Low exciton binding energies from computational predictions de Gier, Hilde Dorothea
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1 Low exciton binding energies from computational predictions de Gier, Hilde Dorothea IMPORTANT NOTE: You are advised to consult the publisher's version (publisher's PDF) if you wish to cite from it. Please check the document version below. Document Version Publisher's PDF, also known as Version of record Publication date: 2016 Link to publication in University of Groningen/UMCG research database Citation for published version (APA): de Gier, H. D. (2016). Low exciton binding energies from computational predictions: Towards the next generation of organic photovoltaics [Groningen]: University of Groningen Copyright Other than for strictly personal use, it is not permitted to download or to forward/distribute the text or part of it without the consent of the author(s) and/or copyright holder(s), unless the work is under an open content license (like Creative Commons). Take-down policy If you believe that this document breaches copyright please contact us providing details, and we will remove access to the work immediately and investigate your claim. Downloaded from the University of Groningen/UMCG research database (Pure): For technical reasons the number of authors shown on this cover page is limited to 10 maximum. Download date:
2 Low exciton binding energies from computational predictions Towards the next generation of organic photovoltaics Hilde D. de Gier
3 Low exciton binding energies from computational predictions Towards the next generation of organic photovoltaics Hilde D. de Gier PhD thesis University of Groningen The Netherlands Zernike Institute PhD thesis series ISSN: ISBN: ISBN: printed version electronic version The research presented in this thesis was performed in the research group Theoretical Chemistry of the Zernike Institute for Advanced Materials at the University of Groningen, The Netherlands. Parts of the work were carried out at the Dutch National Supercomputers Huygens and Cartesius with grants from The Netherlands escience Center and at the Titan Supercomputer at the Oak Ridge Leadership Computing Facility (USA) through an INCITE-DD grant. This PhD project was funded by the Foundation of Fundamental Research on Matter (FOM), which is part of The Netherlands Organisation for Scientific Research (NWO). This is a publication of the FOM-focus group Next Generation Organic Photovoltaics, participating in the Dutch Institute for Fundamental Energy Research (DIFFER) Hilde D. de Gier Printed by Gildeprint Drukkerijen Enschede
4 Low exciton binding energies from computational predictions Towards the next generation of organic photovoltaics Proefschrift ter verkrijging van de graad van doctor aan de Rijksuniversiteit Groningen op gezag van de rector magnificus prof. dr. E. Sterken en volgens besluit van het College voor Promoties. De openbare verdediging zal plaatsvinden op maandag 1 februari 2016 om uur door Hilde Dorothea de Gier geboren op 13 mei 1988 te Dongeradeel
5 Promotores Prof. dr. H.B. Broer-Braam Prof. dr. J.C. Hummelen Copromotor Dr. R.W.A. Havenith Beoordelingscommissie Prof. dr. S.J. Marrink Prof. dr. A. Meijerink Prof. dr. M.A. Ratner
6 C est le temps que tu as perdu pour ta rose qui fait ta rose si importante. Le Petit Prince, 1943 Antoine de Saint-Exupéry Aan mijn grootouders Pie en Rein die met mij meegaan
7
8 Contents 1 Introduction into the field of organic photovoltaics Technology and energy market Operating principle Device architecture Typical donor and acceptor molecules Models for the description of electronic properties Photovoltaic process Exciton binding energy and charge-transfer exciton binding energy Proposed mechanisms for charge separation Aim and approach of the research programme Aim of the theoretical research within the programme and thesis outline References 31 2 Theory Schrödinger equation Born-Oppenheimer approximation Pauli principle Hartree-Fock theory Post Hartree-Fock methods Configuration interaction Multiconfiguration and multireference theories Møller-Plesset many-body perturbation theory Coupled-cluster theory Density Functional Theory Hohenberg-Kohn theorems Kohn-Sham theory Exchange-correlation hole Approximations to the functional for the exchange-correlation energy Self-interaction Time-dependent Density Functional Theory Runge-Gross theorem and time-dependent Kohn-Sham equation Known failures 50
9 Charge-transfer excitations Valence Bond theory Band theory Molecular Dynamics Computational modelling of organic photovoltaics Multiscale modelling Modelling the molecular environment Motivation for the (TD-)DFT approach applied in the studies described in this thesis References 60 3 Non-innocent side-chains with dipole moments in organic solar cells improve charge separation Introduction Computational details Results and discussion Geometry of the central donor-acceptor complex Results for the donor-acceptor complex Results for the donor-acceptor complex Conclusions Acknowledgements References 79 4 Promising strategy to improve charge separation in organic photovoltaics: installing permanent dipoles in PCBM analogues Introduction Computational details Results and discussion Comparison between experimental and calculated electronic and optical properties Isotropic polarisabilities and dipole moments Electronic state diagrams Conclusions Acknowledgements References 97
10 5 Influence of push-pull group substitution patterns on excited state properties of donor-acceptor co-monomers and their trimers Introduction Computational details Results and discussion Monomers Geometries Molecular orbitals Excited state properties Properties relevant for OPV applications Trimers Geometries Molecular orbitals Excited state properties Properties relevant for OPV applications Conclusions Acknowledgements References On the relation between local and charge-transfer exciton binding energies in organic photovoltaic materials Introduction Computational details Charge transfer and charge separation upon excitation Effect of an embedding on the vertical local exciton binding energy Monomer-PCBM complexes Results and discussion Charge transfer and charge separation upon excitation Monomers Trimers Effect of an embedding on the vertical local exciton binding energy Monomer-PCBM complexes Excited state properties Charge-transfer exciton binding energies Conclusions Acknowledgements 146
11 6.6 References Outlook Worm s eye view Bird s eye view Future perspective for organic photovoltaics References 156 Appendix A 159 A.1 Analysis of the TD-DFT (BHandH/DZP) calculations of 1-3 in vacuum, embedded in 4 and embedded in A.2 Analysis of the TD-DFT (BHandH/DZP) calculations of 2-3 in vacuum, embedded in 4 and embedded in A.3 Analysis of the TD-DFT (CAMYB3LYP/DZP) calculation of 1-3 in vacuum 165 Appendix B 167 B.1 Analysis of the TD-DFT (BHandH/DZP) calculations of Si-CPDTBT-PCBDN in vacuum, embedded in PCBBz and embedded in PCBDN 167 Summary 171 Samenvatting 175 Curriculum Vitae 179 Acknowledgements 181
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