Role of Atomic Structure on Exciton Dynamics and Photoluminescence in NIR Emissive InAs/InP/ZnSe Quantum Dots
Abstract
The development of bright, near-infrared-emissive quantum dots (QDs) is a necessary requirement for the realization of important new classes of technology. Specifically, there exist significant needs for brighter, heavy metal-free, near-infrared (NIR) QDs for applications with high radiative efficiency that span diverse applications, including down-conversion emitters for high-performance luminescent solar concentrators. In this work, we use a combination of theoretical and experimental approaches to synthesize bright, NIR luminescent InAs/InP/ZnSe QDs and elucidate fundamental material attributes that remain obstacles for development of near-unity NIR QD luminophores. First, using Monte Carlo ray tracing, we identify the atomic and electronic structural attributes of InAs core/shell, NIR emitters, whose luminescence properties can be tailored by synthetic design to match most beneficially those of high-performance, single-band-gap photovoltaic devices based on important semiconductor materials, such Si or GaAs. Second, we synthesize InAs/InP/ZnSe QDs based on the optical attributes found to maximize LSC performance and develop methods to improve the emissive qualities of NIR emitters with large, tunable Stokes ratios, narrow emission linewidths, and high luminescence quantum yields (here reaching 60 ± 2%). Third, we employ atomistic electronic structure calculations to explore charge carrier behavior at the nanoscale affected by interfacial atomic structures and find that significantmore »
- Authors:
-
[1];
[2];
[4];
[5];
[4];
[7];
[4];
[6];
[4];
[8];
- Department of Chemistry, University of Illinois at Urbana Champaign, Urbana, Illinois 61801, United States, Department of Chemistry, Western Washington University, Bellingham, Washington 98225, United States
- Department of Chemistry, University of California, Berkeley, California 94720, United States
- Department of Chemistry, University of Illinois at Urbana Champaign, Urbana, Illinois 61801, United States
- Department of Applied Physics and Materials Science, California Institute of Technology, Pasadena, California 91125, United States
- Department of Chemistry, University of California, Berkeley, California 94720, United States, Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
- Department of Materials Science and Engineering, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States
- Department of Chemical and Biomolecular Engineering, University of Illinois at Urbana Champaign, Urbana, Illinois 61801, United States
- Department of Chemistry, University of California, Berkeley, California 94720, United States, Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States, The Sackler Center for Computational Molecular and Materials Science, Tel Aviv University, Tel Aviv 69978, Israel
- Department of Chemistry, University of Illinois at Urbana Champaign, Urbana, Illinois 61801, United States, Surface and Corrosion Science, School of Engineering Sciences in Chemistry, Biotechnology and Health, KTH Royal Institute of Technology, Stockholm 10044, Sweden
- Publication Date:
- Research Org.:
- Univ. of Illinois at Urbana-Champaign, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Photonics at Thermodynamic Limits; Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1865203
- Alternate Identifier(s):
- OSTI ID: 1866743; OSTI ID: 1925194
- Grant/Contract Number:
- SC0019140; SC0019323; AC02-05CH11231
- Resource Type:
- Published Article
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Name: Journal of Physical Chemistry. C Journal Volume: 126 Journal Issue: 17; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 77 NANOSCIENCE AND NANOTECHNOLOGY; 14 SOLAR ENERGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; excitons; indium arsenide; materials; quantum dots; thickness
Citation Formats
Enright, Michael J., Jasrasaria, Dipti, Hanchard, Mathilde M., Needell, David R., Phelan, Megan E., Weinberg, Daniel, McDowell, Brinn E., Hsiao, Haw-Wen, Akbari, Hamidreza, Kottwitz, Matthew, Potter, Maggie M., Wong, Joeson, Zuo, Jian-Min, Atwater, Harry A., Rabani, Eran, and Nuzzo, Ralph G. Role of Atomic Structure on Exciton Dynamics and Photoluminescence in NIR Emissive InAs/InP/ZnSe Quantum Dots. United States: N. p., 2022.
