† Corresponding author. E-mail:
Project supported by the National Natural Science Foundation of China (Grant No. 61874029) and the National Key Technologies R&D Program of China (Grant No. 2015ZX02102-003).
Photodetectors based on amorphous InGaZnO (a-IGZO) thin film transistor (TFT) and halide perovskites have attracted attention in recent years. However, such a stack assembly of a halide perovskite layer/an a-IGZO channel, even with an organic semiconductor film inserted between them, easily has a very limited photoresponsivity. In this article, we investigate photoresponsive characteristics of TFTs by using CsPbX3 (X = Br or I) quantum dots (QDs) embedded into the a-IGZO channel, and attain a high photoresponsivity over 103A⋅W−1, an excellent detectivity in the order of 1016 Jones, and a light-to-dark current ratio up to 105 under visible lights. This should be mainly attributed to the improved transfer efficiency of photoelectrons from the QDs to the a-IGZO channel. Moreover, spectrally selective photodetection is demonstrated by introducing halide perovskite QDs with different bandgaps. Thus, this work provides a novel strategy of device structure optimization for significantly improving the photoresponsive characteristics of TFT photodetectors.
Amorphous In–Ga–Zn–O (a-IGZO) thin-film transistors (TFTs) exhibit high field effect mobility, excellent electrical uniformity, flexibility, and low-temperature process, and thus have been extensively investigated in display panels, flexible electronics, and UV detectors.[1–8] However, with respect to detections of visible lights, the a-IGZO TFTs often show limited responsivity because of a rather wide bandgap larger than 3 eV in a-IGZO.[1,2] To achieve significantly improved visible light detections, various light-absorbing materials have been introduced into the devices, including organic semiconductor,[9–13] two-dimensional materials,[14,15] inorganic quantum dots (QDs),[16–19] and halide perovskites.[20–30] Among them, the halide perovskites are of great interest due to their strong light absorption, long carrier diffusion length, low-cost process, high charge carrier mobility, and tunable bandgaps (∼ 1.7–3.2 eV).[31–37] Therefore, the concept of a-IGZO/perovskite hybrid-based photodetectors has been proposed in recent years, and presents enhanced photosensitive performance.[20–24,26]
So far, the reported a-IGZO/perovskite hybrid-based photodetectors include two different device structures, i.e., a-IGZO-covered perovskite channel devices and perovskite-covered a-IGZO channel ones.[20–24,26] The former, in which perovskite nanowires are sandwiched between a-IGZO and gate dielectric, cannot operate like a transistor because of the gate field shielding effect. The latter with perovskite films or QDs on the back side of the a-IGZO channel can maintain relatively high field-effect mobility, however, their photo-responsiveness is still rather limited.[20–24,26]
In this work, we propose a hybrid channel consisting of inorganic halide perovskite (IHP) QDs embedded in the a-IGZO film for TFT photodetector applications, which is inspired by the rather good stabilities and high photoluminescence quantum yields of the IHP QDs.[33–35,38–43] Therefore, the fabricated devices exhibit superior photodetecting performance, including high photoresponsivity, excellent detectivity, and so on. In particular, tunable spectrally-selective photodetections of the devices are realized by introducing different bandgap QDs, and the underlying mechanisms are also discussed.[44,45]
The IHP QDs solution was synthesized at room temperature according to the method reported by Li et al.[46] Firstly, 0.1 mmol PbBr2 and 0.1 mmol CsBr were dissolved in 2.5 mL dimethylformamide (DMF) in atmosphere. Oleic acid (OA, 0.25 mL) and oleylamine (OAm, 0.125 mL) were added to stabilize the precursor solution, then stirred till a transparent solution. Next, 1 mL of the mixture was quickly added to toluene (10 mL) during stirring. In order to obtain pure products, the CsPbBr3 QDs precursor solution was added into 30 mL methyl acetate and centrifuged at 8000 rpm for 2 min. Finally, the precipitate CsPbBr3 QDs were dispersed in n-hexane for further use.
