Degradation of the ZT thermoelectric figure of merit in silicon when nanostructuring: From bulk to nanowires
Since the landmark paper by Hicks and Dresselhaus [Phys. Rev. B 47, 16631(R) (1993)], there has been a general consensus that one-dimensional nanoscale conductors, i.e. nanowires, provide the long sought paradigm to implement the so-called phonon-glass electron-crystal material, which results in lar...
| Autores: | , , |
|---|---|
| Tipo de recurso: | artículo |
| Estado: | Versión publicada |
| Fecha de publicación: | 2024 |
| País: | España |
| Institución: | Consejo Superior de Investigaciones Científicas (CSIC) |
| Repositorio: | DIGITAL.CSIC. Repositorio Institucional del CSIC |
| OAI Identifier: | oai:digital.csic.es:10261/364554 |
| Acceso en línea: | http://hdl.handle.net/10261/364554 https://api.elsevier.com/content/abstract/scopus_id/85186771496 |
| Access Level: | acceso abierto |
| Palabra clave: | Coupled e-ph Boltzmann transport equation Nanowires Phonon drag Thermoelectrics ZT |
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Degradation of the ZT thermoelectric figure of merit in silicon when nanostructuring: From bulk to nanowires |
| title |
Degradation of the ZT thermoelectric figure of merit in silicon when nanostructuring: From bulk to nanowires |
| spellingShingle |
Degradation of the ZT thermoelectric figure of merit in silicon when nanostructuring: From bulk to nanowires Raya Moreno, Martí Coupled e-ph Boltzmann transport equation Nanowires Phonon drag Thermoelectrics ZT |
| title_short |
Degradation of the ZT thermoelectric figure of merit in silicon when nanostructuring: From bulk to nanowires |
| title_full |
Degradation of the ZT thermoelectric figure of merit in silicon when nanostructuring: From bulk to nanowires |
| title_fullStr |
Degradation of the ZT thermoelectric figure of merit in silicon when nanostructuring: From bulk to nanowires |
| title_full_unstemmed |
Degradation of the ZT thermoelectric figure of merit in silicon when nanostructuring: From bulk to nanowires |
| title_sort |
Degradation of the ZT thermoelectric figure of merit in silicon when nanostructuring: From bulk to nanowires |
| dc.creator.none.fl_str_mv |
Raya Moreno, Martí Rurali, Riccardo Cartoixà, Xavier |
| author |
Raya Moreno, Martí |
| author_facet |
Raya Moreno, Martí Rurali, Riccardo Cartoixà, Xavier |
| author_role |
author |
| author2 |
Rurali, Riccardo Cartoixà, Xavier |
| author2_role |
author author |
| dc.contributor.none.fl_str_mv |
Ministerio de Ciencia, Innovación y Universidades (España) Agencia Estatal de Investigación (España) Generalitat de Catalunya Ministerio de Ciencia e Innovación (España) Raya Moreno, Martí [0000-0001-6190-9769] Rurali, Riccardo [0000-0002-4086-4191] Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72] |
| dc.subject.none.fl_str_mv |
Coupled e-ph Boltzmann transport equation Nanowires Phonon drag Thermoelectrics ZT |
| topic |
Coupled e-ph Boltzmann transport equation Nanowires Phonon drag Thermoelectrics ZT |
| description |
Since the landmark paper by Hicks and Dresselhaus [Phys. Rev. B 47, 16631(R) (1993)], there has been a general consensus that one-dimensional nanoscale conductors, i.e. nanowires, provide the long sought paradigm to implement the so-called phonon-glass electron-crystal material, which results in large improvements in the thermoelectric figure of merit ZT. Despite some encouraging—though isolated—experimental results, this idea has never been subjected to a rigorous scrutiny and the effect of the coupled dynamics of electrons and phonons has usually been oversimplified. To bypass these limitations, we have calculated the effective thermoelectric parameters for silicon nanowires (SiNWs) by iteratively solving the coupled electron-phonon Boltzmann transport equation (EPBTE) supplied with first-principles data. This allows for an unprecedented precision in determining the correct dependence of the thermoelectric parameters with system size; including, but not limited to, the figure of merit and its enhancement or degradation due to nanostructuring. Indeed, we demonstrate that the commonly used relaxation time approximation (RTA), or the uncoupled beyond the RTA (iterative) solution fail to describe the correct effect of nanostructuring on the thermoelectric properties and efficiency in SiNWs due to the strong contribution of phonon drag to the Seebeck coefficient, so that the use of fully coupled solution of the EPBTE is essential to obtain the correct effect of nanostructuring. Most importantly, we show that, contrarily to what commonly argued, resorting to NWs is not necessarily beneficial for ZT. Indeed, in a wide range of diameters nanostructuring diminishes the Seebeck coefficient faster than the decrease in thermal conductivity, due to the suppression of very long wavelength phonons responsible for the largest contribution to the phonon drag component of the Seebeck coefficient. This penalty to ZT can be mitigated if the NWs have a very rough surface, providing additional reduction to the thermal conductivity. Additionally, we demonstrate that our methodology provides improved data sets for an accurate determination of doping concentration in NWs through electrical-based inference and excellent agreement with the available experimental data. |
| publishDate |
2024 |
| dc.date.none.fl_str_mv |
2024 2024 2024 |
