A witness for coherent electronic oscillations in ultrafast spectroscopy

Abstract

We report a conceptually straightforward witness that isolates coherent electronic oscillations from their vibronic counterparts in nonlinear optical spectra of molecular aggregates: Coherent oscillations as a function of waiting time in broadband pump/broadband probe spectra correspond to coherent electronic oscillations. Oscillations in individual peaks of 2D electronic spectra do not necessarily yield this conclusion. Our witness is simpler to implement than quantum process tomography and potentially resolves a long-standing controversy on the character of oscillations in ultrafast spectra of photosynthetic light harvesting systems.

4 pages, 2 figures, plus Supplementary Information. Work presented by the first author on March 1, 2012 at APS, Boston, Session W41, Focus Session on Quantum Coherence in Biological Systems

References in corpus (4)

• Environment-Assisted Quantum Walks in Photosynthetic Energy Transfer
• Dephasing assisted transport: Quantum networks and biomolecules
• Vibrational vs. electronic coherences in 2D spectrum of molecular systems
• The nature of the low energy band of the Fenna-Matthews-Olson complex: vibronic signatures

Cited by in corpus (18)

• Does coherence enhance transport in photosynthesis?
• Enhancement of Vibronic and Ground-State Vibrational Coherences in 2D Spectra of Photosynthetic Complexes
• Impact of environmentally induced fluctuations on quantum mechanically mixed electronic and vibrational pigment states in photosynthetic energy transfer and 2D electronic spectra
• Disentangling electronic and vibronic coherences in two-dimensional echo spectra
• Distinguishing electronic and vibronic coherence in 2D spectra by their temperature dependence
• Automatic Feynman diagram generation for nonlinear optical spectroscopies
• Insights into photosynthetic energy transfer gained from free-energy structure: Coherent transport, incoherent hopping, and vibrational assistance revisited
• Practical Witness for Electronic Coherences
• Efficient numerical method for predicting nonlinear optical spectroscopies of open systems
• Transfer of Vibrational Coherence Through Incoherent Energy Transfer Process in Förster Limi
• Multi-color quantum control for suppressing ground state coherences in two-dimensional electronic spectroscopy
• Numerical Method for Nonlinear Optical Spectroscopies: Ultrafast Ultrafast Spectroscopy
• Calculations of coherent two-dimensional electronic spectra using forward and backward stochastic wavefunctions
• Measuring excitation-energy transfer with a real-time time-dependent density functional theory approach
• Towards a Spectroscopic Protocol for Unambiguous Detection of Quantum Coherence in Excitonic Energy Transport
• Influences of quantum mechanically mixed electronic and vibrational pigment states in 2D electronic spectra of photosynthetic systems: Strong electronic coupling cases
• Coherent exciton dynamics in supramolecular light-harvesting nanotubes revealed by ultrafast quantum process tomography
• Toward Witnessing Molecular Exciton Entanglement from Spectroscopy