CN108807683B - Wide-spectral-response multiplication type organic photoelectric detector - Google Patents

Wide-spectral-response multiplication type organic photoelectric detector Download PDF

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CN108807683B
CN108807683B CN201810730910.3A CN201810730910A CN108807683B CN 108807683 B CN108807683 B CN 108807683B CN 201810730910 A CN201810730910 A CN 201810730910A CN 108807683 B CN108807683 B CN 108807683B
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杨天赦
李向领
赵强
刘淑娟
冯腾
黄维
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Nanjing University of Posts and Telecommunications
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Abstract

The invention discloses a wide-spectrum-response multiplication type organic photoelectric detector which comprises a substrate, a transparent conducting layer, an anode modification layer, a photosensitive layer, a hole blocking layer and a cathode layer which are sequentially stacked, wherein the photosensitive layer is made of a material containing an organic micromolecule donor material (BODIPY) and an organic micromolecule acceptor material (PC)61BM or PC71BM); BODIPY is an organic fluorescent dye with high molar absorption coefficient and wide absorption range, has obvious photoelectric response in near infrared light wave band, and realizes the function of wide spectral response of a photoelectric detector; the responsivity or external quantum efficiency of detecting optical signals is also obviously improved, the EQE under forward bias can exceed 100%, and the maximum EQE reaches more than 350%; the device has simple structure and manufacturing process and low cost, can be used for large-area preparation, and has great advantages in the field of organic photoelectric detectors.

