices to the typical values of amorphous Si devices.

OPV devices have the most different device architectures. Typically, OPV devices include at least one organic semiconductor layer between two electrodes. The organic layer may be a mixture of donors and acceptors such as poly3-hexyl-tiophene (P3HT) and phenyl C61 Butyric Acid Methyl Ester (PCBM). These simple device structures only properly achieve efficiencies when interfacial injection layers are used to aid in charge carrier injection / extraction (Liao et al., Appl. Phys. Lett., 2008. 92: p. 173303). Other organic solar cells have multi-layered structures, sometimes even hybrid polymers and small molecule structures. Serial or multi-unit stacks are also known (Ameri et al., Energy & Env. Science, 2009, 2: P.347). Multi-layer devices can be more easily optimized because different layers can include different materials suitable for different functions. Typical functional layers are transmissive layers, optically active layers, injection layers and the like.

Optically active materials are materials that have a high absorption coefficient at least for a particular wavelength range of the solar spectrum, which convert absorbed photons into excitons, which then contribute to the photocurrent. The optically active materials are typically used in donor-acceptor heterojunctions, where at least one of the donor or acceptor is a light absorbing material. The interface of the donor-acceptor heterojunction serves to separate the generated excitons into charge carriers. Heterojunctions may be bulk-heterojunctions (mixing), or planar (also referred to as faces) heterojunctions, and additional layers may also be provided (Hong et al, J. Appl. Phys., 2009. 106: p. 064511).

Loss of recombination should be minimized for high efficiency OPV devices. Thus, the materials in the heterojunction should have high charge carrier mobilities and high exciton diffusion lengths. The excitons must be separated at the heterointerface, and the charge carriers must leave the optically active region before any recombination occurs. For this reason, only a few organic materials are suitable for use in heterojunctions. For example, at present, fullerene (C60, C70, PCBM, etc.) is preferably selected as an acceptor in OPV devices.

Transmission materials for opto-electronic devices are required to transmit at least at the wavelengths at which the device is active and have good semiconductor properties. These semiconductor properties may be intrinsic, for example, energy levels or mobility, or extrinsic, such as charge carrier density. Charge carrier mobility can also be affected externally, for example by doping the material with an electrical dopant.

The formation of OOED requires patterning very often in series, in parallel, or even in mixed connections, to connect organic light emitting diodes or organic solar cells, or for circuits using transistors. Several techniques are known for forming OOEDs. These methods use patterning such as photolithography, shadow masks for vapor deposition more powerfully. Known methods used for opto-electronic organic devices are complex processes, the patterning of several layers of the opto-electronic organic device requires several steps that increase complexity and reduce quality yield and formation throughput. .

It is known that in these devices a laser can be used to remove layers to separate shorted areas or create patterns. In all cases, the laser is used to remove at least one conductive electrode to break the electrical connection.

Several different approaches have been formulated to produce large areas of homogeneous opto-electronic organic devices. The main problem is current distribution across the surface. In general, the electrodes of the device are also current distribution layers (electrical buses), or an extra conductive layer is deposited on the electrode, which should be thin when permeability is required. For large areas, the resistance of these thin conductive layers is very high because the current required for a large area device is very high. For OLEDs, these resistances cause strong heterogeneity in light emission and device degration. In the case of organic solar cells, the resistance causes loss in power conversion due to the reduced fill factor.

One approach for modifying uniformity in opto-electronic organic devices is the use of additional current supply lines, for example a metal grid deposited in connection with an electrode. The grid lowers the resistance but also slightly reduces the active area since it is not permeable. The metal grid also has a limited thickness, again limiting the maximum current that can be supplied to or provided by the device. For higher currents, a denser grid is needed, which reduces the efficiency of the overall device. Sometimes the grid is undesirable, for example in OLEDs, because it again degrades uniformity.

The electrical interconnects (electric buses) of the electrodes, in particular the conductive layers forming the top electrode and their respective current supply layers, are typically made by patterning an organic semiconductor layer (OSL). The OSL is patterned in this manner so that some areas of the bottom conductive layer are not covered with OSL, and the deposition of the top conductive layer forms an electrical contact to the bottom conductive layer due to the direct contact.

In document US 7,049,757 it is disclosed to subdivide a large area of an organic light emitting device into sub-regions (individual OLEDs) and to connect (partially) the sub-regions of N OLEDs in series. The voltage that needs to be applied to these N OLEDs in series is now N times the single OLED voltage, and the current flow through the N OLEDs is only 1 / N of the current flow on this region. However, in order to implement such a serial connection, connection of the cathode of the i-th OLED (i = 1 ... N-1) to the anode of the i + 1-th OLED is required. Generally the anodes are located on the bottom side of the OLED (and therefore directly on the substrate), while the cathodes are located on the top side of the OLED. In order to make this cathode and anode (++ 1) connection, the uniform organic light emitting device (organic layer portion) region must be separated into suitable sub-regions and the uniform top cathode region is appropriate sub-regions. To be separated. Also the layer forming the bottom electrodes must be divided into sub-regions. This is accomplished by patterning the bottom layer (generally ITO) and by using two mask steps during deposition, which in addition requires a sophisticated alignment of the masks to the substrate during the manufacturing process (see FIG. 1). N is the total number of OLEDs in one column (column) of OLEDs electrically connected in series. Because of the practical limitation of the voltage generally used in facilities, the actual upper limit for N is approximately 300.

Known patterning processes are complex and expensive. The alignment precision of the deposition mask defines the gaps visible between the OLEDs, and non-luminescence. Alternatively, if sophisticated masking is not available, the gap between OLEDs will be very large (range of 1 mm and greater) and OLED, which is one of the main advantages of OLEDs over other large area lighting technologies. Will destroy their uniform appearance.

Another cause of efficiency loss is the power lost by the electrical supply connections. Thin film electrical supply connections provide an electrical connection outside the region that is formed and encapsulates on the substrate to the electrode itself that is inside the encapsulated region. The distance of this thin film electrical connection is several centimeters, and in the best case several millimeters. The film can be larger, but not much thicker, because thicker layers will not be practical for deposition and can cause problems with encapsulation.

Standard electrical connections used in organic light emitting devices cause their resistance as well as large losses in power transfer and large currents cause significant heating of the substrate, further degrading the useful life of the device. .

Especially for large area opto-electronic organic devices, such as organic light emitting devices for the lighting sectors, it is of greatest concern to simplify the formation of the devices and to avoid patterning steps. One exemplary area of concern is the formation in a roll-to-roll process, where it is necessary to move the mask to the roll, which is very undesirable.

It is an object of the present invention to provide improved techniques for forming electrical connections in organic electrical devices, in particular in organic opto-electronic devices. It is also desirable to form more complex electrical interconnections in organic opto-electronic devices in an easier way.

According to the invention, a method for forming an electrical interconnect in an organic optoelectronic device according to claim 1, a method for forming an organic optoelectronic device according to claim 11 and an organic light emitting according to claim 19 A device is provided. Advantageous embodiments of the invention are disclosed in the dependent claims.

As used herein, an organic opto-electronic device is a device comprising a series or parallel arrangement of at least one device or individual devices, wherein each individual device comprises a transducer between the optical signals and the electrical signals. transductor). Preferred organic opto-electronic devices are organic light emitting devices comprising organic light emitting diodes as individual devices or organic photovoltaic devices comprising organic solar cells as individual devices.

The present invention overcomes the problems of the prior art by providing a method for creating an electrical interconnect through an organic semiconductor layer, in particular through a closed OSL. The organic semiconductor layer can be provided as a single organic layer or a stack of organic sub-layers. Methods for forming such electrical interconnects through organic semiconductor layers can be used in different kinds of organic electrical devices. No complicated mask or photolithographic patterning is required. There is a process simplification, and in the case of a light emitting device, the uniformity of the emitted light is improved. On organic photovoltaic devices, series resistance and overall conversion efficiency are improved. By means of laser light, a kind of via is provided through the organic layer which electrically connects the metallized regions on opposite sides of the organic layer. This arrangement of layers can be provided in organic photovoltaic devices as well as organic light emitting devices.

The electrical interconnects are formed by laser processing, ie, irradiation of light to the connection areas where the interconnects will be formed. The material modification produced by laser processing may be, for example, a fused material, a recoagulant material or others. The interconnect can be recognized by its typical shape, which is formed by the high energy density of the laser.

