High-Dimensional Quantum Dynamics of Functional Organic Polymer Materials: Coherence, Confinement, and Disorder
Invited
Abstract
This talk addresses quantum dynamical studies of ultrafast photo-induced exciton migration and dissociation in functional organic materials, in view of understanding the intricate interplay of electronic delocalization, coherent nonadiabatic dynamics, and trapping phenomena. Our approach combines first-principles parametrized Hamiltonians, based on TDDFT and/or high-level electronic structure calculations, with accurate quantum dynamics simulations using the Multi-Configuration Time-Dependent Hartree (MCTDH) method [1] and its hierarchical multi-layer (ML-MCTDH) variant [2]. The talk will specifically focus on (i) exciton dissociation and free carrier generation in regioregular donor-acceptor assemblies [3-5], (ii) exciton multiplication in acene materials [6] and (iii) the elementary mechanism of exciton migration and creation of charge-transfer excitons in polythiophene and poly-(p-phenylene vinylene) type materials [7]. Special emphasis is placed on the influence of structural (dis)order and molecular packing, which can act as a determining factor in transfer efficiencies. Against this background, we will comment on the role of temporal and spatial coherence along with a consistent description of the transition to a classical-statistical regime.
[1] G. A. Worth, H.-D. Meyer, H. Köppel, L. S. Cederbaum, and I. Burghardt, Int. Rev. Phys. Chem. 27, 569 (2008).
[2] H. Wang, J. Phys. Chem. A 119, 7951 (2015).
[3] M. Polkehn, H. Tamura, P. Eisenbrandt, S. Haacke, S. Méry, and I. Burghardt, J. Phys. Chem. Lett. 7, 1327 (2016).
[4] M. Polkehn, P. Eisenbrandt, H. Tamura, and I. Burghardt, Int. J. Quantum Chem. 2017, https://doi.org/10.1002/qua.25502.
[5] M. Polkehn, H. Tamura, and I. Burghardt, J. Phys. B: At. Mol. Opt. Phys. 2017, https://doi.org/10.1088/1361-6455/aa93d0.
[6] H. Tamura, M. Huix-Rotllant, I. Burghardt, Y. Olivier, and D. Beljonne, Phys. Rev. Lett. 115, 107401 (2015).
[7] R. Binder, M. Polkehn, T. Ma, and I. Burghardt, Chem. Phys. 482, 16 (2017).
[1] G. A. Worth, H.-D. Meyer, H. Köppel, L. S. Cederbaum, and I. Burghardt, Int. Rev. Phys. Chem. 27, 569 (2008).
[2] H. Wang, J. Phys. Chem. A 119, 7951 (2015).
[3] M. Polkehn, H. Tamura, P. Eisenbrandt, S. Haacke, S. Méry, and I. Burghardt, J. Phys. Chem. Lett. 7, 1327 (2016).
[4] M. Polkehn, P. Eisenbrandt, H. Tamura, and I. Burghardt, Int. J. Quantum Chem. 2017, https://doi.org/10.1002/qua.25502.
[5] M. Polkehn, H. Tamura, and I. Burghardt, J. Phys. B: At. Mol. Opt. Phys. 2017, https://doi.org/10.1088/1361-6455/aa93d0.
[6] H. Tamura, M. Huix-Rotllant, I. Burghardt, Y. Olivier, and D. Beljonne, Phys. Rev. Lett. 115, 107401 (2015).
[7] R. Binder, M. Polkehn, T. Ma, and I. Burghardt, Chem. Phys. 482, 16 (2017).
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Presenters
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Irene Burghardt
Institute of Physical and Theoretical Chemistry, Goethe University Frankfurt
Authors
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Irene Burghardt
Institute of Physical and Theoretical Chemistry, Goethe University Frankfurt