Polariton Dynamics in Two-Dimensional Ruddlesden–Popper Perovskites Strongly Coupled with Plasmonic Lattices
Abstract
Strong coupling between light and matter can produce hybrid eigenstates known as exciton–polaritons. Although polariton dynamics are important photophysical properties, the relaxation pathways of polaritons in different coupling regimes have seen limited attention. This paper reports the dynamics of hybridized states from 2D Ruddlesden–Popper perovskites coupled to plasmonic nanoparticle lattices. The open cavity architecture of Al lattices enables the coupling strength to be modulated by varying either the lead halide perovskite film thickness or the superstrate refractive index. Both experiments and finite-difference time-domain simulations of the optical dispersion diagrams showed avoided crossings that are a signature of strong coupling. Our analytical model also elucidated the correlation between the exciton/plasmon mixing ratio and polariton coupling strength. Using fs-transient absorption spectroscopy, we found that both the upper and lower polaritons have shorter lifetimes than the excitons and that polaritons can show faster excited-state dynamics when they have access to additional energy transfer channels.
- Authors:
-
- Northwestern Univ., Evanston, IL (United States); Gwangju Institute of Science and Technology (GIST) (Korea, Republic of)
- Northwestern Univ., Evanston, IL (United States)
- Northwestern Univ., Evanston, IL (United States); Univ. of South Florida, Tampa, FL (United States)
- Publication Date:
- Research Org.:
- Northwestern Univ., Evanston, IL (United States); Univ. of California, Santa Barbara, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); US DoD; US Department of the Navy, Office of Naval Research (ONR)
- OSTI Identifier:
- 1865235
- Alternate Identifier(s):
- OSTI ID: 1866210; OSTI ID: 1870319
- Grant/Contract Number:
- SC0012541; SC0021314; SC0004752; N00014-21-1-2289; N00014-17-13023; DMR-1720139; ECCS-2025633
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Nano
- Additional Journal Information:
- Journal Volume: 16; Journal Issue: 3; Journal ID: ISSN 1936-0851
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; strong coupling; polariton; plasmonic nanoparticle lattices; 2D perovskite; polariton dynamics; lattices; excitons; lipids; perovskites; strong coupling, polariton, plasmonic nanoparticle lattices, 2D perovskite, polariton dynamics
Citation Formats
Park, Jeong-Eun, López-Arteaga, Rafael, Sample, Alexander D., Cherqui, Charles R., Spanopoulos, Ioannis, Guan, Jun, Kanatzidis, Mercouri G., Schatz, George C., Weiss, Emily A., and Odom, Teri W. Polariton Dynamics in Two-Dimensional Ruddlesden–Popper Perovskites Strongly Coupled with Plasmonic Lattices. United States: N. p., 2022.
Web. doi:10.1021/acsnano.1c09296.
Park, Jeong-Eun, López-Arteaga, Rafael, Sample, Alexander D., Cherqui, Charles R., Spanopoulos, Ioannis, Guan, Jun, Kanatzidis, Mercouri G., Schatz, George C., Weiss, Emily A., & Odom, Teri W. Polariton Dynamics in Two-Dimensional Ruddlesden–Popper Perovskites Strongly Coupled with Plasmonic Lattices. United States. https://doi.org/10.1021/acsnano.1c09296
Park, Jeong-Eun, López-Arteaga, Rafael, Sample, Alexander D., Cherqui, Charles R., Spanopoulos, Ioannis, Guan, Jun, Kanatzidis, Mercouri G., Schatz, George C., Weiss, Emily A., and Odom, Teri W. Wed .
"Polariton Dynamics in Two-Dimensional Ruddlesden–Popper Perovskites Strongly Coupled with Plasmonic Lattices". United States. https://doi.org/10.1021/acsnano.1c09296. https://www.osti.gov/servlets/purl/1865235.
@article{osti_1865235,
title = {Polariton Dynamics in Two-Dimensional Ruddlesden–Popper Perovskites Strongly Coupled with Plasmonic Lattices},
author = {Park, Jeong-Eun and López-Arteaga, Rafael and Sample, Alexander D. and Cherqui, Charles R. and Spanopoulos, Ioannis and Guan, Jun and Kanatzidis, Mercouri G. and Schatz, George C. and Weiss, Emily A. and Odom, Teri W.},
abstractNote = {Strong coupling between light and matter can produce hybrid eigenstates known as exciton–polaritons. Although polariton dynamics are important photophysical properties, the relaxation pathways of polaritons in different coupling regimes have seen limited attention. This paper reports the dynamics of hybridized states from 2D Ruddlesden–Popper perovskites coupled to plasmonic nanoparticle lattices. The open cavity architecture of Al lattices enables the coupling strength to be modulated by varying either the lead halide perovskite film thickness or the superstrate refractive index. Both experiments and finite-difference time-domain simulations of the optical dispersion diagrams showed avoided crossings that are a signature of strong coupling. Our analytical model also elucidated the correlation between the exciton/plasmon mixing ratio and polariton coupling strength. Using fs-transient absorption spectroscopy, we found that both the upper and lower polaritons have shorter lifetimes than the excitons and that polaritons can show faster excited-state dynamics when they have access to additional energy transfer channels.},
doi = {10.1021/acsnano.1c09296},
journal = {ACS Nano},
number = 3,
volume = 16,
place = {United States},
year = {Wed Mar 02 00:00:00 EST 2022},
month = {Wed Mar 02 00:00:00 EST 2022}
}
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