Technique - (2) Theoretical Modeling of Vibronic Exciton Coherence in Molecular Aggregates

Type: Theoretical

Description: Surface-hopping and vibronic-exciton theoretical methods for simulating two-dimensional electronic spectroscopy, used to explain how vibronic coupling sustains excitonic quantum coherence in photosynthetic light-harvesting complexes and organic semiconductor aggregates.

Department(s)/lab(s): School of Chemistry | Kassal Group @ USyd
Summary:

Kassal is the leading Australian theorist of quantum effects in light harvesting. He established the distinction between coherent processes and coherent states in photosynthesis — showing that under incoherent sunlight at steady state, wavelike motion per se does not enhance efficiency, while environment-assisted transport and supertransfer genuinely can — and has since developed a classification of the mechanisms by which coherence (excitonic, vibrational, or of the light field itself) can improve energy transport. He also pioneered quantum-computer algorithms for chemistry. A distinct and directly relevant thread is the theory of spectroscopy with non-classical light: what entangled or squeezed photons can reveal about molecular coherence that classical light cannot. Positioned against the established body of NV-ensemble quantum sensing work — DEER, nanoscale NMR and T1 relaxometry protocols operating at pT/sqrt(Hz) field sensitivity — his work is the theoretical counterpart to the quantum-biology ambitions of the NV community: where NV ensembles at pT/sqrt(Hz) try to detect the magnetic signatures of biological spin chemistry, Kassal asks what quantum coherence is actually doing in those systems and whether quantum light can interrogate it.

Department(s)/lab(s): Chemistry | Tempelaar Team @ Northwestern
Summary:

Tempelaar develops theory and simulation methods (surface-hopping and vibronic exciton models) for two-dimensional electronic spectroscopy, explaining how vibronic coupling sustains excitonic coherence in photosynthetic light-harvesting complexes such as the Fenna-Matthews-Olson complex and LH2, and extending these ideas to singlet fission and organic-semiconductor aggregates. He is a faculty affiliate of Northwestern's Institute for Quantum Information Research and Engineering (INQUIRE).