The CsPbI3 QDs solution was obtained though the displacement reaction of CsPbBr3 QDs and PbI2 solution. Firstly, 0.4 mmol PbI2 was dissolved into 10 mL n-dodecane with 1 mL OA and 0.5 mL OAm, and was stirred till a transparent solution. Then, the PbI2 solution and the above prepared CsPbBr3 QDs solution were mixed in the same volume ratio, and the color change from green to red could be observed. The method of purification was the same as that for the CsPbBr3 QDs solution.
For the hybrid device fabrications, 80 nm Al2O3 gate dielectrics were deposited by atomic layer deposition using trimethylaluminum (TMA) and O2 plasma as precursors on the highly doped p-type silicon wafers (< 0.0015 ω ⋅cm) at room temperature.[47] Next, 20 nm a-IGZO films were deposited on the top of Al2O3 by radio frequency (RF) sputtering using an InGaZnO4 ceramic target. Subsequently, different light absorption layers were prepared as following: the CsPbBr3 or CsPbI3 QDs solution was coated on the surface of the a-IGZO films by spin coating at 1000 rpm for 30 s, followed by drying at room temperature for 24 h in N2. Then, 20 nm a-IGZO films were deposited on the top of the light absorption layers of the QDs as aforementioned. Finally, 30 nm Ti/70 nm Au bilayer electrodes were prepared by electron beam evaporation and a lift-off method. The channel length and width were 10 μm and 40 μm, respectively. A control device (i.e., a-IGZO TFT) employed a single a-IGZO channel, and the other components were the same as mentioned above.
UV–visible absorption spectra were measured on a UV–visible spectrophotometer (Lambda 750). Photoluminescence (PL) spectra were recorded by a spectrophotometer (F-320, Tianjin Gangdong Sci.&Tech. Co., Ltd). The x-ray diffraction (XRD) of the IHP QDs was collected by an x-ray diffractometer (Bruker Advance D8) with Cu Kα radiation (1.54 Å) at 40 kV. The transmission electron microscopy (TEM) image and the surface morphologies of the IHP QDs films were observed by FEI Talos F200X and an atomic force microscope (AFM, Bruker Icon), respectively. The monochromatic lights of different wavelengths were provided by a xenon arc lamp filtered with a double grating monochromator (Omno 330150, Beijing NBeT, China). The electrical characteristics of the photodetectors were measured by an Agilent B1500A semiconductor device analyzer at room temperature in atmosphere.
Figure
Figure
The transfer curves of both the CsPbX3-based hybrid TFTs are further measured as a function of power density under 530 nm and 630 nm lights, respectively, as shown in Fig.
Further, the light power density-dependent threshold voltage (VT) shifts and field effect mobility (μ) are compared between the CsPbBr3- and CsPbI3-based hybrid TFTs, as displayed in Figs.
In order to well evaluate the photosensitive characteristics of the TFT photodetectors, both photoresponsivity (R) and detectivity (D*) are introduced, which can be calculated as[39,50,51]
Moreover, the transient response of the a-IGZO/CsPbBr3 QDs hybrid TFTs to a switching light (λ = 500 nm) was investigated, as shown in Fig.
Finally, the photoresponse mechanisms of the IHP QDs-based hybrid TFTs under different lights are expressed by schematic diagrams of energy band, as shown in Fig.
Table
Photodetectors based on a-IGZO TFT embedded with IHP QDs in the channel were successfully fabricated in this work, which exhibit excellent photosensitive performance with a photoresponsivity over 103 A⋅W−1, an Iphoto/Idark of 105, and a detectivity in the order of 1016 to visible light. The enhanced photoresponsivity, as compared with those of previously reported a-IGZO/perovskite hybrid devices, is mainly attributed to a higher transfer efficiency of the photoelectrons from the perovskite QDs to the effective channel region, as well as the amplifier function of the TFT. Moreover, the CsPbBr3 and CsPbI3 QDs embedded a-IGZO TFTs exhibit different wavelength-responsive cutoffs of 550 nm and 700 nm, respectively, indicating tunable spectrally selective photodetections. By optimizing the device structure, this work provides a novel strategy for further improving the performance of a-IGZO/perovskite hybrid photodetectors.
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