Cross-plane coherent acoustic phonons in two-dimensional organic-inorganic hybrid perovskites

Peijun Guo; Constantinos C. Stoumpos; Lingling Mao; Sridhar Sadasivam; John B. Ketterson; Pierre Darancet; Mercouri G. Kanatzidis; Richard D. Schaller

doi:10.1038/s41467-018-04429-9

Cross-plane coherent acoustic phonons in two-dimensional organic-inorganic hybrid perovskites

Peijun Guo, Constantinos C. Stoumpos, Lingling Mao, Sridhar Sadasivam, John B. Ketterson, Pierre Darancet, Mercouri G. Kanatzidis, Richard D. Schaller^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

86 Scopus citations

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 phonons, which are important for heat management of 2D RP-based devices, have remained unexplored. Here we report on the generation and propagation of coherent longitudinal acoustic phonons along the cross-plane direction of 2D RPs, following separate characterizations of below-bandgap refractive indices. Through experiments on single 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 counterpart. 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. 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.

Original language	English (US)
Article number	2019
Journal	Nature communications
Volume	9
Issue number	1
DOIs	https://doi.org/10.1038/s41467-018-04429-9
State	Published - Dec 1 2018

Funding

The work was performed at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, and supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. This material is based upon work supported by Laboratory Directed Research and Development (LDRD) funding from Argonne National Laboratory, provided by the Director, Office of Science, of the U.S. Department of Energy under contract DE-AC02-06CH11357. Work at Northwestern University was supported by grant SC0012541 from the US Department of Energy, Office of Science (sample synthesis, processing and structural characterization).

ASJC Scopus subject areas

General Physics and Astronomy
General Chemistry
General Biochemistry, Genetics and Molecular Biology

Access to Document

10.1038/s41467-018-04429-9

Cite this

@article{5dd6feff9e2e40f9a5e597d2882a8e52,

title = "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 phonons, which are important for heat management of 2D RP-based devices, have remained unexplored. Here we report on the generation and propagation of coherent longitudinal acoustic phonons along the cross-plane direction of 2D RPs, following separate characterizations of below-bandgap refractive indices. Through experiments on single 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 counterpart. 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. 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.",

author = "Peijun Guo and Stoumpos, {Constantinos C.} and Lingling Mao and Sridhar Sadasivam and Ketterson, {John B.} and Pierre Darancet and Kanatzidis, {Mercouri G.} and Schaller, {Richard D.}",

note = "Funding Information: The work was performed at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, and supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. This material is based upon work supported by Laboratory Directed Research and Development (LDRD) funding from Argonne National Laboratory, provided by the Director, Office of Science, of the U.S. Department of Energy under contract DE-AC02-06CH11357. Work at Northwestern University was supported by grant SC0012541 from the US Department of Energy, Office of Science (sample synthesis, processing and structural characterization). Publisher Copyright: {\textcopyright} 2018 The Author(s).",

year = "2018",

month = dec,

day = "1",

doi = "10.1038/s41467-018-04429-9",

language = "English (US)",

volume = "9",

journal = "Nature communications",

issn = "2041-1723",

publisher = "Nature Research",

number = "1",

}

TY - JOUR

T1 - Cross-plane coherent acoustic phonons in two-dimensional organic-inorganic hybrid perovskites

AU - Guo, Peijun

AU - Stoumpos, Constantinos C.

AU - Mao, Lingling

AU - Sadasivam, Sridhar

AU - Ketterson, John B.

AU - Darancet, Pierre

AU - Kanatzidis, Mercouri G.

AU - Schaller, Richard D.

N1 - Funding Information: The work was performed at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility, and supported by the U.S. Department of Energy, Office of Science, under Contract No. DE-AC02-06CH11357. This material is based upon work supported by Laboratory Directed Research and Development (LDRD) funding from Argonne National Laboratory, provided by the Director, Office of Science, of the U.S. Department of Energy under contract DE-AC02-06CH11357. Work at Northwestern University was supported by grant SC0012541 from the US Department of Energy, Office of Science (sample synthesis, processing and structural characterization). Publisher Copyright: © 2018 The Author(s).

PY - 2018/12/1

Y1 - 2018/12/1

N2 - 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 phonons, which are important for heat management of 2D RP-based devices, have remained unexplored. Here we report on the generation and propagation of coherent longitudinal acoustic phonons along the cross-plane direction of 2D RPs, following separate characterizations of below-bandgap refractive indices. Through experiments on single 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 counterpart. 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. 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.

AB - 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 phonons, which are important for heat management of 2D RP-based devices, have remained unexplored. Here we report on the generation and propagation of coherent longitudinal acoustic phonons along the cross-plane direction of 2D RPs, following separate characterizations of below-bandgap refractive indices. Through experiments on single 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 counterpart. 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. 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.

UR - http://www.scopus.com/inward/record.url?scp=85047726491&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85047726491&partnerID=8YFLogxK

U2 - 10.1038/s41467-018-04429-9

DO - 10.1038/s41467-018-04429-9

M3 - Article

C2 - 29789666

AN - SCOPUS:85047726491

SN - 2041-1723

VL - 9

JO - Nature communications

JF - Nature communications

IS - 1

M1 - 2019

ER -

Cross-plane coherent acoustic phonons in two-dimensional organic-inorganic hybrid perovskites

Abstract

Funding

ASJC Scopus subject areas

Access to Document

Other files and links

Fingerprint

Cite this