WO2014073446A1 - 光電変換素子および固体撮像装置ならびに電子機器 - Google Patents
光電変換素子および固体撮像装置ならびに電子機器 Download PDFInfo
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- WO2014073446A1 WO2014073446A1 PCT/JP2013/079528 JP2013079528W WO2014073446A1 WO 2014073446 A1 WO2014073446 A1 WO 2014073446A1 JP 2013079528 W JP2013079528 W JP 2013079528W WO 2014073446 A1 WO2014073446 A1 WO 2014073446A1
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- photoelectric conversion
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
- H10K30/20—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising organic-organic junctions, e.g. donor-acceptor junctions
- H10K30/211—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising organic-organic junctions, e.g. donor-acceptor junctions comprising multiple junctions, e.g. double heterojunctions
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E10/00—Energy generation through renewable energy sources
- Y02E10/50—Photovoltaic [PV] energy
- Y02E10/549—Organic PV cells
Definitions
- the present disclosure relates to a photoelectric conversion element using an organic photoelectric conversion material, and a solid-state imaging device and an electronic device including such a photoelectric conversion element as a pixel.
- Patent Document 1 in order to prevent performance deterioration due to high-temperature heat treatment (200 ° C. or more), an intermediate layer made of an organic compound having a glass transition temperature of 200 ° C. or more is provided between the photoelectric conversion layer and the electrode. .
- the interposition of such an intermediate layer causes a decrease in quantum efficiency, and also reduces the degree of freedom in material selection of the organic semiconductor. Therefore, it is desirable to realize a method for suppressing the performance deterioration of the photoelectric conversion layer due to the heat treatment without providing such an intermediate layer.
- a photoelectric conversion element includes a first organic semiconductor of a first conductivity type and a second organic semiconductor of a second conductivity type, and one of the first and second organic semiconductors.
- a solid-state imaging device includes a plurality of pixels each including the photoelectric conversion element according to the embodiment of the present disclosure.
- An electronic device includes the solid-state imaging device according to the embodiment of the present disclosure.
- the photoelectric conversion layer includes a first organic semiconductor of a first conductivity type and a second organic semiconductor of a second conductivity type. Or the derivative or the isomer of either one of them is added. Thereby, the aggregation of the first or second organic semiconductor is suppressed in the high temperature heat treatment of the manufacturing process.
- the photoelectric conversion layer includes the first organic semiconductor of the first conductivity type and the second organic semiconductor of the second conductivity type. Furthermore, one of the derivatives or isomers thereof is added. Thereby, in the high-temperature heat treatment of the manufacturing process, the aggregation of the first or second organic semiconductor can be suppressed, and unevenness in film quality in the photoelectric conversion layer can be reduced. Therefore, the performance deterioration of the photoelectric conversion layer due to the heat treatment can be suppressed.
- FIG. 1 is a cross-sectional view illustrating a schematic configuration example of a photoelectric conversion element (pixel) according to an embodiment of the present disclosure. It is a schematic diagram showing an example of the ternary system mixing ratio of the organic semiconductor contained in the photoelectric converting layer shown in FIG.
- FIG. 6 is a perspective view illustrating a configuration example of a photoelectric conversion element according to Comparative Example 1. It is an image which shows the film state after heat processing of the photoelectric converting layer shown in FIG.
- FIG. 6 is a perspective view illustrating a configuration example of a photoelectric conversion element according to Comparative Example 2. It is an image which shows the film state after heat processing of one photoelectric converting layer (intermediate layer: BCP) shown in FIG.
- intermediate layer: BCP intermediate layer
- FIG. 1 It is an image which shows the film state after heat processing of the other photoelectric converting layer (intermediate layer: PTCDI) shown in FIG.
- Embodiment an example of a photoelectric conversion element in which a derivative of an n-type organic semiconductor is added to a photoelectric conversion layer containing a p-type organic semiconductor and an n-type organic semiconductor
- Modification example when other derivative is added
- Overall configuration example of solid-state imaging device Application example (example of electronic device (camera))
- FIG. 1 illustrates a schematic cross-sectional configuration of a pixel (photoelectric conversion element 10) in a solid-state imaging device according to an embodiment of the present disclosure.
- the solid-state imaging device which will be described in detail later, is, for example, a charge coupled device (CCD) or a complementary metal oxide semiconductor (CMOS) image sensor.
