Cargando…

Conformation and Quantum-Interference-Enhanced Thermoelectric Properties of Diphenyl Diketopyrrolopyrrole Derivatives

[Image: see text] Manipulating the connectivity of external electrodes to central rings of carbon-based molecules in single molecule junctions is an effective route to tune their thermoelectrical properties. Here we investigate the connectivity dependence of the thermoelectric properties of a series...

Descripción completa

Detalles Bibliográficos
Autores principales: Almughathawi, Renad, Hou, Songjun, Wu, Qingqing, Liu, Zitong, Hong, Wenjing, Lambert, Colin
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2020
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8021221/
https://www.ncbi.nlm.nih.gov/pubmed/33382942
http://dx.doi.org/10.1021/acssensors.0c02043
_version_ 1783674710537535488
author Almughathawi, Renad
Hou, Songjun
Wu, Qingqing
Liu, Zitong
Hong, Wenjing
Lambert, Colin
author_facet Almughathawi, Renad
Hou, Songjun
Wu, Qingqing
Liu, Zitong
Hong, Wenjing
Lambert, Colin
author_sort Almughathawi, Renad
collection PubMed
description [Image: see text] Manipulating the connectivity of external electrodes to central rings of carbon-based molecules in single molecule junctions is an effective route to tune their thermoelectrical properties. Here we investigate the connectivity dependence of the thermoelectric properties of a series of thiophene-diketopyrrolopyrrole (DPP) derivative molecules using density functional theory and tight-binding modeling, combined with quantum transport theory. We find a significant dependence of electrical conductance on the connectivity of the two thiophene rings attached to the DPP core. Interestingly, for connectivities corresponding to constructive quantum interference (CQI), different isomers obtained by rotating the thiophene rings possess the same electrical conductance while those corresponding to destructive quantum interference (DQI) show huge conductance variations upon ring rotation. Furthermore, we find that DQI connectivity leads to enhanced Seebeck coefficients, which can reach 500–700 μV/K. After including the contribution to the thermal conductance from phonons, the full figure of merit (ZT) for the CQI molecules could reach 1.5 at room temperature and it would further increase to 2 when temperature elevates to 400 K. Finally, we demonstrate that doping with tetracyanoquinodimethane can change the sign of the Seebeck coefficients by forming a charge-transfer system with the DPP.
format Online
Article
Text
id pubmed-8021221
institution National Center for Biotechnology Information
language English
publishDate 2020
publisher American Chemical Society
record_format MEDLINE/PubMed
spelling pubmed-80212212021-04-06 Conformation and Quantum-Interference-Enhanced Thermoelectric Properties of Diphenyl Diketopyrrolopyrrole Derivatives Almughathawi, Renad Hou, Songjun Wu, Qingqing Liu, Zitong Hong, Wenjing Lambert, Colin ACS Sens [Image: see text] Manipulating the connectivity of external electrodes to central rings of carbon-based molecules in single molecule junctions is an effective route to tune their thermoelectrical properties. Here we investigate the connectivity dependence of the thermoelectric properties of a series of thiophene-diketopyrrolopyrrole (DPP) derivative molecules using density functional theory and tight-binding modeling, combined with quantum transport theory. We find a significant dependence of electrical conductance on the connectivity of the two thiophene rings attached to the DPP core. Interestingly, for connectivities corresponding to constructive quantum interference (CQI), different isomers obtained by rotating the thiophene rings possess the same electrical conductance while those corresponding to destructive quantum interference (DQI) show huge conductance variations upon ring rotation. Furthermore, we find that DQI connectivity leads to enhanced Seebeck coefficients, which can reach 500–700 μV/K. After including the contribution to the thermal conductance from phonons, the full figure of merit (ZT) for the CQI molecules could reach 1.5 at room temperature and it would further increase to 2 when temperature elevates to 400 K. Finally, we demonstrate that doping with tetracyanoquinodimethane can change the sign of the Seebeck coefficients by forming a charge-transfer system with the DPP. American Chemical Society 2020-12-31 2021-02-26 /pmc/articles/PMC8021221/ /pubmed/33382942 http://dx.doi.org/10.1021/acssensors.0c02043 Text en © 2020 American Chemical Society Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Almughathawi, Renad
Hou, Songjun
Wu, Qingqing
Liu, Zitong
Hong, Wenjing
Lambert, Colin
Conformation and Quantum-Interference-Enhanced Thermoelectric Properties of Diphenyl Diketopyrrolopyrrole Derivatives
title Conformation and Quantum-Interference-Enhanced Thermoelectric Properties of Diphenyl Diketopyrrolopyrrole Derivatives
title_full Conformation and Quantum-Interference-Enhanced Thermoelectric Properties of Diphenyl Diketopyrrolopyrrole Derivatives
title_fullStr Conformation and Quantum-Interference-Enhanced Thermoelectric Properties of Diphenyl Diketopyrrolopyrrole Derivatives
title_full_unstemmed Conformation and Quantum-Interference-Enhanced Thermoelectric Properties of Diphenyl Diketopyrrolopyrrole Derivatives
title_short Conformation and Quantum-Interference-Enhanced Thermoelectric Properties of Diphenyl Diketopyrrolopyrrole Derivatives
title_sort conformation and quantum-interference-enhanced thermoelectric properties of diphenyl diketopyrrolopyrrole derivatives
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8021221/
https://www.ncbi.nlm.nih.gov/pubmed/33382942
http://dx.doi.org/10.1021/acssensors.0c02043
work_keys_str_mv AT almughathawirenad conformationandquantuminterferenceenhancedthermoelectricpropertiesofdiphenyldiketopyrrolopyrrolederivatives
AT housongjun conformationandquantuminterferenceenhancedthermoelectricpropertiesofdiphenyldiketopyrrolopyrrolederivatives
AT wuqingqing conformationandquantuminterferenceenhancedthermoelectricpropertiesofdiphenyldiketopyrrolopyrrolederivatives
AT liuzitong conformationandquantuminterferenceenhancedthermoelectricpropertiesofdiphenyldiketopyrrolopyrrolederivatives
AT hongwenjing conformationandquantuminterferenceenhancedthermoelectricpropertiesofdiphenyldiketopyrrolopyrrolederivatives
AT lambertcolin conformationandquantuminterferenceenhancedthermoelectricpropertiesofdiphenyldiketopyrrolopyrrolederivatives