Practical Witness for Electronic Coherences
arXiv:1408.3121 · doi:10.1063/1.4903982
Abstract
The origin of the coherences in two-dimensional spectroscopy of photosynthetic complexes remains disputed. Recently it has been shown that in the ultrashort-pulse limit, oscillations in a frequency-integrated pump-probe signal correspond exclusively to electronic coherences, and thus such experiments can be used to form a test for electronic vs. vibrational oscillations in such systems. Here we demonstrate a method for practically implementing such a test, whereby pump-probe signals are taken at several different pulse durations and used to extrapolate to the ultrashort-pulse limit. We present analytic and numerical results determining requirements for pulse durations and the optimal choice of pulse central frequency, which can be determined from an absorption spectrum. Our results suggest that for numerous systems the required experiment could be implemented by many ultrafast spectroscopy laboratories using pulses of tens of femtoseconds in duration. Such experiments could resolve the standing debate over the nature of coherences in photosynthetic complexes.
8 pages + 4 pages appendices
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Cited by in corpus (4)
- Numerical Method for Nonlinear Optical Spectroscopies: Ultrafast Ultrafast Spectroscopy
- Multi-color quantum control for suppressing ground state coherences in two-dimensional electronic spectroscopy
- Towards a Spectroscopic Protocol for Unambiguous Detection of Quantum Coherence in Excitonic Energy Transport
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