Molecularly thin two-dimensional hybrid perovskites with tunable optoelectronic properties due to reversible surface relaxation

Kai Leng; Ibrahim Abdelwahab; Ivan Verzhbitskiy; Mykola Telychko; Leiqiang Chu; Wei Fu; Xiao Chi; Na Guo; Zhihui Chen; Zhongxin Chen; Chun Zhang; Qing Hua Xu; Jiong Lu; Manish Chhowalla; Goki Eda; Kian Ping Loh

doi:10.1038/s41563-018-0164-8

Molecularly thin two-dimensional hybrid perovskites with tunable optoelectronic properties due to reversible surface relaxation

Kai Leng, Ibrahim Abdelwahab, Ivan Verzhbitskiy, Mykola Telychko, Leiqiang Chu, Wei Fu, Xiao Chi, Na Guo, Zhihui Chen, Zhongxin Chen, Chun Zhang, Qing Hua Xu, Jiong Lu, Manish Chhowalla, Goki Eda, Kian Ping Loh

Rutgers University

Research output: Contribution to journal › Article

82 Citations (Scopus)

Abstract

Due to their layered structure, two-dimensional Ruddlesden–Popper perovskites (RPPs), composed of multiple organic/inorganic quantum wells, can in principle be exfoliated down to few and single layers. These molecularly thin layers are expected to present unique properties with respect to the bulk counterpart, due to increased lattice deformations caused by interface strain. Here, we have synthesized centimetre-sized, pure-phase single-crystal RPP perovskites (CH₃(CH₂)₃NH₃)₂(CH₃NH₃)_n−1Pb_nI_3n+1 (n = 1–4) from which single quantum well layers have been exfoliated. We observed a reversible shift in excitonic energies induced by laser annealing on exfoliated layers encapsulated by hexagonal boron nitride. Moreover, a highly efficient photodetector was fabricated using a molecularly thin n = 4 RPP crystal, showing a photogain of 10⁵ and an internal quantum efficiency of ~34%. Our results suggest that, thanks to their dynamic structure, atomically thin perovskites enable an additional degree of control for the bandgap engineering of these materials.

Original language	English
Pages (from-to)	908-914
Number of pages	7
Journal	Nature Materials
Volume	17
Issue number	10
DOIs	https://doi.org/10.1038/s41563-018-0164-8
Publication status	Published - Oct 1 2018

ASJC Scopus subject areas

Chemistry(all)
Materials Science(all)
Condensed Matter Physics
Mechanics of Materials
Mechanical Engineering

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Leng, K., Abdelwahab, I., Verzhbitskiy, I., Telychko, M., Chu, L., Fu, W., Chi, X., Guo, N., Chen, Z., Chen, Z., Zhang, C., Xu, Q. H., Lu, J., Chhowalla, M., Eda, G., & Loh, K. P. (2018). Molecularly thin two-dimensional hybrid perovskites with tunable optoelectronic properties due to reversible surface relaxation. Nature Materials, 17(10), 908-914. https://doi.org/10.1038/s41563-018-0164-8

Molecularly thin two-dimensional hybrid perovskites with tunable optoelectronic properties due to reversible surface relaxation. / Leng, Kai; Abdelwahab, Ibrahim; Verzhbitskiy, Ivan; Telychko, Mykola; Chu, Leiqiang; Fu, Wei; Chi, Xiao; Guo, Na; Chen, Zhihui; Chen, Zhongxin; Zhang, Chun; Xu, Qing Hua; Lu, Jiong; Chhowalla, Manish; Eda, Goki; Loh, Kian Ping.

In: Nature Materials, Vol. 17, No. 10, 01.10.2018, p. 908-914.

Research output: Contribution to journal › Article

Leng, K, Abdelwahab, I, Verzhbitskiy, I, Telychko, M, Chu, L, Fu, W, Chi, X, Guo, N, Chen, Z, Chen, Z, Zhang, C, Xu, QH, Lu, J, Chhowalla, M, Eda, G & Loh, KP 2018, 'Molecularly thin two-dimensional hybrid perovskites with tunable optoelectronic properties due to reversible surface relaxation', Nature Materials, vol. 17, no. 10, pp. 908-914. https://doi.org/10.1038/s41563-018-0164-8

Leng, Kai ; Abdelwahab, Ibrahim ; Verzhbitskiy, Ivan ; Telychko, Mykola ; Chu, Leiqiang ; Fu, Wei ; Chi, Xiao ; Guo, Na ; Chen, Zhihui ; Chen, Zhongxin ; Zhang, Chun ; Xu, Qing Hua ; Lu, Jiong ; Chhowalla, Manish ; Eda, Goki ; Loh, Kian Ping. / Molecularly thin two-dimensional hybrid perovskites with tunable optoelectronic properties due to reversible surface relaxation. In: Nature Materials. 2018 ; Vol. 17, No. 10. pp. 908-914.

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abstract = "Due to their layered structure, two-dimensional Ruddlesden–Popper perovskites (RPPs), composed of multiple organic/inorganic quantum wells, can in principle be exfoliated down to few and single layers. These molecularly thin layers are expected to present unique properties with respect to the bulk counterpart, due to increased lattice deformations caused by interface strain. Here, we have synthesized centimetre-sized, pure-phase single-crystal RPP perovskites (CH3(CH2)3NH3)2(CH3NH3)n−1PbnI3n+1 (n = 1–4) from which single quantum well layers have been exfoliated. We observed a reversible shift in excitonic energies induced by laser annealing on exfoliated layers encapsulated by hexagonal boron nitride. Moreover, a highly efficient photodetector was fabricated using a molecularly thin n = 4 RPP crystal, showing a photogain of 105 and an internal quantum efficiency of ~34%. Our results suggest that, thanks to their dynamic structure, atomically thin perovskites enable an additional degree of control for the bandgap engineering of these materials.",

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AU - Fu, Wei

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AU - Xu, Qing Hua

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AU - Chhowalla, Manish

AU - Eda, Goki

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