CN111048669B - Bionic near-infrared response enhanced photoelectric detector and preparation method thereof - Google Patents

Bionic near-infrared response enhanced photoelectric detector and preparation method thereof Download PDF

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CN111048669B
CN111048669B CN201911193443.6A CN201911193443A CN111048669B CN 111048669 B CN111048669 B CN 111048669B CN 201911193443 A CN201911193443 A CN 201911193443A CN 111048669 B CN111048669 B CN 111048669B
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CN111048669A (en
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徐晓宝
刘贤浩
曹菲
邹友生
曾海波
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Nanjing University of Science and Technology
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Abstract

The invention discloses a bionic near-infrared response enhanced photoelectric detector. The detector is composed of two parts, a micro-cavity structure simulating a butterfly compound eye is arranged as a detector top layer and is a micro-cavity composed of dielectric medium layers, and the bottom layer adopts inorganic halide perovskite prepared by thin film engineering as a device of an optical active layer, so that selective photoresponse in a near-infrared biological window is realized. The invention builds the LiF/NPB artificial optical microcavity by simulating the compound eye of the butterfly, and has the advantages of narrow-band response with the half-peak width less than 50nm and tunability of covering a near-infrared band. By selecting the inorganic halide perovskite CsPb0.5Sn0.5I3 as the photoactive layer of the bottom device, the composite material has comprehensive band gap and film engineering characteristics, and has good comprehensive performance such as high response speed, high resolution, low detection limit and the like in real-time imaging application compared with a common photoelectric detector.