- the photoelectric conversion element 10 is provided, for example, on a substrate 11 having a pixel transistor and a wiring, and is covered with a sealing film and a planarization film (not shown).
- a planarization film for example, an on-chip lens (not shown) is disposed on the planarizing film.
- the photoelectric conversion element 10 is an organic photoelectric conversion element that generates an electron-hole pair by absorbing light of a selective wavelength (for example, color light of any of R, G, and B) using an organic semiconductor. .
- the photoelectric conversion elements 10 (pixels) of the respective colors of R, G, and B are two-dimensionally arranged in parallel.
- a plurality of photoelectric conversion layers made of an organic semiconductor are vertically stacked in one pixel, or a photoelectric conversion layer made of an organic semiconductor and a photoelectric conversion layer made of an inorganic semiconductor are vertically stacked.
- the configuration may be adopted. In this embodiment, the main part configuration of such a photoelectric conversion element will be described with reference to FIG.
- the photoelectric conversion element 10 includes, on a substrate 11, an organic layer 13 as a photoelectric conversion layer, and a pair of electrodes (lower electrode 12 and upper electrode 14) for extracting signal charges from the organic layer 13.
- the lower electrode 12, the organic layer 13 and the upper electrode 14 are covered with an insulating layer 15 having an opening (light receiving opening) H1.
- the lower electrode 12 (first electrode) is electrically connected to the lower contact electrode 16A
- the upper electrode 14 (second electrode) is electrically connected to the upper contact electrode 16B.
- signal charge for example, electrons
- the lower electrode 12 is electrically connected to, for example, a storage layer embedded in the substrate 11 via the lower contact electrode 16A. Be done.
- the lower contact electrode 16A is electrically connected to the lower electrode 12 through an opening (contact hole) H2 provided in the insulating film 15. Electric charges (for example, holes) are discharged from the upper electrode 14 through the upper contact electrode 16B.
- the substrate 11 is made of, for example, silicon (Si).
- a conductive plug or a storage layer (not shown) serving as a transmission path for charges (electrons or holes) extracted from the organic layer 13 is embedded.
- the organic photoelectric conversion layer and the inorganic photoelectric conversion layer are stacked in one pixel as described above, the inorganic photoelectric conversion layer is embedded in the substrate 11.
- the lower electrode 12 is made of, for example, a metal element such as aluminum (Al), chromium (Cr), gold (Au), platinum (Pt), nickel (Ni), copper (Cu), tungsten (W) or silver (Ag). It is composed of a single element or an alloy.
- the lower electrode 12 may be made of, for example, a transparent conductive film such as ITO (indium tin oxide).
- ITO indium tin oxide
- a tin oxide (TO), a tin oxide (SnO 2 ) based material added with a dopant, or a zinc oxide based material obtained by adding a dopant to zinc oxide (ZnO) is used.
- the zinc oxide based material for example, aluminum zinc oxide (AZO) to which aluminum (Al) is added as a dopant, gallium zinc oxide (GZO) to which gallium (Ga) is added, and indium zinc oxide to which indium (In) is added (IZO).
- AZO aluminum zinc oxide
- GZO gallium zinc oxide
- IZO indium zinc oxide to which indium (In) is added
- CuI, InSbO 4 , ZnMgO, CuInO 2 , MgIN 2 O 4 , CO, ZnSnO 3 or the like may be used.
- the insulating film 15 is formed of, for example, a single layer film made of one of silicon oxide, silicon nitride and silicon oxynitride (SiON) or a laminated film made of two or more of these. These insulating films 15 have a function of electrically separating the lower electrodes 12 of the respective pixels when the photoelectric conversion element 10 is used as a pixel of a solid-state imaging device.
- the organic layer 13 is configured to include p-type (first conductivity type) and n-type (second conductivity type) organic semiconductors that absorb light in a selective wavelength range and perform photoelectric conversion.
- p-type organic semiconductors and n-type organic semiconductors include various organic pigments.
- quinacridone derivatives quinacridone such as quinacridone, dimethyl quinacridone, diethyl quinacridone, dibutyl quinacridone, etc.
- dihalogen quinacridone such as dichloro quinacridone
- phthalocyanines Derivatives phthalocyanine, SubPC, CuPC, ZnPC, H2PC, PbPC
- oxadiazole derivatives NDO, PBD
- stilbene derivatives TPB
- perylene derivatives PTCDA, PTCDI, PTCBI, Bipyrene
- TCNQ, F4-TCNQ tetracyanoquinodimethane derivatives
- Bphen Anthracene, Rubrene, Bianthrone
- naphthalene derivatives, pyrene derivatives and fluoranthene derivatives may be used.
