Loading…
Symmetry Breaking Induced Anisotropic Carrier Transport and Remarkable Thermoelectric Performance in Mixed Halide Perovskites CsPb(I1–x Br x )3
We present a combination of first-principles calculations and the Boltzmann transport theory to understand the carrier transport and thermoelectric performance of mixed halide perovskite alloys CsPb(I1–x Br x )3 with different Br compositions. Our computational results correlate the conduction band...
Saved in:
Published in: | ACS applied materials & interfaces 2020-09, Vol.12 (36), p.40453-40464 |
---|---|
Main Authors: | , , , , |
Format: | Article |
Language: | English |
Subjects: | |
Citations: | Items that this one cites Items that cite this one |
Online Access: | Get full text |
Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
cited_by | cdi_FETCH-LOGICAL-a222t-5ee0c43f73d52fd6121e7c11f01dbb2f4ddb33998dae9796a7b1e1564e684fa53 |
---|---|
cites | cdi_FETCH-LOGICAL-a222t-5ee0c43f73d52fd6121e7c11f01dbb2f4ddb33998dae9796a7b1e1564e684fa53 |
container_end_page | 40464 |
container_issue | 36 |
container_start_page | 40453 |
container_title | ACS applied materials & interfaces |
container_volume | 12 |
creator | Yan, Lifu Wang, Mingchao Zhai, Chenxi Zhao, Lingling Lin, Shangchao |
description | We present a combination of first-principles calculations and the Boltzmann transport theory to understand the carrier transport and thermoelectric performance of mixed halide perovskite alloys CsPb(I1–x Br x )3 with different Br compositions. Our computational results correlate the conduction band splitting in CsPb(I1–x Br x )3 to the significant anisotropy in their carrier transport properties, such as effective masses and deformation potential constants. Such band splitting originates from the symmetry-broken crystal structures of CsPb(I1–x Br x )3 polymorphs: with residue stresses/strains in asymmetric CsPb(I1–x Br x )3, nondegenerate orbitals reconstruct the conduction band and reduce the Pb-halide antibonding character along certain directions. While the Seebeck coefficient (S) and the relaxation time-normalized electrical conductivity (σ/τ) show weak directional anisotropy, the carrier relaxation time (τ) is highly direction-dependent. The reconstruction of the conduction band finally leads to significantly anisotropic and enhanced thermoelectric power factors (PF = S 2σ) in CsPb(I1–x Br x )3 compared to those in pure CsPbI3 and CsPbBr3, showing anomalous nonlinear alloy behavior. A delicate balance between S 2σ and combined measurement of the carrier effective mass and deformation potential constant, m*E DP, is confirmed. The lattice thermal conductivities of CsPb(I1–x Br x )3 are significantly suppressed compared to those of their pure counterparts due to strong mass disordering and strain fields upon halogen substitution. As a result, symmetry breaking in CsPb(I1–x Br x )3 leads to anisotropy in carrier transport, high PF, and scattered phonon transport (ultralow thermal conductivity), concurrently contributing to their promising thermoelectric figures of merit (ZT) up to 1.7 at room temperature. The principles behind the asymmetry-induced factors would serve as new design concepts to tailor the thermoelectric properties of alloys, mixtures, superlattices, and low-dimensional materials. |
doi_str_mv | 10.1021/acsami.0c07501 |
format | article |
fullrecord | <record><control><sourceid>proquest_cross</sourceid><recordid>TN_cdi_proquest_miscellaneous_2434472338</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>2434472338</sourcerecordid><originalsourceid>FETCH-LOGICAL-a222t-5ee0c43f73d52fd6121e7c11f01dbb2f4ddb33998dae9796a7b1e1564e684fa53</originalsourceid><addsrcrecordid>eNp1kM9OwkAQxhujiYpePe8RTcD915YekaiQYDSK52a7O9WVdhdni4Gbr2B8Q5_EEog3TzOZ-X2T-b4oOmO0zyhnl0oHVds-1TSNKduLjlgmZW_AY77_10t5GB2H8EZpIjiNj6Kvp3VdQ4NrcoWg5ta9kIkzSw2GDJ0NvkG_sJqMFKIFJDNULiw8NkQ5Qx6hVjhXRQVk9gpYe6hAN9jyD4Clx1o5DcQ6cmdX7cGxqqyBzc5_hLltIJBReCi6E_bz-b1qHyArci5OooNSVQFOd7UTPd9cz0bj3vT-djIaTnuKc970YgCqpShTYWJemoRxBqlmrKTMFAUvpTGFEFk2MAqyNEtUWjBgcSIhGchSxaITdbd3F-jflxCavLZBQ1UpB34Zci6FlCkXYtCi_S2q0YeAUOYLtK31dc5ovsk-32af77JvBRdbQTvP3_wSXevkP_gXW1aJQA</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>2434472338</pqid></control><display><type>article</type><title>Symmetry