• Photonics Research
  • Vol. 9, Issue 5, 781 (2021)
Tengteng Li1、†, Qingyan Li1、†, Xin Tang1, Zhiliang Chen1, Yifan Li1, Hongliang Zhao1, Silei Wang1, Xin Ding1、2, Yating Zhang1、*, and Jianquan Yao1、3
Author Affiliations
  • 1Key Laboratory of Opto-Electronics Information Technology, Ministry of Education, School of Precision Instruments and Opto-Electronics Engineering, Tianjin University, Tianjin 300072, China
  • 2e-mail: dingxin@tju.edu.cn
  • 3e-mail: jqyao@tju.edu.cn
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    DOI: 10.1364/PRJ.416580 Cite this Article Set citation alerts
    Tengteng Li, Qingyan Li, Xin Tang, Zhiliang Chen, Yifan Li, Hongliang Zhao, Silei Wang, Xin Ding, Yating Zhang, Jianquan Yao. Environment-friendly antisolvent tert-amyl alcohol modified hybrid perovskite photodetector with high responsivity[J]. Photonics Research, 2021, 9(5): 781 Copy Citation Text show less

    Abstract

    The preparation of high-quality perovskite films with optimal morphologies is important for achieving high-performance perovskite photodetectors (PPDs). An effective strategy to optimize the morphologies is to add antisolvents during the spin-coating steps. In this work, a novel environment-friendly antisolvent tert-amyl alcohol (TAA) is employed first to improve the quality of perovskite films, which can effectively regulate the formation of an intermediate phase staged in between a liquid precursor phase and a solid perovskite phase due to its moderate polarity and further promote the homogeneous nucleation and crystal growth, thus leading to the formation of high-quality perovskite films and enhanced photodetector performance. As a result, the responsivity of the PPD reaches 1.56 A/W under the illumination of 532 nm laser with the power density of 6.37 μW/cm2 at a bias voltage of -2 V, which is good responsivity for PPDs with the vertical structure and only CH3NH3PbI3 perovskite as the photosensitive material. The corresponding detectivity reaches 1.47×1012 Jones, while the linear dynamic range reaches 110 dB. These results demonstrate that our developed green antisolvent TAA has remarkable advantages for the fabrication of high-performance PPDs and can provide a reference for similar research work.

    1. INTRODUCTION

    Photodetectors (PDs) that can convert hard-to-quantify optical signals into electrical ones that can be accurately detected are of great importance for a lot of industrial and scientific applications such as imaging, optical communications, chemical/biological sensing, and environmental monitoring [16]. For PDs, the most critical is the semiconductor material, which is used to absorb the incident photons and generate effective carriers (electrons and holes) upon photo-excitation. Then, the separated electrons and holes are transferred to the cathode and anode under the action of a built-in or applied electric field to produce an electric current [7]. At present, commercially available PDs mainly use inorganic semiconductor materials, such as GaN, Si, and InGaAs [811]. PDs using such materials have the advantages of a mature and reliable preparation process and a clear working mechanism, but the disadvantages are that the preparation process is complex and expensive [12], coupled with mechanical inflexibility and high driving voltage [13], which greatly limit their application scope. In the past few years, low-cost, solution-processable optoelectronic materials, such as organic materials, nanomaterials, and nanocomposites have shown great application potential in the preparation of flexible and large-area PDs [1420], but shortcomings that cannot be ignored greatly hindered their broader applications and further development of the devices based on these materials, such as the low carrier mobility. Recently, perovskite materials have been widely used in solar cells [2124], LEDs [25,26], lasers [27], and PDs [28,29] because of their unique characteristics, such as high carrier mobility, high optical absorption coefficient, long carrier diffusion length, and adjustable direct bandgap [3032]. Perovskite PDs (PPDs) are suitable for visible light communication and imaging applications with a vertical structure because of the advantages of short carrier transmission distance, fast frequency response, and linear correlation between photocurrent and incident light intensity. Liu et al. and Sutherland et al. fabricated vertical PDs with CH3NH3PbI3 (MAPbI3) as the photosensitive layer material and obtained less-than-ideal responsivities of 0.34 A/W and 0.4 A/W under monochromatic illumination at wavelengths of 500 and 600 nm, respectively. The reasons for the unsatisfactory performance of PDs were greatly attributed to the poor morphologies of perovskite films and the defects existing on the grain boundaries and film surface. Therefore, it is important for improving the performance of PPDs to construct high-quality films with larger grain sizes, fewer grain boundaries, better crystallinity, and uniform morphologies. In order to better control the morphologies of the films, an effective method is to add antisolvents in the process of perovskite spin-coating, such as toluene, chlorobenzene, ethyl acetate, or mixed antisolvents, to regulate the formation of perovskite crystal nucleus and crystal grains growth, so as to obtain uniform and dense perovskite films without pinholes.

