Ultrafast vibronic dynamics of functional organic polymer materials: Coherence, confinement, and disorder

Burghardt, Irene

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https://hdl.handle.net/2142/100542 Copy

Description

Title

Ultrafast vibronic dynamics of functional organic polymer materials: Coherence, confinement, and disorder

Author(s)

Burghardt, Irene

Issue Date

2018-06-18

Keyword(s)

Plenary

Abstract

This talk addresses quantum dynamical studies of ultrafast photo-induced energy and charge transfer in functional organic materials, complementing time-resolved spectroscopic observations [1] which underscore that the elementary transfer events in these molecular aggregate systems can be guided by quantum coherence, despite the presence of static and dynamic disorder. The intricate interplay of electronic delocalization, coherent vibronic dynamics, and trapping phenomena requires a quantum dynamical treatment that goes beyond conventional mixed quantum-classical simulations. 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 [2]. The talk will specifically focus on (i) exciton dissociation and free carrier generation in regioregular donoracceptor 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] A. De Sio and C. Lienau, Phys. Chem. Chem. Phys. 19, 18813 (2017). [2] G. A. Worth, H.-D. Meyer, H. Koppel, L. S. Cederbaum, and I. Burghardt, Int. Rev. Phys. Chem. 27, 569 (2008). [3] M. Polkehn, H. Tamura, P. Eisenbrandt, S. Haacke, S. Mery, and I. Burghardt, J. Phys. Chem. Lett. 7, 1327 (2016). ´ [4] M. Polkehn, P. Eisenbrandt, H. Tamura, and I. Burghardt, Int. J. Quantum Chem. 118:e25502. (2018). [5] M. Polkehn, H. Tamura, and I. Burghardt, J. Phys. B: At. Mol. Opt. Phys. 51, 014003 (2018). [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).

Publisher

International Symposium on Molecular Spectroscopy

Type of Resource

text

Language

eng

Permalink

http://hdl.handle.net/2142/100542

DOI

10.15278/isms.2018.MA02

Copyright and License Information

Copyright 2018 Irene Burghardt

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