Breaking Induced Anisotropic Carrier Transport and Remarkable Thermoelectric Performance in Mixed Halide Perovskites CsPb(I1–x Br x )3</title><source>American Chemical Society:Jisc Collections:American Chemical Society Read & Publish Agreement 2022-2024 (Reading list)</source><creator>Yan, Lifu ; Wang, Mingchao ; Zhai, Chenxi ; Zhao, Lingling ; Lin, Shangchao</creator><creatorcontrib>Yan, Lifu ; Wang, Mingchao ; Zhai, Chenxi ; Zhao, Lingling ; Lin, Shangchao</creatorcontrib><description>We present a combination of first-principles calculations and the Boltzmann transport theory to understand the carrier transport and thermoelectric performance of mixed halide perovskite alloys CsPb(I1–x Br x )3 with different Br compositions. Our computational results correlate the conduction band splitting in CsPb(I1–x Br x )3 to the significant anisotropy in their carrier transport properties, such as effective masses and deformation potential constants. Such band splitting originates from the symmetry-broken crystal structures of CsPb(I1–x Br x )3 polymorphs: with residue stresses/strains in asymmetric CsPb(I1–x Br x )3, nondegenerate orbitals reconstruct the conduction band and reduce the Pb-halide antibonding character along certain directions. While the Seebeck coefficient (S) and the relaxation time-normalized electrical conductivity (σ/τ) show weak directional anisotropy, the carrier relaxation time (τ) is highly direction-dependent. The reconstruction of the conduction band finally leads to significantly anisotropic and enhanced thermoelectric power factors (PF = S 2σ) in CsPb(I1–x Br x )3 compared to those in pure CsPbI3 and CsPbBr3, showing anomalous nonlinear alloy behavior. A delicate balance between S 2σ and combined measurement of the carrier effective mass and deformation potential constant, m*E DP, is confirmed. The lattice thermal conductivities of CsPb(I1–x Br x )3 are significantly suppressed compared to those of their pure counterparts due to strong mass disordering and strain fields upon halogen substitution. As a result, symmetry breaking in CsPb(I1–x Br x )3 leads to anisotropy in carrier transport, high PF, and scattered phonon transport (ultralow thermal conductivity), concurrently contributing to their promising thermoelectric figures of merit (ZT) up to 1.7 at room temperature. The principles behind the asymmetry-induced factors would serve as new design concepts to tailor the thermoelectric properties of alloys, mixtures, superlattices, and low-dimensional materials.</description><identifier>ISSN: 1944-8244</identifier><identifier>EISSN: 1944-8252</identifier><identifier>DOI: 10.1021/acsami.0c07501</identifier><language>eng</language><publisher>American Chemical Society</publisher><subject>Functional Inorganic Materials and Devices</subject><ispartof>ACS applied materials & interfaces, 2020-09, Vol.12 (36), p.40453-40464</ispartof><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a222t-5ee0c43f73d52fd6121e7c11f01dbb2f4ddb33998dae9796a7b1e1564e684fa53</citedby><cites>FETCH-LOGICAL-a222t-5ee0c43f73d52fd6121e7c11f01dbb2f4ddb33998dae9796a7b1e1564e684fa53</cites><orcidid>0000-0002-1532-7247 ; 0000-0002-6810-1380 ; 0000-0003-0245-8472</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,780,784,27924,27925</link.rule.ids></links><search><creatorcontrib>Yan, Lifu</creatorcontrib><creatorcontrib>Wang, Mingchao</creatorcontrib><creatorcontrib>Zhai, Chenxi</creatorcontrib><creatorcontrib>Zhao, Lingling</creatorcontrib><creatorcontrib>Lin, Shangchao</creatorcontrib><title>Symmetry Breaking Induced Anisotropic Carrier Transport and Remarkable Thermoelectric Performance in Mixed Halide Perovskites CsPb(I1–x Br x )3</title><title>ACS applied materials & interfaces</title><addtitle>ACS Appl. Mater. Interfaces</addtitle><description>We present a combination of first-principles calculations and the Boltzmann transport theory to understand the carrier transport and thermoelectric performance of mixed halide perovskite alloys CsPb(I1–x Br x )3 with different Br compositions. Our computational results correlate the conduction band splitting