    In this work, tert-amyl alcohol (TAA) as a novel green antisolvent was first employed to prepare high-quality perovskite films with a smooth and mirror-like surface, which greatly improved the performance of the PPDs. Through this method, the responsivity of the PDs reached 1.56 A/W under the illumination of 532 nm laser with a power density of 6.37  μW/cm2 at a bias voltage of 2  V, which is a good responsivity we have known for PPDs with the vertical structure of glass/ITO/PEDOT:PSS/perovskite/PC61BM/BCP/Ag and only MAPbI3 perovskite as the photosensitive material. The corresponding detectivity reached 1.47×1012 Jones, while the LDR reached 110 dB. In addition, we prepared PDs using isopropanol (IPA) and n-butanol (nBA) with polarity greater than TAA and toluene (TL) and chlorobenzene (CB) with polarity less than TAA as antisolvents for comparison. Judging from the obtained results, the PDs with TAA as the antisolvent had the best performance. We supposed that these results should be attributed to the better modification-assisted selectivity characteristics of TAA with moderate polarity than that of the other antisolvents, which would effectively regulate the formation of an MAIPbI2·DMSO intermediate phase staged in between a liquid precursor phase and a solid perovskite phase and further promote the homogeneous nucleation and crystal growth in the subsequent annealing process, thus leading to the formation of high-quality perovskite films and enhanced PD performance. Moreover, it is worth noting that TAA is a green and environment-friendly antisolvent material. Compared with TL, CB, and other high-risk antisolvents, it has the advantages of low toxicity, low cost, and easy availability. These results provide a reference for the preparation of high-performance and environment-friendly PPDs in the future.

    2. EXPERIMENTAL SECTION

    A. Materials Preparation

    Poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS), lead iodide (PbI2, >99.99%), methylammonium iodide (CH3NH3I, MAI, >99.5%), phenyl-C61-butyric acid methyl ester (PC61BM, >99%), and bathocuproine (BCP, >99%) were all purchased from Xi’an Polymer Light Technology Corp., Ltd. N,N-dimethylformamide (DMF, 99.5%), dimethylsulfoxide (DMSO, 99.5%), and tert-amyl alcohol (TAA) were all purchased from Aladdin.

    B. Device Fabrication

    The prepatterned glass/ITO was first cleaned ultrasonically in the order of glass cleaner, deionized water, acetone, and isopropanol; then, the ITO glass was treated with UV-ozone for 15 min to enhance its wettability. The MAPbI3 perovskite solution was prepared by dissolving PbI2 and CH3NH3I with a molar ratio of 1:1.05 in a mixed-solvent system with DMF and DMSO at a volume ratio of 9:1. A 100 μL perovskite precursor solution was spin-coated on the ITO/PEDOT:PSS substrate at 6000 r/min for 30 s, and 250 μL TAA was slowly dropped on the wet film at about one tenth of a second during the spin-coating process; then, the film was briefly annealed at 100°C for 15 s, while the film turned black. All the spin-coating processes mentioned above were carried out in a glove box filled with nitrogen. Next, the samples were annealed in ambient air at 100°C for 15 min and then annealed at DMSO atmosphere at 100°C for 10 min. Subsequently, the chlorobenzene solution of PC61BM (20 mg/mL) and ethanol solution of BCP (0.7 mg/mL) were successively spin-coated on the perovskite film. Finally, 100 nm thick silver was evaporated as the electrode.

