Inverting pump-probe spectroscopy for state tomography of excitonic systems
arXiv:1209.6625 · doi:10.1063/1.4800800
Abstract
We propose a two-step protocol for inverting ultrafast spectroscopy experiments on a molecular aggregate to extract the time-evolution of the excited state density matrix. The first step is a deconvolution of the experimental signal to determine a pump-dependent response function. The second step inverts the quantum state of the system from this response function, given a model for how the system evolves following the probe interaction. We demonstrate this inversion analytically and numerically for a dimer model system, and evaluate the feasibility of scaling it to larger molecular aggregates such as photosynthetic protein-pigment complexes. Our scheme provides a direct alternative to the approach of determining all Hamiltonian parameters and then simulating excited state dynamics.
15 pages, 6 figures. This is the accepted version for publication in the Journal of Chemical Physics
References in corpus (8)
- Quantum Process Tomography: Resource Analysis of Different Strategies
- Atomistic study of the long-lived quantum coherences in the Fenna-Matthews-Olson complex
- Exciton dynamics and Quantumness of energy transfer in the Fenna-Matthews-Olson complex
- Conformation of self-assembled porphyrin dimers in liposome vesicles by phase-modulation 2D fluorescence spectroscopy
- Computational Methodologies and Physical Insights into Electronic Energy Transfer in Photosynthetic Light-Harvesting Complexes
- Quantum process tomography of molecular dimers from two-dimensional electronic spectroscopy I: General theory and application to homodimers
- Coherent open-loop optimal control of light-harvesting dynamics
- Spatial propagation of excitonic coherence enables ratcheted energy transfer