Charge-transport-layer-free 2D/3D perovskite photodetector with high performance and stability

doi:10.1016/j.jmst.2026.01.028

Abstract

Abstract: Perovskite photodetectors (PPDs) without charge transport layers (CTLs) have recently garnered significant attention due to the limitations associated with organic and inorganic CTLs in conventional vertically structured PPDs. However, CTL-free PPDs reported so far have suffered from poor performance and stability, primarily due to charge extraction losses, non-radiative recombination at interfaces, and surface degradation caused by air and moisture. In this study, we propose a self-powered CTL-free PPD based on 2D/3D perovskite heterojunction to address these challenges. We demonstrate CTL-free 2D/3D PPDs featuring a metal electrode/2D perovskite/3D perovskite/transparent conducting oxide (TCO) structure, in which the 2D perovskite layer is derived from n-hexyl trimethyl ammonium bromide (HTABr). Our CTL-free 2D/3D PPDs exhibit markedly improved photoresponse properties compared to 3D-only PPDs, attributable to surface passivation and enhanced charge extraction facilitated by the 2D perovskite layer. Notably, the CTL-free 2D/3D PPD exhibits comparable performance to conventional CTL-based 3D PPD (metal electrode/CTL/3D perovskite/CTL/TCO), with a faster response time and improved long-term stability. To gain deeper insights into the 2D perovskite materials, computational calculations are performed along with the detailed characterization of HTABr-based thin films. Overall, this study offers a promising approach for developing efficient, stable, and cost-effective PPDs for next-generation optoelectronic applications.

Key words: Halide perovskite, Photodetector, Dimensional heterojunction, 2D/3D-perovskite, Charge-transporting-layer-free

Yeonghun Yun, Min Ju Jeong, Hanbyeol Cho, Dong Hyun Kim, Won Chang Choi, Jina Jung, Sunwoo Kim, Ji-Sang Park, Jun Hong Noh, Sangwook Lee. Charge-transport-layer-free 2D/3D perovskite photodetector with high performance and stability[J]. J. Mater. Sci. Technol., 2026, 270: 26-35.

References

[1] T.T. Li, Q.Y. Li, H.J. Zhang, H.L. Zhao, S.L. Wang, M.Y. Li, X. Tang, X. Ding, Y.T. Zhang, J.Q. Yao, J. Mater. Chem. C 10 (2022) 6846-6856.
[2] X.Y. Liu, Z.Y. Liu, J.J. Li, X.H. Tan, B. Sun, H. Fang, S. Xi, T.L. Shi, Z.R. Tang, G.L. Liao, J. Mater. Chem. C 8 (2020) 3337-3350.
[3] S.F. Hu, K. Otsuka, R. Murdey, T. Nakamura, M.A. Truong, T. Yamada, T. Handa, K. Matsuda, K. Nakano, A. Sato, K. Marumoto, K. Tajima, Y. Kanemitsu, A. Wakamiya, Energy Environ. Sci. 15(2022) 2096-2107.
[4] H.Y. Wang, Y. Sun, J. Chen, F.C. Wang, R.Y. Han, C.Y. Zhang, J.F. Kong, L. Li, J. Yang, Nanomaterials 12 (2022) 4390.
[5] Y. Yun, G.S. Han, G.N. Park, J. Kim, J. Park, D. Vidyasagar, J. Jung, W.C. Choi, Y.J. Choi, K. Heo, J. Kang, J.S. Park, H.S. Jung, S. Lee, Adv. Mater. 34(2022) 2206932.
[6] Y. Zhao, C.L. Li, J.Z. Jiang, B.M. Wang, L. Shen, Small 16 (2020) 2001534.
[7] Y.W. Hsiao, B.S. Cheng, H.C. Hsu, S.H. Wu, H.T. Wu, C.C. Leu, C.F. Shih, Adv. Funct. Mater. 33(2023) 2300169.
[8] P.H. Wangyang, C.H. Gong, G.F. Rao, K. Hu, X.P. Wang, C.Y. Yan, L.P. Dai, C.Y. Wu, J. Xiong, Adv. Opt. Mater. 6(2018) 30.
[9] C.L. Li, Y. Ma, Y.F. Xiao, L. Shen, L.M. Ding, Infomat 2 (2020) 1247-1256.