    C. Characterization and Measurement

    The cross-sectional images and surface morphologies of the different perovskite films were characterized using scanning electron microscopy (SEM, HITACHI SU 8020, Japan) and atomic force microscopy (AFM, CSPM5500, China). The cross-sectional EDS mapping images of different elements for each layer were characterized by a Talos F200X (FEI, America). The absorption of different antisolvent-processed perovskite films was measured by a Shimadzu UV-2600, Japan. The X-ray diffraction (XRD) measurement of perovskite films was performed by a D/MAX-2500, Japan. The steady-state and time-resolved photoluminescence spectra were recorded by a fluorescence spectrum (FLS 1000, Edinburgh Instruments, Britain). The Fourier transform infrared spectrum was recorded using the Nicolet iN10-FTIR microscope (Thermo Scientific, America). The I-V characteristics of all PDs under 405, 532, and 808 nm lasers illumination were measured using a Keithley 2400 source meter instrument.

    3. RESULTS AND DISCUSSION

    (a) Device architecture of PDs. (b) Cross-sectional SEM image of each layer in the device with a structure of (a). (c), (d) Cross-sectional EDS mapping images of different elements for each layer of the device in (a). (e) Schematic processing scheme of the antisolvent-assisted perovskite deposition process; the dashed parts are the chemical structures of antisolvents used in this work (TAA, TL, CB, nBA, and IPA).

    Figure 1.(a) Device architecture of PDs. (b) Cross-sectional SEM image of each layer in the device with a structure of (a). (c), (d) Cross-sectional EDS mapping images of different elements for each layer of the device in (a). (e) Schematic processing scheme of the antisolvent-assisted perovskite deposition process; the dashed parts are the chemical structures of antisolvents used in this work (TAA, TL, CB, nBA, and IPA).

    (a) Photograph of TAA-PSK film on ITO glass before annealing. (b) FTIR spectra of TAA-PSK films with and without annealing. (c) Photographs of different antisolvents processed films after annealing.

    Figure 2.(a) Photograph of TAA-PSK film on ITO glass before annealing. (b) FTIR spectra of TAA-PSK films with and without annealing. (c) Photographs of different antisolvents processed films after annealing.

    Energy band and charge transfer diagram of PDs.

    Figure 3.Energy band and charge transfer diagram of PDs.

    Optical properties of different antisolvent-processed films. (a) Absorption spectra. (b) XRD patterns. (c) Steady-state PL spectra; inset plots the corresponding emission peak position. (d) TRPL spectra; inset plots the values of τ1 and τ2.

    Figure 4.Optical properties of different antisolvent-processed films. (a) Absorption spectra. (b) XRD patterns. (c) Steady-state PL spectra; inset plots the corresponding emission peak position. (d) TRPL spectra; inset plots the values of τ1 and τ2.

    Morphologies of different antisolvents processed perovskite films. (a)–(e) Top-view SEM images; the scale bar is 1 μm. (f)–(j) AFM images; the scanned area is 5 μm×5 μm, and the scale bar is 1 μm. (k)–(o) Top-view SEM images; the scale bar is 5 μm.

    Figure 5.Morphologies of different antisolvents processed perovskite films. (a)–(e) Top-view SEM images; the scale bar is 1 μm. (f)–(j) AFM images; the scanned area is 5  μm×5  μm, and the scale bar is 1 μm. (k)–(o) Top-view SEM images; the scale bar is 5 μm.

    Grain-size distribution histograms of films based on (a) TAA-PSK, (b) TL-PSK, (c) CB-PSK, (d) nBA-PSK, and (e) IPA-PSK measured by SEM images with the scale bar of 1 μm.

    Figure 6.Grain-size distribution histograms of films based on (a) TAA-PSK, (b) TL-PSK, (c) CB-PSK, (d) nBA-PSK, and (e) IPA-PSK measured by SEM images with the scale bar of 1 μm.

