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Journal article
Exciton Modulation in Perylene-Based Molecular Crystals Upon Formation of a Metal-Organic Interface From Many-Body Perturbation Theory
Frontiers in chemistry, Vol.9, 743391
20/Sep/2021
Abstract
Excited-state processes at organic-inorganic interfaces consisting of molecular crystals are essential in energy conversion applications. While advances in experimental methods allow direct observation and detection of exciton transfer across such junctions, a detailed understanding of the underlying excitonic properties due to crystal packing and interface structure is still largely lacking. In this work, we use many-body perturbation theory to study structure-property relations of excitons in molecular crystals upon adsorption on a gold surface. We explore the case of the experimentally-studied octyl perylene diimide (C8-PDI) as a prototypical system, and use the GW and Bethe-Salpeter equation (BSE) approach to quantify the change in quasiparticle and exciton properties due to intermolecular and substrate screening. Our findings provide a close inspection of both local and environmental structural effects dominating the excitation energies and the exciton binding and nature, as well as their modulation upon the metal-organic interface composition.
Details
- Title
- Exciton Modulation in Perylene-Based Molecular Crystals Upon Formation of a Metal-Organic Interface From Many-Body Perturbation Theory
- Creators
- Liran Shunak - 972WIS_INST___98Olugbenga Adeniran - Wayne State UniversityGuy Voscoboynik - 972WIS_INST___98Zhen-Fei Liu - Wayne State UniversitySivan Refaely-Abramson - 972WIS_INST___98
- Resource Type
- Journal article
- Publication Details
- Frontiers in chemistry, Vol.9, 743391; 20/Sep/2021
- Number of pages
- 9
- Publisher
- Frontiers Media S.A
- Language
- English
- DOI
- https://doi.org/10.3389/fchem.2021.743391
- Grant note
- We thank Boris Rybtchinski and Angelica Elkan for valuable discussions, Mark Vilensky for administrative support, and Diana Qiu and Felipe da Jornada for helpful discussions. This research was supported by a grant from the United States-Israel Binational Science Foundation (BSF), Jerusalem, Israel, awarded to Z-FL and SR-A (Grant Number 2018113). OA acknowledges A. Paul and Carole C. Schaap Endowed Distinguished Graduate Award and Rumble Fellowship from Wayne State University. Z-FL acknowledges start-up funds and an Ebbing faculty development award from Wayne State University. SR-A is an incumbent of the Leah Omenn Career Development Chair, and acknowledges research grants from the Peter and Patricia Gruber Awards and an Alon Fellowship. This research used computational resources within a PRACE Allocation Grant, Project No. 2019204916, at the Barcelona Supercomputing Center (BSC-CNS), as well as at the Chemfarm cluster at the Weizmann Institute of Science and at the Center for Functional Nanomaterials, which is a U.S. Department of Energy Office of Science Facility, at Brookhaven National Laboratory under Contract No. DE-SC0012704. Additional computational resources were provided by the National Energy Research Scientific Computing Center (NERSC), a U.S. Department of Energy Office of Science User Facility operated under Contract No. DE-AC02-05CH11231. LS performed most of the DFT, GW, and GW-BSE computations presented in this work. OA performed the interface calculations using the substrate screening GW approach. GV performed DFT and GW examination to explore additional packing effects. Z-FL constructed and led the substrate screening GW calculations. SR-A is the corresponding author in this work and instructed the DFT, GW, and GW-BSE computations. All authors contributed to the manuscript writing.
- Record Identifier
- 993298747303596
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