[10] F.M. Rombach, S.A. Haque, T.J. Macdonald, Energy Environ. Sci. 14(2021) 5161-5190.
[11] V.M.Le Corre, M.Stolterfoht, L.P. Toro, M. Feuerstein, C. Wolff, L. Gil-Escriger, H.J. Bolink, D. Neher, L.J.A. Koster, ACS Appl. Energy Mater. 2(2019) 6280-6287.
[12] C.M. Wolff, P. Caprioglio, M. Stolterfoht, D. Neher, Adv. Mater. 31(2019) 1902762.
[13] I. Grill, M.F. Aygüler, T. Bein, P. Docampo, N.F. Hartmann, M. Handloser, A. Hartschuh, ACS Appl. Mater. Interfaces 9 (2017) 37655-37661.
[14] D. Glowienka, D. Zhang, F. Di Giacomo, M. Najafi, S. Veenstra, J. Szmytkowski, Y. Galagan, Nano Energy 67 (2020) 104186.
[15] Z. Li, C.X. Xiao, Y. Yang, S.P. Harvey, D.H. Kim, J.A. Christians, M.J. Yang, P. Schulz, S.U. Nanayakkara, C.S. Jiang, J.M. Luther, J.J. Berry, M.C. Beard, M.M.Al-Jassim, K.Zhu, Energy Environ. Sci. 10(2017) 1234-1242.
[16] J. Thiesbrummel, S.H. Shah, E. Gutierrez-Partida, F.S. Zu, F. Pena-Camargo, S. Zeiske, J. Diekmann, F.Y. Ye, K.P. Peters, K.O. Brinkmann, P. Caprioglio, A. Dasgupta, S. Seo, F.A. Adeleye, J. Warby, Q. Jeangros, F.L. Lang, S. Zhang, S. Albrecht, T. Riedl, A. Armin, D. Neher, N. Koch, Y.Z. Wu, V.M. Le Corre, H. Snaith, M. Stolterfoht, Nat. Energy 9 (2024) 664-676.
[17] Y.G. Yao, C.D. Cheng, C.Y. Zhang, H.L. Hu, K. Wang, S. De Wolf, Adv. Mater. 34(2022) 2203794.
[18] T. Chen, J. Xie, P. Gao, Adv. Energy Sustain. Res. 3(2022) 2100218.
[19] X.N. Zhang, X.Y. Liu, B. Sun, Z.R. Liu, Z.G. Zhang, L.X. Kong, G.L. Li, M.K. Wang, Z.Y. Liu, G.L. Liao, J. Mater. Chem. C 10 (2022) 14892-14904.
[20] X.N. Zhang, X.Y. Liu, B. Sun, H.B. Ye, C.H. He, L.X. Kong, G.L. Li, Z.Y. Liu, G.L. Liao, ACS Appl. Mater. Interfaces 13 (2021) 35949-35960.
[21] P.B. Gui, J.S. Li, X.L. Zheng, H.B. Wang, F. Yao, X.Z. Hu, Y.J. Liu, G.J. Fang, J. Mater. Chem. C 8 (2020) 6804-6812.
[22] Y.Y. Pan, H.L. Wang, Y.X. Wang, Y.Y. Wang, X.G. Li, Y.T. Liu, L.L Deng, K. Liu, T.X. Hu, F.C. Liu, Z.J. Shi, C.Y. Li, J. Wang, A.R. Yu, X.L. Zhang, Y.Q. Zhan, Adv. Electron. Mater. 9(2023) 2201028.
[23] E.H. Jung, N.J. Jeon, E.Y. Park, C.S. Moon, T.J. Shin, T.Y. Yang, J.H. Noh, J. Seo, Nature 567 (2019) 511-515.
[24] Y.W. Jang, S. Lee, K.M. Yeom, K. Jeong, K. Choi, M. Choi, J.H. Noh, Nat. Energy 6 (2021) 63-71.
[25] S. Lee, H. Cho, S. Kang, O.J. Oh, D.H. Kim, J.H. Noh, Energy Environ. Sci. 17(2024) 6234-6244.
[26] Y. Chen, X. Peng, W. Qin, S. Li, L. Zhang, Y. Wang, Z. Chen, B. Yang, Y. Yuan, J. He, Adv. Funct. Mater. 34(2024) 2403942.
