Deciphering the Role of Solvent in Molecular Properties and Reactions
The solvent environment plays an essential role in chemical processes, including catalysis, photochemical reactions, and the stability of materials. Recent years, new experimental techniques have been introduced to characterize liquid-phase reactions. This places an urgent need for efficient computational models to further predict the effect of solvents on the rate and product distribution. I aim at developing methods and protocols for efficient modeling of reactions in realistic experimental conditions.
I developed the graphical processing units (GPUs) algorithms to accelerate the widely used implicit solvent model, the conductor-like polarizable continuum model (C-PCM) With 10X-100X speed-ups for ground-state Hartree Fock (HF) or density functional theory (DFT) calculation, my algorithm keeps the world’s fastest record. More importantly, these award-winning method developments enable more realistic simulation of large biomolecular systems in solution phase: the bulk solvent effects can now be simulated with little computational overhead.
F. Liu, N. Luehr, H. J. Kulik, and T. J. Martínez. “Quantum chemistry for solvated molecules on graphical processing units using polarizable continuum models.” Journal of chemical theory and computation 11 (2015): 3131-3144.
B. D. Mar., H. W. Qi, F. Liu, and H. J. Kulik. “Ab Initio screening approach for the discovery of lignin polymer breaking pathways.” The Journal of Physical Chemistry A 119 (2015): 6551-6562.
Solvent effects for excited state properteis and photophysical processes
The significances of solvent effects also lie in the simulation of spectroscopy and photochemistry, which involves evaluation of excited-state properties. To this end, time-dependent density functional theory (TDDFT) has been increasingly employed in recent years due to its superior computational scalability. To study the excited-state properties of solvated molecules, I implemented the TDDFT algorithm in the C-PCM solvent model with GPU acceleration, with 40-150X speed-ups. The implementation includes both the equilibrium and non-equilibrium solvation schemes that can describe fluorescence and vertical excitations, respectively. This method enables PCM-TDDFT for systems with ca. 1000 atoms, making the excited-state simulation in combined implicit/explicit solvent model practical.
F Liu, D. M. Sanchez, H J. Kulik, and T. J. Martínez. “Exploiting graphical processing units to enable quantum chemistry calculation of large solvated molecules with conductor-like polarizable continuum models.” International Journal of Quantum Chemistry 119 (2019): e25760