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info:eu-repo/semantics/article http://purl.org/coar/resource_type/c_6501 Publisher's version info:eu-repo/semantics/publishedVersion |
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article |
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publishedVersion |
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http://hdl.handle.net/10261/364554 https://api.elsevier.com/content/abstract/scopus_id/85186771496 |
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http://hdl.handle.net/10261/364554 https://api.elsevier.com/content/abstract/scopus_id/85186771496 |
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Inglés |
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Inglés |
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Elsevier |
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Elsevier |
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Degradation of the ZT thermoelectric figure of merit in silicon when nanostructuring: From bulk to nanowiresRaya Moreno, MartíRurali, RiccardoCartoixà, XavierCoupled e-ph Boltzmann transport equationNanowiresPhonon dragThermoelectricsZTSince the landmark paper by Hicks and Dresselhaus [Phys. Rev. B 47, 16631(R) (1993)], there has been a general consensus that one-dimensional nanoscale conductors, i.e. nanowires, provide the long sought paradigm to implement the so-called phonon-glass electron-crystal material, which results in large improvements in the thermoelectric figure of merit ZT. Despite some encouraging—though isolated—experimental results, this idea has never been subjected to a rigorous scrutiny and the effect of the coupled dynamics of electrons and phonons has usually been oversimplified. To bypass these limitations, we have calculated the effective thermoelectric parameters for silicon nanowires (SiNWs) by iteratively solving the coupled electron-phonon Boltzmann transport equation (EPBTE) supplied with first-principles data. This allows for an unprecedented precision in determining the correct dependence of the thermoelectric parameters with system size; including, but not limited to, the figure of merit and its enhancement or degradation due to nanostructuring. Indeed, we demonstrate that the commonly used relaxation time approximation (RTA), or the uncoupled beyond the RTA (iterative) solution fail to describe the correct effect of nanostructuring on the thermoelectric properties and efficiency in SiNWs due to the strong contribution of phonon drag to the Seebeck coefficient, so that the use of fully coupled solution of the EPBTE is essential to obtain the correct effect of nanostructuring. Most importantly, we show that, contrarily to what commonly argued, resorting to NWs is not necessarily beneficial for ZT. Indeed, in a wide range of diameters nanostructuring diminishes the Seebeck coefficient faster than the decrease in thermal conductivity, due to the suppression of very long wavelength phonons responsible for the largest contribution to the phonon drag component of the Seebeck coefficient. This penalty to ZT can be mitigated if the NWs have a very rough surface, providing additional reduction to the thermal conductivity. Additionally, we demonstrate that our methodology provides improved data sets for an accurate determination of doping concentration in NWs through electrical-based inference and excellent agreement with the available experimental data.M.R-M and R.R acknowledge financial support from MCIN/AEI/10.13039/501100011033 under grant PID2020-119777GB-I00 , and the Severo Ochoa Centres of Excellence Program under grant CEX2019-000917-S , and by the Generalitat de Catalunya under grant 2021 SGR 01519 . X.C acknowledges financial support by Spain's Ministerio de Ciencia, Innovación y Universidades under Grant No. RTI2018-097876-B-C21 (MCIU/AEI/FEDER, UE), and Ministerio de Ciencia e Innovación under Grant No. PID2021-127840NB-I00 (MICINN/AEI/FEDER, UE). The authors thankfully acknowledge the computer resources, technical expertise and assistance provided by the Centro de Supercomputación de Galicia (CESGA).With funding from the Spanish government through the ‘Severo Ochoa Centre of Excellence’ accreditation (CEX2019-000917-S).Peer reviewedElsevierMinisterio de Ciencia, Innovación y Universidades (España)Agencia Estatal de Investigación (España)Generalitat de CatalunyaMinisterio de Ciencia e Innovación (España)Raya Moreno, Martí [0000-0001-6190-9769]Rurali, Riccardo [0000-0002-4086-4191]Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202420242024info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Publisher's versioninfo:eu-repo/semantics/publishedVersionhttp://hdl.handle.net/10261/364554https://api.elsevier.com/content/abstract/scopus_id/85186771496reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/MICIU/Plan Estatal de investigación Científica y Técnica y de Innovación 2017-2020/PID2020-119777GB-I00 ,info:eu-repo/grantAgreement/AEI/Plan Estatal de investigación Científica y Técnica y de Innovación 2017-2020/CEX2019-000917-Sinfo:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/RTI2018-097876-B-C21info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2021-2023/PID2021-127840NB-I00International Journal of Heat and Mass Transferhttp://doi.org/10.1016/j.ijheatmasstransfer.2024.125385Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/3645542026-05-22T06:33:51Z |
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15,811543 |