    Electrical properties of PDs. (a) I-V characteristics of the PDs processed by different antisolvents in dark condition and the illumination of 532 nm laser with a power density of 6.37 mW/cm2. (b) I-V characteristics of the TAA-PD under the illumination of 532 nm laser with different power densities. (c) Dependences of photoresponsivity of the PDs processed by different antisolvents on the incident power density at 532 nm; VBias=−2 V. (d) Dependences of detectivity of the PDs processed by different antisolvents on the incident power density at 532 nm; VBias=−2 V. (e) Dependences of EQE of the PDs processed by different antisolvents on the incident power density at 532 nm; VBias=−2 V. (f) Dependences of photocurrent of the PDs processed by different antisolvents on the incident power density at 532 nm; VBias=0 V. The linear goodness values of the fitted curves are in brackets.

    Figure 7.Electrical properties of PDs. (a) I-V characteristics of the PDs processed by different antisolvents in dark condition and the illumination of 532 nm laser with a power density of 6.37  mW/cm2. (b) I-V characteristics of the TAA-PD under the illumination of 532 nm laser with different power densities. (c) Dependences of photoresponsivity of the PDs processed by different antisolvents on the incident power density at 532 nm; VBias=2  V. (d) Dependences of detectivity of the PDs processed by different antisolvents on the incident power density at 532 nm; VBias=2  V. (e) Dependences of EQE of the PDs processed by different antisolvents on the incident power density at 532 nm; VBias=2  V. (f) Dependences of photocurrent of the PDs processed by different antisolvents on the incident power density at 532 nm; VBias=0  V. The linear goodness values of the fitted curves are in brackets.

    Responsivity (R) as a crucial figure of merit to evaluate the performance of the PDs can be calculated by the equation [41]R=IillIdarkAEe,where Iill and Idark represent the photocurrent and dark current, respectively, A is the effective illumination area (0.04  cm2), and Ee is the power density of the incident light. Figure 7(c) plots R as a function of Ee using a double-logarithmic scale at the applied bias of 2  V. A linear dependence between log (R) and log (Ee) is observed for all of the PDs, and the values of R decrease with the increase of power density. Under a weak illumination of 6.37  μW/cm2, the TAA-PD shows the best performance with an R value of 1.56 A/W, which is a good responsivity for PDs with the same vertical structures and only MAPbI3 perovskite as the photosensitive layer. The other four control groups obtain R values of 0.46 A/W (TL-PD), 0.61 A/W (CB-PD), 0.35 A/W (nBA-PD), and 0.30 A/W (IPA-PD), respectively. The key performance parameters of this work and previously reported PDs with similar vertical structures and using MAPbI3 perovskite as the single photosensitive material are summarized in Table 2, which indicates that the TAA-PD exhibits better device performance than the reported works and the other four antisolvent-processed PDs in comparison groups of this work. In addition to the responsivity, the specific detectivity (D*) is another critical performance parameter to characterize the sensitivity of a PD and can be expressed as [48]D*=R·A2eIdark,where Idark is the dark current. As plotted in Fig. 7(d), the values of D* show linear dependence on the power density of incident light similar to the R curves. It is worth noting that the TAA-PD has a significant performance advantage over the other comparison groups in terms of the D* values. Under the illumination of 6.37  μW/cm2, the D* of TAA-PD reaches 1.47×1012 Jones, which is much higher than that of PDs processed by TL, CB, nBA, and IPA, corresponding to the D* values of 1.78×1011 Jones, 2.58×1011 Jones, 1.56×1011 Jones, and 1.48×1011 Jones, respectively. As one of the important indexes of PDs, external quantum efficiency (EQE) is often used to evaluate the efficiency of PDs to generate free carriers by absorbing photon energy and can be calculated by [49]EQE=R×hceλ×100%,where h is the Planck’s constant, c is the velocity of light, and λ represents the wavelength of incident light. In Fig. 7(e), the maximum EQE value 363.56% is obtained by TAA-PD when the power density is 6.37  μW/cm2 and the bias is 2  V. With the increase of power density, the EQE shows a linear decreasing dependence. The EQE values of PDs processed by TL, CB, nBA, and IPA are 107.98%, 140.95%, 82.63%, and 71.18% under the same conditions. The LDR is a crucial figure of merit for PDs to evaluate the detection range in which the current response is linear with the light intensity. It can be given in a logarithmic scale as [13]LDR=20logIupperIdarkIlowerIdark,where Iupper and Ilower represent the upper and lower photocurrent values at which the current response deviates from linearity, respectively. Figure 7(f) plots the LDR curves measured under the illumination of a 532 nm laser, and, with the range of light intensities from 254.78  nW/cm2 to 178.34  mW/cm2, the bias is 0 V. The corresponding LDR of TAA-PD is 110 dB, which is higher than the corresponding values of 105 dB (TL-PD), 106 dB (CB-PD), 100 dB (nBA-PD), and 91 dB (IPA-PD) in comparison groups. All of the LDR performance of these PDs is much better than that of InGaAs PDs [42].