Description

Bionic near-infrared response enhanced photoelectric detector and preparation method thereof
Technical Field
The invention relates to a bionic near-infrared response enhanced photoelectric detector and a preparation method thereof, belonging to the technical field of photoelectric detection.
Background
Near infrared photodetectors (NIR-PDS) have attracted considerable attention in recent decades due to their great potential in medical instrumentation. Hemoglobin, tissue and lipids account for the major absorption of visible light from 540nm to 700nm, whereas water has a significant absorption of photons with wavelengths greater than 900nm, as opposed to the range where the optical signal is strongly transmitted in vivo from 700nm to 900nm, and is therefore encoded as the "optical window" for in vivo imaging. (S.Luo, E.Zhang, Y.Su, T.Cheng, C.Shi, Biomaterials 2011,32,7127 and 7138.) the detection and imaging of fluorescence photons in this range has been considered a powerful real-time technique for medical diagnosis, surgery or treatment.
The realization of near infrared band photon sensing mainly depends on inorganic narrow bandgap materials. For example, gallium arsenide, silicon, lead selenide, and indium gallium arsenide have been widely studied as photoactive layers for near infrared photodetectors. However, the preparation process of these inorganic narrow bandgap materials includes alloying, doping, etching, epitaxy, etc., which is very complicated and expensive. (M.Garcia, C.Edmeison, T.York, R.Marinov, S.Mondal, N.Zhu, G.P.Sudlow, W.J.Akers, J.Margenthaller, S.Achileff, R.Liang, M.A.Zayed, M.Y.Pepino, V.Gruev, Optica 2018,5,413-422) worse, when both the excitation and fluorescence photons are within a narrow near infrared spectrum, the broadband response determined by the band gap in these near infrared spectra makes them unable to selectively sense the characteristic fluorescence of the near infrared spectrum, since the noise of the excitation photons cannot be effectively rejected. (R.Yousefi, M.R.Mahmoudian, A.Sa' aedi, M.Cheraghizade, F.Jamali-Sheini, M.Azarang, Ceram. int.2016,42,15209-
Disclosure of Invention
The invention aims to provide a near infrared photoelectric detector applied to a biological window. The structure in the butterfly compound eye is simulated and used for a bionic near-infrared response enhanced photoelectric detector. By constructing a micro-cavity formed by bionic dielectric medium layers and adopting inorganic halide perovskite prepared by thin film engineering as an optical active layer, the near-infrared selective optical response detection and the enhancement of near-infrared detection response applied to a biological window are realized.
A preparation method of a bionic near-infrared response enhanced photoelectric detector comprises the following steps:
alternately evaporating multiple LiF/NPB layers to the non-ITO surface of the ITO glass sheet in a positive and negative way, and building an optical microcavity;
the other side of the glass sheet was used as a substrate, CsPb 0.5 Sn 0.5 I 3 The solution is used as a precursor of a light activity layer of the photoelectric detection device, and the photoelectric detection device is prepared by spin coating.
Further, in step 1), the optical microcavity is formed by alternating LiF/NPB layers, the optical thickness of each layer is one n times of the target wavelength, n is a positive number greater than 0, the optical microcavity is formed by alternating m layers of LiF/NPB layers, m is a positive number greater than 0, and the LiF/NPB layers are alternately evaporated on the glass sheet in a positive and negative manner.
Further, the molar ratio of Cs, Pb, Sn and I adopted in the step 2) is 1: 0.5: 0.5: 3.
further, the target wavelength is a near infrared wavelength.
Further, the refractive index of LiF was 1.33 and the refractive index of NPB was 2.1.
The bionic near-infrared response enhanced photoelectric detector prepared by the method simulates a micro-cavity structure of a butterfly compound eye, is arranged as the top layer of the detector and is an optical micro-cavity consisting of dielectric medium layers; the bottom layer adopts inorganic halide perovskite prepared by thin film engineering as a device of a light active layer.
Compared with the prior art, the invention has the following advantages: the invention builds up LiF/NPB artificial optical microcavity and selects inorganic halide perovskite CsPb 0.5 Sn 0.5 I 3 As a light active layer, the strong selectivity of the bionic optical microcavity in the near infrared band and CsPb are utilized 0.5 Sn 0.5 I 3 Reasonable band structure and characteristics of the active layer: 1) the tunable filter has the advantages of narrow-band response with the half-peak width less than 50nm and tunability covering near-infrared bands, and has signal selectivity; 2) compared with a common photoelectric detector, the photoelectric detector has good comprehensive performance such as high response speed, high resolution, low detection limit and the like in real-time imaging application; 3) the array is easy to manufacture.
Drawings
FIG. 1 is a microscopic structure of a butterfly fly's eye.
Fig. 2a is an SEM image of a photodetection cross section of the present invention, fig. 2b is a schematic structural view of an optical microcavity, and fig. 2c is a schematic structural view of a photodetector of the present invention.
Fig. 3 is a simulation diagram of the optical field distribution in the tunable optical microcavity of the present invention.
FIG. 4 is a transmission spectrum obtained from a simulation of a tunable optical microcavity in accordance with the present invention.
FIG. 5 is an image of the external quantum efficiency of a biomimetic photodetector for a particular near infrared photon at zero bias in the present invention.
FIG. 6 is a graph showing the detection rate of three bionic photoelectric detectors PD-1, PD-2 and PD-3 in the invention.
Detailed Description
The invention is further described below by means of specific examples.
The invention provides a bionic near-infrared response enhanced photoelectric detector and a preparation method thereof. The compound eye of the butterfly (see fig. 1) has a number of alternating layers of air and cellular material proximal to the striated muscle of each microspore, which act as optical microcavities, selectively allowing photons of a particular wavelength. We have simulated this structure in butterfly compound eye and designed bionic CsPb 0.5 Sn 0.5 I 3 A photodetector (see fig. 2a, 2 c). The optical microcavity consists of two parts, an optical microcavity is built at the top (as shown in fig. 2b), the optical microcavity consists of alternating LiF (d is 1.33, d is refractive index)/NPB (N, N '-bis (naphthalene-1-yl) -N, N' -bis (phenyl) benzidine, and d is 2.1), and the peak wavelength of transmitted light is adjusted between 700nm and 900nm by adjusting the thickness of a dielectric medium. The bottom is based on CsPb 0.5 Sn 0.5 I 3 The solution is used as a precursor, and is prepared into an optical activity layer of the photoelectric detector through spin coating, so that the photoelectric detector is prepared. The optical microcavity is used for realizing the selection of near infrared light, and the device generates an electric signal after being excited by the near infrared light, so that the enhancement of the near infrared selective light response detection and the near infrared detection response applied to the biological window is realized.
Example 1
In this example, we fabricated a biomimetic photodetector. An optical microcavity based on alternating LiF (d 1.33, d is refractive index)/NPB (N, N '-bis (naphthalene-1-yl) -N, N' -bis (phenyl) benzidine) layers is built on the top, and CsPb is arranged on the bottom 0.5 Sn 0.5 I 3 The photoelectric device with the solution as the precursor of the photoactivation layer specifically comprises the following steps:
