Panadés Barrueta, Ramón LorenzoMartínez Núñez, EmilioPeláez, Daniel2020-04-062020-04-062019Panadés-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.2019.005762296-2646http://hdl.handle.net/10347/21211We 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 propagationsengCopyright © 2019 Panadés-Barrueta, Martínez-Núñez and Peláez. This is an open-access article distributed under the terms of the Creative Commons Attribution License (CC BY). The use, distribution or reproduction in other forums is permitted, provided the original author(s) and the copyright owner(s) are credited and that the original publication in this journal is cited, in accordance with accepted academic practice. No use, distribution or reproduction is permitted which does not comply with these termshttps://creativecommons.org/licenses/by/4.0/PESSums-of-productsTensor-decompositionQuantum dynamicsReparametrized semiempiricalTSSCDSGlobal optimizationjournal article10.3389/fchem.2019.00576open access