RT Journal Article
T1 Specific Reaction Parameter Multigrid POTFIT (SRP-MGPF): Automatic Generation of Sum-of-Products Form Potential Energy Surfaces for Quantum Dynamical Calculations
A1 Panadés Barrueta, Ramón Lorenzo
A1 Martínez Núñez, Emilio
A1 Peláez, Daniel
K1 PES
K1 Sums-of-products
K1 Tensor-decomposition
K1 Quantum dynamics
K1 Reparametrized semiempirical
K1 TSSCDS
K1 Global optimization
AB We present Specific Reaction Parameter Multigrid POTFIT (SRP-MGPF), an automated methodology for the generation of global potential energy surfaces (PES), molecular properties surfaces, e.g., dipole, polarizabilities, etc. using a single random geometry as input. The SRP-MGPF workflow integrates: (i) a fully automated procedure for the global topographical characterization of a (intermolecular) PES based on the Transition State Search Using Chemical Dynamical Simulations (TSSCDS) family of methods;i (ii) the global optimization of the parameters of a semiempirical Hamiltonian in order to reproduce a given level of electronic structure theory; and (iii) a tensor decomposition algorithm which turns the resulting SRP-PES into sum of products (Tucker) form with the Multigrid POTFIT algorithm. The latter is necessary for quantum dynamical studies within the Multiconfiguration Time-Dependent Hartree (MCTDH) quantum dynamics method. To demonstrate our approach, we have applied our methodology to the cis-trans isomerization reaction in HONO in full dimensionality (6D). The resulting SRP-PES has been validated through the computation of classical on-the-fly dynamical calculations as well as calculations of the lowest vibrational eigenstates of HONO as well as high-energy wavepacket propagations
PB Frontiers Media
SN 2296-2646
YR 2019
FD 2019
LK http://hdl.handle.net/10347/21211
UL http://hdl.handle.net/10347/21211
LA eng
NO Panadés-Barrueta RL, Martínez-Núñez E and Peláez D (2019) Specific Reaction Parameter Multigrid POTFIT (SRP-MGPF): Automatic Generation of Sum-of-Products Form Potential Energy Surfaces for Quantum Dynamical Calculations. Front. Chem. 7:576. doi: 10.3389/fchem.2019.00576
NO RP-B thanks the Région Hauts-de-France and the Université de Lille for a Ph.D. Fellowship. RP-B and DP thank the Région Hauts-de-France and the Ministére de l'Enseignement Supérieur et de la Recherche (CPER Climibio), and the European Fund for Regional Economic Development for their financial support. This work has been partially supported by the Agence Nationale de la Recherche through the Labex CaPPA (ANR-11-LABX-0005-01). EM-N thanks Xunta de Galicia (Research Grant No. ED431C 2017/17)
DS Minerva
RD 3 may 2026