- polymers such as phenylene vinylene, fluorene, carbazole, indole, pyrene, pyrrole, picoline, thiophene, acetylene, diacetylene and derivatives thereof may be used.
- metal complex dyes rhodamine dyes, cyanine dyes, merocyanine dyes, phenylxanthene dyes, triphenylmethane dyes, rhodacyanine dyes, xanthene dyes, macrocyclic azaannulene dyes, azulene dyes, naphthoquinones , Anthraquinone dyes, chain compounds in which fused polycyclic aromatic and aromatic rings or heterocyclic compounds such as anthracene and pyrene are condensed, or quinoline, benzothiazole, benzoxazole having squarylium group and croconicut methine group as a bonding chain And the like, or dyes similar to cyanine-based dyes linked by squarylium groups and crocoxicmetin groups, and the like can be preferably used.
- the metal complex dye is preferably an aluminum complex (Alq3, Balq), a dithiol metal complex dye, a metal phthalocyanine dye, a metal porphyrin dye, or a ruthenium complex dye, but is not limited thereto.
- Alq3, Balq aluminum complex
- dithiol metal complex dye dithiol metal complex dye
- metal phthalocyanine dye a metal phthalocyanine dye
- metal porphyrin dye e.g., ruthenium complex dye
- ruthenium complex dye ruthenium complex dye
- other organic materials such as fullerene (C60) and BCP (Bathocuproine) may be laminated on the organic layer 13 as an electrode structure adjusting layer.
- the organic layer 13 contains two of the above materials as a p-type organic semiconductor and an n-type organic semiconductor (hereinafter referred to as organic semiconductors A and B), and one of their analogues (derivatives or An isomer (hereinafter, referred to as an organic semiconductor C1) is formed by adding a predetermined amount.
- the organic layer 13 is, for example, a co-evaporated film (formed by a co-evaporation method described later) including the organic semiconductors A, B, and C1.
- the organic layer 13 may be a coated film (formed by a coating method described later) or a printed film (formed by a printing method described later) containing the organic semiconductors A, B, and C1.
- the organic semiconductors A, B, and C1 can be alternately stacked in film thicknesses of about 10 nm or less.
- the organic semiconductor C1 is a more cohesive (relatively aggregation prone) one of the organic semiconductors A and B.
- cohesive indicates the ease of aggregation at a temperature of, for example, about 150 ° C. to 600 ° C. by the action of an intermolecular force or the like.
- FIG. 2 shows one example of the ternary mixture ratio of these organic semiconductors A, B and C1.
- a quartz substrate substrate temperature 60 ° C.
- the organic layer 13 as described above can be formed on the lower electrode 12 as follows, for example. That is, the organic semiconductor C1 is further added to the lower electrode 12 in which two types (organic semiconductors A and B) of the p-type and n-type organic semiconductor materials are dissolved in a predetermined solvent.
- a mixed solution containing organic semiconductors A, B and C1 is prepared.
- the mixing ratio of the organic semiconductors A, B and C1 in this mixed solution can be, for example, the mixing ratio as shown in r2, r4 and r5 shown in FIG.
- By co-evaporating the mixed solution thus prepared for example, it is possible to form the organic layer 13 containing the organic semiconductors A, B, and C1 at a predetermined mixing ratio.
- a film of the mixed solution by various coating methods such as spin coating, slit coating, and dip coating.
- various printing methods such as reverse offset printing and letterpress printing.
- multistage vapor deposition in which solutions containing the organic semiconductors A, B and C1 are sequentially formed by vapor deposition It can be formed.
- a solution in which the organic semiconductors A and C1 are mixed and a solution containing the organic semiconductor B may be sequentially deposited.
- the upper electrode 14 is formed of the transparent conductive film mentioned in the lower electrode 12. When the signal charge is extracted from the lower electrode 12 side as in the present embodiment, the upper electrode 14 is provided in common to each pixel.
