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In this work, we demonstrate the fabrication of MHP-VFETs by using two-dimensional (2D) tin halide perovskite (PEA)2SnI4 as the semiconductor layer and MXene (Ti3C2Tx) as the source electrodes. The optimized MHP-VFETs exhibit high on/off ratio up to 105 and high current density of 6 mA cm−2, which shows their promising applications as backplane TFTs. In addition, owing to the excellent optoelectronic properties of (PEA)2SnI4, the MHP-VFETs function well as high-performance phototransistors, with the responsivity of 2.1 × 103 A W−1 and a high detectivity of 7.84 × 1015 Jones. This work not only demonstrates the viability of constructing VFETs with perovskite semiconductors but also shows the promising prospects of MHP-VFETs for high-performance phototransistors.
For the VFET structure, a continuous metal source electrode would completely screen the gate electric field and result in failure in device operation. Hence, an essential requirement for VFET is that the source electrode should be perforated so that the gate electric field can penetrate into the active layer. There have been several methods for the fabrication of perforated electrodes for VFETs, such as the preparation of patterned mesh electrodes by photolithography, the deposition of ultrathin aluminum films, or spin-coating of conductive nanowires (Ag nanowires) or nanosheet films. In this study, we employed MXenes (Ti3C2Tx) nanosheets for the fabrication of perovskite VFETs because of their superior structural stability, high electrical conductivity, optical transparency, and hydrophilic surfaces. In particular, MXenes can be readily dispersed in various solvents and processed into coatable/printable inks, which can then form porous films by the simple solution process. As such, porous MXene films are very promising for usage as source electrodes of VFETs, given that they also have high electrical conductivity.15–1915. H. Kim, Z. Wang, and H. N. Alshareef, Nano Energy 60, 179 (2019). https://doi.org/10.1016/j.nanoen.2019.03.02016. Z. Liu and H. N. Alshareef, Adv. Electron. Mater. 7(9), 2100295 (2021). https://doi.org/10.1002/aelm.20210029517. B. Lyu, M. Kim, H. Jing, J. Kang, C. Qian, S. Lee, and J. H. Cho, ACS Nano 13(10), 11392 (2019). https://doi.org/10.1021/acsnano.9b0473118. H. Xu, A. Ren, J. Wu, and Z. Wang, Adv. Funct. Mater. 30(24), 2000907 (2020). https://doi.org/10.1002/adfm.20200090719. Y. Wang and Y. Wang, SmartMat 4(1), e1130 (2023). https://doi.org/10.1002/smm2.1130 In fact, Guo et al. recently demonstrated VOFETs with ultralow subthreshold swing (SS) by utilizing the 2D MXene film as the source electrode,2020. E. Li, C. Gao, R. Yu, X. Wang, L. He, Y. Hu, H. Chen, H. Chen, and T. Guo, Nat. Commun. 13(1), 2898 (2022). https://doi.org/10.1038/s41467-022-30527-w which shows the great potential of MXenes in achieving high-performance VFETs.Figure 1(a) schematically shows the structure of MXene (Ti3C2Tx), from which we see the single-layer Ti3C2Tx nanosheet consists of two carbon atoms bonded to three titanium (Ti) atoms, with the outside Ti layers terminating with functional groups (Tx), such as O, OH, and F, which are randomly distributed on the MXene surface.2121. A. Agresti, A. Pazniak, S. Pescetelli, A. Di Vito, D. Rossi, A. Pecchia, M. Auf der Maur, A. Liedl, R. Larciprete, D. V. Kuznetsov, D. Saranin, and A. Di Carlo, Nat. Mater. 18(11), 1228 (2019). https://doi.org/10.1038/s41563-019-0478-1 Figure 1(b) shows the scanning electron microscopy (SEM) images of MXene films processed from solutions with different concentrations. MXene nanosheets with size about 0.2–5 μm are stacked and form perforated MXene films. With increasing solution concentration, the MXene nanosheets are more densely packed, and so the perforated area gets reduced. The conductivity of the MXene films was measured by using the four-point probe method (see Fig. S1 for more information). As shown in Fig. 1(c), when the MXene concentration increased from 1 to 8 g l−1, the conductivity increased from 50 to 500 S cm−1. The porous feature as well as the conductive nature of the MXene films ensures their usage as source electrodes for VFETs.Among the various MHP semiconductors, two-dimensional (2D) tin halide perovskite (PEA)2SnI4 has attracted much attention due to their relatively good stability and promising prospects in high-mobility FETs.22,2322. Y. Reo, H. Zhu, J.