Inverting pump-probe spectroscopy for state tomography of excitonic systems
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 this response function to obtain the quantum state of the system, 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.
Document Details
- Document Type
- Pub Defense Publication
- Publication Date
- Apr 22, 2013
- Source ID
- 10.1063/1.4800800
Entities
People
- K. Birgitta Whaley
- Stephan Hoyer
Organizations
- Defense Advanced Research Projects Agency
- University of California