    Performance Parameters of PPDs with Vertical Structure

    Device StructureWavelength(nm)Responsivity(A/W)Detectivity(Jones)Response Time Rise/Fall TimeReferences
    ITO/PEDOT:PSS/CH3NH3PbI3/PCBM/BCP/Al5000.879.1×1011-/26.1  μs[42]
    ITO/TiO2/PCBM/CH3NH3PbI3/P3HT/MoO3/Ag5000.344.8×1012[43]
    FTO/TiO2/AlO3/PCBM/CH3NH3PbI3/Spiro/Au/Ag6000.410121.2 μs/3.2 μs[44]
    ITO/PEDOT:PSS/CH3NH3PbI3/PCBM/Al6700.3144 μs/3 μs[45]
    ITO/PEDOT:PSS/CH3NH3PbI3/PCBM/AZO/Al7000.3[46]
    FTO/TiO2/CH3NH3PbI3/Spiro/Au6600.186.3×1010[47]
    ITO/PEDOT:PSS/CH3NH3PbI3/PCBM/BCP/Ag(TAA-PSK)5321.561.47×1012204 ns/358 nsThis work
    ITO/PEDOT:PSS/CH3NH3PbI3/PCBM/BCP/Ag(TL-PSK)5320.461.78×1011320 ns/720 nsThis work
    ITO/PEDOT:PSS/CH3NH3PbI3/PCBM/BCP/Ag(CB-PSK)5320.612.58×1011304 ns/656 nsThis work
    ITO/PEDOT:PSS/CH3NH3PbI3/PCBM/BCP/Ag(nBA-PSK)5320.351.56×1011348 ns/768 nsThis work
    ITO/PEDOT:PSS/CH3NH3PbI3/PCBM/BCP/Ag(IPA-PSK)5320.301.48×1011364 ns/744 nsThis work

    Photoswitching properties of the PDs. (a) Photoswitching characteristics of the TAA-PD measured alternately in dark and under 532 nm laser illumination (1.27 mW/cm2, VBias=0 V). (b) The switching time of the TAA-PD during one ON/OFF illumination switching cycle. (c) Photocurrent stability measurement of TAA-PD for 1000 continuous switching cycles. Photoswitching characteristics of the TAA-PD under (d) 532 nm, (e) 405 nm, and (f) 808 nm laser illumination with different power densities. (g) Photoswitching characteristics of the PDs processed by different antisolvents measured alternately in dark and under 532 nm laser illumination (1.27 mW/cm2, VBias=0 V). (h) Photoswitching characteristics of the PDs processed by different antisolvents measured alternately in dark and under 405, 532, and 808 nm laser illumination (1.27 mW/cm2, VBias=0 V), respectively. (i) Photocurrent distribution of the PDs processed by different antisolvents measured alternately in dark and under 405, 532, and 808 nm laser illumination (1.27 mW/cm2, VBias=0 V), respectively. (j) Test schematic diagram of response time.