-Y. Go, K. In Shim, A. Liu, T. Zou, H. Jung, H. Kim, J. Hong, J. Woo Han, and Y.-Y. Noh, Chem. Mater. 33(7), 2498 (2021). https://doi.org/10.1021/acs.chemmater.0c0478623. T. Matsushima, S. Hwang, A. S. Sandanayaka, C. Qin, S. Terakawa, T. Fujihara, M. Yahiro, and C. Adachi, Adv. Mater. 28(46), 10275 (2016). https://doi.org/10.1002/adma.201603126 Figure 2(a) shows the molecular structure of (PEA)2SnI4, i.e., a perfect organic–inorganic layered structure with a well-connected SnI6 octahedral cage. The bulky organic chain can effectively inhibit ion migration along the out-of-plane direction, which leads to the reduced ion-migration effect in 2D layered perovskites compared to their three-dimensional (3D) analogs.2424. H. Tsai, W. Nie, J. C. Blancon, C. C. Stoumpos, R. Asadpour, B. Harutyunyan, A. J. Neukirch, R. Verduzco, J. J. Crochet, S. Tretiak, L. Pedesseau, J. Even, M. A. Alam, G. Gupta, J. Lou, P. M. Ajayan, M. J. Bedzyk, and M. G. Kanatzidis, Nature 536(7616), 312 (2016). https://doi.org/10.1038/nature18306 Figure 2(b) shows the device structure of the MHP-VFETs, where the drain electrode, semiconductor layer, and MXene are vertically stacked, and, thus, the holes transport through (PEA)2SnI4 from the bottom MXene source electrode to the top drain electrode when a negative drain voltage is applied. The channel length is determined by the thickness of (PEA)2SnI4, which is about 80 nm according to the atomic force microscopy (AFM) results shown in Fig. S2.In order to further understand the lattice arrangement of (PEA)2SnI4 on MXene, we used x-ray diffraction (XRD) to probe the film structure. As shown in Fig. 2(c), XRD patterns of pristine and the (PEA)2SnI4 film on MXene show similar diffraction peaks, which are assigned to the strong (00 l) (l = 2, 4, 6, 8, 10, 12, and 14) diffractions at 5.5°, 10.9°, 16.4°, 21.9°, 27.4°, 33.0°, and 38.7°, respectively, suggesting that the (PEA)2SnI4 film spin-coated on MXene adopts the in-plane layered structure.3,223. Y. Liu, P. A. Chen, X. Qiu, J. Guo, J. Xia, H. Wei, H. Xie, S. Hou, M. He, X. Wang, Z. Zeng, L. Jiang, L. Liao, and Y. Hu, iScience 25(4), 104109 (2022). https://doi.org/10.1016/j.isci.2022.10410922. Y. Reo, H. Zhu, J.-Y. Go, K. In Shim, A. Liu, T. Zou, H. Jung, H. Kim, J. Hong, J. Woo Han, and Y.-Y. Noh, Chem. Mater. 33(7), 2498 (2021). https://doi.org/10.1021/acs.chemmater.0c04786 Figure 2(d) presents the topography of perovskite films on MXene characterized by scanning electron microscopy (SEM), from which we see the domain structure of (PEA)2SnI4 films, similar to that of pristine (PEA)2SnI4 films (Fig. S3), suggesting that the MXene has little influence on the morphology of (PEA)2SnI4.For the operation of VFETs, the holes are accumulated at the interface between (PEA)2SnI4 and SiO2 in the openings of MXene under negative gate voltage, resulting in energy level bending of (PEA)2SnI4 and subsequent reduction of equivalent Schottky barrier (SB) height. Consequently, carriers can tunnel from the MXene to the (PEA)2SnI4 when drain voltage is applied, leading to the on-state current of device. However, when a positive gate voltage is applied, the equivalent SB height increases, and the holes are unable to cross the potential barrier, resulting in an off-state current (see Fig. S4 for more information). Tessler et al. defined the ratio between the sum of the perforations area to the whole device area as Fill Factor (FF), which can significantly affect the current modulation of a VFET by gate voltage.2525. A. J. Ben-Sasson and N. Tessler, J. Appl. Phys. 110(4), 044501 (2011). https://doi.org/10.1063/1.3622291 In order to obtain a VFET with excellent performance, a suitable FF value is essential.2626. X. Qiu, J. Guo, P. A. Chen, K. Chen, Y. Liu, C. Ma, H. Chen, and Y. Hu, Small 17(32), 2101325 (2021). https://doi.org/10.1002/smll.202101325 Based on the aforementioned considerations, we investigated the influence of FF on the device performance of MHP-VFETs. Different MXene films were obtained by spin-coating solutions with different concentrations (1, 2, 4, and 8 g l−1) and