Web. doi:10.1021/acs.jpcc.2c01499.
Enright, Michael J., Jasrasaria, Dipti, Hanchard, Mathilde M., Needell, David R., Phelan, Megan E., Weinberg, Daniel, McDowell, Brinn E., Hsiao, Haw-Wen, Akbari, Hamidreza, Kottwitz, Matthew, Potter, Maggie M., Wong, Joeson, Zuo, Jian-Min, Atwater, Harry A., Rabani, Eran, & Nuzzo, Ralph G. Role of Atomic Structure on Exciton Dynamics and Photoluminescence in NIR Emissive InAs/InP/ZnSe Quantum Dots. United States. https://doi.org/10.1021/acs.jpcc.2c01499
Enright, Michael J., Jasrasaria, Dipti, Hanchard, Mathilde M., Needell, David R., Phelan, Megan E., Weinberg, Daniel, McDowell, Brinn E., Hsiao, Haw-Wen, Akbari, Hamidreza, Kottwitz, Matthew, Potter, Maggie M., Wong, Joeson, Zuo, Jian-Min, Atwater, Harry A., Rabani, Eran, and Nuzzo, Ralph G. Tue .
"Role of Atomic Structure on Exciton Dynamics and Photoluminescence in NIR Emissive InAs/InP/ZnSe Quantum Dots". United States. https://doi.org/10.1021/acs.jpcc.2c01499.
@article{osti_1865203,
title = {Role of Atomic Structure on Exciton Dynamics and Photoluminescence in NIR Emissive InAs/InP/ZnSe Quantum Dots},
author = {Enright, Michael J. and Jasrasaria, Dipti and Hanchard, Mathilde M. and Needell, David R. and Phelan, Megan E. and Weinberg, Daniel and McDowell, Brinn E. and Hsiao, Haw-Wen and Akbari, Hamidreza and Kottwitz, Matthew and Potter, Maggie M. and Wong, Joeson and Zuo, Jian-Min and Atwater, Harry A. and Rabani, Eran and Nuzzo, Ralph G.},
abstractNote = {The development of bright, near-infrared-emissive quantum dots (QDs) is a necessary requirement for the realization of important new classes of technology. Specifically, there exist significant needs for brighter, heavy metal-free, near-infrared (NIR) QDs for applications with high radiative efficiency that span diverse applications, including down-conversion emitters for high-performance luminescent solar concentrators. In this work, we use a combination of theoretical and experimental approaches to synthesize bright, NIR luminescent InAs/InP/ZnSe QDs and elucidate fundamental material attributes that remain obstacles for development of near-unity NIR QD luminophores. First, using Monte Carlo ray tracing, we identify the atomic and electronic structural attributes of InAs core/shell, NIR emitters, whose luminescence properties can be tailored by synthetic design to match most beneficially those of high-performance, single-band-gap photovoltaic devices based on important semiconductor materials, such Si or GaAs. Second, we synthesize InAs/InP/ZnSe QDs based on the optical attributes found to maximize LSC performance and develop methods to improve the emissive qualities of NIR emitters with large, tunable Stokes ratios, narrow emission linewidths, and high luminescence quantum yields (here reaching 60 ± 2%). Third, we employ atomistic electronic structure calculations to explore charge carrier behavior at the nanoscale affected by interfacial atomic structures and find that significant exciton occupation of the InP shell occurs in most cases despite the InAs/InP type I bulk band alignment. Furthermore, the density of the valence band maximum state extends anisotropically through the (111) crystal planes to the terminal InP surfaces/interfaces, indicating that surface defects, such as unpassivated phosphorus dangling bonds, located on the (111) facets play an outsized role in disrupting the valence band maximum and quenching photoluminescence.},
doi = {10.1021/acs.jpcc.2c01499},
journal = {Journal of Physical Chemistry. C},
number = 17,
volume = 126,
place = {United States},
year = {Tue Apr 26 00:00:00 EDT 2022},
month = {Tue Apr 26 00:00:00 EDT 2022}
}
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