Linear, third- and fifth-order nonlinear spectroscopy of a charge transfer system coupled to an underdamped vibration
arXiv:1502.06410 · doi:10.1063/1.4917025
Abstract
We study hole, electron and exciton transport in a charge transfer system in the presence of underdamped vibrational motion. We analyze the signature of these processes in the linear and third-, and fifth-order nonlinear electronic spectra. Calculations are performed with a numerically exact hierarchical equations of motion method for an underdamped Brownian oscillator spectral density. We find that combining electron, hole and exciton transfer can lead to non-trivial spectra with more structure than with excitonic coupling alone. Traces taken during the waiting time of a two-dimensional spectrum are dominated by vibrational motion and do not reflect the electron, hole, and exciton dynamics directly. We find that the fifth-order nonlinear response is particularly sensitive to the charge transfer process. While third-order 2D spectroscopy detects the correlation between two coherences, fifth-order 2D spectroscopy (2D population spectroscopy) is here designed to detect correlations between the excited states during two different time periods.
References in corpus (7)
- Dephasing assisted transport: Quantum networks and biomolecules
- Long-Lived Electronic Coherence in Dissipative Exciton-Dynamics of Light-Harvesting Complexes
- Reduced hierarchical equations of motion in real and imaginary time: Correlated initial states and thermodynamic quantities
- High-performance solution of hierarchical equations of motions for studying energy-transfer in light-harvesting complexes
- On the alternatives for bath correlators and spectral densities from mixed quantum-classical simulations
- Real-Time and Imaginary-Time Quantum Hierarchal Fokker-Planck Equations
- An approach to quantum transport based on reduced hierarchy equations of motion: Application to a resonant tunneling diode