used as the source electrodes. Figure 3(a) illustrates the transfer characteristic of the corresponding VFET devices (see more information in Fig. S5). It is observed that the on-current is gradually increased as the concentration of MXene solution increases. This is because with a higher density of MXene (lower FF), the charge injection area is larger, which leads to higher on-current. However, the off-current gets enhanced accordingly, and, finally, the devices show high off-current with weak gate modulation because the gate electric field is screened by the MXene films.2020. E. Li, C. Gao, R. Yu, X. Wang, L. He, Y. Hu, H. Chen, H. Chen, and T. Guo, Nat. Commun. 13(1), 2898 (2022). https://doi.org/10.1038/s41467-022-30527-w Notably, the currents observed in the + VGS regime for the 1 and 2 g l−1 devices are caused by gate leakage current rather than ambipolarity (see more information in Fig. S6). These results indicate that the MXene films processed from 2 g l−1 solution are optimal for the fabrication of MHP-VFETs. Indeed, we also prepared MHP-VFETs based on Ag nanowires (Ag NWs) under the same conditions, but the device did not exhibit normal transistor performance (Fig. S7). These results indicate the importance of using MXene as source electrodes for MHP-VFETs.Furthermore, we investigated the influence of the drain electrodes on device performance by using three different metals, Al, Ag, and Au, as shown in Fig. 3(b). In VOFETs, the drain contact is thought to be not as that important as the source contact. However, when gold was used as the top electrode of MHP-VFETs, the devices switched on at smaller voltage, and the on-current is much higher compared to that of the other two devices. This can be explained in terms of energy level matching, i.e., the work function of Au electrode has better match with the valence band (VB) of (PEA)2SnI4, as illustrated in Fig. 3(c).5,20,275. J. Guo, Y. Liu, P. Chen, X. Qiu, H. Wei, J. Xia, H. Chen, Z. Zeng, L. Liao, and Y. Hu, Adv. Electron. Mater. 8(7), 2200148 (2022). https://doi.org/10.1002/aelm.20220014820. E. Li, C. Gao, R. Yu, X. Wang, L. He, Y. Hu, H. Chen, H. Chen, and T. Guo, Nat. Commun. 13(1), 2898 (2022). https://doi.org/10.1038/s41467-022-30527-w27. F. Liu, L. Wang, J. Wang, F. Wang, Y. Chen, S. Zhang, H. Sun, J. Liu, G. Wang, Y. Hu, and C. Jiang, Adv. Funct. Mater. 31(1), 2005662 (2020). https://doi.org/10.1002/adfm.202005662 In principle, MXene can also be used as the drain electrode of the device. However, the integration of MXene on top of (PEA)2SnI4 by the solution process is a challenge due to the sensitivity of (PEA)2SnI4 to water and its extremely hydrophobic surface.2828. T. Matsushima, S. Terakawa, M. R. Leyden, T. Fujihara, C. Qin, and C. Adachi, J. Appl. Phys. 125(23), 235501 (2019). https://doi.org/10.1063/1.5097433Based on the aforementioned results, we obtained optimized MHP-VFETs, which show typical saturation output curves of FETs [Fig. 3(d)], with on-current being over 6 mA cm−2 (at VGS = −60 V, VDS = −60 V) and on/off ratio as high as 105 [see red curve in Fig. 3(b)]. The comparison of the transistor performance of MHP-VFETs with other reported vertical transistors is summarized in Table S1. Since there is still no established method for calculating the mobility of VFETs, we compared current density instead. It is found that the current density and on/off ratio of MHP-VFETs reported in our work are comparable or even higher than the reported values. It deserves to be mentioned that the current density of the MHP-VFETs is high enough for driving OLEDs for displays,29–3129. H. Yu, S. Ho, N. Barange, R. Larrabee, and F. So, Org. Electron. 55, 126 (2018). https://doi.org/10.1016/j.orgel.2018.01.03030. B. Chen, B. Liu, J. Zeng, H. Nie, Y. Xiong, J. Zou, H. Ning, Z. Wang, Z. Zhao, and B. Z. Tang, Adv. Funct. Mater. 28(40), 1803369 (2018). https://doi.org/10.1002/adfm.20180336931. H. Gao, J. Liu, Z. Qin, T. Wang, C. Gao, H. Dong, and W. Hu, Nanoscale 12(35), 18371 (2020). https://doi.org/10.1039/D0NR03569F suggesting the promising prospects of employing the VFET structure for the construction of MHP-FETs. However, the SS of the MHP-VFETs is about 5 V dec−1, which is not ideal. We believe this may be due to the hydrophobicity of (PEA)2SnI4, which results in poor contact with the dielectric layer interface, and thus, large SS values.11. Y. Liu, P.