Two-dimensional electronic spectroscopy (2DES) can be realized in increasing nonlinear orders of interaction with the electric field, bringing new information about single- and multi-particle properties and dynamics. Furthermore, signals can be detected both coherently (C-2DES) and by fluorescence (F-2DES), with fundamental and practical differences. We directly compare the simultaneous measurements of four- and six-wave mixing C-2DES and F-2DES on an excitonic heterodimer of squaraine molecules. Spectral features are described in increasing orders of nonlinearity by an explicit excitonic model. We demonstrate that the four-wave-mixing spectra are sensitive to one-exciton energies, their delocalization and dynamics, while the six-wave-mixing spectra include information on bi-exciton and higher excited states including the state energies, electronic coupling, and exciton–exciton annihilation. We focus on the possibility to extract the dynamics arising from exciton–exciton interaction directly from the six-wave-mixing spectra. To this end, in analogy to previously demonstrated fifth-order coherently detected exciton–exciton-interaction 2DES (EEI2D spectroscopy), we introduce a sixth-order fluorescence-detected EEI2D spectroscopy variant.
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14 October 2020
Research Article|
October 14 2020
Signatures of exciton dynamics and interaction in coherently and fluorescence-detected four- and six-wave-mixing two-dimensional electronic spectroscopy
Special Collection:
Excitons: Energetics and Spatio-temporal Dynamics
Pavel Malý
;
Pavel Malý
1
Institut für Physikalische und Theoretische Chemie, Universität Würzburg
, Am Hubland, 97074 Würzburg, Germany
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Stefan Mueller;
Stefan Mueller
1
Institut für Physikalische und Theoretische Chemie, Universität Würzburg
, Am Hubland, 97074 Würzburg, Germany
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Julian Lüttig;
Julian Lüttig
1
Institut für Physikalische und Theoretische Chemie, Universität Würzburg
, Am Hubland, 97074 Würzburg, Germany
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Christoph Lambert
;
Christoph Lambert
2
Institut für Organische Chemie, Universität Würzburg
, Am Hubland, 97074 Würzburg, Germany
3
Center for Nanosystems Chemistry (CNC), Universität Würzburg
, Theodor-Boveri-Weg, 97074 Würzburg, Germany
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Tobias Brixner
Tobias Brixner
a)
1
Institut für Physikalische und Theoretische Chemie, Universität Würzburg
, Am Hubland, 97074 Würzburg, Germany
3
Center for Nanosystems Chemistry (CNC), Universität Würzburg
, Theodor-Boveri-Weg, 97074 Würzburg, Germany
a)Author to whom correspondence should be addressed: [email protected]
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Pavel Malý
1
Stefan Mueller
1
Julian Lüttig
1
Christoph Lambert
2,3
Tobias Brixner
1,3,a)
1
Institut für Physikalische und Theoretische Chemie, Universität Würzburg
, Am Hubland, 97074 Würzburg, Germany
2
Institut für Organische Chemie, Universität Würzburg
, Am Hubland, 97074 Würzburg, Germany
3
Center for Nanosystems Chemistry (CNC), Universität Würzburg
, Theodor-Boveri-Weg, 97074 Würzburg, Germany
a)Author to whom correspondence should be addressed: [email protected]
Note: This paper is part of the JCP Special Topic on Excitons: Energetics and Spatio-temporal Dynamics.
J. Chem. Phys. 153, 144204 (2020)
Article history
Received:
July 23 2020
Accepted:
September 25 2020
Citation
Pavel Malý, Stefan Mueller, Julian Lüttig, Christoph Lambert, Tobias Brixner; Signatures of exciton dynamics and interaction in coherently and fluorescence-detected four- and six-wave-mixing two-dimensional electronic spectroscopy. J. Chem. Phys. 14 October 2020; 153 (14): 144204. https://doi.org/10.1063/5.0022743
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