[27] H. Li, X. Liu, T. Yang, C. Ma, Y. Du, P. Xu, L. Zhang, X. Song, Q. Cui, S. Zhao, ACS Energy Lett. 9(2023) 64-74.
[28] Z. Liao, L. Qiu, T. Chen, W. Qian, Y. Wang, S. Yang, T. Sun, G. Yang, A.K. Srivastava, H. Zhou, Adv. Mater. Technol. 8(2023) 2300714.
[29] H. Liang, J. Zhang, Y. Gao, P. Guo, L. Li, Z. Guo, Y. Wu, J. Huang, Sci. China Mater. 67(2024) 2193-2200.
[30] P.E. Blöchl, Phys. Rev. B 50 (1994) 17953-17979.
[31] G. Kresse, J. Furthmüller, Phys. Rev. B 54 (1996) 11169-11186.
[32] J.P. Perdew, K. Burke, M. Ernzerhof, Phys. Rev. Lett. 77(1996) 3865-3868.
[33] S. Grimme, S. Ehrlich, L. Goerigk, J. Comput. Chem. 32(2011) 1456-1465.
[34] J. Heyd, G.E. Scuseria, M. Ernzerhof, J. Chem. Phys. 118(2003) 8207-8215.
[35] R. Sahani, N. Kumar, C.A.R. Perini, A. Rahmani, D. Muñoz, D. LaFollette, J. Lawton, K. Datta, R.P. Li, J.P. Correa-Baena, T. Jurca, C.Y. Lai, D.R. Radu, Adv. Mater. Interfaces 12 (2025) 2400823.
[36] W.H. Gao, J.K. Ding, Q.X. Ma, H. Zhang, J.J. Zhang, Z.L. Zhang, M.J. Li, Y. Wang, B.X. Zhang, T. Pauporté, J.X. Tang, J.Z. Chen, C. Chen, Adv. Mater. 37(2025) 12.
[37] T. Zhang, S.B. Li, Nanoscale Res. Lett. 16(2021) 6.
[38] A.H. Proppe, A. Johnston, S. Teale, A. Mahata, R. Quintero-Bermudez, E.H. Jung, L. Grater, T. Cui, T. Filleter, C.Y. Kim, S.O. Kelley, F. De Angelis, E.H. Sargent, Nat. Commun. 12(2021) 3472.
[39] Y.H. Liu, S. Akin, L.F. Pan, R. Uchida, N. Arora, J.V. Milic, A. Hinderhofer, F. Schreiber, A.R. Uhl, S.M. Zakeeruddin, A. Hagfeldt, M.I. Dar, M. Grätzel, Sci. Adv. 5 (2019) eaaw2543.
[40] Y. Zeng, R.Q. Wang, K.X. Chen, X. Gao, X.R. Liu, F. Wu, L.N. Zhu, Sol. RRL 8 (2024) 9.
[41] S. Sidhik, Y. Wang, M. De Siena, R. Asadpour, A.J. Torma, T. Terlier, K. Ho, W. Li, A.B. Puthirath, X. Shuai, Science 377 (2022) 1425-1430.
[42] J. Li, P. Xiang, X.Y. Tan, B.W. Li, K. Zhang, Y. Zhu, Y.Q. Ren, X.B. Chen, J. Mater. Sci.: Mater. Electron. 34(2023) 11.
[43] J.W. Liang, X.Z. Hu, C. Wang, C. Liang, C. Chen, M. Xiao, J.S. Li, C. Tao, G.C. Xing, R. Yu, W.J. Ke, G.J. Fang, Joule 6 (2022) 816-833.
[44] L.G. Wang, H.P. Zhou, J.N. Hu, B.L. Huang, M.Z. Sun, B.W. Dong, G.H.J. Zheng, Y. Huang, Y.H. Chen, L. Li, Z.Q. Xu, N.X. Li, Z. Liu, Q. Chen, L.D. Sun, C.H. Yan, Science 363 (2019) 265-270.
[45] A.A. Sutanto, P. Caprioglio, N. Drigo, Y.J. Hofstetter, I. Garcia-Benito, V.I.E. Queloz, D. Neher, M.K. Nazeeruddin, M. Stolterfoht, Y. Vaynzof, G. Grancini, Chem 7 (2021) 1903-1916.
