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Polaron formation and optical absorption in PEDOT and its selenium and tellurium derivatives: density functional calculations
KTH, School of Engineering Sciences (SCI), Applied Physics.ORCID iD: 0000-0001-9970-5710
KTH, School of Biotechnology (BIO), Theoretical Chemistry and Biology. KTH, Centres, SeRC - Swedish e-Science Research Centre.ORCID iD: 0000-0002-9720-5429
KTH, School of Engineering Sciences (SCI), Applied Physics. KTH, Centres, SeRC - Swedish e-Science Research Centre. Department of Physics and Astronomy, Materials Theory Division, Uppsala University,.
(English)Manuscript (preprint) (Other academic)
Abstract [en]

We present a density functional theory (DFT) study on polaron formation and optical properties of PEDOT and its selenium and tellurium derivatives. Comparing a number of combinations of basis set and approximations to the exchange-correlation functional, we find that the ωB97XD functional is an overall good choice giving well-localized polarons and optical spectra in good agreement with experiment. This functional has the correct long-range  asymptotic behavior, and also includes some short-range Hartree-Fock exchange. Despite the  long-range Hartree-Fock exchange part present in this functional, the spin contamination remains relatively limited and it also stably produces results that are virtually independent of the basis set used.

National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:kth:diva-214935OAI: oai:DiVA.org:kth-214935DiVA, id: diva2:1144229
Note

QC 20170928

Available from: 2017-09-25 Created: 2017-09-25 Last updated: 2017-10-30Bibliographically approved
In thesis
1. Electronic and optical properties of conducting polymers from quantum mechanical computations
Open this publication in new window or tab >>Electronic and optical properties of conducting polymers from quantum mechanical computations
2017 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

    Conductive polymers are also known as "organic metals" due to their semiconducting properties. They are found in a wide range of applications in the field of organic electronics. However, the growing number of experimental works is not widely supported with theoretical calculations. Hence, the field of conductive polymers is experiencing lack of understanding of mechanisms occurring in the polymers. In this PhD thesis, the aim is to increase understanding of conductive polymers by performing theoretical calculations.       

The polymers poly(3,4-ethylenedioxythiophene) (PEDOT) together with its selenium (PEDOS) and tellurium (PEDOTe) derivatives, poly(p-phenylene) (PPP) and naphthobischalcogenadiazoles (NXz) were studied. Several computational methods were applied for analysis of mentioned structures, including density functional theory (DFT), tight-binding modelling (TB), and Car-Parrinello molecular dynamics (CPMD) calculations. The combination of CPMD and DFT calculations was applied to investigate the PEDOT, PEDOS and PEDOTe. The polymers were studied using four different functionals in order to investigate the full picture of structural changes, electronic and optical properties. Temperature effects were studied using molecular dynamics simulations. Wide statistics for structural and molecular orbitals analysis were collected.        

The TB method was employed for PPP. The formation and motion of the excitations, polarons and bipolarons, along the polymer backbone was investigated in presence of electric and magnetic fields. The influence of non-magnetic and magnetic impurities was determined.       

The extended π-conjugated structures of NXz were computed using B3LYP and ωB97XD functionals in combination with the 6-31+G(d) basis set. Here, the structural changes caused by polaron formation were analyzed. The combined analysis of densities of states and absorption spectra was used for understanding of the charge transition.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2017. p. 54
Series
TRITA-FYS, ISSN 0280-316X ; 2017:59
Keyword
density functional theory, DFT, Car-Parrinello molecular dynamics, CPMD, tigh-binding, poly(3, 4-ethylenedioxythiophene), PEDOT, selenium, PEDOS, tellurium, PEDOTe, poly(p-phenylene), poly(para-phenylene), poly(1, 4-phenylene), naphthobischalcogenadiazoles
National Category
Condensed Matter Physics Polymer Chemistry
Research subject
Physics
Identifiers
urn:nbn:se:kth:diva-214979 (URN)978-91-7729-529-7 (ISBN)
Public defence
2017-10-27, Sal C, Kistagången 16, Kista, 10:00 (English)
Opponent
Supervisors
Note

QC 20170928

Available from: 2017-09-28 Created: 2017-09-27 Last updated: 2017-09-28Bibliographically approved

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