- the photoelectric conversion element 10 of the present embodiment for example, as a pixel of a solid-state imaging device, signal charges are acquired as follows. That is, when light is incident on the photoelectric conversion element 10 through an on-chip lens (not shown), the incident light is photoelectrically converted in the organic layer 13. Specifically, first, predetermined color light (red light, green light or blue light) is selectively detected (absorbed) in the organic layer 13 to generate electron-hole pairs. Among the generated electron-hole pairs, for example, electrons are extracted from the lower electrode 12 side and accumulated in the substrate 11, while holes are discharged from the upper electrode 14 side via a wiring layer (not shown). By reading out the light reception signals of the respective colors accumulated in this manner to the vertical signal line Lsig described later, it is possible to obtain imaging data of the respective colors of red, green and blue.
- predetermined color light red light, green light or blue light
- FIG. 3 is a perspective view showing the configuration of a sample (sample 100a) of a photoelectric conversion element according to a comparative example (comparative example 1) of the present embodiment.
- an organic layer 102 composed of a binary co-deposited film of quinacridone and SubPC is deposited on a substrate 101 composed of quartz, and then an electrode 103 composed of ITO is deposited and subjected to high temperature annealing (250 ° C.
- Sample 100a was produced by applying the degree, for several minutes.
- a cross section of the organic layer 102 of the sample 100a is photographed using an optical microscope, and a bright field image is shown in FIG. 4 (A) and a dark field image is shown in FIG. 4 (B).
- FIG. 5 is a perspective view showing a configuration of a sample (sample 100b) of a photoelectric conversion element according to a comparative example (comparative example 2-1) of the present embodiment.
- Comparative Example 2-1 after the organic layer 102 (codeposited film of quinacridone and SubPC) is deposited on the substrate 101 via the intermediate layer 104 made of BCP (low glass transition temperature), the electrode 103 is formed. The film was subjected to high temperature annealing (about 250 ° C., for several minutes) to prepare a sample 100 b. A cross section of the organic layer 102 of the sample 100b is photographed using an optical microscope, and a bright field image is shown in FIG. 6 (A) and a dark field image is shown in FIG. 6 (B). As described above, even in Comparative Example 2-1 in which the intermediate layer 104 made of BCP is provided between the organic layer 102 and the substrate 101, it is understood that spots occur and unevenness in the film quality occurs.
- the organic layer 102 composed of a co-deposited film containing a p-type organic semiconductor and an n-type organic semiconductor, spots or the like are generated due to the manufacturing process (high temperature heat treatment), and unevenness in the film quality occurs. . It is considered that this is because one of the p-type organic semiconductor and the n-type organic semiconductor (here, quinacridone as the p-type organic semiconductor) preferentially aggregates to cause phase separation in the organic layer 102. .
- the organic layer 13 including the p-type organic semiconductor A (for example, quinacridone) and the n-type organic semiconductor B (for example, SubPC) Semiconductor C1 (dimethyl quinacridone) is added.
- the organic layer 13 further includes the analogue (organic semiconductor C1) of the more cohesive one (organic semiconductor A) among them.
- the regular arrangement of the molecules of the organic semiconductor A (QD molecules 130a) is broken (disrupted) by the molecules of the organic semiconductor C1 (dimethyl QD molecules 130b). It is for. Specifically, quinacridone molecules tend to aggregate due to intermolecular force, but for example, by using a derivative in which a methyl group is disposed at the 2, 9 position with respect to quinacridone, spots do not significantly change electrical characteristics. Occurrence is suppressed.
- FIG. 9 shows a band diagram of the device structure of this embodiment.
- a ternary co-deposited film of an organic semiconductor A, B, C1 is provided between an electrode made of ITO (work function 4.8 eV) and an electrode made of aluminum (work function 4.3 eV).
- the energy level of the highest occupied molecular orbital (HOMO) of quinacridone is about 5.3 eV
- the energy level of the lowest unoccupied molecular orbital (LUMO) is about 3.2 eV. is there.
- the energy level of the highest occupied atomic orbital of SubPC is about 5.4 eV
- the energy level of the lowest unoccupied orbital is about 3.3 eV.
- the organic semiconductor C1 which is a derivative of the organic semiconductor A, is added to the organic layer 13 containing the p-type organic semiconductor A and the n-type organic semiconductor B.
- the aggregation of the organic semiconductor A is suppressed, and the unevenness of the film quality in the organic layer 13 can be reduced. Therefore, performance degradation of the organic layer 13 (photoelectric conversion layer) resulting from the heat treatment can be suppressed.
- FIG. 11 shows one example of a ternary mixture ratio of the organic semiconductors (organic semiconductors A, B, C2) contained in the organic layer 13 according to the modification.