[46] S. Jeong, S. Seo, H. Yang, H. Park, S. Shin, H. Ahn, D. Lee, J.H. Park, N.G. Park, H. Shin, Adv. Energy Mater. 11(2021) 2102236.
[47] H. Chen, S. Teale, B. Chen, Y. Hou, L. Grater, T. Zhu, K. Bertens, S.M. Park, H.R. Atapattu, Y.J. Gao, M.Y. Wei, A.K. Johnston, Q.L. Zhou, K.M. Xu, D.N. Yu, C.C. Han, T. Cui, E.H. Jung, C. Zhou, W.J. Zhou, A.H. Proppe, S. Hoogland, F. Laquai, T. Filleter, K.R. Graham, Z.J. Ning, E.H. Sargent, Nat. Photonics 16 (2022) 352-358.
[48] M.C. Biesinger, X-ray photoelectron spectroscopy (XPS) reference pages, https://www.xpsfitting.com/2009/04/relative-sensitivity-factors-rsf.html, January 26, 2026.
[49] P. Fu, Y. Liu, S.W. Yu, H. Yin, B.W. Yang, S. Ahmad, X. Guo, C. Li, Nano Energy 88 (2021) 106249.
[50] R. Liu, X. Hu, M.X. Xu, H.R. Ren, H. Yu, Chemsuschem 16 (2023) e202300736.
[51] J. Gong, M.W. Hao, Y.L. Zhang, M.Z. Liu, Y.Y. Zhou, Angew. Chem. Int. Ed. 61(2022) e202112022.
[52] C.M.M.Soe, C.C. Stoumpos, M. Kepenekian, B.Traoré, H. Tsai, W.Y. Nie, B.H. Wang, C. Katan, R. Seshadri, A.D. Mohite, J. Eyen, T.J. Marks, M.G. Kanatzidis, J. Am. Chem. Soc. 139(2017) 16297-16309.
[53] D.B. Mitzi, S. Wang, C.A. Feild, C.A. Chess, A.M. Guloy, Science 267 (1995) 1473-1476.
[54] S. Aharon, B. El Cohen, L. Etgar, J. Phys. Chem. C 118 (2014) 17160-17165.
[55] R. Kour, S. Arya, S. Verma, J. Gupta, P. Bandhoria, V. Bharti, R. Datt, V. Gupta, Glob. Chall. 3(2019) 37.
[56] S. Wang, B.C. Kang, S.J. Park, T.J. Ha, L.K. Jagadamma, J. Phys. Mater. 6(2023) 12.
[57] Q. Lou, X.X. Xu, Z.J. Xu, T.T. Dai, H. Zhang, L. Zhao, F. Wang, E.J. Zhou, F. Gao, H. Zhou, Cell Rep. Phys. Sci. 6(2025) 12.
[58] Y.Q. Yang, Q. Xiong, J.H. Wu, Y.G. Tu, T.X. Sun, G.X. Li, X.P. Liu, X.B. Wang, Y.T. Du, C.Y. Deng, L.A. Tan, Y.L. Wei, Y. Lin, Y.F. Huang, M.L. Huang, W.H. Sun, L.Q. Fan, Y.M. Xie, J.M. Lin, Z. Lan, V. Stacchinii, A. Musiienko, Q. Hu, P. Gao, A. Abate, M.K. Nazeeruddin, Adv. Mater. 36(2024) 10.
[59] D.D. Xu, Z.M. Gong, Y. Jiang, Y.C. Feng, Z. Wang, X.S. Gao, X.B. Lu, G.F. Zhou, J.M. Liu, J.W. Gao, Nat. Commun. 13(2022) 8.
[60] Z.Y.L. Zhang, W.T. Zhang, Q.B. Jiang, Z.M. Wei, M.Y. Deng, D.D. Chen, W.D. Zhu, J.C. Zhang, H.L. You, ACS Appl. Mater. Interfaces 12 (2020) 6607-6614.
[61] J.W. Lim, H. Wang, C.H. Choi, H. Kwon, L.N. Quan, W.T. Park, Y.Y. Noh, D.H. Kim, Nano Energy 57 (2019) 761-770.
[62] S. Shaﬁque, A. Qadir, T. Iqbal, M. Sulaman, L. Yang, Y.N. Hou, Y.C. Miao, J. Wu, Y.H. Wang, F. Zheng, X. Wang, Z.Y. Hu, J. Alloy. Compd. 1004(2024) 11.
