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Mirsakiyeva, A., Hugosson, H. W., Crispin, X. & Delin, A. (2017). Quantum Molecular Dynamical Calculations of PEDOT 12-Oligomer and its Selenium and Tellurium Derivatives. Paper presented at 35th International Conference on Thermoelectrics (ICT), Wuhan, China, 2016. Journal of Electronic Materials, 46(5), 3071-3075
Open this publication in new window or tab >>Quantum Molecular Dynamical Calculations of PEDOT 12-Oligomer and its Selenium and Tellurium Derivatives
2017 (English)In: Journal of Electronic Materials, ISSN 0361-5235, E-ISSN 1543-186X, Vol. 46, no 5, p. 3071-3075Article in journal (Refereed) Published
Abstract [en]

We present simulation results, computed with the Car–Parrinello molecular dynamics method, at zero and ambient temperature (300 K) for poly(3,4-ethylenedioxythiophene) [PEDOT] and its selenium and tellurium derivatives PEDOS and PEDOTe, represented as 12-oligomer chains. In particular, we focus on structural parameters such as the dihedral rotation angle distribution, as well as how the charge distribution is affected by temperature. We find that for PEDOT, the dihedral angle distribution shows two distinct local maxima whereas for PEDOS and PEDOTe, the distributions only have one clear maximum. The twisting stiffness at ambient temperature appears to be larger the lighter the heteroatom (S, Se, Te) is, in contrast to the case at 0 K. As regards point charge distributions, they suggest that aromaticity increases with temperature, and also that aromaticity becomes more pronounced the lighter the heteroatom is, both at 0 K and ambient temperature. Our results agree well with previous results, where available. The bond lengths are consistent with substantial aromatic character both at 0 K and at ambient temperature. Our calculations also reproduce the expected trend of diminishing gap between the highest occupied molecular orbital and the lowest unoccupied molecular orbital with increasing atomic number of the heteroatom.

Keywords
Aromatization; Atoms; Charge distribution; Density functional theory; Molecular dynamics; Molecular orbitals; Selenium; Tellurium; Tellurium compounds; Temperature, Dynamical calculations; Highest occupied molecular orbital; Lowest unoccupied molecular orbital; Molecular dynamics methods; PEDOS; PEDOT; PEDOTe; Poly-3, 4-ethylenedioxythiophene, Dihedral angle
National Category
Electrical Engineering, Electronic Engineering, Information Engineering
Identifiers
urn:nbn:se:hig:diva-23282 (URN)10.1007/s11664-016-5161-6 (DOI)000398937900075 ()2-s2.0-85001037983 (Scopus ID)
Conference
35th International Conference on Thermoelectrics (ICT), Wuhan, China, 2016
Funder
Swedish Research CouncilThe Royal Swedish Academy of SciencesKnut and Alice Wallenberg FoundationCarl Tryggers foundation Swedish Energy Agency
Note

Funders: Vetenskapsradet (VR), The Royal Swedish Academy of Sciences (KVA), the Knut and Alice Wallenberg Foundation (KAW), Carl Tryggers Stiftelse (CTS), Swedish Energy Agency (STEM), Swedish Foundation for Strategic Research (SSF), and Erasmus Mundus Action 2 TARGET II consortium

Available from: 2017-01-12 Created: 2017-01-11 Last updated: 2018-03-13Bibliographically approved
Mirsakiyeva, A., Hugosson, H. W., Linares, M. & Delin, A. (2017). Temperature dependence of band gaps and conformational disorder in PEDOT and its selenium and tellurium derivatives: Density functional calculations. Journal of Chemical Physics, 147(13), Article ID 134906.
Open this publication in new window or tab >>Temperature dependence of band gaps and conformational disorder in PEDOT and its selenium and tellurium derivatives: Density functional calculations
2017 (English)In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 147, no 13, article id 134906Article in journal (Refereed) Published
Abstract [en]

The conducting polymer poly(3,4-ethylenedioxythiophene), or PEDOT, is an attractive material for flexible electronics. We present combined molecular dynamics and quantum chemical calculations, based on density functional theory, of EDOT oligomers and isoelectronic selenium and tellurium derivatives (EDOS and EDOTe) to address the effect of temperature on the geometrical and electronic properties of these systems. With finite size scaling, we also extrapolate our results to the infinite polymers, i.e., PEDOT, PEDOS, and PEDOTe. Our computations indicate that the most favourable oligomer conformations at finite temperature are conformations around the flat trans-conformation and a non-flat conformation around 45° from the cis-conformation. Also, the dihedral stiffness increases with the atomic number of the heteroatom. We find excellent agreement with experimentally measured gaps for PEDOT and PEDOS. For PEDOT, the gap does not increase with temperature, whereas this is the case for its derivatives. The conformational disorder and the choice of the basis set both significantly affect the calculated gaps.

National Category
Physical Sciences
Identifiers
urn:nbn:se:hig:diva-25412 (URN)10.1063/1.4998509 (DOI)000412321600030 ()28987116 (PubMedID)2-s2.0-85031789300 (Scopus ID)
Funder
Swedish Research CouncilThe Royal Swedish Academy of SciencesKnut and Alice Wallenberg FoundationCarl Tryggers foundation Swedish Energy Agency
Note

Ytterligare finansiär:

Swedish Foundation for Strategic Research (SSF) 

Available from: 2017-10-16 Created: 2017-10-16 Last updated: 2018-03-13Bibliographically approved
Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0001-9970-5710

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