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Title:ULTRAFAST VIBRONIC DYNAMICS OF FUNCTIONAL ORGANIC POLYMER MATERIALS: COHERENCE, CONFINEMENT, AND DISORDER
Author(s):Burghardt, Irene
Subject(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 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. \noindent[1] A. De Sio and C. Lienau, Phys. Chem. Chem. Phys. 19, 18813 (2017). \noindent[2] G. A. Worth, H.-D. Meyer, H. Köppel, L. S. Cederbaum, and I. Burghardt, Int. Rev. Phys. Chem. 27, 569 (2008). \noindent[3] M. Polkehn, H. Tamura, P. Eisenbrandt, S. Haacke, S. Méry, and I. Burghardt, J. Phys. Chem. Lett. 7, 1327 (2016). \noindent[4] M. Polkehn, P. Eisenbrandt, H. Tamura, and I. Burghardt, Int. J. Quantum Chem. 118:e25502. (2018). \noindent[5] M. Polkehn, H. Tamura, and I. Burghardt, J. Phys. B: At. Mol. Opt. Phys. 51, 014003 (2018). \noindent[6] H. Tamura, M. Huix-Rotllant, I. Burghardt, Y. Olivier, and D. Beljonne, Phys. Rev. Lett. 115, 107401 (2015). \noindent[7] R. Binder, M. Polkehn, T. Ma, and I. Burghardt, Chem. Phys. 482, 16 (2017).
Issue Date:06/18/18
Publisher:International Symposium on Molecular Spectroscopy
Citation Info:APS
Genre:Conference Paper / Presentation
Type:Text
Language:English
URI:http://hdl.handle.net/2142/100542
DOI:10.15278/isms.2018.MA02
Other Identifier(s):MA02
Date Available in IDEALS:2018-08-17
2018-12-12


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