Mesoscale quantum dynamics in molecular aggregates
Doran Bennett, Southern Methodist University
Photophysical processes of molecular materials depend on the diffusion of excited-state carriers on the 10 nm to 1 μm length-scale. Spatially resolved non-linear spectroscopies can probe exciton dynamics on this mesoscale, but the corresponding computational simulations remain intractable for most systems of interest. The challenge is two-fold: the number of molecules is massive and yet the material parameters tend to fall into the broad “intermediate regime” where perturbative techniques breakdown. In this talk, I will describe a formally exact quantum dynamics technique my group has developed with the goal of performing mesoscale simulations. I will first present the physical motivation underpinning the theoretical approach and then discuss proof-of-concept calculations on model systems containing 1000 pigments. I will finish with a brief discussion of the strengths/weaknesses of the current technique and our plans for continued development of computational tools for simulating mesoscale quantum dynamics.