Forming an interconnect using a laser requires that the laser does not remove the layers; Therefore, it is desirable that the laser power is lower than the power used for removal. The power of the laser is 200mW to 15W, more preferably 200mW to 8W for an infrared laser having a wavelength of 800 to 10 mu m; For lasers with shorter wavelengths in the range from 300 to 800 nm, the power is preferably between 200 mW and 3 W, more preferably between 200 mW and 1 W, even more preferably between 200 and 500 mW.

Laser radiation may range from 300 to 500 nm, in particular from 300 to 450 nm; In this range, the absorption of the metal layer becomes stronger and it becomes easier to promote heating. Any laser can be used and preferred lasers are triple or quadruple Nd lasers, excimer lasers, or semiconductor lasers.

Non-limiting examples of such short wavelength lasers include InGaN blue violet laser, triple Nd: YAG, XeF excimer layer.

Lasers used for electrical interconnects can also have a wavelength of 500-1500 μm. Exemplary lasers are Nd lasers that operate within their dominant wavelength, typically in the range of 1020-1050 nm, but dual frequencies may be used as well as other bands. Examples of such lasers include Nd: YAG at 1064 nm or 532 nm; Nd: YVO 4 at 914, 1064 or 1342 nm; Nd: YLF at 1047 or 1053 nm. Semiconductor or fiber lasers can be used as well as gas and excimer lasers. The laser can also match the absorption of the transparent oxide layer (if it is used as an electrode); It can also match the absorption wavelength of the OSL.

Primarily, pulsed lasers are used to more easily control the laser power per unit shot, the shot forming an electrical interconnect between the top and bottom electrodes.

For diode-pumped Nd: YAG (1064 nm), ns Q-switching lasers, good results are obtained using pulses with energy higher than or equal to 10 μJ. About 1000 shots at 10 μJ lead to good contact.

In a Q-switched laser by ps diode-pumped Nd: YAG (1064 nm), a Pockels cell, the best results were obtained at powers above 300 mW. Repetition rates tested were between 10 kHz and 640 kHz.

Since the number and materials of layers used in the OLED can vary depending on the application, a calibration step of the laser can be provided prior to the use of the laser in production.

In another preferred embodiment, the organic layer is provided as a redox doped layer adjacent to the top-electrode.

The absence of inorganic tunneling layer (s) in the layer (s) between the top and bottom electrodes is further desirable. In exceptional cases where such tunneling layers can be provided if these tunneling layers are non-closed layers, these non-closed layers have a typical thickness of less than 5 nm, but the non-closed layers are completely avoided. It is desirable to be saved. Examples of inorganic tunneling layers are inorganic salt layers such as LiF, NaCs, and other examples include inorganic insulators such as SiO ₂ , silicon nitride, and the like. These layers increase the operating voltage of the devices due to their high resistance. In addition, the process of fabricating these layers imposes excessive energy on the organic layers resulting in degradation of the material. These layers are also unnecessary for electrical interconnections by the laser.

In a preferred embodiment, the layer (s) between the top and bottom electrodes are free of inorganic contact layer (s). Examples of such inorganic contact layers are layers of ITO used as intermediate connectors or intermediate electrodes.

It is more preferred that each monolayer, separate layer, organic layer thicker than 35 nm is made of a material or material composition having a temperature of less than Tg <

The OSL used in all embodiments can be deposited by any known method. Preferably, the OSL is deposited by vacuum thermal vapor deposition (VTE). Another preferred method is OVPD (organic vapor phase deposition). Methods for casting organic semiconductors from solution may also be used. Examples of such methods are drop casting, blade coating, stamp coating, spin coating, slot die coating, and spray coating. Alternatively, non-patterned deposition by inkjet may also be used.

In a preferred embodiment, the substrate is made of a material selected from the group of the following materials: metal, glass and plastic. The method can be applied on OOED fabricated on a metal substrate. For example, OLEDs on metal substrates are top-spinning by definition because the metal substrate is not transmissive. If OOED is fabricated on a metal substrate, an electrically insulating layer (also referred to herein as an insulating layer) is required. The insulating layer is required to support the conductive layer layer without creating a short circuit, while the conductive layer forms a bottom electrode or is connected to the bottom or top electrode. At least one conductive layer; It can also be multiple. If the metal substrate is electrically connected to the OOED, the insulating layer must be patterned. This patterning step can be accomplished by any known method.

According to a further embodiment, manufacturing the conductive structure includes manufacturing a metal layer over the substrate, and manufacturing a patterned insulating layer over the conductive layer.

In a further embodiment, the method further comprises manufacturing a patterned insulating layer over the substrate.

According to a preferred embodiment, manufacturing the patterned insulating layer includes manufacturing an insulating layer over the substrate, and patterning the insulating layer.

In another preferred embodiment, patterning the insulating layer comprises patterning the insulating layer by laser ablation.

In a preferred embodiment, manufacturing the conductive structure includes depositing a conductive layer over the substrate, and patterning the conductive layer.

According to a further embodiment, patterning the conductive layer includes patterning the conductive layer by laser ablation.

In a further embodiment, manufacturing the conductive structure comprises depositing a layer of photoresist material over the substrate, depositing a conductive layer over the photoresist layer, and patterning the conductive layer by partially removing the photoresist material. It includes.

According to a preferred embodiment, manufacturing the conductive structure includes providing region B by the metal substrate.

In a further preferred embodiment, the method comprises encapsulating the organic light emitting diode and forming an electrical short between the top electrode and the feed contact by irradiation of laser light before or after the encapsulating organic light emitting diode. It further includes. When forming the electrical short, the laser light is irradiated through the previously manufactured encapsulation. In an alternative procedure, laser light is irradiated before depositing the encapsulation.

The following preferred embodiments are described in further detail.

For metal substrates, preferably, providing the substrate further includes fabricating a patterned insulating layer over the substrate. Alternatively, providing a substrate further includes (i) fabricating an unpatterned insulating layer over the substrate, and (ii) patterning the insulating layer by removing the determined region. Step (ii) here can be made by lifting off the underlying photoresists, for example, or can be removed by laser ablation. In a preferred embodiment, the insulating layer is a photoresist, and step (ii) includes developing the photoresist and removing the determined regions.

Non-limiting examples of metal substrates include stainless steel, austenitic stainless steel, martensitic stainless steel, aluminum alloys, 6063 aluminum alloys, Alanod Ltd. (United Kingdom) Aluminum plate produced by Steel Plates from Arcelor Mittal.

A current supply layer, which may generally be referred to as a feed contact or feed layer, is essentially deposited over the insulating layer to provide electrical connections to the top electrode later. Obviously the number of current supply layers is not limited to one. In addition, additional current supply layer (s) may be deposited over and / or over the insulating layer and / or electrical and mechanical contacts to the metal substrate. These additional current supply layer (s) provide electrical connections to the OSL by forming the bottom electrode. In this embodiment, an additional layer is required to improve the reflectivity of the bottom electrode. This may also have an additional planarization effect, especially if deposited over the insulating layer to avoid shorts caused by the roughness of the substrate.

To simplify manufacturing, the conductive layer forming the bottom electrode and the conductive layer connected to the top electrode are formed in parallel by the same deposition step. Conductive layers connected to the top electrode form feed contacts to the top electrode. The layer is patterned during or after lamination. This patterned layer may be referred to as SML. Non-limiting examples of SMLs are: metal layers such as Cu, Ag or Al.

There are several alternatives for making SMLs. Producing the SML may further include depositing a metal layer on the substrate, and patterning the metal layer to form the SML.

Alternatively, the substrates can be non-metallic and non-conductive substrates. Non-limiting examples of non-metallic substrates are glass and plastic substrates.

If non-metallic substrates are used, a relatively thick conductive layer used as a current distributing layer, which may be referred to as CDL, will preferentially be deposited over the substrate or alternatively over the top electrode. Such CDL has a general thickness in the range from 50 nm to 5 μm, preferably from 150 nm to 500 nm. The CDL is preferably thicker than the top electrode.

The method of making OOED on a non-metallic substrate with a CDL is the same as that used for metal substrates.

