Simulation of absorption spectra of molecular aggregates: a Hierarchy of Stochastic Pure States approach

Abstract

The 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 aggregares 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 apply adaptive HOPS methods for the simulation of absorption spectra and also to a formulation for non-linear spectroscopy that is perturbative with respect to interactions with the electric field.

References in corpus (10)

• Perspective: Numerically "exact" approach to open quantum dynamics: The hierarchical equations of motion (HEOM)
• On the alternatives for bath correlators and spectral densities from mixed quantum-classical simulations
• Open system dynamics with non-Markovian quantum jumps
• Exact open quantum system dynamics using the Hierarchy of Pure States (HOPS)
• Forster resonance energy transfer, absorption and emission spectra in multichromophoric systems: III. Exact stochastic path integral evaluation
• Hierarchical equations for open system dynamics in fermionic and bosonic environments
• Non-Markovian Quantum State Diffusion for Temperature-Dependent Linear Spectra of Light Harvesting Aggregates
• Chebyshev Hierarchical Equations of Motion for Systems with Arbitrary Spectral Densities and Temperatures
• Exciton Transfer in Organic Photovoltaic Cells: A Role of Local and Nonlocal Electron-Phonon Interactions in a Donor Domain
• Optical response of laser-driven charge-transfer complex described by Holstein-Hubbard model coupled to heat baths: Hierarchical equations of motion approach

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• Machine learning meets $\mathfrak{su}(n)$ Lie algebra: Enhancing quantum dynamics learning with exact trace conservation
• Toward Quantum-Aware Machine Learning: Improved Prediction of Quantum Dissipative Dynamics via Complex Valued Neural Networks