    Figure 8.Photoswitching properties of the PDs. (a) Photoswitching characteristics of the TAA-PD measured alternately in dark and under 532 nm laser illumination (1.27  mW/cm2, VBias=0  V). (b) The switching time of the TAA-PD during one ON/OFF illumination switching cycle. (c) Photocurrent stability measurement of TAA-PD for 1000 continuous switching cycles. Photoswitching characteristics of the TAA-PD under (d) 532 nm, (e) 405 nm, and (f) 808 nm laser illumination with different power densities. (g) Photoswitching characteristics of the PDs processed by different antisolvents measured alternately in dark and under 532 nm laser illumination (1.27  mW/cm2, VBias=0  V). (h) Photoswitching characteristics of the PDs processed by different antisolvents measured alternately in dark and under 405, 532, and 808 nm laser illumination (1.27  mW/cm2, VBias=0  V), respectively. (i) Photocurrent distribution of the PDs processed by different antisolvents measured alternately in dark and under 405, 532, and 808 nm laser illumination (1.27  mW/cm2, VBias=0  V), respectively. (j) Test schematic diagram of response time.

    Electrical and photoswitching properties of TL-PD. (a) I-V characteristics under the illumination of 532 nm laser with different power densities. (b) Photoswitching characteristics measured alternately in dark and under 532 nm laser illumination (1.27 mW/cm2, VBias=0 V). (c) Switching time of the TL-PD during one ON/OFF illumination switching cycle. Photoswitching characteristics under (d) 532 nm, (e) 405 nm, and (f) 808 nm laser illumination with different power densities.

    Figure 9.Electrical and photoswitching properties of TL-PD. (a) I-V characteristics under the illumination of 532 nm laser with different power densities. (b) Photoswitching characteristics measured alternately in dark and under 532 nm laser illumination (1.27  mW/cm2, VBias=0  V). (c) Switching time of the TL-PD during one ON/OFF illumination switching cycle. Photoswitching characteristics under (d) 532 nm, (e) 405 nm, and (f) 808 nm laser illumination with different power densities.

    Electrical and photoswitching properties of CB-PD. (a) I-V characteristics under the illumination of 532 nm laser with different power densities. (b) Photoswitching characteristics measured alternately in dark and under 532 nm laser illumination (1.27 mW/cm2, VBias=0 V). (c) Switching time of the CB-PD during one ON/OFF illumination switching cycle. Photoswitching characteristics under (d) 532 nm, (e) 405 nm, and (f) 808 nm laser illumination with different power densities.

    Figure 10.Electrical and photoswitching properties of CB-PD. (a) I-V characteristics under the illumination of 532 nm laser with different power densities. (b) Photoswitching characteristics measured alternately in dark and under 532 nm laser illumination (1.27  mW/cm2, VBias=0  V). (c) Switching time of the CB-PD during one ON/OFF illumination switching cycle. Photoswitching characteristics under (d) 532 nm, (e) 405 nm, and (f) 808 nm laser illumination with different power densities.

    Electrical and photoswitching properties of nBA-PD. (a) I-V characteristics under the illumination of 532 nm laser with different power densities. (b) Photoswitching characteristics measured alternately in dark and under 532 nm laser illumination (1.27 mW/cm2, VBias=0 V). (c) Switching time of the nBA-PD during one ON/OFF illumination switching cycle. Photoswitching characteristics under (d) 532 nm, (e) 405 nm, and (f) 808 nm laser illumination with different power densities.

    Figure 11.Electrical and photoswitching properties of nBA-PD. (a) I-V characteristics under the illumination of 532 nm laser with different power densities. (b) Photoswitching characteristics measured alternately in dark and under 532 nm laser illumination (1.27  mW/cm2, VBias=0  V). (c) Switching time of the nBA-PD during one ON/OFF illumination switching cycle. Photoswitching characteristics under (d) 532 nm, (e) 405 nm, and (f) 808 nm laser illumination with different power densities.

