Simulation of absorption spectra of molecular aggregates: A hierarchy of stochastic pure state approach
Lipeng Chen, Doran I. G. Bennett, Alexander Eisfeld
Abstract
Simulation of spectroscopic observables for molecular aggregates with strong and structured coupling of electronic excitation to vibrational degrees of freedom is an important but challenging task. The Hierarchy of Pure States (HOPS) provides a formally exact solution based on local, stochastic trajectories. Exploiting the localization of HOPS for the simulation of absorption spectra in large aggregates requires a formulation in terms of normalized trajectories. Here, we provide a normalized dyadic equation where the ket- and bra-states are propagated in different electronic Hilbert spaces. This work opens the door to applying adaptive HOPS methods for the simulation of absorption spectra.
Topics & Concepts
HierarchyObservableAbsorption (acoustics)ExcitationCoupling (piping)Work (physics)Spectral lineStatistical physicsAbsorption spectroscopyHilbert spaceState (computer science)Degrees of freedom (physics and chemistry)Computer scienceMolecular physicsMaterials sciencePhysicsQuantum mechanicsAlgorithmOpticsLawMetallurgyPolitical scienceSpectroscopy and Quantum Chemical StudiesAdvanced Chemical Physics StudiesPhotochemistry and Electron Transfer Studies