(1) and (3) sequentially carrying out ultrasonic cleaning on the ITO glass sheet for 10 minutes by using a detergent, deionized water, acetone and isopropanol.
(2) The substrate was dried with a nitrogen stream and treated with uv-ozone for 20 minutes.
(3) Optical microcavities were prepared on the glass side. The optical microcavity consists of alternating LiF (d is 1.33, d is refractive index)/NPB (n, n '-bis (naphthalene-1-yl) -n, n' -bis (phenyl) benzidine), and d is 2.1), evaporation is carried out by an optical film coater, the thickness of each layer is adjusted to be 200nm, LiF/NPB structural layers are overlapped on the glass surface in seven pairs alternately in a positive and negative mode, and the optical microcavity PD-1 with the projection peak of 800nm is prepared.
(4) The PEDOT: PSS (AL 4083) solution was spin-coated on clean ITO glass at 5000 rpm for 30 seconds and annealed in air at 150 ℃ for 10 minutes.
(5) Preparation of CsPb 0.5 Sn 0.5 I 3 In the case of perovskite precursor solution, CsI (259.8mg) and PbI are added 2 (230.5mg)、SnI 2 (186mg) and SnF 2 (8mg) was dissolved in a mixed solvent of dimethylformamide (DMF; 700. mu.l) and dimethyl sulfoxide (DMSO; 300. mu.l).
(6) 35 μ l of the perovskite precursor was dipped on a PEDOT: PSS layer and spin coated in a glove box at 5000 rpm for 35 s. Toluene (700. mu.l) was added dropwise to the substrate at 10 seconds. The perovskite thin film is annealed for 3min at 100 ℃.
(7) PCBM solution (20mg/ml in chlorobenzene) was then spin coated onto the perovskite film at 2000 rpm for 30 seconds. Finally, under high vacuum: (<2×10 -6 torr) a silver electrode with a thickness of 120nm was evaporated.
Based on the structure of the optical microcavity, fig. 3 shows a simulation of the optical field distribution in the proposed tunable microcavity, and fig. 4 shows its projection spectrum, which clearly shows the selectivity and compatibility of the optical microcavity with respect to near-infrared light, with a narrowing of the transmission spectrum in this microcavity. Figure 5 shows the External Quantum Efficiency (EQE) of a biomimetic PDS prepared at zero bias for a specific near infrared photon, which shows that the 10 response spectra in the near infrared range effectively narrow to a unimodal line (FWHM <25 nm). In biomedical fluorescence imaging, a narrow response to near infrared photons is desirable, which ensures efficient discrimination of near infrared fluorescence from excitation photons.
As shown in FIG. 6, the peak detection rate (d;) of PD-1 was 5.25X 10 14 jones. These values are comparable to the values of the high sensitivity commercial silicon PDS, indicating its potential for weak light sensing.
Example 2
Similar to example 1, except that the thickness of each layer (LiF/NPB) of the optical microcavity in step (1) of example 1 was changed to 213nm, and the other conditions were kept the same, the biomimetic photodetector PD-2 was prepared. The simulation of the optical field distribution in the optical microcavity of the bionic photoelectric device based on the optical microcavity is shown in fig. 3, the projection spectrogram is shown in fig. 4, the external quantum efficiency is shown in fig. 5, the detection rate is shown in fig. 6, the projection peak of the bionic optical detector is 850nm, and the bionic optical detector has the characteristics of strong near infrared light selectivity, high response speed, high resolution and low detection limit.
Example 3
Similar to example 1, except that the thickness of each layer (LiF/NPB) of the optical microcavity in step (1) of example 1 was changed to 225nm, and the other conditions were kept the same, a biomimetic photodetector PD-3 was prepared. The simulation of the optical field distribution in the optical microcavity of the bionic photoelectric device based on the optical microcavity is shown in fig. 3, the projection spectrogram is shown in fig. 4, the external quantum efficiency is shown in fig. 5, the detection rate is shown in fig. 6, the projection peak of the bionic optical detector is 900nm, and the bionic optical detector has the characteristics of strong near infrared light selectivity, high response speed, high resolution and low detection limit.
Example 4
Similar to example 1, except that the number of layers of the optical microcavity in step (1) in example 1 is changed to 5, and other conditions are kept consistent, the detection performance of the bionic photodetector based on the optical microcavity is consistent with that in example 1.
Example 5
Similar to example 1, except that the number of layers of the optical microcavity in step (1) in example 1 is changed to 6, and other conditions are kept consistent, the detection performance of the bionic photodetector based on the optical microcavity is consistent with that of example 1.
Example 6
Similar to example 1, except that the number of layers of the optical microcavity in step (1) in example 1 is changed to 8 layers, and other conditions are kept consistent, the detection performance of the bionic photodetector based on the optical microcavity is consistent with that of example 1.
Example 7
Similar to example 1, except that the number of layers of the optical microcavity in step (1) in example 1 is changed to 9, and other conditions are kept consistent, the detection performance of the bionic photodetector based on the optical microcavity is consistent with that in example 1.
Comparative example 1
Similar to example 1, the difference is that the number of layers of the optical microcavity in step (1) in example 1 is changed to 4 layers, and other conditions are kept consistent, and the bionic photodetector based on the optical microcavity has too strong light transmittance and cannot have good selectivity for the near-infrared band.
Comparative example 2
Similar to example 1, the difference is that the number of layers of the optical microcavity in step (1) in example 1 is changed to 10, and other conditions are kept consistent, and the bionic photodetector based on the optical microcavity has too weak light transmittance and cannot have good selectivity for the near-infrared band.
Comparative example 3
Similar to example 1, the difference is that the evaporation mode of the optical microcavity in step (1) in example 1 is changed from alternating positive and negative LiF/NPB layers to repeated LiF/NPB layers, other conditions are kept consistent, and the bionic photodetector based on the optical microcavity has no good selectivity for the near-infrared band.
Comparative example 4
Similar to example 1, the difference is that the evaporation method of the optical microcavity in step (1) of example 1 is changed from alternating positive and negative LiF/NPB layers to a single LiF layer, and other conditions are consistent, and the bionic photodetector based on the optical microcavity has no good selection capability for the near-infrared band.
Comparative example 5
Similar to example 1, the difference is that the evaporation method of the optical microcavity in step (1) of example 1 is changed from alternating positive and negative LiF/NPB layers to a single NPB layer, and other conditions are consistent, and the bionic photodetector based on the optical microcavity has no good selection capability for the near-infrared band.
The above description is only an embodiment of the present invention, and is not intended to limit the scope of the present invention, and all modifications and equivalents of the structure and flow diagrams described in the present specification and drawings can be used directly or indirectly in other related fields, and are intended to be included within the scope of the present invention.