For non-limiting substrates, a patterned barrier layer as described above is deposited over the CDL.

Preferably, for non-metallic substrates, providing the substrate further comprises preparing a thick metal layer (TML) over the substrate and manufacturing a patterned insulating layer over the thick metal layer.

It is pointed out that all the necessary patterning of the bottom layer-all layers between the substrate and the OSL (SML, insulating layer)-can be performed prior to the deposition of the OSL.

Technical problems exist in implementing laser interconnect processes in common OOED manufacturing tools. In OOED, most of the layers need to be processed in a highly controlled atmosphere. The addition of an intermediate step using a laser can require complex and expensive modifications to existing tools. In the present invention, it is possible to fabricate an interconnect from an already encapsulated OOED. The encapsulation provides a transparent window. The same window is preferably used for the laser interconnect.

In an advanced mode of the present invention, the interconnecting step is later than the next step of encapsulating the organic light emitting diode. Lasers that perform electrical interconnection are preferably irradiated through the encapsulation.

In some cases, color filters, UV filters, or other layers (films) are made over the encapsulation. Deposition of these layers is preferably performed after electrical interconnection. The encapsulation can be a glass cover or a thin film encapsulation. It is necessary that the encapsulation does not absorb the laser light (absorption <2%). Highly transmissive encapsulation (having more than 98% transmission relative to the wavelength of the laser used) is preferred.

In an advanced mode of the present invention, some electrical interconnects electrically connect the top electrode to a metal substrate (or CDL) to increase homogeneity of large area OLEDs or reduce series resistance of large area solar cells. To be performed. The connections are made in defined regions RB where there is no bottom electrode, so that the layers defining the bottom electrode must be patterned. The connections have a minimum side distance between each other of 5 mm to 100 mm and preferably have a minimum side distance of 10 to 45 mm. Longer distances do not provide the required homogeneity of luminescence. Shorter distances are not due to laser spots with diameters of several micrometers to several hundred micrometers, but are generally required patterning of the bottom electrode, which is much larger than the electrical interconnects (at least three times the diameter of the laser spot) to avoid alignment problems. Will damage the whole area.

A preferred method for creating interconnects on the structured SML is to deposit the unstructured SML and pattern the SML by laser ablation. In addition, the step of making electrical interconnects may include the use of a light alignment method: a low intensity laser (without modifying layers, power <50 mW) prior to using the laser to create an interconnect, the laser It is used for light detection with feedback to a laser scanner to determine and adjust position. In the optical alignment method, the interconnects can be made smaller because the insulating area of the SML can be very small.

It is a particular advantage of the present invention that all patterning is done by laser ablation.

In an alternative embodiment of the invention, a glass substrate is used, and there is no step of depositing an insulating layer on the glass substrate prior to SML. There is also no deposition of CDL. In this mode, the SML is deposited in several regions, where at least two are not electrically shorted to each other. The first region may be used to form the bottom electrode, or additional conductive layers may be deposited by at least partially overlapping the first region to form the bottom electrode. A second region of the SML that is not electrically connected to the first region provides electrical connection to the top electrode through the electrical interconnect.

Preferably, the SML is deposited directly on the glass substrate. Preferably, the SML is deposited as parallel stripes, which do not necessarily have to be rectangular in shape.

Optionally, the stripes that are electrically connected to or form the bottom electrode are electrically connected in parallel. The electrical interconnection of the layer forming the second region of the SML and the top electrode is provided by the laser interconnect method of the present invention.

In another embodiment, the serial connection is made with a laser interconnect. Here, the first region of the SML is connected to or forms a bottom electrode on the first individual device, and additionally the first region is connected to the top electrode of the second individual device via an electrical interconnect. The top electrode must be patterned, for example by laser ablation or shadow mask deposition. Preferentially three or more individual devices (eg organic light emitting diodes or organic solar cells) are electrically connected in series by using this method.

In another advanced embodiment, the method provides an easy path for the fabrication of large area OOEDs electrically connected in series. It has been found that the longer operation of the deposition device using shadow masks needs to be maintained very often, because the shadow mask accumulates very much evaporated material. Therefore, maskless deposition of the top electrode is preferred.

The method comprises depositing a transparent conductive layer (TCL) over an OSL, wherein the deposition is essentially maskless and the following steps (i) are electrically isolated from one another in this manner to form individual devices: Partially removing the metal layers to form regions, preferably stripes, and (ii) making the interconnect by forming a series connection between the individual devices. Steps (i) and (ii) can be done before encapsulation, but preferably after encapsulation.

In another mode of the invention, OSL is deposited over TCL and SML is deposited over OSL. In this embodiment, the substrate is transmissive.

For large area OOED, the area of the device is preferentially larger than about 25 cm 2, preferentially larger than about 100 cm 2. Each individual device is preferentially larger than about 1 cm 2 (OOED includes one or more individual devices). Preferably, the large area organic light emitting device is a non-pixelated device (pixels are pixels).

Next, further aspects of a method for forming an organic opto-electronic device are described.

The electrical interconnection step is always performed after (not during) deposition of the top electrode, organic layer (OSL) and bottom electrode.

In one embodiment, the provided method allows for the deposition of organic layers without using a deposition shadow mask, since they are 'break' (or interrupt) in a non-conductive (insulating) separator. The same can be said for the top electrode. If the top electrode is a cathode, the cathode is also interrupted in the non-conductive separator. Electrical interconnects provide electrical connections between the cathode and the anode of adjacent individual devices of the series connections. The same process and design works naturally similarly if the anode and cathode are exchanged (inverted OLED or inverted solar cell).

The serial connection can be made without using a shadow mask. There is also no need for laser ablation between the deposition steps of the organic layers, top electrode, and optional encapsulation. The bottom electrode and separator can be made, for example, by lithography or other process without requiring a vacuum or inert atmosphere.

In a preferred embodiment, the individual devices are free from any other conductive layer upon direct contact with the bottom conductive layer. However, conductive layers can be provided on the boundaries of the entire device, and the conductive layers provide external electrical connections.

For all arrangements (at least some of the large area devices) in which the individual devices are connected in series, the series electrical interconnect, which may also be referred to as the top-electrode-bottom-electrode connection, is a separate device adjacent to the top electrode of one individual device. An electrical connection provided between the lowermost electrodes of. The electrical interconnects provide electrical series connections. The electrical interconnects are formed by laser processing as described above.

In a preferred embodiment, generating the electrical interconnects in series by laser processing comprises irradiating laser light through the substrate. Additionally or alternatively, laser light can be emitted from the top.

According to another embodiment, the method further comprises providing an encapsulation on the top electrode.

In yet another embodiment, providing a serial connection of the plurality of individual devices is performed after providing an encapsulation. The laser light may be irradiated through the substrate or through the encapsulation. The electrical interconnect is made by laser processing and no vacuum or inert atmosphere is required in the steps of laser processing.

According to a preferred embodiment, a number of individual devices are created on a substrate by a maskless deposition process comprising maskless deposition of materials at least in the active region. However, masking such as simple frames can be used to prevent material deposition outside the active area of the device provided by the outer periphery of the individual device. The connection area may be provided in an area outside the active area.

In another preferred embodiment, the bottom electrode is provided as a transparent bottom electrode. The transmissive electrode is, for example, by thin metal layers (eg, Ag, Au, Al, Cu in the range of 5 to 30 nm), or degenerated inorganic semiconductors, usually IZO (indium-zinc-oxide) Can be realized by oxides such as ITO (indium-tin-oxide). Since ITO or IZO cannot be thermally annealed due to the temperature limitations of the underlying organic layers, the resistance of the ITO or IZO top electrode is generally above 100 ohms / square.

In a preferred embodiment, the top electrode is provided as a transparent top electrode. Again, the transmissive electrode can be formed by thin metal layers (eg, Ag, Au, Al, Cu in the range of 5 to 30 nm) or by ITO (indium zinc oxide) of degenerated inorganic semiconductors, generally IZO (in general). Indium-tin-oxide) type oxides. Since ITO or IZO cannot be thermally annealed due to temperature limitations of the underlying organic layers, the resistance of the ITO or IZO top electrode is generally above 100 ohms / square.

According to a further embodiment, the separator is provided as a tapered separator. In one embodiment, the tapered separator is provided in the form of a mushroom.

