Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites

Blancon, J. -C.; Tsai, H.; Nie, W.; Stoumpos, C. C.; Pedesseau, L.; Katan, C.; Kepenekian, M.; Soe, C. M. M.; Appavoo, K.; Sfeir, M. Y.; Tretiak, S.; Ajayan, P. M.; Kanatzidis, M. G.; Even, J.; Crochet, J. J.; Mohite, A. D.

doi:10.1126/science.aal4211

Title: Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites

Journal Article · Thu Mar 09 00:00:00 EST 2017 · Science

DOI:https://doi.org/10.1126/science.aal4211· OSTI ID:1434400

; Tsai, H.; Nie, W.;

;

; Appavoo, K.;

;

; Ajayan, P. M.; Kanatzidis, M. G.;

;

Understanding and controlling charge and energy flow in state-of-the-art semiconductor quantum wells has enabled high-efficiency optoelectronic devices. Two-dimensional (2D) Ruddlesden-Popper perovskites are solution-processed quantum wells wherein the band gap can be tuned by varying the perovskite-layer thickness, which modulates the effective electron-hole confinement. We report that, counterintuitive to classical quantum-confined systems where photogenerated electrons and holes are strongly bound by Coulomb interactions or excitons, the photophysics of thin films made of Ruddlesden-Popper perovskites with a thickness exceeding two perovskite-crystal units (>1.3 nanometers) is dominated by lower-energy states associated with the local intrinsic electronic structure of the edges of the perovskite layers. Furthermore, these states provide a direct pathway for dissociating excitons into longer-lived free carriers that substantially improve the performance of optoelectronic devices.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: 300034; 300035; SC0012541; 300033; AC52-06NA25396; SC0012704

OSTI ID:: 1434400

Alternate ID(s):: OSTI ID: 1414133; OSTI ID: 1437943

Report Number(s):: LA-UR-17-20088; BNL-204650-2018-JAAM; /sci/355/6331/1288.atom

Journal Information:: Science, Journal Name: Science Vol. 355 Journal Issue: 6331; ISSN 0036-8075

Publisher:: American Association for the Advancement of Science (AAAS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 714 works

