Multiorbital exciton formation in an organic semiconductor

Fuente: arXiv
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Auteurs principaux: Bennecke, Wiebke, Windischbacher, Andreas, Schmitt, David, Bange, Jan Philipp, Hemm, Ralf, Kern, Christian S., D`Avino, Gabriele, Blase, Xavier, Steil, Daniel, Steil, Sabine, Aeschlimann, Martin, Stadtmueller, Benjamin, Reutzel, Marcel, Puschnig, Peter, Jansen, G. S. Matthijs, Mathias, Stefan
Format: Preprint
Publié: 2023
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author Bennecke, Wiebke
Windischbacher, Andreas
Schmitt, David
Bange, Jan Philipp
Hemm, Ralf
Kern, Christian S.
D`Avino, Gabriele
Blase, Xavier
Steil, Daniel
Steil, Sabine
Aeschlimann, Martin
Stadtmueller, Benjamin
Reutzel, Marcel
Puschnig, Peter
Jansen, G. S. Matthijs
Mathias, Stefan
author_facet Bennecke, Wiebke
Windischbacher, Andreas
Schmitt, David
Bange, Jan Philipp
Hemm, Ralf
Kern, Christian S.
D`Avino, Gabriele
Blase, Xavier
Steil, Daniel
Steil, Sabine
Aeschlimann, Martin
Stadtmueller, Benjamin
Reutzel, Marcel
Puschnig, Peter
Jansen, G. S. Matthijs
Mathias, Stefan
contents Harnessing the optoelectronic response of organic semiconductors requires a thorough understanding of the fundamental light-matter interaction that is dominated by the excitation of correlated electron-hole pairs, i.e. excitons. The nature of these excitons would be fully captured by knowing the quantum-mechanical wavefunction, which, however, is difficult to access both theoretically and experimentally. Here, we use femtosecond photoemission orbital tomography in combination with many-body perturbation theory to gain access to exciton wavefunctions in organic semiconductors. We find that the coherent sum of multiple electron-hole pair contributions that typically make up a single exciton can be experimentally evidenced by photoelectron spectroscopy. For the prototypical organic semiconductor buckminsterfullerene (C$_{60}$), we show how to disentangle such multiorbital contributions and thereby access key properties of the exciton wavefunctions including localization, charge-transfer character, and ultrafast exciton formation and relaxation dynamics.
format Preprint
id arxiv_https___arxiv_org_abs_2303_13904
institution arXiv
publishDate 2023
record_format arxiv
spellingShingle Multiorbital exciton formation in an organic semiconductor
Bennecke, Wiebke
Windischbacher, Andreas
Schmitt, David
Bange, Jan Philipp
Hemm, Ralf
Kern, Christian S.
D`Avino, Gabriele
Blase, Xavier
Steil, Daniel
Steil, Sabine
Aeschlimann, Martin
Stadtmueller, Benjamin
Reutzel, Marcel
Puschnig, Peter
Jansen, G. S. Matthijs
Mathias, Stefan
Mesoscale and Nanoscale Physics
Harnessing the optoelectronic response of organic semiconductors requires a thorough understanding of the fundamental light-matter interaction that is dominated by the excitation of correlated electron-hole pairs, i.e. excitons. The nature of these excitons would be fully captured by knowing the quantum-mechanical wavefunction, which, however, is difficult to access both theoretically and experimentally. Here, we use femtosecond photoemission orbital tomography in combination with many-body perturbation theory to gain access to exciton wavefunctions in organic semiconductors. We find that the coherent sum of multiple electron-hole pair contributions that typically make up a single exciton can be experimentally evidenced by photoelectron spectroscopy. For the prototypical organic semiconductor buckminsterfullerene (C$_{60}$), we show how to disentangle such multiorbital contributions and thereby access key properties of the exciton wavefunctions including localization, charge-transfer character, and ultrafast exciton formation and relaxation dynamics.
title Multiorbital exciton formation in an organic semiconductor
topic Mesoscale and Nanoscale Physics
url https://arxiv.org/abs/2303.13904