- the organic layer 13 includes the organic semiconductor A (quinacridone) and the organic semiconductor B (subphthalocyanine) similar to those in the above-described embodiment, and an organic semiconductor different from the organic semiconductor C1 as a derivative of the organic semiconductor A C2 (dichloroquinacridone) is added.
- the organic semiconductor A quinacridone
- the organic semiconductor B subphthalocyanine
- a quartz substrate substrate temperature 60 ° C.
- the derivative of the organic semiconductor A is not limited to the organic semiconductor C1 (dimethyl quinacridone) of the above embodiment, but the organic semiconductor C2 (dichloroquinacridone) may be used.
- it can be used as an aggregation inhibitor of organic semiconductor A as long as it is a derivative or an analogue of organic semiconductor A, it is not limited to the above-mentioned substances, and various other substances can be used as a ternary system. It can be used as an additive in Further, the organic semiconductors A and B are not limited to the combinations of quinacridone and subphthalocyanine exemplified in FIGS. 2 and 11, and various combinations are selected from the various p-type and n-type organic semiconductors described above. be able to.
- FIG. 12 is a functional block diagram of a solid-state imaging device (solid-state imaging device 1) using the photoelectric conversion element described in the above embodiment for each pixel.
- the solid-state imaging device 1 is a CMOS image sensor, has a pixel portion 1a as an imaging area, and includes, for example, a circuit portion 130 including a row scanning portion 131, a horizontal selection portion 133, a column scanning portion 134, and a system control portion 132.
- the circuit portion 130 may be provided in the peripheral region of the pixel portion 1a, or may be provided in the peripheral region of the pixel portion 1a, or may be laminated with the pixel portion 1a (opposed to the pixel portion 1a. It may be provided in the area).
- the pixel unit 1a includes, for example, a plurality of unit pixels P (corresponding to the photoelectric conversion elements 10) arranged two-dimensionally in a matrix.
- this unit pixel P for example, pixel drive lines Lread (specifically, row selection lines and reset control lines) are wired for each pixel row, and vertical signal lines Lsig are wired for each pixel column.
- the pixel drive line Lread transmits a drive signal for reading out a signal from the pixel.
- One end of the pixel drive line Lread is connected to an output end corresponding to each row of the row scanning unit 131.
- the row scanning unit 131 is a pixel driving unit that is configured of a shift register, an address decoder, and the like, and drives each pixel P of the pixel unit 1 a in, for example, a row unit.
- a signal output from each pixel P of the pixel row selectively scanned by the row scanning unit 131 is supplied to the horizontal selection unit 133 through each of the vertical signal lines Lsig.
- the horizontal selection unit 133 is configured of an amplifier, a horizontal selection switch, and the like provided for each vertical signal line Lsig.
- the column scanning unit 134 is configured of a shift register, an address decoder, and the like, and drives the horizontal selection switches of the horizontal selection unit 133 in order while scanning them.
- the signal of each pixel transmitted through each vertical signal line Lsig is sequentially transmitted to the horizontal signal line 135 by the selective scanning by the column scanning unit 134, and is output to the outside through the horizontal signal line 135.
- the system control unit 132 receives an externally supplied clock, data instructing an operation mode, and the like, and outputs data such as internal information of the solid-state imaging device 1.
- the system control unit 132 further includes a timing generator that generates various timing signals, and the row scanning unit 131, the horizontal selection unit 133, the column scanning unit 134, and the like based on the various timing signals generated by the timing generator. Drive control is performed.
- FIG. 13 shows a schematic configuration of the electronic device 2 (camera) as an example.
- the electronic device 2 is, for example, a video camera capable of capturing still images or moving images, and drives the solid-state imaging device 1, an optical system (optical lens) 310, a shutter device 311, the solid-state imaging device 1 and the shutter device 311 And a signal processing unit 312.
- the optical system 310 guides image light (incident light) from a subject to the pixel unit 1 a of the solid-state imaging device 1.
- the optical system 310 may be composed of a plurality of optical lenses.
- the shutter device 311 controls a light irradiation period and a light shielding period to the solid-state imaging device 1.
- the drive unit 313 controls the transfer operation of the solid-state imaging device 1 and the shutter operation of the shutter device 311.
- the signal processing unit 312 performs various signal processing on the signal output from the solid-state imaging device 1.
- the video signal Dout after signal processing is stored in a storage medium such as a memory or output to a monitor or the like.