-A. Chen, and Y. Hu, J. Mater. Chem. C 8(47), 16691 (2020). https://doi.org/10.1039/D0TC03693E Nevertheless, the SS of the MHP-VFETs is much superior to that of planar structure MHP-FETs (see more information in Table S2). In addition, the bias-stress stability of the MHP-VFET device was evaluated, and the results show the device can operate reliably with high bias-stress stability (Fig. S8).The aforementioned results show the feasibility of achieving high current density in MHP-VFETs. In addition to this benefit, MHP-VFETs may possess advantages when they are applied as phototransistors for the following reasons: (1) MHP semiconductors intrinsically have excellent optoelectronic properties, namely, large absorption coefficient, long charge carrier lifetime, and diffusion length.32,3332. R. Ollearo, A. Caiazzo, J. Li, M. Fattori, A. van Breemen, M. M. Wienk, G. H. Gelinck, and R. A. J. Janssen, Adv. Mater. 34(40), 2205261 (2022). https://doi.org/10.1002/adma.20220526133. K. M. Yeom, S. U. Kim, M. Y. Woo, J. H. Noh, and S. H. Im, Adv. Mater. 32(51), 2002228 (2020). https://doi.org/10.1002/adma.202002228 (2) The vertical device structure with nanoscale channel length can greatly reduce the probability of dissociated charge carriers being trapped or recombined, which is beneficial to enhance the photodetection efficiency. Thus, in the following paragraphs, we investigated the photodetection performance of the MHP-VFETs.Figure 4(a) shows the absorption spectra of pristine (PEA)2SnI4 and MXene/(PEA)2SnI4 films, which almost overlap because the MXene film is thin. To understand the interfacial charge transfer properties between the (PEA)2SnI4 and MXene, time-resolved photoluminescence (TR-PL) spectra of (PEA)2SnI4 and MXene/(PEA)2SnI4 films are investigated, as shown in Fig. 4(b). A reduced lifetime of excitons is observed in the (PEA)2SnI4/MXene samples, indicating that the (PEA)2SnI4 on MXene can boost exciton dissociation efficiency, which is important to the enhancement of responsivity (see Fig. S9 for more information).3434. Y. Yan, Q. Chen, X. Wang, Y. Liu, R. Yu, C. Gao, H. Chen, and T. Guo, ACS Appl. Mater. Interfaces 13(6), 7498 (2021). https://doi.org/10.1021/acsami.0c20704 Figure 4(c) schematically describes the operating mechanism of the phototransistors. In specific, when the device is exposed to light illumination, photo-induced electron–hole pairs or excitons are generated in the (PEA)2SnI4 layer. Then, the excitons dissociate into free carriers easily because of the small binding energy between them, and this dissociation process is further enhanced due to the existence of (PEA)2SnI4/MXene interfaces. Following that, the electrons are transferred to the MXene source electrode, while the holes drift to the top drain electrode, resulting in the generation of photocurrent.To evaluate the photodetection performance of MHP-VFETs, the device was illuminated by 532 nm light with different light intensities, and the measured transfer characteristics are shown in Fig. 4(d). Obvious photoresponse was observed in the device as the transfer curves shifted significantly upon illumination. In Fig. 4(e), we show the photocurrent density (Jlight − Jdark) of the MHP-VFETs as a function of power density in the log –log scale. It is seen that the slope decreases as the gate voltage increases, which is an indication of the combined photoconductive and photo-gating effect in the devices.27,3527. F. Liu, L. Wang, J. Wang, F. Wang, Y. Chen, S. Zhang, H. Sun, J. Liu, G. Wang, Y. Hu, and C. Jiang, Adv. Funct. Mater. 