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Title: Scaling law for excitons in 2D perovskite quantum wells

Ruddlesden–Popper halide perovskites are 2D solution-processed quantum wells with a general formula A 2A’ n-1M n X 3n+1, where optoelectronic properties can be tuned by varying the perovskite layer thickness (n-value), and have recently emerged as efficient semiconductors with technologically relevant stability. However, fundamental questions concerning the nature of optical resonances (excitons or free carriers) and the exciton reduced mass, and their scaling with quantum well thickness, which are critical for designing efficient optoelectronic devices, remain unresolved. Here, using optical spectroscopy and 60-Tesla magneto-absorption supported by modeling, we unambiguously demonstrate that the optical resonances arise from tightly bound excitons with both exciton reduced masses and binding energies decreasing, respectively, from 0.221 m 0 to 0.186 m 0 and from 470 meV to 125 meV with increasing thickness from n equals 1 to 5. Based on this study we propose a general scaling law to determine the binding energy of excitons in perovskite quantum wells of any layer thickness.
Authors:
ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [2] ; ORCiD logo [1] ; ORCiD logo [3] ; ORCiD logo [4] ;  [5] ; ORCiD logo [4] ;  [6] ;  [6] ; ORCiD logo [6] ; ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [4] ;  [3] ; ORCiD logo [1] ; ORCiD logo [7] ; ORCiD logo [6]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Rice Univ., Houston, TX (United States)
  3. Northwestern Univ., Evanston, IL (United States)
  4. Univ Rennes, ENSCR, INSA Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes) (France)
  5. Univ Rennes, INSA Rennes, CNRS (France)
  6. Rice Univ., Houston, TX (United States)
  7. Unive. Rennes, CNRS
Publication Date:
Report Number(s):
LA-UR-18-30029
Journal ID: ISSN 2041-1723
Grant/Contract Number:
AC52-06NA25396
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC); USDOE Laboratory Directed Research and Development (LDRD) Program
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1479902

Blancon, Jean-Christophe Robert, Stier, Andreas V, Tsai, Hsinhan, Nie, Wanyi, Stoumpos, Costas C., Traore, B., Pedesseau, L., Kepenekian, M., Katsutani, F, Noe, G. T., Kono, J., Tretiak, Sergei, Crooker, Scott A., Katan, C., Kanatzidis, M G., Crochet, Jared John, Even, Jacky, and Mohite, Aditya D.. Scaling law for excitons in 2D perovskite quantum wells. United States: N. p., Web. doi:10.1038/s41467-018-04659-x.
Blancon, Jean-Christophe Robert, Stier, Andreas V, Tsai, Hsinhan, Nie, Wanyi, Stoumpos, Costas C., Traore, B., Pedesseau, L., Kepenekian, M., Katsutani, F, Noe, G. T., Kono, J., Tretiak, Sergei, Crooker, Scott A., Katan, C., Kanatzidis, M G., Crochet, Jared John, Even, Jacky, & Mohite, Aditya D.. Scaling law for excitons in 2D perovskite quantum wells. United States. doi:10.1038/s41467-018-04659-x.
Blancon, Jean-Christophe Robert, Stier, Andreas V, Tsai, Hsinhan, Nie, Wanyi, Stoumpos, Costas C., Traore, B., Pedesseau, L., Kepenekian, M., Katsutani, F, Noe, G. T., Kono, J., Tretiak, Sergei, Crooker, Scott A., Katan, C., Kanatzidis, M G., Crochet, Jared John, Even, Jacky, and Mohite, Aditya D.. 2018. "Scaling law for excitons in 2D perovskite quantum wells". United States. doi:10.1038/s41467-018-04659-x. https://www.osti.gov/servlets/purl/1479902.
@article{osti_1479902,
title = {Scaling law for excitons in 2D perovskite quantum wells},
author = {Blancon, Jean-Christophe Robert and Stier, Andreas V and Tsai, Hsinhan and Nie, Wanyi and Stoumpos, Costas C. and Traore, B. and Pedesseau, L. and Kepenekian, M. and Katsutani, F and Noe, G. T. and Kono, J. and Tretiak, Sergei and Crooker, Scott A. and Katan, C. and Kanatzidis, M G. and Crochet, Jared John and Even, Jacky and Mohite, Aditya D.},
abstractNote = {Ruddlesden–Popper halide perovskites are 2D solution-processed quantum wells with a general formula A2A’n-1M n X3n+1, where optoelectronic properties can be tuned by varying the perovskite layer thickness (n-value), and have recently emerged as efficient semiconductors with technologically relevant stability. However, fundamental questions concerning the nature of optical resonances (excitons or free carriers) and the exciton reduced mass, and their scaling with quantum well thickness, which are critical for designing efficient optoelectronic devices, remain unresolved. Here, using optical spectroscopy and 60-Tesla magneto-absorption supported by modeling, we unambiguously demonstrate that the optical resonances arise from tightly bound excitons with both exciton reduced masses and binding energies decreasing, respectively, from 0.221 m0 to 0.186 m0 and from 470 meV to 125 meV with increasing thickness from n equals 1 to 5. Based on this study we propose a general scaling law to determine the binding energy of excitons in perovskite quantum wells of any layer thickness.},
doi = {10.1038/s41467-018-04659-x},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {6}
}

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