Cross-plane coherent acoustic phonons in two-dimensional organic-inorganic hybrid perovskites
Abstract
Two-dimensional, Ruddlesden-Popper organic-inorganic hybrid layered perovskites (2D-RPs) are solution-grown semiconductors with prospective applications in next-generation optoelectronics. The heat-carrying, low-energy acoustic vibrations of 2D-RPs, which are important for heat management of 2D-RP-based devices, have remained unexplored. Here we report on the propagation of coherent longitudinal acoustic phonons along the cross-plane direction of 2D-RPs, following separate characterizations of below-bandgap refractive index for each 2D-RP. Through experiments on crystals of systematically varied perovskite layer thickness, we demonstrate significant reduction in both group velocity and propagation length of acoustic phonons in 2D-RPs as compared to the three-dimensional methylammonium lead iodide. As borne out by a minimal coarse-grained model, these vibrational properties arise from a large acoustic impedance mismatch between the alternating layers of perovskite sheets and bulky organic cations. Furthermore, our results inform on thermal transport in highly impedance-mismatched crystal sub-lattices and provide insights towards design of materials that exhibit highly anisotropic thermal dissipation properties.
- Authors:
-
- Argonne National Lab. (ANL), Lemont, IL (United States)
- Northwestern Univ., Evanston, IL (United States)
- Argonne National Lab. (ANL), Lemont, IL (United States); Northwestern Univ., Evanston, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
- OSTI Identifier:
- 1461512
- Grant/Contract Number:
- AC02-06CH11357
- Resource 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
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Guo, Peijun, Stoumpos, Constantinos C., Mao, Lingling, Sadasivam, Sridhar, Ketterson, John B., Darancet, Pierre, Kanatzidis, Mercouri G., and Schaller, Richard D. Cross-plane coherent acoustic phonons in two-dimensional organic-inorganic hybrid perovskites. United States: N. p., 2018.
Web. doi:10.1038/s41467-018-04429-9.
Guo, Peijun, Stoumpos, Constantinos C., Mao, Lingling, Sadasivam, Sridhar, Ketterson, John B., Darancet, Pierre, Kanatzidis, Mercouri G., & Schaller, Richard D. Cross-plane coherent acoustic phonons in two-dimensional organic-inorganic hybrid perovskites. United States. https://doi.org/10.1038/s41467-018-04429-9
Guo, Peijun, Stoumpos, Constantinos C., Mao, Lingling, Sadasivam, Sridhar, Ketterson, John B., Darancet, Pierre, Kanatzidis, Mercouri G., and Schaller, Richard D. Tue .
"Cross-plane coherent acoustic phonons in two-dimensional organic-inorganic hybrid perovskites". United States. https://doi.org/10.1038/s41467-018-04429-9. https://www.osti.gov/servlets/purl/1461512.
@article{osti_1461512,
title = {Cross-plane coherent acoustic phonons in two-dimensional organic-inorganic hybrid perovskites},
author = {Guo, Peijun and Stoumpos, Constantinos C. and Mao, Lingling and Sadasivam, Sridhar and Ketterson, John B. and Darancet, Pierre and Kanatzidis, Mercouri G. and Schaller, Richard D.},
abstractNote = {Two-dimensional, Ruddlesden-Popper organic-inorganic hybrid layered perovskites (2D-RPs) are solution-grown semiconductors with prospective applications in next-generation optoelectronics. The heat-carrying, low-energy acoustic vibrations of 2D-RPs, which are important for heat management of 2D-RP-based devices, have remained unexplored. Here we report on the propagation of coherent longitudinal acoustic phonons along the cross-plane direction of 2D-RPs, following separate characterizations of below-bandgap refractive index for each 2D-RP. Through experiments on crystals of systematically varied perovskite layer thickness, we demonstrate significant reduction in both group velocity and propagation length of acoustic phonons in 2D-RPs as compared to the three-dimensional methylammonium lead iodide. As borne out by a minimal coarse-grained model, these vibrational properties arise from a large acoustic impedance mismatch between the alternating layers of perovskite sheets and bulky organic cations. Furthermore, our results inform on thermal transport in highly impedance-mismatched crystal sub-lattices and provide insights towards design of materials that exhibit highly anisotropic thermal dissipation properties.},
doi = {10.1038/s41467-018-04429-9},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {Tue May 22 00:00:00 EDT 2018},
month = {Tue May 22 00:00:00 EDT 2018}
}
Web of Science
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