- the present disclosure content is not limited to the above-mentioned embodiment etc., and various modification is possible.
- the (ternary) organic layer 13 containing three types of organic semiconductors is exemplified in the above embodiment and the like, the organic layer of the present disclosure contains at least the three types of organic semiconductors as described above. And any other organic semiconductor may be included.
- the present disclosure may have the following configurations.
- a third organic semiconductor comprising a first organic semiconductor of a first conductivity type and a second organic semiconductor of a second conductivity type, and a derivative or isomer of one of the first and second organic semiconductors And a photoelectric conversion layer to which A photoelectric conversion element comprising: first and second electrodes provided to sandwich the photoelectric conversion layer.
- a photoelectric conversion element comprising: first and second electrodes provided to sandwich the photoelectric conversion layer.
- the photoelectric conversion element is A third organic semiconductor comprising a first organic semiconductor of a first conductivity type and a second organic semiconductor of a second conductivity type, and a derivative or isomer of one of the first and second organic semiconductors And a photoelectric conversion layer to which An electronic apparatus comprising a solid-state imaging device comprising: first and second electrodes provided with the photoelectric conversion layer interposed therebetween.
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Abstract
Description
1.実施の形態(p型有機半導体およびn型有機半導体を含む光電変換層に、n型有機半導体の誘導体が添加されてなる光電変換素子の例)
2.変形例(他の誘導体が添加される場合の例)
3.固体撮像装置の全体構成例
4.適用例(電子機器(カメラ)の例)
[構成]
図1は、本開示の一実施の形態の固体撮像装置における画素(光電変換素子10)の概略断面構成を表すものである。固体撮像装置は、詳細は後述するが、例えばCCD(Charge Coupled Device)またはCMOS(Complementary Metal Oxide Semiconductor)イメージセンサなどである。光電変換素子10は、例えば画素トランジスタや配線を有する基板11上に設けられ、図示しない封止膜および平坦化膜によって被覆されている。この平坦化膜上には例えば図示しないオンチップレンズが配設される。