    Electrical and photoswitching properties of IPA-PD. (a) I-V characteristics under the illumination of 532 nm laser with different power densities. (b) Photoswitching characteristics measured alternately in dark and under 532 nm laser illumination (1.27 mW/cm2, VBias=0 V). (c) Switching time of the IPA-PD during one ON/OFF illumination switching cycle. Photoswitching characteristics under (d) 532 nm, (e) 405 nm, and (f) 808 nm laser illumination with different power densities.

    Figure 12.Electrical and photoswitching properties of IPA-PD. (a) I-V characteristics under the illumination of 532 nm laser with different power densities. (b) Photoswitching characteristics measured alternately in dark and under 532 nm laser illumination (1.27  mW/cm2, VBias=0  V). (c) Switching time of the IPA-PD during one ON/OFF illumination switching cycle. Photoswitching characteristics under (d) 532 nm, (e) 405 nm, and (f) 808 nm laser illumination with different power densities.

    Meanwhile, as a control, we studied the photoswitching characteristics of the five PDs under the 532 nm laser illumination of 1.27  mW/cm2 at the bias of 0 V; the results are shown in Fig. 8(g). Compared with the other four comparison groups, TAA-PD has a more prominent photocurrent response under the same light conditions, indicating that TAA as an antisolvent to modify perovskite has great advantages compared with other antisolvents, which can effectively improve the quality of perovskite film and thus improve the photoelectric performance of the PD. In order to further understand the photoswitching characteristics of PDs, we also measured the photoresponse of the PDs under 405 and 808 nm laser illumination with a specific incident power density of 1.27  mW/cm2 and bias voltage of 0 V and compared the result with the photoresponse illuminated by 532 nm. As shown in Fig. 8(h), all PDs processed by different antisolvents have noticeable and fast photocurrent response under the illumination of three wavelengths of lasers. Remarkably, the photoswitching performance of TAA-PD under three wavelengths of illumination is significantly better than that of other comparison groups, further proving that the TAA is superior to TL, CB, nBA, and IPA in improving the performance of perovskite PDs; further, the histograms corresponding to the photocurrent response under three wavelengths of light irradiation given in Fig. 8(i)confirm this conclusion more intuitively. In addition, all PDs are more sensitive to the 532 nm laser, and the photocurrent response intensity to 405 and 808 nm light illumination decreases in turn, which is consistent with the absorption spectra in Fig. 4(a). Figure 8(j) displays the schematic diagram of the response time test system of the PDs. The pulse frequency of laser was controlled by a signal generator and was 100 kHz in this work. The pulse laser converged through lenses M1 and M2 and then illuminated to the perovskite PDs that connected to an oscilloscope with 50  Ω input resistance compensation after being restrained by an aperture diaphragm of proper size. The analog signals of response time were obtained by the oscilloscope monitoring.

    4. CONCLUSIONS

    In summary, we developed an effective solution-processed method for the fabrication of high-performance organometal trihalide PPDs. By introducing the novel and environment-friendly TAA as antisolvents for the first time, the responsivity of the PD reached 1.56 A/W under 532 nm laser illumination of 6.37  μW/cm2, which is good responsivity for PPDs with the vertical structure of glass/ITO/PEDOT:PSS/MAPbI3/PC61BM/BCP/Ag. The superior performance of the TAA-PDcompared with other PDs in the comparison groups is mainly ascribed to the better modification-assisted selectivity characteristics of TAA with moderate polarity than those of the other antisolvents, which would effectively regulate the formation of an intermediate phase staged in between a liquid precursor phase and a solid perovskite phase and further promote the homogeneous nucleation and crystal growth in the subsequent annealing process, thus leading to the formation of high-quality perovskite films and enhanced PD performance. Moreover, compared with traditional antisolvents such as TL, CB, nBA, and IPA, TAA has less toxicity, which is more beneficial for management of the environment and health in the preparation process. Together, with the characteristics of low cost and easy availability, TAA is a great environment-friendly antisolvent with remarkable advantages for the fabrication of high-performance PPDs in the future and could provide a reference for similar research work.

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