In yet a further embodiment, the separator is provided with a plurality of sub-separators, for example double separators which are essentially two parallel separators located in close proximity. Alternatively, the separator can be provided as a single piece separator.

According to a preferred embodiment, the series electrical interconnect is provided adjacent the electrode edge of the bottom electrode, wherein the separator is provided adjacent the series electrical interconnect on the side of the series electrical interconnect facing away from the electrode edge. In a preferred embodiment, the distance between the series electrical interconnects and the electrode edges of the bottom electrode is less than about 1/10 of one lateral dimension of the emitting area, preferably less than about 1 mm, more preferred. Preferably less than about 300 μm.

The separation in the lateral direction rather than in the direction of the serially connected development devices can be performed by a vertical single non-conductive separator approach, for example in the form of a mushroom. In the meantime, serially connected development devices can be electrically connected in parallel to the next series of individual devices connected in series.

Typical sizes of individual devices range from 0.5 cm x 0.5 cm to 3 cm x 3 cm. For example, a large area organic light emitting device of about 10 x 10 cm 2 can be implemented while having an individual device size of 1 cm x 1 cm and N = 10. This means that the length (perpendicular to the connection direction and parallel to the substrate) to the next anode of the cathode connector is about 0.5 to 3 cm in length.

Typical layer thicknesses of the organic layers of the individual devices are about 50 to about 1000 nm, preferably about 100 nm to about 300 nm, and the layer thickness of the ITO bottom electrode is in the range of about 10 to about 500 nm, preferably Is from about 20 nm to about 200 nm. The non-conductive separator height (each thickness) must be greater than the thickness of the layer stack (sum of the thicknesses of all the layers deposited on top of the bottom electrode) and range from about 500 nm to about 5 μm.

The separator has a non-conductive surface topography that provides patterning of layers deposited on top, such as organic and top conductive layers. The separator preferably forms an in-situ shadow mask of square shape, inverted isosceles trapezoid shape, or mushroom shape. It is preferred that the end of the separator away from the substrate is larger than the end closer to the substrate. The separator is preferably formed by positive or negative photoresist or by using two layers of positive / negative photoresist. The separator is preferably made by lithography. Alternative methods for the deposition of the separator may be used, for example screen printing.

The height of the separator (perpendicular to the substrate direction) is greater than the sum of the thickness of the organic layer and the thickness of the top conductive layer, preferably 5 times, more preferably 10 times larger.

Hereinafter, terms used in the specification and / or claims will be described in more detail.

Metal substrate: The metal substrate is preferentially stainless steel or aluminum plate. The metal substrate should have a small roughness, preferably the RMS roughness is less than half the thickness of the insulating layer. It is also desirable for the stainless steel to have at least one surface that is electrically polished.

In the case where OOED is fabricated on a metal substrate, an electrically insulating layer is required. An insulating layer is required to support the conductive layer without creating a short circuit, the conductive layer forming a bottom or top electrode or connected to the bottom or top electrode. There is at least one conductive layer, and a plurality may be sufficient.

Patterned or Structured: It is considered that this layer is patterned or structured when one layer contains functional geometric features much smaller than the smallest substrate lateral dimension. It is also contemplated that this layer is also patterned or structured if one layer comprises several separate regions, a non-limiting example being two parallel stripes formed by the same layer but not in direct contact with each other.

Top electrode: The top electrode is a transparent conductive electrode. The top electrode is an electrode further away from the substrate; It is between the OSL and the encapsulation.

Reflective: The reflectance in the wavelength region corresponding to light emitted by the OSL is greater than 85%, preferably greater than 95%.

Transparent: The transmittance in the wavelength region corresponding to the light emitted by OSL is greater than 70%, preferably greater than 90%.

Maskless (or essentially maskless): In this method the deposition region is defined by a shadow mask that defines only the limiting external borders of the layer, the shadow mask being convex or concave, preferably convex, more It preferably has an opening (through hole) defined by one closed geometry, which may be a rectangular closed cone cross section or another closed curved shape. A non-limiting example is a rectangular frame with one rectangular opening, where one rectangular opening defines the deposition area across the entire substrate except for the boundaries that need to be insulated, and no additional structure exists.

Current distribution layer: This layer provides electrical connection to the top electrode but does not form the electrode itself. The current distributing layer can also be referred to as feed contact.

An individual device refers to a device that is an individual component, such as a single diode, such as an organic light emitting diode (OLED) or a single solar cell, wherein the solar cell is also a diode. In embodiments with a serial connection, the term organic opto-electronic device (OOED) refers to the arrangement of individual devices.

The interconnect or electrical interconnect is used as synonyms. The serial interconnect or serial electrical interconnect is a kind of electrical interconnect.

Insulation layer: The insulation layer is at least one electrical insulation layer. Optionally, one or more insulating layers can be used. Non-limiting examples include polyimide, PVC, polyurethane, PMMA, aluminum oxide. Non-limiting examples of double insulation layers are polyimide / aluminum oxides. The thickness of the insulating layer is typically 200 nm to 100 m, preferably 200 nm to 10 m, and more preferably 500 nm to 7 m. The insulating layer may also be used as a planarization layer for smoothing out the roughness of the metal substrate. In metal substrates, the planarization layer is preferably thicker than 1 μm.

Structured metal layer: this is a layer forming one of the electrodes; It may extend beyond the area of the electrode to provide an area for electrical connection. In metal substrates, the SML is the bottom electrode. In transmissive substrates, the SML can be a top electrode or a bottom electrode.

Organic Semiconductor Layer (OSL): An organic semiconductor layer, or stack of organic semiconductor layers, comprising at least one optically active layer, such as a light emitting layer or an absorbing layer. This is a layer comprising at least one organic semiconductor layer. The OSL of the organic light emitting device includes at least one light emitting layer. Typically OSL is a stack of several organic layers, for example OLED description and paragraphs of EP 1 336 208 B1 ("prinzipielle Aufbau"), [0023] ("Vorteilhafte Ausfuehrung"), and [0037] (" bevorzugtes Ausfuehrungsbeispiel "); See also US 2009 / 0,045,728, in particular paragraphs [0078]-[0085] (“A light emitting device comprises m electroluminescent units”) and examples 1 to 7 thereof. OSL may also be polymeric or hybrid, non-limiting examples are given in US 2005 / 0,110,009 A1, in particular paragraphs [0004-0009] (“organic light-emitting diodes in the form of PLEDs”), and [ 0017-0025 ("pin heterostructure"). Examples of top emitting OLEDs are shown in the preferred embodiment of US 7,274,141, in particular column 4, wherein the blocking layers are optional, the embodiment also having a non-inverted type (more on the substrate than the anode). Near cathode). These cited documents describe a stack of organic layers, which stack can be applied to the electrodes presented herein. The OSL of an organic solar cell is a layer or stack of organic layers that includes at least one material that absorbs light, and the light contributes to the photocurrent. Typically, the OSL of an organic solar cell comprises a donor-acceptor heterojunction. The heterojunction may be a bulk-heterojunction (blend (mix)), or a planar (also referred to as facet) heterojunction, and additional layers may also be provided (Hong et al., J. Appl. Phys. , 2009. 106: p. 064511). Exemplary stacks of organic solar cells are shown in US2007090371A1.

Permeable conductive layer: a layer forming a permeable electrode; It may extend beyond the area of the electrode to provide an area for electrical connection. In metal substrates, the TCL is the top electrode. In transparent substrates, the TCL can be a top electrode or a bottom electrode.

In the following, the invention will be described in further detail by way of example with reference to different embodiments.

1 is a method for providing an interconnect for a device on a metal substrate.
2 illustrates a method of providing an interconnect to a device on a metal substrate or non-conductive substrate / metal layer, wherein the top electrode is electrically connected to the metal layer or metal substrate on the non-conductive substrate via the interconnect. Connected.
3 is a diagram of a method of providing an interconnect to a device on a non-conductive substrate.
4 is a top view of a device in which interconnects are formed in lines and individual devices consist of parallel stripes.
5 is a top view of a possible configuration of an insulating layer and a CDL on a metal substrate.
6 is a top view of a large area high homogeneous discrete device made without a mask or photolithographic pattern, using laser patterning and laser interconnection.
FIG. 7A is a diagram of a bottommost radiation OOED comprising a plurality of serially connected discrete devices in accordance with the prior art. FIG.
7B is the bottommost radiating device.
8 is a view of a top emitting device.
9 is a transmissive device.
10 is a top view of an array of individual devices connected in series in accordance with the present invention.
11 shows an alternative connection pattern for a wide area OOED.
12 is a detailed view of a preferred mode for an isolation separator.
13 is a diagram illustrating an embodiment of an electrical interconnect.

