Simulation of Excitation by Sunlight in Mixed Quantum-Classical Dynamics

2020/06/24 by Mario Barbatti · 1 voice · 24 citations
Biochemistry, Genetics and Molecular Biology · Chemistry · Neuroscience · Physics and Astronomy · #Chemistry #Computational physics #Excitation #Excited state #Isomerization #Microsecond #Optics #Photoisomerization #Photoreceptor and optogenetics research #Photosynthetic Processes and Mechanisms #Physics #Population #Quantum #Quantum mechanics #Spectroscopy and Quantum Chemical Studies #Statistical physics

paper · pdf · doi:10.1021/acs.jctc.0c00501

published in Journal of Chemical Theory and Computation 16(8), 4849-4856 (American Chemical Society)

openalex publication_date 2020/06/24 · openalex created_date 2025/10/10 · openalex updated_date 2026/08/04

Abstract

This paper proposes a method to simulate nonadiabatic dynamics initiated by thermal light, including solar radiation, in the frame of mixed quantum-classical (MQC) methods, like surface hopping. The method is based on the Chenu-Brumer approach, which treats the thermal radiation as an ensemble of coherent pulses. It is composed of three steps: (1) sampling initial conditions from a broad blackbody spectrum, (2) dynamics propagation using conventional methods, and (3) ensemble averaging considering the field and realization time of the pulses. The application of MQC dynamics with pulse ensembles (MQC-PE) to a model system of nucleic acid photophysics showed the emergence of a steady excited-state population. In another test case, modeling retinal photophysics, MQC-PE predicted that although the photoisomerization occurs within 200 fs, it may take tens of microseconds of continuous solar irradiation to photoactivate a single retinal. Such emergent long timescales may impact our understanding of biological and technological phenomena occurring under solar radiation.

Cited by

• Roadmap for Molecular Benchmarks in Nonadiabatic Dynamics
• Assessing Nonadiabatic Dynamics Methods in Long Timescales
• The Quest to Simulate Excited-State Dynamics of Transition Metal Complexes. [europepmc]
• Simulations of molecular photodynamics in long timescales. [europepmc]
• A Theoretical Perspective on the Actinic Photochemistry of 2-Hydroperoxypropanal. [europepmc]
• Newton-X Platform: New Software Developments for Surface Hopping and Nuclear Ensembles. [europepmc]
• Deciphering the Influence of Ground-State Distributions on the Calculation of Photolysis Observables. [europepmc]
• Perspective on Theoretical and Experimental Advances in Atmospheric Photochemistry. [europepmc]
• Toward a Correct Description of Initial Electronic Coherence in Nonadiabatic Dynamics Simulations. [europepmc]
• Selecting Initial Conditions for Trajectory-Based Nonadiabatic Simulations. [europepmc]
• Roadmap for Molecular Benchmarks in Nonadiabatic Dynamics. [europepmc]
• The Newton-X platform for mixed quantum-classical dynamics. [europepmc]

Discussions

• Something amazing to start the day:🧪 Under a short laser pulse in the lab, retinal, the visual chromophore, isomerizes within 0.0001 ns. Under moonlight, its isomerization takes 1000 ns! The diff [bsky, 14 points, 0 comments]

Related

• Thermal-Light-Induced Coherent Dynamics in Atoms and Molecules -- an Exact Quantum Mechanical Treatment
• Photo-induced dynamics with continuous and discrete quantum baths
• Can Natural Sunlight Induce Coherent Exciton Dynamics?
• Natural Light Harvesting Systems: Unraveling the quantum puzzles
• Thermalization of quantum light induced by classical nonlinear wave dynamics