有機層13は、選択的な波長域の光を吸収して光電変換するp型(第1導電型)およびn型(第2導電型)の有機半導体を含んで構成されている。p型有機半導体およびn型有機半導体としては、様々な有機顔料が挙げられるが、例えばキナクリドン誘導体(キナクリドン,ジメチルキナクリドン,ジエチルキナクリドン,ジブチルキナクリドン等のキナクリドン類、あるいはジクロロキナクリドン等のジハロゲンキナクリドン)、フタロシアニン誘導体(フタロシアニン,SubPC,CuPC,ZnPC,H2PC,PbPC)が挙げられる。また、この他にも、オキサジアゾール誘導体(NDO,PBD)、スチルベン誘導体(TPB)、ペリレン誘導体(PTCDA,PTCDI,PTCBI,Bipyrene)、テトラシアノキノジメタン誘導体(TCNQ,F4-TCNQ)、およびフェナントロリン誘導体(Bphen,Anthracene,Rubrene,Bianthrone)が挙げられる。但し、この他にも、例えばナフタレン誘導体、ピレン誘導体、およびフルオランテン誘導体が用いられていてもよい。あるいは、フェニレンビニレン、フルオレン、カルバゾール、インドール、ピレン、ピロール、ピコリン、チオフェン、アセチレン、ジアセチレン等の重合体やその誘導体が用いられていてもよい。加えて、金属錯体色素、ローダーミン系色素、シアニン系色素、メロシアニン系色素、フェニルキサンテン系色素、トリフェニルメタン系色素、ロダシアニン系色素、キサンテン系色素、大環状アザアヌレン系色素、アズレン系色素、ナフトキノン、アントラキノン系色素、アントラセンおよびピレン等の縮合多環芳香族および芳香環ないし複素環化合物が縮合した鎖状化合物、または、スクアリリウム基およびクロコニツクメチン基を結合鎖として持つキノリン、ベンゾチアゾール、ベンゾオキサゾール等の二つの含窒素複素環、または、スクアリリウム基およびクロコニツクメチン基により結合したシアニン系類似の色素等を好ましく用いることができる。尚、上記金属錯体色素としては、アルミニウム錯体(Alq3,Balq)、ジチオール金属錯体系色素、金属フタロシアニン色素、金属ポルフィリン色素、またはルテニウム錯体色素が好ましいが、これに限定されるものではない。また、有機層13には、上記のような顔料以外にも、フラーレン(C60)や、BCP(Bathocuproine)等の他の有機材料が、電極構造調整層として積層されていてもよい。
本実施の形態の光電変換素子10では、例えば固体撮像装置の画素として、次のようにして信号電荷が取得される。即ち、光電変換素子10に、図示しないオンチップレンズを介して光が入射すると、この入射光は、有機層13において光電変換される。具体的には、まず、所定の色光(赤色光,緑色光または青色光)が、有機層13に選択的に検出(吸収)されることにより、電子・ホール対を発生する。発生した電子・ホール対のうち、例えば電子が下部電極12側から取り出され、基板11内へ蓄積される一方、ホールは、上部電極14側から、図示しない配線層を介して排出される。このようにして蓄積された各色の受光信号がそれぞれ、後述の垂直信号線Lsigに読み出されることにより、赤、緑、青の各色の撮像データを得ることができる。
図3は、本実施の形態の比較例(比較例1)に係る光電変換素子のサンプル(サンプル100a)の構成を表す斜視図である。比較例1として、石英からなる基板101上に、キナクリドンとSubPCとの2元系共蒸着膜からなる有機層102を蒸着した後、ITOからなる電極103を成膜して、高温アニール(250℃程度、数分間)を施すことにより、サンプル100aを作製した。このサンプル100aの有機層102の断面を光学顕微鏡を用いて撮影し、明視野像を図4(A)に、暗視野像を図4(B)にそれぞれ示す。このように、キナクリドンとSubPCとの2元系共蒸着膜からなる有機層102を用いた比較例1では、材料のマイグレーションにより構造体が形成され、膜質にむらが生じていることがわかる。また、キナクリドンが優先的に凝集して相分離が生じている。
図11は、変形例に係る有機層13に含まれる有機半導体(有機半導体A,B,C2)の3元系混合比の一例について表したものである。本変形例では、有機層13が、上記実施の形態と同様の有機半導体A(キナクリドン)および有機半導体B(サブフタロシアニン)を含むと共に、有機半導体Aの誘導体として、有機半導体C1とは異なる有機半導体C2(ジクロロキナクリドン)が添加されている。図11では、有機半導体A,B,C2の3元系混合比(A:B:C2)=s1(50:50:0),s2(25:50:25),s3(0:50:50),s4(50:25:25),s5(25:25:50)およびs6(50:0:50)と、これらの各場合における有機層13の斑点発生の有無が示されている。尚、これは、上記実施の形態と同様、有機半導体A,B,C2を上記混合比s1~s6により混合したものを、石英基板(基板温度60℃および0℃)上に共蒸着させた後、高温アニール(250℃程度,数分間)して形成した有機層13の断面を観察し、斑点の有無を評価した結果に基づくものである。s1~s6の各点において、斑点発生が見られなかったものには「○」のマーク、斑点発生が見られたものには「△」のマークをそれぞれ付している。また、これらのマークは、基板温度60℃の場合を実線、0℃の場合を破線により示している。
図12は、上記実施の形態において説明した光電変換素子を各画素に用いた固体撮像装置(固体撮像装置1)の機能ブロック図である。この固体撮像装置1は、CMOSイメージセンサであり、撮像エリアとしての画素部1aを有すると共に、例えば行走査部131、水平選択部133、列走査部134およびシステム制御部132からなる回路部130を有している。この画素部1aの周辺領域あるいは画素部1aと積層されて、回路部130は、画素部1aの周辺領域に設けられていてもよいし、画素部1aと積層されて(画素部1aに対向する領域に)設けられていてもよい。
上述の固体撮像装置1は、例えばデジタルスチルカメラやビデオカメラ等のカメラシステムや、撮像機能を有する携帯電話など、撮像機能を備えたあらゆるタイプの電子機器に適用することができる。図13に、その一例として、電子機器2(カメラ)の概略構成を示す。この電子機器2は、例えば静止画または動画を撮影可能なビデオカメラであり、固体撮像装置1と、光学系(光学レンズ)310と、シャッタ装置311と、固体撮像装置1およびシャッタ装置311を駆動する駆動部313と、信号処理部312とを有する。