Description

Wide-spectral-response multiplication type organic photoelectric detector
Technical Field
The invention belongs to the technical field of photoelectric materials, and particularly relates to a multiplication type organic photoelectric detector with wide spectral response.
Background
The photodetector is a device that converts an optical signal into an electrical signal (current or voltage), and the system can respond to the optical signal through subsequent processing of a circuit system, and can also restore the electrical signal into the optical signal. The photodetectors can be classified into wide spectral response photodetectors and narrow spectral response photodetectors according to their response wavelength ranges. Among them, the wide-spectrum response photodetector has important applications in image sensing, remote control, day and night monitoring, and other aspects.
The two-end photoelectric detectors can be divided into a photodiode and an avalanche photodiode which belong to photovoltaic devices, wherein the photodiode has no internal gain, the upper limit of External Quantum Efficiency (EQE) of the photodiode is 100 percent, namely, the two-end photoelectric detectors have no multiplication effect on incident light signals; the avalanche photodiode can generate multiplication effect on photogenerated carriers, so the external quantum efficiency can exceed 100%, but the avalanche photodiode is generally prepared by inorganic semiconductor materials, the manufacturing process is complex, the cost is high, the external bias voltage during working is high (100V and 200V), the dark current is high, the avalanche photodiode needs to work in a low-temperature environment, and the restrictive condition is more.
Compared with an inorganic photoelectric detector, the organic photoelectric detector has the advantages of good flexibility, low manufacturing cost, large-area preparation, wide material selection range and the like, but the response range of the organic photoelectric detector is generally limited to the near ultraviolet to visible light wave band, so far, the reports on the organic photoelectric detector with high responsivity in the near infrared light are few, and the main reasons are as follows: in a donor-acceptor system commonly used for preparing a photoelectric detector, certain energy level difference exists between donor-acceptor materials when photoproduction excitons are separated into free carriers, a smaller energy gap is needed when near infrared light is detected, and the reduction of the energy gap makes it difficult to obtain materials with high energy level matching degree with the acceptor materials; the reduction of the energy gap makes exciton recombination easy to reduce carrier generation efficiency. In addition, there are few reports on organic photodetectors having a multiplication effect on near-infrared light, and almost all photodetectors operate under a reverse bias (anode is connected to a negative voltage), and a photodetector capable of operating under a forward bias and having a multiplication effect has not been reported yet.
Therefore, designing and fabricating an organic photodetector that can operate under forward bias while having a broad spectral response and multiplication effect would be an important addition to the type of photodetector device.
Disclosure of Invention
In view of the above existing problems, the present invention aims to provide an organic photodetector having a wide spectral response with a response range covering the ultraviolet-near infrared region and having a multiplication effect. The organic photoelectric detector has the advantages of low preparation cost, simple preparation process, excellent performance, wide application range and the like, and can be used for large-area preparation.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows: a multiplied organic photoelectric detector with wide spectral response comprises a substrate, a transparent conducting layer, an anode modification layer, a photosensitive layer, a hole blocking layer and a cathode layer which are sequentially stacked, wherein the photosensitive layer is made of a material containing an organic small molecule donor material (BODIPY) and an organic small molecule acceptor material (PC)61BM or PC71BM) from a mixture of said PC61BM is C60The PC71BM is C70A derivative of (1).
Further, the BODIPY material is selected from any one of the following structures:
Figure BDA0001720862990000021
further, PC61The BM structure is:
Figure BDA0001720862990000022
further, PC71The BM structure is:
Figure BDA0001720862990000023
furthermore, the preparation materials of the transparent electrode layer comprise various high-work-function metals, ITO and graphene.
Furthermore, the preparation material of the anode modification layer comprises poly (3, 4-ethylenedioxythiophene) -poly (styrenesulfonic acid) (PEDOT: PSS) and molybdenum oxide (M)OO3)。
Further, the preparation material of the hole blocking layer comprises C60、 C 701,3, 5-tris (1-phenyl-1H-benzimidazol-2-yl) benzene (TPBi), Ca and Mg。
Further, the preparation material of the cathode layer comprises low work function metals Al and Ag.
Further, the thickness of the transparent conducting layer is 100-150 nm; the thickness of the anode modification layer is 30-50 nm; the thickness of the photosensitive layer is 100-250 nm; the thickness of the hole blocking layer is 3-10 nm; the thickness of the cathode layer is 80-150 nm.
The invention has the beneficial effects that: the device structure and the manufacturing process of the wide spectral response multiplication type organic photoelectric detector are simple; the BODIPY organic fluorescent dye with high molar absorption coefficient and wide absorption range is added into the photosensitive layer, so that the detector has photoelectric response in a near infrared light band, and the function of wide spectral response is realized; the photoelectric detector has a multiplication effect on incident light signals, and can remarkably improve the responsivity and the detection rate of detecting light signals; the cost is low, and the preparation method can be used for large-area preparation; the method can be used for preparing flexible photoelectric detectors and has wide application range.
Drawings
FIG. 1 is a schematic diagram of the structural composition of a broad spectral response multiplication organic photodetector of the present invention;
FIG. 2 is a graph of normalized absorption spectrum of a BODIPY-1 thin film in a photosensitive layer of an organic photodetector prepared according to the present invention;
FIG. 3 is a graph of current-voltage curves of an organic photodetector prepared according to the present invention in a dark state and under illumination;
FIG. 4 is a graph of the external quantum efficiency of the organic photodetector prepared according to the present invention under-5V bias voltage as a function of the wavelength of incident light;
FIG. 5 is a graph showing the external quantum efficiency of the organic photodetector under +4.2V bias as a function of the wavelength of incident light.
The solar cell comprises a substrate 1, a transparent conducting layer 2, an anode modification layer 3, a photosensitive layer 4, a hole blocking layer 5 and a cathode layer 6.
Detailed Description
In order to make those skilled in the art better understand the technical solution of the present invention, the following further describes the technical solution of the present invention with reference to the drawings and the embodiments.
It is to be understood that the described embodiments are merely exemplary of the presently preferred embodiments of the invention. This invention may be embodied in many different forms and should not be construed as limited to the embodiments set forth herein, but rather should be construed as broadly as the present disclosure will be understood by those skilled in the art. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any inventive step, shall be considered as simple modifications of the invention, which shall fall within the scope of protection of the invention.