1 illustrates the critical steps of a method for generating an OOED using a laser interconnect. A substrate is provided.

The substrate is coated with an insulating layer in step 1.a. Preferably, the deposition is done by reactive CVD, spin coating, sputtering, VTE (vapor thermal vapor deposition), spraying, ink jet, or blade coating. After this step, the SML is deposited in step (1.b) and the desired structure is obtained by depositing the layer only over the desired areas, or by depositing the layer over the entire area and by subsequent patterning (1.c). Can lose. Non-limiting examples of such methods are shadow mask deposition by VTE, shadow mask deposition by sputtering, deposition using subsequent laser patterning, and deposition using subsequent lift-off of the underlying patterned layer. The pattern of the SML allows at least two electrically separated regions to be formed. In FIG. 1, three regions can be seen from left to right: region A (RA) will partially form the bottom electrode, region B (RB) will form an electrical connection to the top electrode, and further region A will partially form the bottom electrode of the additional OOED.

In step 1.d of FIG. 1, the OSL is deposited by conventional techniques. OSL includes low molecular materials, low molecular layers, polymer layers, or low molecular and polymer layers. TCL is deposited on the OSL, in step 1.e. Deposition of TCL is preferentially performed by VTE or sputtering and is essentially maskless.

At least one electrical interconnect between SML and TCL is formed by a laser in step 1.f electrically interconnecting the top electrode to region RB.

2 shows steps of a method of generating an OOED using laser interconnects. This alternative embodiment takes advantage of the electrically conductive properties of the substrate. Alternatively a metal substrate is provided which can be a non-conductive substrate coated with a metal layer. Examples of metal substrates have been described above. Non-limiting examples of coated non-conductive substrates are glass coated with aluminum, glass coated with copper, polyethylene terephthalate (PET) coated with copper, and polyimide coated with silver.

Step 2.a is deposition of the insulating layer on the substrate. The deposition may be in a patterned manner, optionally, the deposition is not patterned, and the layer is later patterned. Preferred modes are also photoresists and insulating layers that can be patterned by photolithography. Another preferred mode is that the insulating layer is patterned by laser ablation.

The SML is deposited in step 2.b, and furthermore, the SML needs to be defined in regions RA and RB that are electrically separated from each other. The pattern of SML may be defined during deposition or patterned by an additional step (2.c). The functions of the regions RA and RB are the same as described above in FIG. 1.

Alternatively, the insulating layer and the SML are deposited without a pattern, and the two layers are patterned in one step, in which case at least one region RB (intermediate SML region of FIG. 2 (step 2.d)) is also removed. do. A preferred mode for patterning two layers is by lift off when the insulating layer is also photoresist. Another preferred mode is that the two layers are patterned by laser ablation.

Step 2.e corresponds to step 1.d of FIG. Step 2.f corresponds to step 1.e of FIG.

Step 2g is an interconnect step, wherein if an electrical interconnect is made between TCL and (RB) or the region RB is removed, then the interconnect layer of the TCL is provided on a non-conductive substrate. Or made directly on a metal substrate.

3 shows a method of making an OOED on a non-conductive substrate. Non-conductive substrates are provided (eg glass, plastic, etc.). SML is deposited on the non-conductive substrate in step 3.a as described in FIGS. 1 and 2. The patterning step (3.b) can optionally be followed if the SML is not deposited in a structured way.

The SML of FIG. 3 has at least two regions as described in FIG. 1. Step 3.c corresponds to step 1.d of FIG. Step 3.d corresponds to step 1.e of FIG. Step 3.e corresponds to step 1.f of FIG.

The OOED may be a light emitting device powered by a power source that applies a voltage between regions A (RA) and regions B (RB). If OOED is an organic photovoltaic device, the external electrical contacts of the device connect to areas A and B.

4 is a top view of an OOED formed of parallel stripes. FIG. 4 shows a substrate 40 comprising an SML 43 structured in parallel with wider and narrower regions (providing regions A and B, respectively), where the wider regions are formed of an insulating layer ( 41) formed on the top. Unpatterned OSL 42 is deposited over SML 43 and TCL 44 is deposited over OSL 42. Narrower SML regions 43 are regions RB that supply current to TCL 44 via electrical interconnects 45. Regions RB are not necessary if the substrate is a metal substrate or if the substrate is coated with a metal layer, in which case interconnects 45 can be made directly between the TCL 44 and the substrate 40.

An exemplary alternative pattern for insulating layer 51 and SML 52 over substrate 50 is shown in FIG. 5. Here, the substrate 50 is a metal substrate or a substrate coated with a metal layer. SML 52 is provided only over insulating layer 51. OSL and TCL are deposited on top (not shown). In this embodiment, the interconnects of the TCL are made on regions that do not include the insulating layer 51.

6 shows another embodiment in which a substrate 60 is provided, which is a metal substrate or a substrate coated with a metal layer. The substrate 60 is coated with the insulating layer 61; The insulating layer 61 is patterned by forming a matrix of holes defined by the outer circle 64 of points. The SML is not shown to simplify the drawing, but is formed under the OSL 62 and is patterned using holes (also defined by the outer circle 64 of points) at the same location as the insulating layer 62. do. TCL is deposited on the rectangular region defined by the dashed line. The interconnects are made by laser and defined by black (full) circles 64.

In FIG. 6, if OOED is an organic light emitting device, the OLED is connected to a power source or other external circuit in the case of an organic photovoltaic device or to a conductive layer on the substrate if the substrate is non-conductive through the extension of the SML and the electrical connection to the substrate. Can be electrically connected.

In all embodiments, it is desirable that encapsulation takes place before the interconnecting step.

Subsequently, different embodiments are described. Unless otherwise specified, the following deposition techniques are used in the embodiments;

SML is deposited by the VTE using a shadow mask for patterning.

OSL is deposited by the VTE.

TCL is deposited by the VTE, but can also be done by sputtering or other methods.

The interconnecting step of the non-encapsulated devices is done under an inert atmosphere.

Patterned non-conductive layer:

Embodiments often use a patterned non-conductive layer formed as follows: A 2.3 μm thick photodefineable polyimide layer (HD-8820 from HD microsystems) onto the substrate by spin coating at 3500 rpm. Is deposited. The polyimide layer is heated at 120 ° C. for 3 minutes; The pattern is defined by exposure to a light pattern for 50 seconds, developed for 120 seconds and heated at 180 ° C. for 30 minutes.

Example 1) electricity Interconnects  Organic light-emitting device

100 mm × 100 mm glass substrates were provided. A 90 mm x 78 mm metal layer (SML) was deposited on the organic substrate. The metal layer forming parallel stripes is patterned; Wide stripes (RA-area A) have dimensions of 90 mm × 20 mm and narrow stripes (RB-area B) have dimensions of 90 mm × 3 mm; There is always a gap of 1 mm between the stripes. The stripes are formed in the following configuration: (RB)-3 x ((RA)-(RB)) ("-" denotes horizontal layer separation). This configuration is similar to the SML of FIG.

A non-patterned 80 mm × 78 mm OSL comprising the following layers was deposited on the SML as follows; 50 nm thick NPD doped with F4TCNQ; 10 nm thick non-doped NPD layer; A 20 nm blue emitter host layer doped with a fluorescent emitter; 10 nm BPhen; 60 nm BPhen doped with Cs. And 20 nm Ag was deposited as TCL.

The overlap between the OSL, the RA, and the TCL forms a bottom electrode. (RB) is the feed contact to the top electrode.

The electrical interconnection was formed by applying laser pulses to the regions RB; The laser was applied from the top side (in other words, without passing through the substrate). The laser used in this example was a DPSS Nd; YAG laser operating at 1064 nm. The interconnecting points were made over a length of 80 mm of each of the regions RB (length does not overlap with the OSL) at a linear density of 1 point / 250 μm.