31(1), 2005662 (2020). https://doi.org/10.1002/adfm.20200566235. K. Chen, X. Zhang, P. A. Chen, J. Guo, M. He, Y. Chen, X. Qiu, Y. Liu, H. Chen, Z. Zeng, X. Wang, J. Yuan, W. Ma, L. Liao, T. Q. Nguyen, and Y. Hu, Adv. Sci. 9(12), 2105856 (2022). https://doi.org/10.1002/advs.202105856 For phototransistors, the responsivity R, detectivity D*, and photosensitivity P are critical parameters. Figure 4(f) shows the values of R, D*, and P as a function of illumination density, indicating both R and D* decrease with the illumination density, while P increases with it (see Fig. S10 for the calculation of R, D*, and P and more information). Under illumination intensity of 0.001 mW cm−2, the device exhibits responsivity of 2.1 × 103 A W−1, detectivity of 7.84 × 1015 Jones, and photosensitivity of 104 (VDS = −60 V, VGS = 5 V).In addition, the transient response of MHP-VFETs was investigated by repeatedly switching on/off illumination. We see the device shows good stability during repeated cycles of measurements. Noticeably, the device could not return to its off-state immediately upon the switching off of illumination, which is likely to be caused by the trapped electrons in dielectric. This phenomenon can be minimized by applying a negative gate pulse (−40 V) as shown in Fig. 4(g), and it promises the prospects of such devices for usage as photo memory devices. Overall, the phototransistors based on the MHP-VFETs exhibit remarkably high performance, and the performance parameters stand out even if we compare them with those of the best vertical phototransistors ever reported in literatures,20,36–4120. E. Li, C. Gao, R. Yu, X. Wang, L. He, Y. Hu, H. Chen, H. Chen, and T. Guo, Nat. Commun. 13(1), 2898 (2022). https://doi.org/10.1038/s41467-022-30527-w36. K. Yeliu, J. Zhong, X. Wang, Y. Yan, Q. Chen, Y. Ye, H. Chen, and T. Guo, Org. Electron. 67, 200 (2019). https://doi.org/10.1016/j.orgel.2019.01.01837. J. Liu, K. Zhou, J. Liu, J. Zhu, Y. Zhen, H. Dong, and W. Hu, Adv. Mater. 30(44), 1803655 (2018). https://doi.org/10.1002/adma.20180365538. Y. Fang, X. Wu, S. Lan, J. Zhong, D. Sun, H. Chen, and T. Guo, ACS Appl. Mater. Interfaces 10(36), 30587 (2018). https://doi.org/10.1021/acsami.8b0662539. J. S. Kim, Y. J. Choi, H. J. Woo, J. Yang, Y. J. Song, M. S. Kang, and J. H. Cho, Adv. Funct. Mater. 27(48), 1770286 (2017). https://doi.org/10.1002/adfm.20177028640. Q. Zhang, E. Li, Y. Wang, C. Gao, C. Wang, L. Li, D. Geng, H. Chen, W. Chen, and W. Hu, Adv. Mater. 35(3), 2208600 (2023). https://doi.org/10.1002/adma.20220860041. A. Subramanian, S. Hussain, N. Din, G. Abbas, A. Shuja, W. Lei, J. Chen, Q. Khan, and K. Musselman, ACS Appl. Electron. Mater. 2(12), 3871 (2020). https://doi.org/10.1021/acsaelm.0c00707 as shown in Fig. 4(h). In spite of this, we have to point out that the performances of our MHP-VFETs are underestimated here because the top drain electrodes are not transparent. Thus, higher photodetection performance can be expected if drain electrodes are replaced by transparent ones.In summary, we have demonstrated the fabrication of MHP-VFETs via a simple solution process by using MXenes as the perforated source electrodes. The devices show high on/off ratio up to 105 and current density approaching 6 mA cm−2. Furthermore, the MHP-VFETs exhibit outstanding optoelectronic properties with a high detectivity of 7.84 × 1015 Jones and photoresponsivity of 2.1 × 103 A W−1. We believe the demonstration of MHP-VFETs may pave the way for the developments of other vertical perovskite electronic and optoelectronic devices and circuits, which, thus, in turn, serve as a versatile platform for fundamental studies in this field.
The author acknowledges the National Key Research and Development Program (Nos. 2022YFB3603802 and 2021YFA1200700), the National Natural Science Foundation of China (Nos. 62222403, 62074054, and U21A20497), the Natural Science Foundation of Hunan Province (Nos. 2022JJ10019, 2019GK2245, and 2020JJ1002), and the Shenzhen Science and Technology Innovation Commission (No. RCYX20200714114537036) for financial support.
Conflict of Interest
The authors have no conflicts to disclose.
Author Contributions
Haihong Xie: Writing – original draft (lead). Yuanyuan Hu: Investigation (equal); Resources (equal); Supervision (equal); Writing – original draft (equal); Writing – review & editing (equal). Ping-An Chen: Investigation (supporting). Xincan Qiu: Investigation (equal). Yu Liu: Investigation (supporting). Jiangnan Xia: Investigation (supporting). Jing Guo: Investigation (supporting). Huan Wei: Investigation (supporting). Zhenqi Gong: Investigation (supporting). Jiaqi Ding: Investigation (supporting).
The data that support the findings of this study are available from the corresponding author upon reasonable request.
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