Since the existing photodetectors based on inorganic semiconductor materials are basically of a photovoltaic type, and the External Quantum Efficiency (EQE) does not exceed 100%, in practical applications, a complex signal amplification circuit is usually disposed in the circuit. The avalanche photodiode with the photomultiplier effect is generally prepared from an inorganic semiconductor, and has the advantages of complex manufacturing process, higher cost, higher external bias voltage during working, larger dark current and the need of working in a low-temperature environment. Although the photomultiplier has strong photoelectric response capability and large current gain and has a remarkable amplification effect on optical signals, the photomultiplier has a complex structure and a large volume, generally works under a very high voltage (the power supply voltage is generally more than 1000V), and is not beneficial to safe operation.
Many photodetectors based on organic materials do not have a photomultiplier effect, and even though some documents report a photomultiplier type photodetector, the response range is limited to a visible light region, and a photodetector having a photomultiplier effect and a photoelectric response to near infrared light has been rarely reported.
In this example we utilized a class of BODIPY-1 materials with near infrared absorption and the electron transport material PC commonly used in organic photovoltaics61BM, an organic photodetector with a wide spectral response and a photoelectric response capability in an ultraviolet to near-infrared region (300-900nm) is manufactured, the photodetector has a multiplication effect at the same time, namely the external quantum efficiency exceeds 100%, and the photodetector can also work under forward bias.
Wherein the specific structure of BODIPY-1 is as follows:
Figure BDA0001720862990000041
PC61the concrete structure of BM is:
Figure BDA0001720862990000051
the specific preparation method of the wide spectral response multiplication type organic photodetector provided by the embodiment of the invention is as follows:
(1) preparing a transparent conductive layer: firstly, cleaning a substrate, drying, and then depositing ITO on the substrate by adopting a magnetron sputtering method to form a transparent conducting layer, wherein the deposition thickness of the transparent conducting layer is 120 nm;
(2) and (3) processing the transparent conductive layer: the substrate deposited with the ITO transparent conducting layer is respectively placed into acetone and ethanol detergents for ultrasonic cleaning for 15min, then placed into a drying oven, heated to 80 ℃ to remove the detergents, so that the dryness is ensured, and then the formed ITO transparent conducting layer is treated by ultraviolet ozone plasmas to remove organic impurities on the surface of the ITO, increase the viscosity of the surface of the ITO and facilitate the formation of a subsequent anode modification layer;
(3) preparing an anode modification layer: the anode modification layer is PEDOT: the PSS film is coated on the transparent conducting layer in a spin coating mode, the spin coating time is 60s, the rotating speed is 3000rpm in the spin coating process, and finally a film layer with the thickness of 30nm is formed;
(4) and (3) processing the anode modification layer: and (3) after the anode modification layer is spin-coated, putting the anode modification layer into an oven with the temperature of 80 ℃ for baking for 30min to remove PEDOT: the solvent water in the PSS to facilitate the formation of the photosensitive layer, followed by cooling;
(5) preparation of photosensitive layer: firstly, BODIPY-1 and PC are mixed according to the proportion of 3:1061BM is dissolved in 1, 2-dichlorobenzene as a solvent to form a mixed solution, and then the formed mixed solution is coated on the anode modification layer in a spin coating mode to form a thick layerA thin film layer with a thickness of 200 nm;
(6) and (3) processing the photosensitive layer: placing the material with the photosensitive layer coated in a spin coating manner on a heating table at the temperature of 80 ℃ and baking for 30min to remove the solvent, wherein the process is carried out in a glove box filled with nitrogen atmosphere;
(7) preparation of a hole blocking layer: TPBi is plated on the upper surface of the photosensitive layer in a vacuum evaporation mode, wherein the thickness of a hole blocking layer formed by the TPBi is 3 nm;
(8) preparing a cathode layer: and evaporating Al on the upper surface of the hole blocking layer by using a vacuum evaporation method to form a cathode layer with the thickness of 100 nm.
And (3) performance characterization test:
referring to fig. 2-5, fig. 2 is a graph of normalized absorption spectrum of the BODIPY-1 film in the photosensitive layer, and it can be seen that the material absorbs light of 300-900nm in the film state, and has a wider absorption range.
FIG. 3 is a graph showing the relationship between current and voltage of the organic photodetector prepared in this example under dark state and illumination conditions, from which it can be seen that the device has a lower dark current density and a higher photocurrent density, and the dark current and the photocurrent density at-5V are 3.02 × 10-4A/cm2And 3.02X 10-1A/cm2(ii) a Dark current and photocurrent densities at +5V were 1.40X 10, respectively-2A/cm2And 1.40X 101A/cm2. The device has low dark current noise and strong light response capability.
Fig. 4 is a graph showing the variation of external quantum efficiency of the organic photodetector prepared in this example with the wavelength of incident light, and it can be seen from the graph that the external quantum efficiency of the device under reverse bias voltage is not more than 100%, and not more than 50%, indicating that no multiplication phenomenon occurs. The curve of EQE as a function of wavelength has the same trend as the absorption spectrum of BODIPY-1.
Fig. 5 is a graph showing the relationship between the external quantum efficiency of the organic photodetector prepared in this embodiment and the wavelength change of incident light under the bias voltage of +4.2V, and it can be seen from the graph that the external quantum efficiency of the detector prepared in this embodiment to near-infrared light exceeds 100% under the bias voltage of +4.2V, and the maximum external quantum efficiency exceeds 350%, so that the response capability of the detector with a wide spectrum is realized, and the organic photodetector has a photomultiplier effect.
In the embodiment of the invention, the organic photoelectric detector is made of organic semiconductor materials, so that the organic photoelectric detector with large area and low cost can be prepared on substrates made of various different materials, and meanwhile, when the substrate has a good flexible function, the organic photoelectric detector can be used for preparing a flexible photoelectric detector, so that the application scenes of the detector can be increased; meanwhile, the organic photoelectric detector has a multiplication effect on incident light signals, and the device can amplify the light signals, so that the circuit structure can be simplified in practical application, the complexity of a circuit system is reduced, and the organic photoelectric detector has great practical significance.
The foregoing illustrates and describes the principles, general features, and advantages of the present invention. However, the above description is only an example of the present invention, the technical features of the present invention are not limited thereto, and any other embodiments that can be obtained by those skilled in the art without departing from the technical solution of the present invention should be covered by the claims of the present invention.