Finally, to test the device, the extremities of regions RB (not overlapping with the OSL) were connected to the cathode of the voltage supply, and the ends of the regions RA were the anode of the voltage supply. Connected to This device was formed of three luminous regions connected in parallel, all three regions being operated through the luminous surface with high luminous intensity and high uniform luminous intensity.

Example 2) metal substrate and electricity Interconnects  Luminescence on Pinterest device

A 0.8 mm thick stainless steel sheet with transverse dimensions of 100 mm x 100 mm was provided as a substrate. A 2.3 μm thick polyimide layer (PI2555 from HD Microsystems) was deposited on the metal substrate by spin coating at 3500 rpm and heated to 180 ° C. for 30 minutes. The steps of Example 1) were repeated (except for the first one: to provide a glass substrate). The device worked as expected in Example 1).

Example 3) metal substrate and electricity Interconnects  Luminescence on Pinterest device

A 0.8 mm thick stainless steel sheet with transverse dimensions of 100 mm x 100 mm was provided as a substrate. The patterned non-conductive layer was deposited as described above. As shown in FIG. 4, a 100 nm thick SML layer of Ag was deposited on the polyamide layer RA and on the exposed substrate regions RB. In this case, the feed contact is provided by the substrate itself (regions RB). The steps of depositing OSL and TCL are repeated as in Example 1).

The electrical interconnection was formed by applying laser pulses on regions RB; The laser was applied from the top side (in other words, without passing through the substrate). The laser used in this example was a pulsed Nd: YVO 4 laser operating at 1064 nm. The interconnecting points were made over a length of 80 mm of each of the regions RB (length does not overlap with the OSL) at a linear density of 1 point / 250 μm.

The method leads to the desired effect.

Example 4) metal substrate and electricity Interconnects  Luminescence on Pinterest device

Example 3 was repeated with the following variations. The polyimide layer was patterned as shown in FIG. The SML is not deposited in contact with the metal substrate, but is patterned to deposit only on the polyimide layer as shown in FIG. 5.

Example 5 electricity Interconnects  Having organic light emitting device

A 0.8 mm thick stainless steel sheet with transverse dimensions of 100 mm x 100 mm was provided as a substrate. A patterned non-conductive layer of polyimide was deposited as described above. The polyimide layer is patterned to expose the substrate as a matrix of holes. The spacing between the rows and columns of the matrix is 20 mm, each hole having a diameter of 1 mm. A 100 nm thick SML layer of Ag is deposited on the polyimide layer.

The frequency doubled Nd: YAG laser is used to remove the SML and insulating layer in the holes, exposing the substrate. Alternatively, although increasing complexity, a photosensitive polyimide layer or additional photoresist may be used to pattern the SML.

The steps of depositing OSL and TCL are repeated in Example 1).

An electrical interconnect is formed by applying laser pulses to the center of each hole forming three adjacent interconnects; The laser is applied from the top-side (ie without passing through the substrate). The laser used in this example is a pulsed Nd: YAG laser operating at 1064 nm and having a pulse duration of 8 ps.

This method leads to the device shown in FIG. OLEDs show a high homogeneity of the light emitted through the surface of the device.

Example 6): electrical Interconnects  Eggplants Encapsulated Organic Luminescence device

Although Example 5 is repeated, the device is encapsulated with a glass cover and the steps of forming electrical interconnects are made after encapsulation, and irradiate a laser through the glass cover. The advantage is that the interconnection step can be made in air, while for encapsulated samples that are sensitive to oxygen, moisture and dust, they must be made under inert gas.

Example 7): Electrical through glass Interconnects  Eggplants Encapsulated Organic Luminescence device

Example 6 is repeated, but the following modifications are made: A relatively thick, non-patterned, glass substrate comprising a 500 nm metal layer (TML) was used in place of the metal substrate.

Example 8): Maskless  Organic light emission through deposition device

A 0.8 mm thick stainless steel sheet with lateral ranges of 100 mm x 100 mm is provided as a substrate. A 2.3 μm thick polyimide layer (PI2555 from HD microsystems) is deposited on the metal substrate by spin coating at 3500 rpm and heated at 180 ° C. for 30 minutes. A 100 nm thick SML layer of Ag is deposited on the polyimide layer.

Holes are made in the polyimide layer and the SML is immediately patterned using an Nd: YAG laser to remove both layers.

The steps of depositing OSL and TCL are repeated as in Example 1), which essentially defines a region that is non-patterned but where electrical connections from the power source can be made to the electrodes.

An electrical interconnect is formed by applying laser pulses to the center of each hole forming the interconnects; The laser was applied from the top-side (ie without passing through the substrate) using optical alignment (but can also be done without optical alignment). The interconnects are made in 1 / mm in matrix format.

OLEDs operate to have very high homogeneity as expected. Through this very simplified method, it is possible to make large areas of light emitting organic devices without any mask or lithographic patterning step.

Organic photovoltaic device

Organic photovoltaic devices are made in the form of one, large area organic solar cell. A 0.8 mm thick stainless steel sheet with lateral dimensions of 100 mm x 100 mm is provided as a substrate. A patterned non-conductive polyimide layer is deposited as described above. The polyimide layer is patterned to expose the substrate as a matrix of holes. The spacing between the rows and columns of the matrix is 20 mm, each hole having a diameter of 1 mm. A 100 nm thick SML layer of Ag is deposited on the polyimide layer.

The frequency doubled Nd: YAG laser is used to remove the SML and insulating layer in the holes, exposing the substrate. Alternatively, a photosensitive polyimide layer or additional photoresist may be used to pattern the SML, although increasing complexity.

The following layer was deposited as OSL:

A 5% (molar) p-doped (Cu-phthalocyanine) CuPc layer of 10 nm thickness was deposited over the ITO through a shadow mask;

A 10 nm undoped CuPc layer was deposited over the doped CuPc layer;

30 nm thick mixed layers of fullerene C60 and CuPc were deposited at a molar ratio of 2 (C60): 1 (CuPu);

40 nm thick C60 was deposited on top of the mixed layer;

A 10 nm BPhen (4,7-diphenyl-1,10-phenanthroline) layer was deposited on top of the C60 layer.

20 nm of silver was deposited as TCL.

The electrical interconnect was formed by applying laser pulses to the center of the outer holes forming three adjacent interconnects on each hole; The laser was applied from the top side (ie not penetrating the substrate). The laser used in this example was a pulsed Nd: YAG laser operating at 1064 nm.

The device showed an I-V curve with a characteristic large series resistance. After the experimental characterization, electrical interconnects were made in all other holes, in a matrix-orthogonal grid-format, with significantly lower series resistance. 6 shows the geometry of such a device. Short circuit current is improved by more than 100%.

Subsequently, further preferred embodiments of organic electronic devices comprising serial interconnects are described. Reference is made to FIGS. 7 to 13.

The arrows indicate the direction in which light is emitted when the device is an organic light emitting device, and these arrows are used to show the mode of the device: when the device is top emitting (absorbing), it is bottom emitting (absorbing) If, or completely permeable.

7a shows a bottommost emissive organic light emitting device comprising individual devices connected in series according to the prior art. FIG. 7A illustrates a stacked structure over a transmissive substrate 70a that includes a transmissive bottom electrode 71a, at least one organic semiconductor layer 72a, and a reflective top electrode 73a. At least one organic semiconductor layer 72a and top electrode 73a need to be patterned directly by, for example, shadow masks or ink-jet printing. The arrows indicated the direction in which light is emitted when the device is an OLED, which is opposite the absorption of light for the photovoltaic device.

FIG. 7B shows a bottommost light emitting device that includes a bottom electrode 71b pre-patterned over the substrate 70b and an electrically insulated separator 75b. Organic layer (s) 72b and top electrode 73b are created without shadow masks. Separation of the individual devices is provided by separators 75b that are electrically insulated during the deposition of the layers. A series electrical interconnect 74b, also referred to as an electrical top-electrode-bottom-electrode connection, is made by a laser process.

FIG. 8 shows a top light emitting device (or having a stacked structure comprising a bottom electrode 81 and at least one organic semiconductor layer 82 between a bottom electrode 81 and a top electrode 83 on a substrate 80. Top absorbing photovoltaic device), where top electrode 83 is transmissive and substrate 80 and / or bottom electrode 81 is reflective. Separation of the individual devices is provided by electrically insulating separators 85 during the deposition of the layers. The electrical interconnects 84 in series are made by lasers.