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Controllable growth of two-dimensional perovskite microstructures Fang, Chen; Li, Junze; Wang, Jun CrystEngComm, Vol. 20, Issue 41 https://doi.org/10.1039/c8ce01087k	journal	January 2018
Inter-phase charge and energy transfer in Ruddlesden–Popper 2D perovskites: critical role of the spacing cations Zheng, Kaibo; Chen, Yani; Sun, Yong Journal of Materials Chemistry A, Vol. 6, Issue 15 https://doi.org/10.1039/c8ta01518j	journal	January 2018
Multi-layered hybrid perovskites templated with carbazole derivatives: optical properties, enhanced moisture stability and solar cell characteristics Herckens, Roald; Van Gompel, Wouter T. M.; Song, Wenya Journal of Materials Chemistry A, Vol. 6, Issue 45 https://doi.org/10.1039/c8ta08019d	journal	January 2018
Emission enhancement and bandgap retention of a two-dimensional mixed cation lead halide perovskite under high pressure Chen, Yaping; Fu, Ruijing; Wang, Lingrui Journal of Materials Chemistry A, Vol. 7, Issue 11 https://doi.org/10.1039/c8ta11992a	journal	January 2019
Photophysics behind highly luminescent two-dimensional hybrid perovskite (CH ₃ (CH ₂ ) ₂ NH ₃ ) ₂ (CH ₃ NH ₃ ) ₂ Pb ₃ Br ₁₀ thin films Ramirez, Daniel; Uribe, José Ignacio; Francaviglia, Luca Journal of Materials Chemistry C, Vol. 6, Issue 23 https://doi.org/10.1039/c8tc01582a	journal	January 2018
Superlattices based on van der Waals 2D materials Ryu, Yu Kyoung; Frisenda, Riccardo; Castellanos-Gomez, Andres Chemical Communications, Vol. 55, Issue 77 https://doi.org/10.1039/c9cc04919c	journal	January 2019
Liquid-phase growth and optoelectronic properties of two-dimensional hybrid perovskites CH ₃ NH ₃ PbX ₃ (X = Cl, Br, I) Bai, Yu; Zhang, Haixin; Zhang, Mingjing Nanoscale, Vol. 12, Issue 2 https://doi.org/10.1039/c9nr07981e	journal	January 2020
Guanidinium induced phase separated perovskite layer for efficient and highly stable solar cells Zhang, Weihai; Xiong, Juan; Li, Jinhua Journal of Materials Chemistry A, Vol. 7, Issue 16 https://doi.org/10.1039/c9ta01893j	journal	January 2019
Negative electron affinity driven broadband absorption of Cs _3+n Pb _n Sb ₂ I _9+3n /GaN van der Waals heterostructures Yang, Xiao-dong; Shu, Hai-bo; Wang, Xin-xin Journal of Materials Chemistry A, Vol. 7, Issue 39 https://doi.org/10.1039/c9ta08458d	journal	January 2019
Janus electrochemical exfoliation of two-dimensional materials Fang, Yiyun; Li, Xinzhe; Li, Jing Journal of Materials Chemistry A, Vol. 7, Issue 45 https://doi.org/10.1039/c9ta10487a	journal	January 2019
Ultrathin two-dimensional π–d conjugated coordination polymer Co ₃ (hexaaminobenzene) ₂ nanosheets for highly efficient oxygen evolution Li, Chun; Shi, Lingling; Zhang, Lili Journal of Materials Chemistry A, Vol. 8, Issue 1 https://doi.org/10.1039/c9ta10644h	journal	January 2020
Energy transfer mechanisms in layered 2D perovskites Williams, Olivia F.; Guo, Zhenkun; Hu, Jun The Journal of Chemical Physics, Vol. 148, Issue 13 https://doi.org/10.1063/1.5009663	journal	April 2018
A transient-electroluminescence study on perovskite light-emitting diodes Xu, Mengmeng; Peng, Qiming; Zou, Wei Applied Physics Letters, Vol. 115, Issue 4 https://doi.org/10.1063/1.5099277	journal	July 2019
Long-lived charge separation in two-dimensional ligand-perovskite heterostructures Deng, Shibin; Snaider, Jordan M.; Gao, Yao The Journal of Chemical Physics, Vol. 152, Issue 4 https://doi.org/10.1063/1.5131801	journal	January 2020
Observation of Rydberg exciton polaritons and their condensate in a perovskite cavity Bao, Wei; Liu, Xiaoze; Xue, Fei Proceedings of the National Academy of Sciences, Vol. 116, Issue 41 https://doi.org/10.1073/pnas.1909948116	journal	September 2019
Highly efficient and stable 2D–3D perovskite solar cells fabricated by interfacial modification Zou, Yuqin; Cui, Yong; Wang, Hao-Yi Nanotechnology, Vol. 30, Issue 27 https://doi.org/10.1088/1361-6528/ab10f3	journal	April 2019
Synthesis and optical applications of low dimensional metal-halide perovskites Liu, Jingying; Chen, Keqiang; Khan, Sayed Ali Nanotechnology, Vol. 31, Issue 15 https://doi.org/10.1088/1361-6528/ab5a19	journal	January 2020
Fabrication of single phase 2D homologous perovskite microplates by mechanical exfoliation Li, Junze; Wang, Jun; Zhang, Yingjun 2D Materials, Vol. 5, Issue 2 https://doi.org/10.1088/2053-1583/aaa5d4	journal	January 2018
Synthesis, Hirshfeld surface analysis, optical and electronic properties of the functional hybrid perovskite [NH ₃ –(CH ₂ ) ₂ –NH ₃ ] CdCl ₄ : a combined experimental and theoretical study Tahiri, Obaida; Kassou, Said; El Mrabet, Rajae Materials Research Express, Vol. 6, Issue 7 https://doi.org/10.1088/2053-1591/ab11ae	journal	April 2019
Dual excitonic emissions and structural phase transition of octylammonium lead iodide 2D layered perovskite single crystal Sheikh, Tariq; Shinde, Aparna; Mahamuni, Shailaja Materials Research Express, Vol. 6, Issue 12 https://doi.org/10.1088/2053-1591/ab53a1	journal	November 2019
Efficient and accurate calculation of band gaps of halide perovskites with the Tran-Blaha modified Becke-Johnson potential Traoré, Boubacar; Bouder, Gaëlle; Lafargue-Dit-Hauret, William Physical Review B, Vol. 99, Issue 3 https://doi.org/10.1103/physrevb.99.035139	journal	January 2019
Distinct conducting layer edge states in two-dimensional (2D) halide perovskite Wang, Kai; Wu, Congcong; Jiang, Yuanyuan Science Advances, Vol. 5, Issue 7 https://doi.org/10.1126/sciadv.aau3241	journal	July 2019
Ultrahydrophobic 3D/2D fluoroarene bilayer-based water-resistant perovskite solar cells with efficiencies exceeding 22% Liu, Yuhang; Akin, Seckin; Pan, Linfeng Science Advances, Vol. 5, Issue 6 https://doi.org/10.1126/sciadv.aaw2543	journal	June 2019
Promises and challenges of perovskite solar cells Correa-Baena, Juan-Pablo; Saliba, Michael; Buonassisi, Tonio Science, Vol. 358, Issue 6364 https://doi.org/10.1126/science.aam6323	journal	November 2017
Enhanced optoelectronic performance of 2D organic-inorganic hybrid perovskite through light-illumination Song, Yiling; Liu, Weiwei; Fang, Chen Optics Express, Vol. 27, Issue 21 https://doi.org/10.1364/oe.27.030618	journal	January 2019
Recent Research Progress in Surface Ligand Exchange of PbS Quantum Dots for Solar Cell Application You, Hyung Ryul; Park, Jin Young; Lee, Duck Hoon Applied Sciences, Vol. 10, Issue 3 https://doi.org/10.3390/app10030975	journal	February 2020
Nanostructured Perovskite Solar Cells McDonald, Calum; Ni, Chengsheng; Maguire, Paul Nanomaterials, Vol. 9, Issue 10 https://doi.org/10.3390/nano9101481	journal	October 2019

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