Claims (6)

1. The multiplied organic photoelectric detector with wide spectral response is characterized by comprising a substrate, a transparent conducting layer, an anode modification layer, a photosensitive layer, a hole blocking layer and a cathode layer which are sequentially stacked, wherein the photosensitive layer is made of a BODIPY material and PC61Prepared from a mixture of BM, said PC61BM is C60A derivative of (a);
the BODIPY material has the following structure:
Figure FDA0002976251510000011
the PC61The BM structure is:
Figure FDA0002976251510000012
2. the wide spectral response multiplied organic photodetector of claim 1, wherein said transparent conductive layer is fabricated from materials including high work function metals, ITO and graphene.
3. The wide spectral response multiplied organic photodetector of claim 2, wherein said anode modifying layer is fabricated from a material comprising PEDOT: PSS and MOO3。
4. The wide spectral response multiplied organic photodetector of claim 3, wherein said hole blocking layer is formed from a material comprising C60、C70TPBi, Ca and Mg.
5. The wide spectral response multiplying organic photodetector of claim 4, wherein said cathode layer is fabricated from materials including low work function metals Al and Ag.
6. The wide spectral response multiplied organic photodetector of claim 5, wherein said transparent conductive layer has a thickness of 100 to 150 nm; the thickness of the anode modification layer is 30-50 nm; the thickness of the photosensitive layer is 100-250 nm; the thickness of the hole blocking layer is 3-10 nm; the thickness of the cathode layer is 80-150 nm.
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