9 shows a transmissive device having at least one organic semiconductor layer 92 between electrodes 91 and 93, wherein top electrode 93, bottom electrode 91, and substrate 90 are transmissive. . Isolation separator 95 and electrical interconnect 94 in series provide for serial connection of the individual devices (i + 1, i, i-1, ...).

10 shows an array of individual devices connected in series (columns ..., i + 1, i, i-1), with columns connected in parallel (rows). FIG. 10 shows the patterned bottom electrodes 101, insulation separator 102, and electrical interconnect 104 in succession. The black lines 104 show where the laser is applied, and obviously the electrical interconnect is only formed where the top and bottom electrodes are provided. The columns may be connected in parallel by the conductive layers 105 and 106. Alternatively, the columns can be driven in groups or individually. Alternatively or in addition, the layer forming the bottom electrodes can be patterned continuously between adjacent columns. The bottom electrodes of the row can optionally be made of single layers (eg, stripes). The layer 103 which also provides the top electrode is only partially shown (for clarity reasons).

Layer 106 is provided in electrical contact with the bottom electrodes on top before deposition of organic layers. Alternatively or alternatively, electrical interconnect 107 may be used to provide interconnection between conductive layer 106 and bottom electrodes. Other variations can be made, for example, the conductive layer 106 does not overlap with the bottom electrodes, the top conductive layer forming the top electrodes, plus the required electrical interconnects, provide the necessary electrical paths. The same idea can be applied to the conductive layer 105 and to other embodiments. The conductive layer 105 may optionally be an extension of the top electrode layer and may be provided over the organic layer (this also applies to other embodiments).

Figure 11 shows an array of individual devices connected in series (columns ...., i-1, i, i + 1), the columns being connected in parallel (rows). FIG. 11 shows patterned bottom electrodes 111, insulation separator 112, and in series electrical interconnects 114. The columns may be connected in parallel by conductive layers 115 and 116. The layer 113 which also provides the top electrode is only partially shown (for clarity reasons). In this embodiment, insulation separator 112 is patterned in regions 112 and 117, and regions 117 (parallel to the columns) are used to define the radiation regions. Alternatively or additionally, the layer forming the bottom electrodes 111 may be patterned continuously between adjacent columns. The bottom electrodes 111 of the row may optionally be a single layer (eg, a stripe).

12 illustrates a stacked structure including a substrate 120, a bottom electrode 121, at least one organic layer 122, and a top electrode 123. Insulation separator 125 is used to separate at least one organic layer 122 and top electrode 123 into two regions. Insulation separator 125 preferentially has a conical (mushroom) format. This can be realized by constructing the insulation separator 125 from the two photoresists at different etch rates (the bottom part should have a higher etch rate).

Figure 13 shows a mode for electrical interconnects that can be used for all embodiments of the present invention. FIG. 13 shows a stacked structure including a substrate 130, a bottom electrode 131, at least one organic layer 132, and a top electrode 133. Electrical interconnection is always through closed OSL. In other words, the OSL is formed as a closed layer and the IC provides a local connection of the two opposing electrodes via the OSL. After fabricating the electrical interconnect by the laser method as described above, the top electrode is in direct contact with the bottom electrode. The layer forming the top electrode does not necessarily have to be interrupted as shown in FIG.

Further embodiments are described below with reference to device examples.

Organic luminescence device  Examples

The following terms are used: Spiro-TTB-rooftop-toryl-9,9'-spirobi [fluorene] -2,2 ', 7,7'-tetraamine-2,2', 7, 7'-tetrakis (N, N-di-p-methylphenylamino) -9,9'-spirobifluorene (octap-tolyl-9,9'-spirobi [fluorene] -2,2 ', 7,7 '-tetraamine-2,2', 7,7'-tetrakis (N, N-di-p-methylphenylamino) -9,9'-spirobifluorene, F4TCNQ -2,3,5,6-tetrafluor-7,7 , 8,8-tetracyanokinomidimethane (2,3,5,6-Tetrafluor-7,7,8,8-tetracyanochinodimethan), Spiro-TAD-2,2 ', 7,7'-tetrakis ( N, N-diphenylamino) -9,9'-spirobifluorene (2,2 ', 7,7'-Tetrakis (N, N-diphenylamino) -9,9'-spirobifluorene, Ir (ppy) 3 Tris (2-phenylpyridine) iridium, TPBI-1,3,5-tris (1-phenyl-1H-benzimidazol-2-yl) benzene (1,3,5 -Tris (1-phenyl-1H-benzimidazol-2-yl) benzene, and BPhen-2,9-bis (naphthalen-2-yl) -4,7-diphenyl-1,10-phenanthroline (2, 9-Bis (naphthalen-2-yl) -4,7-diphenyl-1,10-phenanthroline.

A 0.8 mm thick glass substrate with side dimensions of 100 mm x 100 mm was provided as a substrate. The glass substrate has eight stripes spaced by 500 μm with side dimensions of 80 mm × 9.5 mm, except for the first stripe with an extension to the edge A of the substrate used to power the device. Patterned, pre-patterned ITO layer.

The patterned non-conductive layer was deposited as described above. Insulation separators are provided 300 μm away from one edge of each patterned ITO stripe. An area of 300 μm between the insulation separator and the edge is used for the top-electrode-bottom-electrode connection. Insulation separators are provided as seven lines with a length of 82 mm.

The stack of organic semiconductor layers was deposited by VTE over an area of 82 mm by 82 mm that completely covers the ITO stripes, except for the first stripe with an extension to the edge of the substrate used to power the device. . The stack of organic layers is made of the following layers:

Hole transport layer: 78 nm Spiro-TTB p-doped with 2 mol% of F4TCNQ

Electron transport layer: Spiro-TAD at 10 nm

10 nm Spiro-TAD doped with 5 mol% of emitter layer 1, Ir (ppy) 3

10 nm TPBI doped with 9 mol% of emitter layer 2, Ir (ppy) 3

Electron transport layer, 10 nm BPhen, and

Electron transport layer, 30 nm BPhen (molar ratio 1: 1) doped with Cs

The top electrode of 100 nm Al was deposited over an 80 mm x 90 mm area, overlapping the ITO stripes, extending to the edge of the substrate located opposite the edge A, and providing an external electron supply layer.

The top electrode was interrupted by insulation separators that electrically insulated the individual devices onto the desired locations.

The device was encapsulated using a rigid glass encapsulation cover adhered to the glass substrate; The encapsulation also includes an oxygen and moisture getter.

The electrical top-electrode-bottom-electrode connection was formed by forming seven rows between the insulation separator and the edges of the ITO stripes, and applying laser pulses on the edges of the ITO stripes forming the electrical connection in series. The laser used in this example was a pulsed Nd: YAG laser operating at 1064 nm. Laser processing was done in the air because the device was encapsulated. This may be done in an inert atmosphere prior to encapsulation, but this can increase process complexity.

Laser pulses are applied through the encapsulation, but may be applied through the substrate.

The organic light emitting device with eight single light emitting diodes connected in series worked as expected.

The above example was repeated and an insulating separator was provided at a distance of 100 μm of the edge of the ITO stripe. Electrical interconnects were formed on this 100 μm wide and 80 nm long region. When using this method, not only the process is greatly simplified, but also the connection area can be minimized. Gaps between ITO stripes of as small as 100 μs μm may be used, which reduces the total dead area (the area used for connection rather than light emission) to less than 300 μm.

Organic photovoltaic device

A glass substrate having a side dimension of 100 mm x 100 mm and having a thickness of 0.8 mm was provided as a substrate. The glass substrate has side dimensions of 80 mm by 9.5 mm and is patterned into eight stripes spaced by 500 μm except for a first stripe that extends to the edge A of the substrate used to power the device. It includes a pre-patterned ITO layer.

