We fabricate our MAPbCl
3/GaN PD and the control single-layer at the optimal concentration (2M) of the precursor solution of MAPbCl
3. The concentration of the precursor solution, as well as the thickness of the MAPbCl
3 film deposited on the GaN surface, is initially optimized to minimize the dark current level and maximize the light current level.
Figure S3a,b, respectively, compares the dark current and photocurrent levels of MAPbCl
3/GaN and control PDs with different concentrations of MAPbCl
3 precursor. The thickness of the MAPbCl
3 layer increases with the precursor concentration, to suppress the dark current of the MAPbCl
3/GaN PD. The photocurrent of MAPbCl
3/GaN PD reaches the maximum for precursor concentrations above 1 M. To maximize the light over dark on/off ratio, the optimal concentration to deposit the MAPbCl
3 film is chosen as 2M. The optimal thickness of the MAPbCl
3 film is measured to be around 516 nm by cross-sectional SEM, as shown in
Figure S4.
Figure 1d shows the comparison of the typical current–voltage (
I–
V) characteristics of the MAPbCl
3/GaN PD and the corresponding control devices under dark and 365 nm light illumination. Unlike the MAPbCl
3 PD with a low dark/light current level and the GaN PD with a high dark/light current level, the dark current of MAPbCl
3/GaN PD is about 4 orders of magnitude suppressed compared with the one of GaN PD, while the light current is increased by more than 300 times compared to the MAPbCl
3 PD. The significantly enhanced light over dark on/off ratio of MAPbCl
3/GaN PD cannot be only attributed to the optimized MAPbCl
3 film quality on the GaN surface, as the charge transfer properties of the MAPbCl
3/GaN PD are also very different from those of the control devices.
Figure 1e shows the linear-scale
I–
V curves of our MAPbCl
3/GaN PD under different illumination levels. Under both negative and positive bias, the photocurrents of the heterogeneous device sharply increase below the 0.5 V range and then saturate above the 0.5 V range. Moreover, the saturated photocurrent of MAPbCl
3/GaN PD increases linearly with the light intensity, which is highly similar to the characteristic output curves of a BJT with common emitter configuration.
(32) As shown in
Figure 1f, the bias is applied on the lateral electrodes of the heterogeneous device (as emitter and collector, respectively) for photocurrent collection, with the optical pump on the GaN film as the base terminal to inject the photogenerated carriers. The linear-scale
I–
V curves of our MAPbCl
3/GaN PD and the control devices under dark conditions are also compared in
Figure S5. It is clearly shown that the MAPbCl
3 film forms an Ohmic contact and the GaN film forms a Schottky contact with the gold electrodes. The saturated trend can still be observed in the dark current of MAPbCl
3/GaN PD, which confirms that the electric field is applied on the heterostacked layers.
With the comparisons of the dark and light
I–
V characteristics between the heterogeneous and single-layer devices, we can summarize that the MAPbCl
3/GaN heterointerface plays an important role in the photocurrent generation, as schematically illustrated by the photocarrier dynamics model in
Figure 1f. At 365 nm, the GaN film contributes the most photogenerated carriers, with a large absorption coefficient and bottom-illumination scheme. The electron–hole pairs generated in the GaN film diffuse to the MAPbCl
3/GaN interface, and are then separated by the heterojunction and extracted by MAPbCl
3 and the electrodes. That is, the photocurrent flows through the perovskite and GaN layers dominate the photoresponse of our MAPbCl
3/GaN PD. We further measured the
I–
V curves of one MAPbCl
3/GaN device with a discontinuous (split in the middle of the electrodes) perovskite film under 365 nm illumination, as shown in
Figure S6. Even the perovskite film covering the GaN film is discontinuous; a similar output characteristic curve can still be obtained as the continuous one.
The photosensing mechanism of the heterogeneous device is further investigated under 395 nm illumination, with the
I–
V characteristics comparison shown in
Figure 1g. The corresponding linear-scale
I–
V curves of the MAPbCl
3/GaN PD under different illumination levels are shown in
Figure 1h, with a similar saturated photocurrent output. Especially, although the GaN layer has no photoresponse at 395 nm, the photocurrent of MAPbCl
3/GaN PD increases by more than 300 times compared with the one of the control MAPbCl
3 PD. This indicates that the MAPbCl
3/GaN heterointerface facilitates the photocurrent generation with efficient electron–hole pair separation and higher carrier mobility in the GaN layer, while the single-layer MAPbCl
3 PD suffers from a large charge carrier recombination loss. As schematically illustrated by the photocarrier dynamics model in
Figure 1i, the electron–hole pairs generated in the perovskite film tend to diffuse to the MAPbCl
3/GaN interface and are separated by the heterojunction and extracted by the electrodes. Therefore, the photocurrent flows through the perovskite and GaN layers dominate the photoresponse, even though the light is only absorbed by the perovskite film.