2021

Nottoli, M., Bondanza, M., Lipparini, F. & Mennucci, B.
An enhanced sampling QM/AMOEBA approach: The case of the excited state intramolecular proton transfer in solvated 3-hydroxyflavone
J. Chem. Phys. 154, 184107 (2021).  <Read>
We present an extension of the polarizable quantum mechanical (QM)/AMOEBA approach to enhanced sampling techniques. This is achieved by connecting the enhanced sampling PLUMED library to the machinery based on the interface of Gaussian and Tinker to perform QM/AMOEBA molecular dynamics. As an application, we study the excited state intramolecular proton transfer of 3-hydroxyflavone in two solvents: methanol and methylcyclohexane. By using a combination of molecular dynamics and umbrella sampling, we find an ultrafast component of the transfer, which is common to the two solvents, and a much slower component, which is active in the protic solvent only. The mechanisms of the two components are explained in terms of intramolecular vibrational redistribution and intermolecular hydrogen-bonding, respectively. Ground and excited state free energies along an effective reaction coordinate are finally obtained allowing for a detailed analysis of the solvent mediated mechanism.

Nottoli, M., Cupellini, L., Lipparini, F., Granucci, G. & Mennucci, B.
Multiscale Models for Light-Driven Processes
Annual Review of Physical Chemistry 72, 489-513 (2021).  <Read>
Multiscale models combining quantum mechanical and classical descriptions are a very popular strategy to simulate properties and processes of complex systems. Many alternative formulations have been developed, and they are now available in all of the most widely used quantum chemistry packages. Their application to the study of light-driven processes, however, is more recent, and some methodological and numerical problems have yet to be solved. This is especially the case for the polarizable formulation of these models, the recent advances in which we review here. Specifically, we identify and describe the most important specificities that the polarizable formulation introduces into both the simulation of excited-state dynamics and the modeling of excitation energy and electron transfer processes.

Cardoso Ramos, F., Cupellini, L. & Mennucci, B.
Computational Investigation of Structural and Spectroscopic Properties of LOV-Based Proteins with Improved Fluorescence.
J. Phys. Chem. B 125, 1768–1777 (2021). <Read>

Macaluso, V., Salvadori, G., Cupellini, L. & Mennucci, B.
The structural changes in the signaling mechanism of bacteriophytochromes in solution revealed by a multiscale computational investigation.
Chemical Science (2021). doi:10.1039/D1SC00186H  <Read>

Mascoli, V. , Liguori, N., Cupellini, L., Mennucci, B., Croce, R.
Uncovering the interactions driving carotenoid binding in light-harvesting complexes.
Chemical Science (2021). doi:10.1039/D1SC00071C  <Read>