A 2.3 μm thick photosensitive polyimide layer (HD-8820 from HD microsystems) was deposited on the substrate by spin coating. The polyimide layer is heated to 120 ° C. for 3 minutes; Double insulated separators (two insulated separators spaced in parallel, 500 μm apart) are defined by exposing the polyimide layer to the light pattern for 50 seconds, developing for 120 seconds, and heating at 180 ° C. for 30 minutes. . Double insulation separators are provided 500 μm apart at one edge of the patterned ITO stripe. An area of 500 μm between the double insulation separator and the edge is used for connecting series electrical interconnects. Double insulation separators are provided as seven double lines with a length of 82 mm.

A stack of organic semiconductor layers was deposited by the VTE over an area of 82 mm x 82 mm mm that completely covers the ITO stripes, except for the first stripe that extends to the edge of the substrate used to power the device. The stack of organic layers is made of the following layers:

A 10 nm thick 5% (mol) p-doped (Cu-Phthalocyanine) CuPc layer was deposited through a shadow mask over ITO;

A 10 nm undoped CuPc layer was deposited over the doped CuPc layer:

A mixed layer of 30 nm thick fullerene C60 and CuPc was deposited at a molar ratio of 2 (C60): 1 (CuPc).

40 nm thick C60 layer is deposited on top of the mixed layer.

A 10 nm BPhen (4,7-dipienyl-1, 10-phenanthroline) layer is deposited on top of the C60 layer.

The top electrode of 100 nm Al is deposited over an area of 80 mm x 90 mm, overlapping with the ITO stripes and extending to the edge of the substrate opposite the edge (A) and providing an external electrical supply layer.

The top electrode is interrupted by double insulation separators at the desired locations, which electrically insulate the individual devices.

The device is encapsulated using a rigid glass encapsulation cover adhered to the glass substrate, which encapsulation also includes oxygen and moisture getters.

The electrical interconnects are formed by supplying laser pulses on the edges of the ITO stripes that form seven rows between the edges of the ITO stripes and the isolation separator, forming a series of electrical connections. The laser used in this example is a pulsed Nd: YAG laser operating at 1064 nm. Since the laser processing device is encapsulated, it is performed in air. This can also be done in an inert atmosphere before encapsulation, but this can increase process complexity. Laser pulses may also be applied through the substrate.

The organic photovoltaic device has eight single organic solar cells connected in series and operates as expected to deliver a total open circuit voltage of 3.7 V.

Other lasers are also tested and the parameters for each different laser can be easily adjusted to provide an interconnect.

Features disclosed in at least one of the description, the claims, and the drawings may be material for recognizing the invention in various embodiments, taken alone or in various combinations.

Claims (19)

A method for forming an electrical interconnect in an organic electronic device,
Providing a first conductive layer;
Depositing an organic semiconductor layer over the first conductive layer;
Depositing a second conductive layer over the organic semiconductor layer; And
Electricity between the first conductive layer and the second conductive layer in the connection region by electrically interconnecting the first conductive layer and the second conductive layer through the organic semiconductor layer by irradiating a laser light into the connection region. Forming a short circuit
Including,
A method for forming an electrical interconnect. The method of claim 1,
Providing the first conductive layer as a first metal layer; And
Depositing the second conductive layer as a second metal layer
Further comprising at least one of,
A method for forming an electrical interconnect. The method according to claim 1 or 2,
The method for forming the electrical interconnect further includes forming the electronic device as an organic photo-electronic diode, wherein forming the electronic device comprises:
Providing a substrate,
Providing a first conductive layer, thereby producing a conductive structure made of a conductive material over the substrate, the conductive structure providing a feed contact to a region A and a top electrode that provides a bottom electrode; Region B, wherein regions A and B are electrically isolated from each other;
Providing the top electrode by depositing the second conductive layer over the organic semiconductor layer, and
Irradiating a laser light into the connection region to electrically interconnect the top electrode and the feed contact through the organic semiconductor layer to form an electrical short between the top electrode and the feed contact in the connection region.
Including,
A method for forming an electrical interconnect. The method of claim 3, wherein manufacturing the conductive structure comprises:
Fabricating a metal layer on the substrate, and
Fabricating a patterned insulating layer over the metal layer
Including,
A method for forming an electrical interconnect. The method of claim 3, wherein the method for forming the electrical interconnect further comprises fabricating a patterned insulating layer over the substrate.
A method for forming an electrical interconnect. The method of claim 3, wherein manufacturing the conductive structure comprises:
Depositing a metal layer on the substrate, and
Patterning the metal layer
Including,
A method for forming an electrical interconnect. 7. The method of claim 5 or 6, wherein producing the patterned insulating layer and / or patterning the metal layer comprises removing the layer by laser ablation.
A method for forming an electrical interconnect. The method of claim 3, wherein manufacturing the conductive structure comprises:
Depositing a layer of photoresist material on the substrate,
Depositing a metal layer over the photoresist layer, and
Patterning the metal layer by partially removing the photoresist material
Including,
A method for forming an electrical interconnect. The method of claim 3, wherein fabricating the conductive structure comprises providing the second conductive layer by a metal substrate.
A method for forming an electrical interconnect. 10. The method of claim 3, wherein the method for forming the electrical interconnects comprises:
Encapsulating the organic photo-electronic diode, and
Forming the electrical short between the top electrode and the feed contact by irradiation of laser light before or after encapsulating the organic photo-electronic diode
Further comprising,
A method for forming an electrical interconnect. As a method for forming an organic opto-electronic device,
The method for forming the organic opto-electronic device
Providing a plurality of organic photo-electronic diodes on a substrate, wherein providing the plurality of organic photo-electronic diodes comprises:
Providing a bottom electrode for each of the plurality of organic photo-electronic diodes by depositing a first conductive layer on the substrate,
Providing a separator on the first conductive layer,
Providing an organic layer on each of the plurality of organic photo-electronic diodes on the first conductive layer, and
Providing a top electrode for each of the plurality of organic photo-electronic diodes by depositing a second conductive layer on the organic layer, wherein the top electrodes of adjacent organic photo-electronic diodes are separated by the separator.
It includes; And
The method for forming the organic opto-electronic device
Providing a series connection of the plurality of organic opto-electronic diodes, wherein providing the series connection comprises:
Forming series of electrical interconnections in the connection area,
Providing respective electrical interconnects by electrically interconnecting a top electrode and a bottom electrode of adjacent organic photo-electronic diodes of the plurality of organic photo-electronic diodes, and
Forming the electrical interconnections by laser processing
Including,
A method for forming an organic opto-electronic device. The method of claim 11, wherein forming the electrical connections by the laser processing comprises irradiating laser light through the substrate.
A method for forming an organic opto-electronic device. 13. The method of claim 11 or 12, wherein the method for forming the organic optoelectronic device further comprises providing an encapsulation on the top electrode, and providing a series connection of the plurality of organic optoelectronic diodes. Is performed after the step of providing the encapsulation,
A method for forming an organic opto-electronic device. 14. The maskless deposition process of claim 11, wherein the plurality of organic photo-electronic diodes comprises maskless deposition of materials within at least an active region. Generated on the substrate,
A method for forming an organic opto-electronic device. The separator according to claim 11, wherein the separator is provided as a tapered separator.
A method for forming an organic opto-electronic device. The method of claim 11, wherein the separator is provided with a plurality of sub-separators.
A method for forming an organic opto-electronic device. 17. The electrical interconnect of claim 11, wherein the electrical interconnect is provided adjacent an electrode edge of the bottom electrode, and the separator is a side of the electrical interconnect facing away from the electrode edge. Provided adjacent said electrical interconnection on
A method for forming an organic opto-electronic device. 18. The method of claim 11, wherein the organic layer is provided with a redox doped layer adjacent to the top-electrode.
A method for forming an organic opto-electronic device. An organic light emitting device made by the method according to at least one of claims 11 to 18,
A plurality of organic photo-electronic diodes on a substrate, each of the organic photo-electronic diodes comprising a bottom electrode, a top electrode and an organic layer disposed between the bottom and bottom electrodes;
An electrical separator for electrically separating top electrodes of adjacent organic photo-electronic diodes of the plurality of organic photo-electronic diodes, and
Electrical interconnects electrically connecting the top and bottom electrodes of adjacent organic photo-electronic diodes of the plurality of organic photo-electronic diodes, the electrical interconnects being a series connection of the plurality of organic photo-electronic diodes Provides laser-generated connections
Including,
Organic light emitting device.

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