Journal article
Signatures of Coherent Phonon Transport in Ultralow Thermal Conductivity Two-Dimensional Ruddlesden–Popper Phase Perovskites
ACS nano, Vol.15(3), pp.4165-4172
23 Mar 2021
PMID: 33661603
Featured in Collection : UN Sustainable Development Goals @ Drexel
Abstract
An emerging class of methylammonium lead iodide (MAPbI3)-based Ruddlesden–Popper (RP) phase perovskites, BA2MA n–1Pb n I3n+1 (n = 1–7), exhibit enhanced stability to environmental conditions relative to MAPbI3, yet still degrade at elevated temperatures. We experimentally determine the thermal conductivities of these layered RP phases for n = 1–6, where n defines the number of repeated perovskite octahedra per layer. We measure thermal conductivities of 0.37 ± 0.13/0.12, 0.17 ± 0.08/0.07, 0.21 ± 0.05/0.04, and 0.19 ± 0.04/0.03 W/m·K in thin films of n = 1–4 and 0.08 ± 0.06/0.04, 0.06 ± 0.04/0.03, 0.06 ± 0.03/0.03, and 0.08 ± 0.07/0.04 W/m·K in single crystals of n = 3–6. With the exception of n = 1, these thermal conductivities are lower than the range of 0.34–0.50 W/m·K reported for single-crystal MAPbI3. Reduced-order lattice dynamics modeling suggests that the initially decreasing trend of thermal conductivity in similarly oriented perovskites with increasing n may result from the transport properties of coherent phonons, emergent from the superstructure, that do not scatter at the interfaces of organic butylammonium chains and perovskite octahedra. Reduced group velocity of coherent phonons in n = 3–6, a consequence of band flattening in the phonon dispersion, is primarily responsible for their ultralow thermal conductivities. Similar effects on thermal conductivity have been experimentally demonstrated in deposited superlattices, but never in naturally defined materials such as RP phases. GIWAXS measurements reveal that higher n RP phase thin films are less orientationally controlled and therefore possess apparently elevated thermal conductivities relative to single crystals of the same n.
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Details
- Title
- Signatures of Coherent Phonon Transport in Ultralow Thermal Conductivity Two-Dimensional Ruddlesden–Popper Phase Perovskites
- Creators
- Alexander D Christodoulides - Carnegie Mellon UniversityPeijun Guo - Argonne National LaboratoryLingyun Dai - Carnegie Mellon UniversityJustin M Hoffman - Northwestern UniversityXiaotong Li - Northwestern UniversityXiaobing Zuo - Argonne National LaboratoryDaniel Rosenmann - Argonne National LaboratoryAlexandra Brumberg - Northwestern UniversityMercouri G Kanatzidis - Northwestern UniversityRichard D Schaller - Argonne National LaboratoryJonathan A Malen - Carnegie Mellon UniversityArgonne National Lab. (ANL), Argonne, IL (United States)
- Publication Details
- ACS nano, Vol.15(3), pp.4165-4172
- Publisher
- American Chemical Society
- Number of pages
- 8
- Resource Type
- Journal article
- Language
- English
- Academic Unit
- Chemistry
- Web of Science ID
- WOS:000634569100038
- Scopus ID
- 2-s2.0-85103449850
- Other Identifier
- 991022053795604721
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- Collaboration types
- Domestic collaboration
- Web of Science research areas
- Chemistry, Multidisciplinary
- Chemistry, Physical
- Materials Science, Multidisciplinary
- Nanoscience & Nanotechnology