(1)
第1導電型の第1の有機半導体および第2導電型の第2の有機半導体を含むと共に、前記第1および第2の有機半導体のうちの一方の誘導体または異性体よりなる第3の有機半導体が添加されてなる光電変換層と、
前記光電変換層を挟んで設けられた第1および第2の電極と
を備えた光電変換素子。
(2)
前記第3の有機半導体は、前記第1および第2の有機半導体のうちのより凝集性の高い方の誘導体または異性体である
上記(1)に記載の光電変換素子。
(3)
前記光電変換層は、前記第1ないし第3の有機半導体を含む共蒸着膜である
上記(1)または(2)に記載の光電変換素子。
(4)
前記光電変換層は、前記第1ないし第3の有機半導体を含む塗布膜または印刷膜である
上記(1)または(2)に記載の光電変換素子。
(5)
前記光電変換層は、前記第1ないし第3の有機半導体を含む積層膜である
上記(1)または(2)に記載の光電変換素子。
(6)
各々が光電変換素子を含む複数の画素を有し、
前記光電変換素子は、
第1導電型の第1の有機半導体および第2導電型の第2の有機半導体を含むと共に、前記第1および第2の有機半導体のうちの一方の誘導体または異性体よりなる第3の有機半導体が添加されてなる光電変換層と、
前記光電変換層を挟んで設けられた第1および第2の電極と
を備えた固体撮像装置。
(7)
各々が光電変換素子を含む複数の画素を有し、
前記光電変換素子は、
第1導電型の第1の有機半導体および第2導電型の第2の有機半導体を含むと共に、前記第1および第2の有機半導体のうちの一方の誘導体または異性体よりなる第3の有機半導体が添加されてなる光電変換層と、
前記光電変換層を挟んで設けられた第1および第2の電極と
を備えた固体撮像装置を有する電子機器。
Claims (7)
- 第1導電型の第1の有機半導体および第2導電型の第2の有機半導体を含むと共に、前記第1および第2の有機半導体のうちの一方の誘導体または異性体よりなる第3の有機半導体が添加されてなる光電変換層と、
前記光電変換層を挟んで設けられた第1および第2の電極と
を備えた光電変換素子。 - 前記第3の有機半導体は、前記第1および第2の有機半導体のうちのより凝集性の高い方の誘導体または異性体である
請求項1に記載の光電変換素子。 - 前記光電変換層は、前記第1ないし第3の有機半導体を含む共蒸着膜である
請求項1に記載の光電変換素子。 - 前記光電変換層は、前記第1ないし第3の有機半導体を含む塗布膜または印刷膜である
請求項1に記載の光電変換素子。 - 前記光電変換層は、前記第1ないし第3の有機半導体を含む積層膜である
請求項1に記載の光電変換素子。 - 各々が光電変換素子を含む複数の画素を有し、
前記光電変換素子は、
第1導電型の第1の有機半導体および第2導電型の第2の有機半導体を含むと共に、前記第1および第2の有機半導体のうちの一方の誘導体または異性体よりなる第3の有機半導体が添加されてなる光電変換層と、
前記光電変換層を挟んで設けられた第1および第2の電極と
を備えた固体撮像装置。 - 各々が光電変換素子を含む複数の画素を有し、
前記光電変換素子は、
第1導電型の第1の有機半導体および第2導電型の第2の有機半導体を含むと共に、前記第1および第2の有機半導体のうちの一方の誘導体または異性体よりなる第3の有機半導体が添加されてなる光電変換層と、
前記光電変換層を挟んで設けられた第1および第2の電極と
を備えた固体撮像装置を有する電子機器。
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Also Published As
Publication number | Publication date |
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US9680104B2 (en) | 2017-06-13 |
TW201421718A (zh) | 2014-06-01 |
KR20150082246A (ko) | 2015-07-15 |
JPWO2014073446A1 (ja) | 2016-09-08 |
TWI613833B (zh) | 2018-02-01 |
EP2919277A1 (en) | 2015-09-16 |
EP2919277A4 (en) | 2016-07-20 |
JP6252485B2 (ja) | 2017-12-27 |
EP2919277B1 (en) | 2020-09-23 |
EP3767697A1 (en) | 2021-01-20 |
CN204720453U (zh) | 2015-10-21 |
KR102146142B1 (ko) | 2020-08-19 |
KR102224334B1 (ko) | 2021-03-08 |
US20150311445A1 (en) | 2015-10-29 |
KR20200098722A (ko) | 2020-08-20 |
CN103811518A (zh) | 2014-05-21 |
CN103811518B (zh) | 2017-07-14 |
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