in CsPb(I1–x Br x )3 to the significant anisotropy in their carrier transport properties, such as effective masses and deformation potential constants. Such band splitting originates from the symmetry-broken crystal structures of CsPb(I1–x Br x )3 polymorphs: with residue stresses/strains in asymmetric CsPb(I1–x Br x )3, nondegenerate orbitals reconstruct the conduction band and reduce the Pb-halide antibonding character along certain directions. While the Seebeck coefficient (S) and the relaxation time-normalized electrical conductivity (σ/τ) show weak directional anisotropy, the carrier relaxation time (τ) is highly direction-dependent. The reconstruction of the conduction band finally leads to significantly anisotropic and enhanced thermoelectric power factors (PF = S 2σ) in CsPb(I1–x Br x )3 compared to those in pure CsPbI3 and CsPbBr3, showing anomalous nonlinear alloy behavior. A delicate balance between S 2σ and combined measurement of the carrier effective mass and deformation potential constant, m*E DP, is confirmed. The lattice thermal conductivities of CsPb(I1–x Br x )3 are significantly suppressed compared to those of their pure counterparts due to strong mass disordering and strain fields upon halogen substitution. As a result, symmetry breaking in CsPb(I1–x Br x )3 leads to anisotropy in carrier transport, high PF, and scattered phonon transport (ultralow thermal conductivity), concurrently contributing to their promising thermoelectric figures of merit (ZT) up to 1.7 at room temperature. The principles behind the asymmetry-induced factors would serve as new design concepts to tailor the thermoelectric properties of alloys, mixtures, superlattices, and low-dimensional materials.</description><subject>Functional Inorganic Materials and Devices</subject><issn>1944-8244</issn><issn>1944-8252</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2020</creationdate><recordtype>article</recordtype><recordid>eNp1kM9OwkAQxhujiYpePe8RTcD915YekaiQYDSK52a7O9WVdhdni4Gbr2B8Q5_EEog3TzOZ-X2T-b4oOmO0zyhnl0oHVds-1TSNKduLjlgmZW_AY77_10t5GB2H8EZpIjiNj6Kvp3VdQ4NrcoWg5ta9kIkzSw2GDJ0NvkG_sJqMFKIFJDNULiw8NkQ5Qx6hVjhXRQVk9gpYe6hAN9jyD4Clx1o5DcQ6cmdX7cGxqqyBzc5_hLltIJBReCi6E_bz-b1qHyArci5OooNSVQFOd7UTPd9cz0bj3vT-djIaTnuKc970YgCqpShTYWJemoRxBqlmrKTMFAUvpTGFEFk2MAqyNEtUWjBgcSIhGchSxaITdbd3F-jflxCavLZBQ1UpB34Zci6FlCkXYtCi_S2q0YeAUOYLtK31dc5ovsk-32af77JvBRdbQTvP3_wSXevkP_gXW1aJQA</recordid><startdate>20200909</startdate><enddate>20200909</enddate><creator>Yan, Lifu</creator><creator>Wang, Mingchao</creator><creator>Zhai, Chenxi</creator><creator>Zhao, Lingling</creator><creator>Lin, Shangchao</creator><general>American Chemical Society</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0002-1532-7247</orcidid><orcidid>https://orcid.org/0000-0002-6810-1380</orcidid><orcidid>https://orcid.org/0000-0003-0245-8472</orcidid></search><sort><creationdate>20200909</creationdate><title>Symmetry Breaking Induced Anisotropic Carrier Transport and Remarkable Thermoelectric Performance in Mixed Halide Perovskites CsPb(I1–x Br x )3</title><author>Yan, Lifu ; Wang, Mingchao ; Zhai, Chenxi ; Zhao, Lingling ; Lin, Shangchao</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a222t-5ee0c43f73d52fd6121e7c11f01dbb2f4ddb33998dae9796a7b1e1564e684fa53</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2020</creationdate><topic>Functional Inorganic Materials and Devices</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Yan, Lifu</creatorcontrib><creatorcontrib>Wang, Mingchao</creatorcontrib><creatorcontrib>Zhai, Chenxi</creatorcontrib><creatorcontrib>Zhao, Lingling</creatorcontrib><creatorcontrib>Lin, Shangchao</creatorcontrib><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><jtitle>ACS applied materials & interfaces</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Yan, Lifu</au><au>Wang, Mingchao</au><au>Zhai, Chenxi</au><au>Zhao, Lingling</au><au>Lin, Shangchao</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Symmetry Breaking Induced Anisotropic Carrier Transport and Remarkable Thermoelectric Performance in Mixed Halide Perovskites CsPb(I1–x Br x )3</atitle><jtitle>ACS applied materials & interfaces</jtitle><addtitle>ACS