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Title: Design principles for electronic charge transport in solution-processed vertically stacked 2D perovskite quantum wells

State-of-the-art quantum-well-based devices such as photovoltaics, photodetectors, and light-emission devices are enabled by understanding the nature and the exact mechanism of electronic charge transport. Ruddlesden–Popper phase halide perovskites are two-dimensional solution-processed quantum wells and have recently emerged as highly efficient semiconductors for solar cell approaching 14% in power conversion efficiency. However, further improvements will require an understanding of the charge transport mechanisms, which are currently unknown and further complicated by the presence of strongly bound excitons. Here, we unambiguously determine that dominant photocurrent collection is through electric field-assisted electron–hole pair separation and transport across the potential barriers. This is revealed by in-depth device characterization, coupled with comprehensive device modeling, which can self-consistently reproduce our experimental findings. These findings establish the fundamental guidelines for the molecular and device design for layered 2D perovskite-based photovoltaics and optoelectronic devices, and are relevant for other similar quantum-confined systems.
Authors:
ORCiD logo [1] ; ORCiD logo [2] ;  [3] ;  [4] ; ORCiD logo [5] ;  [6] ;  [4] ;  [2] ; ORCiD logo [1] ; ORCiD logo [3]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Rice Univ., Houston, TX (United States)
  2. Purdue Univ., West Lafayette, IN (United States)
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  4. Northwestern Univ., Evanston, IL (United States)
  5. Univ Rennes, INSA Rennes (France)
  6. Rice Univ., Houston, TX (United States)
Publication Date:
Report Number(s):
LA-UR-18-30079
Journal ID: ISSN 2041-1723
Grant/Contract Number:
AC52-06NA25396; FOA-0001647-1544; AC02-06CH11357
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)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1479905

Tsai, Hsinhan, Asadpour, Reza, Blancon, Jean-Christophe, Stoumpos, Constantinos C., Even, Jacky, Ajayan, Pulickel M., Kanatzidis, Mercouri G., Alam, Muhammad Ashraful, Mohite, Aditya D., and Nie, Wanyi. Design principles for electronic charge transport in solution-processed vertically stacked 2D perovskite quantum wells. United States: N. p., Web. doi:10.1038/s41467-018-04430-2.
Tsai, Hsinhan, Asadpour, Reza, Blancon, Jean-Christophe, Stoumpos, Constantinos C., Even, Jacky, Ajayan, Pulickel M., Kanatzidis, Mercouri G., Alam, Muhammad Ashraful, Mohite, Aditya D., & Nie, Wanyi. Design principles for electronic charge transport in solution-processed vertically stacked 2D perovskite quantum wells. United States. doi:10.1038/s41467-018-04430-2.
Tsai, Hsinhan, Asadpour, Reza, Blancon, Jean-Christophe, Stoumpos, Constantinos C., Even, Jacky, Ajayan, Pulickel M., Kanatzidis, Mercouri G., Alam, Muhammad Ashraful, Mohite, Aditya D., and Nie, Wanyi. 2018. "Design principles for electronic charge transport in solution-processed vertically stacked 2D perovskite quantum wells". United States. doi:10.1038/s41467-018-04430-2. https://www.osti.gov/servlets/purl/1479905.
@article{osti_1479905,
title = {Design principles for electronic charge transport in solution-processed vertically stacked 2D perovskite quantum wells},
author = {Tsai, Hsinhan and Asadpour, Reza and Blancon, Jean-Christophe and Stoumpos, Constantinos C. and Even, Jacky and Ajayan, Pulickel M. and Kanatzidis, Mercouri G. and Alam, Muhammad Ashraful and Mohite, Aditya D. and Nie, Wanyi},
abstractNote = {State-of-the-art quantum-well-based devices such as photovoltaics, photodetectors, and light-emission devices are enabled by understanding the nature and the exact mechanism of electronic charge transport. Ruddlesden–Popper phase halide perovskites are two-dimensional solution-processed quantum wells and have recently emerged as highly efficient semiconductors for solar cell approaching 14% in power conversion efficiency. However, further improvements will require an understanding of the charge transport mechanisms, which are currently unknown and further complicated by the presence of strongly bound excitons. Here, we unambiguously determine that dominant photocurrent collection is through electric field-assisted electron–hole pair separation and transport across the potential barriers. This is revealed by in-depth device characterization, coupled with comprehensive device modeling, which can self-consistently reproduce our experimental findings. These findings establish the fundamental guidelines for the molecular and device design for layered 2D perovskite-based photovoltaics and optoelectronic devices, and are relevant for other similar quantum-confined systems.},
doi = {10.1038/s41467-018-04430-2},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {5}
}

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