[63] Y. Deng, W.F. Tai, Q. Zhang, J. Tang, J.P. Li, K. Wang, H.M. Yu, J. Mater. Chem. C 11 (2023) 600-608.
[64] M. He, Z.H. Xu, C. Zhao, Y. Gao, K.H. Ke, N. Liu, X.X. Yao, F.Y. Kang, Y. Shen, L.W. Lin, G.D. Wei, Adv. Funct. Mater. 33(2023) 11.
[65] C.W. Shan, F. Meng, J.H. Yu, Z.X. Wang, W.H. Li, D.Y. Fan, R. Chen, H.B. Ma, G.Q. Li, A.K.K. Kyaw, J. Mater. Chem. C 9 (2021) 7632-7642.
[66] C. Liu, K. Wang, C. Yi, X.J. Shi, P.C. Du, A.W. Smith, A. Karim, X. Gong, J. Mater. Chem. C 3 (2015) 6600-6606.
[67] R. Chen, L.N. Shen, L.Y. Zheng, T. Zhu, Y.H. Liu, L. Liu, J. Zheng, X. Gong, ACS Appl. Mater. Interfaces 13 (2021) 49104-49113.
[68] G.X. Li, Y.K. Wang, L.X. Huang, W.H. Sun, ACS Appl. Electron. Mater. 4(2022) 1485-1505.
[69] J. Yang, C.X. Bao, W.H. Ning, B. Wu, F.X. Ji, Z.B. Yan, Y.T. Tao, J.M. Liu, T.C. Sum, S. Bai, J.P. Wang, W. Huang, W.J. Zhang, F. Gao, Adv. Opt. Mater. 7(2019) 1801732.
[70] W.D. Xu, L.J.F.Hart, B. Moss, P.Caprioglio, T.J. Macdonald, F. Furlan, J. Panidi, R.D.J. Oliver, R.A. Pacalaj, M. Heeney, N. Gasparini, H.J. Snaith, P.R.F. Barnes, J.R. Durrant, Adv. Energy Mater. 13(2023) 2301102.
[71] Z. Ahmad, A. Mishra, S.M. Abdulrahim, D. Taguchi, P. Sanghyun, F. Aziz, M. Iwamoto, T. Manaka, J. Bhadra, N.J.Al-Thani, M.K. Nazeeruddin, F. Touati, A. Belaidi, S.A. Al-Muhtaseb, Sci. Rep. 11(2021) 33.
[72] R.K. Gunasekaran, J. Jung, S.W. Yang, D. Im, W.C. Choi, Y. Yun, S. Lee, ACS Energy Lett. 9(2023) 102-109.
[73] Y. Zhao, C. Li, L. Shen, InfoMat 1 (2019) 164-182.
[74] L. Krückemeier, Z. Liu, T. Kirchartz, U. Rau, Adv. Mater. 35(2023) 2300872.
[75] C.R.McNeill, I. Hwang, N.C. Greenham, J. Appl. Phys. 106(2009) 024507.
[76] W. Xu, T. Du, M. Sachs, T.J. Macdonald, G. Min, L. Mohan, K. Stewart, C.T. Lin, J. Wu, R. Pacalaj, Cell Rep. Phys. Sci. 3(2022) 100890.
[77] Y. Liu, Y. Zhang, X. Zhu, Z. Yang, W. Ke, J. Feng, X. Ren, K. Zhao, M. Liu, M.G. Kanatzidis, Sci. Adv. 7 (2021) eabc8844.
[78] J.W. Lee, S.H. Bae, N. De Marco, Y.T. Hsieh, Z.H. Dai, Y. Yang, Mater. Today Energy 7 (2018) 149-160.
[79] Q. Wang, B. Chen, Y. Liu, Y.H. Deng, Y. Bai, Q.F. Dong, J.S. Huang, Energy Environ. Sci. 10(2017) 516-522.
[80] H.F. Xu, G.Z. Liu, X.X. Xu, S.D. Xu, L.Y. Zhang, X.J. Chen, H.Y. Zheng, X. Pan, Sol. RRL 4 (2020) 2000647.
[81] X. He, M. Wang, F.R. Cao, W. Tian, L. Li, J. Mater. Sci.Technol. 124(2022) 243-251.