Appl. Mater. Interfaces</addtitle><date>2020-09-09</date><risdate>2020</risdate><volume>12</volume><issue>36</issue><spage>40453</spage><epage>40464</epage><pages>40453-40464</pages><issn>1944-8244</issn><eissn>1944-8252</eissn><abstract>We present a combination of first-principles calculations and the Boltzmann transport theory to understand the carrier transport and thermoelectric performance of mixed halide perovskite alloys CsPb(I1–x Br x )3 with different Br compositions. Our computational results correlate the conduction band splitting in CsPb(I1–x Br x )3 to the significant anisotropy in their carrier transport properties, such as effective masses and deformation potential constants. Such band splitting originates from the symmetry-broken crystal structures of CsPb(I1–x Br x )3 polymorphs: with residue stresses/strains in asymmetric CsPb(I1–x Br x )3, nondegenerate orbitals reconstruct the conduction band and reduce the Pb-halide antibonding character along certain directions. While the Seebeck coefficient (S) and the relaxation time-normalized electrical conductivity (σ/τ) show weak directional anisotropy, the carrier relaxation time (τ) is highly direction-dependent. The reconstruction of the conduction band finally leads to significantly anisotropic and enhanced thermoelectric power factors (PF = S 2σ) in CsPb(I1–x Br x )3 compared to those in pure CsPbI3 and CsPbBr3, showing anomalous nonlinear alloy behavior. A delicate balance between S 2σ and combined measurement of the carrier effective mass and deformation potential constant, m*E DP, is confirmed. The lattice thermal conductivities of CsPb(I1–x Br x )3 are significantly suppressed compared to those of their pure counterparts due to strong mass disordering and strain fields upon halogen substitution. As a result, symmetry breaking in CsPb(I1–x Br x )3 leads to anisotropy in carrier transport, high PF, and scattered phonon transport (ultralow thermal conductivity), concurrently contributing to their promising thermoelectric figures of merit (ZT) up to 1.7 at room temperature. The principles behind the asymmetry-induced factors would serve as new design concepts to tailor the thermoelectric properties of alloys, mixtures, superlattices, and low-dimensional materials.</abstract><pub>American Chemical Society</pub><doi>10.1021/acsami.0c07501</doi><tpages>12</tpages><orcidid>https://orcid.org/0000-0002-1532-7247</orcidid><orcidid>https://orcid.org/0000-0002-6810-1380</orcidid><orcidid>https://orcid.org/0000-0003-0245-8472</orcidid></addata></record> |
fulltext | fulltext |
identifier | ISSN: 1944-8244 |
ispartof | ACS applied materials & interfaces, 2020-09, Vol.12 (36), p.40453-40464 |
issn | 1944-8244 1944-8252 |
language | eng |
recordid | cdi_proquest_miscellaneous_2434472338 |
source | American Chemical Society:Jisc Collections:American Chemical Society Read & Publish Agreement 2022-2024 (Reading list) |
subjects | Functional Inorganic Materials and Devices |
title | Symmetry Breaking Induced Anisotropic Carrier Transport and Remarkable Thermoelectric Performance in Mixed Halide Perovskites CsPb(I1–x Br x )3 |
url | http://sfxeu10.hosted.exlibrisgroup.com/loughborough?ctx_ver=Z39.88-2004&ctx_enc=info:ofi/enc:UTF-8&ctx_tim=2024-12-25T09%3A01%3A01IST&url_ver=Z39.88-2004&url_ctx_fmt=infofi/fmt:kev:mtx:ctx&rfr_id=info:sid/primo.exlibrisgroup.com:primo3-Article-proquest_cross&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.genre=article&rft.atitle=Symmetry%20Breaking%20Induced%20Anisotropic%20Carrier%20Transport%20and%20Remarkable%20Thermoelectric%20Performance%20in%20Mixed%20Halide%20Perovskites%20CsPb(I1%E2%80%93x%20Br%20x%20)3&rft.jtitle=ACS%20applied%20materials%20&%20interfaces&rft.au=Yan,%20Lifu&rft.date=2020-09-09&rft.volume=12&rft.issue=36&rft.spage=40453&rft.epage=40464&rft.pages=40453-40464&rft.issn=1944-8244&rft.eissn=1944-8252&rft_id=info:doi/10.1021/acsami.0c07501&rft_dat=%3Cproquest_cross%3E2434472338%3C/proquest_cross%3E%3Cgrp_id%3Ecdi_FETCH-LOGICAL-a222t-5ee0c43f73d52fd6121e7c11f01dbb2f4ddb33998dae9796a7b1e1564e684fa53%3C/grp_id%3E%3Coa%3E%3C/oa%3E%3Curl%3E%3C/url%3E&rft_id=info:oai/&rft_pqid=2434472338&rft_id=info:pmid/&rfr_iscdi=true |