Analytical Nuclear Gradients for the Multiconfigurational Self-Consistent Field Method Coupled with the Polarizable Fluctuating Charges Model
Francesco Mazza, Marco Trinari, Chiara Sepali, Chiara Cappelli
TL;DR
This paper introduces a new method combining quantum and classical models to accurately simulate how aromatic molecules interact with water.
Contribution
The novel contribution is deriving analytical nuclear gradients for the MCSCF/FQ model and validating its use in simulating vibronic spectra.
Findings
Analytical nuclear gradients were successfully derived and implemented in OpenMolcas.
The MCSCF/FQ model accurately reproduced experimental vibronic spectra of benzene and phenol in water.
The method captures both solute flexibility and solvent dynamics in simulations.
Abstract
The multiscale model combining the multiconfigurational self-consistent field (MCSCF) method with the fully atomistic polarizable Fluctuating Charges (FQ) force field (Sepali, C.; et al. J. Chem. Theory Comput. 2024, 20, 9954–9967) is here extended to the calculation of analytical nuclear gradients. The gradients are derived from first-principles, implemented in the OpenMolcas package, and validated against numerical references. The resulting MCSCF/FQ nuclear gradients are employed to simulate vibronic absorption spectra of aromatic molecules in aqueous solution, namely benzene and phenol. By integrating this approach with molecular dynamics simulations, both solute conformational flexibility and the dynamical aspects of solvation are properly captured. The computed spectra reproduce experimental profiles and relative band intensities with remarkable accuracy, demonstrating the…
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Taxonomy
TopicsSpectroscopy and Quantum Chemical Studies · Photochemistry and Electron Transfer Studies · Molecular spectroscopy and chirality