Bright magnetic dipole radiation from two-dimensional lead-halide perovskites
Abstract
Light-matter interactions in semiconductors are uniformly treated within the electric dipole approximation; multipolar interactions are considered “forbidden.” We experimentally demonstrate that this approximation inadequately describes light emission in two-dimensional (2D) hybrid organic-inorganic perovskites (HOIPs), solution processable semiconductors with promising optoelectronic properties. By exploiting the highly oriented crystal structure, we use energy-momentum spectroscopies to demonstrate that an exciton-like sideband in 2D HOIPs exhibits a multipolar radiation pattern with highly directed emission. Electromagnetic and quantum-mechanical analyses indicate that this emission originates from an out-of-plane magnetic dipole transition arising from the 2D character of electronic states. Symmetry arguments and temperature-dependent measurements suggest a dynamic symmetry-breaking mechanism that is active over a broad temperature range. These results challenge the paradigm of electric dipole–dominated light-matter interactions in optoelectronic materials, provide new perspectives on the origins of unexpected sideband emission in HOIPs, and tease the possibility of metamaterial-like scattering phenomena at the quantum-mechanical level.
- Authors:
-
[1];
[1];
[1];
[1];
[1];
[1];
[2];
[1]
- Univ. of California, Santa Barbara, CA (United States)
- Brown Univ., Providence, RI (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of California, Santa Barbara, CA (United States); Univ. of California, San Diego, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); US Air Force Office of Scientific Research (AFOSR)
- OSTI Identifier:
- 1626044
- Grant/Contract Number:
- AC02-05CH11231; SC0012541; SC0010689; SC0019273; DMR-1454260; OIA-1538893; FA9550-16-1-0393; DMR 1720256
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Science Advances
- Additional Journal Information:
- Journal Volume: 6; Journal Issue: 6; Journal ID: ISSN 2375-2548
- Publisher:
- AAAS
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 42 ENGINEERING; Science & Technology - Other Topics
Citation Formats
DeCrescent, Ryan A., Venkatesan, Naveen R., Dahlman, Clayton J., Kennard, Rhys M., Zhang, Xie, Li, Wenhao, Du, Xinhong, Chabinyc, Michael L., Zia, Rashid, and Schuller, Jon A. Bright magnetic dipole radiation from two-dimensional lead-halide perovskites. United States: N. p., 2020.
Web. doi:10.1126/sciadv.aay4900.
DeCrescent, Ryan A., Venkatesan, Naveen R., Dahlman, Clayton J., Kennard, Rhys M., Zhang, Xie, Li, Wenhao, Du, Xinhong, Chabinyc, Michael L., Zia, Rashid, & Schuller, Jon A. Bright magnetic dipole radiation from two-dimensional lead-halide perovskites. United States. https://doi.org/10.1126/sciadv.aay4900
DeCrescent, Ryan A., Venkatesan, Naveen R., Dahlman, Clayton J., Kennard, Rhys M., Zhang, Xie, Li, Wenhao, Du, Xinhong, Chabinyc, Michael L., Zia, Rashid, and Schuller, Jon A. Fri .
"Bright magnetic dipole radiation from two-dimensional lead-halide perovskites". United States. https://doi.org/10.1126/sciadv.aay4900. https://www.osti.gov/servlets/purl/1626044.
@article{osti_1626044,
title = {Bright magnetic dipole radiation from two-dimensional lead-halide perovskites},
author = {DeCrescent, Ryan A. and Venkatesan, Naveen R. and Dahlman, Clayton J. and Kennard, Rhys M. and Zhang, Xie and Li, Wenhao and Du, Xinhong and Chabinyc, Michael L. and Zia, Rashid and Schuller, Jon A.},
abstractNote = {Light-matter interactions in semiconductors are uniformly treated within the electric dipole approximation; multipolar interactions are considered “forbidden.” We experimentally demonstrate that this approximation inadequately describes light emission in two-dimensional (2D) hybrid organic-inorganic perovskites (HOIPs), solution processable semiconductors with promising optoelectronic properties. By exploiting the highly oriented crystal structure, we use energy-momentum spectroscopies to demonstrate that an exciton-like sideband in 2D HOIPs exhibits a multipolar radiation pattern with highly directed emission. Electromagnetic and quantum-mechanical analyses indicate that this emission originates from an out-of-plane magnetic dipole transition arising from the 2D character of electronic states. Symmetry arguments and temperature-dependent measurements suggest a dynamic symmetry-breaking mechanism that is active over a broad temperature range. These results challenge the paradigm of electric dipole–dominated light-matter interactions in optoelectronic materials, provide new perspectives on the origins of unexpected sideband emission in HOIPs, and tease the possibility of metamaterial-like scattering phenomena at the quantum-mechanical level.},
doi = {10.1126/sciadv.aay4900},
journal = {Science Advances},
number = 6,
volume = 6,
place = {United States},
year = {Fri Feb 07 00:00:00 EST 2020},
month = {Fri Feb 07 00:00:00 EST 2020}
}
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Figure 1: Structure and energy-momentum photoluminescence spectra of BA2PbI4. (A) Schematic crystal structure of BA2PbI4. Thin films exhibit a vertically layered morphology with repeated PbI4 monolayers separated in the z direction by BA2 spacer layers. (B) Experimental GIWAXS patterns of a spin-cast BA2PbI4 thin film. (C) Experimental geometry: Momentum- (k‖)more »
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