Claims (8)

1. A preparation method of a bionic near-infrared response enhanced photoelectric detector is characterized by comprising the following steps:
1) alternately evaporating multiple LiF/NPB layers to the non-ITO surface of the ITO glass sheet in a positive and negative way, and building an optical microcavity;
2) the other side of the glass sheet was used as a substrate, CsPb 0.5 Sn 0.5 I 3 The solution is used as a precursor of a light activity layer of the photoelectric detection device, and the photoelectric detection device is prepared by spin coating.
2. The method according to claim 1, wherein in step 1), the optical microcavity is formed by alternating LiF/NPB layers, each layer has an optical thickness of n times of a target wavelength, n is a positive number greater than 0, the optical microcavity is formed by alternating m layers of LiF/NPB, m is a positive number greater than 0, and the LiF/NPB layers are alternately evaporated on the glass sheet in a positive and negative manner.
3. The method for preparing a bionic near-infrared response-enhanced photodetector as claimed in claim 1, wherein the molar ratio of Cs, Pb, Sn and I adopted in the step 2) is 1: 0.5: 0.5: 3.
4. the method of claim 2, wherein the target wavelength is near infrared wavelength.
5. The method of claim 1, wherein the refractive index of LiF is 1.33 and the refractive index of NPB is 2.1.
6. A bionic near-infrared response enhanced photoelectric detector is characterized by comprising a micro-cavity structure simulating a butterfly compound eye, an optical micro-cavity, a first optical micro-cavity and a second optical micro-cavity, wherein the micro-cavity structure is arranged as a detector top layer and is composed of dielectric medium layers; the bottom layer adopts inorganic halide perovskite prepared by thin film engineering as a device of a light active layer; the optical microcavity is composed of alternating LiF/NPB layers, the optical thickness of each layer is one n times of the target wavelength, n is a positive number larger than 0, the optical microcavity is composed of alternating m LiF/NPB layers, m is a positive number larger than 0, and the LiF/NPB layers are alternately evaporated on a glass sheet in a positive and negative way; the inorganic halide perovskite is CsPb 0.5 Sn 0.5 I 3 。
7. The biomimetic near-infrared response enhanced photodetector of claim 6, wherein the target wavelength is a near-infrared wavelength.
8. The biomimetic near infrared response enhanced photodetector of claim 6, wherein the refractive index for LiF is 1.33 and the refractive index for NPB is 2.1.
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