Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 7, Issue 3, Pages 382-386Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.5b02793
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Funding
- Max Planck-Society
- excellence cluster The Hamburg Center for Ultrafast Imaging - Structure, Dynamics and Control of Matter at the Atomic Scale - Deutsche Forschungsgemeinschaft
- Joachim Herz-Stiftung (Hamburg) within the PIER Fellowship Program
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We derive a reduced model for the nonadiabatic quantum dynamics of an electronic wave packet moving through a conical intersection in the presence of strong vibrational damping. Starting from the dissipative two-state two-model model, we transform the tuning and the coupling mode to the bath. The resulting quantum two-state model with two highly structured environments is solved numerically exactly in the regime of strong vibrational damping. We find negative cross peaks in the ultrafast optical 2D spectra as clear signatures of the conical intersection. They arise from secondary excitations of the wave packet after having passed through the photophysical energy funnel. This feature is in agreement with recent transient absorption measurements of rhodopsin.
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