Nuclear-Electronic All-Particle Density Matrix Renormalization Group 1 1 1 1, Andrea Muolo, Alberto Baiardi, Robin Feldmann, and Markus Reiher ∗ 1ETH Z¨urich,Laboratory of Physical Chemistry, Vladimir-Prelog-Weg 2, 8093 Z¨urich,Switzerland Abstract We introduce the Nuclear Electronic All-Particle Density Matrix Renormalization Group (NEAP-DMRG) method for solving the time-independent Schr¨odingerequation simultaneously for electrons and other quantum species. In contrast to already existing multicomponent approaches, in this work we construct from the outset a multi-reference trial wave function with stochastically optimized non-orthogonal Gaussian orbitals. By iterative refining of the Gaussians' positions and widths, we obtain a compact multi-reference expansion for the multicomponent wave function. We extend the DMRG algorithm to multicomponent wave functions to take into account inter- and intra-species correlation effects. The efficient parametrization of the total wave function as a ma- trix product state allows NEAP-DMRG to accurately approximate full configuration interaction energies of molecular systems with more than three nuclei and twelve particles in total, which is currently a major challenge for other multicomponent approaches. We present NEAP-DMRG + results for two few-body systems, i.e., H2 and H3 , and one larger system, namely BH3. arXiv:2003.04446v2 [physics.chem-ph] 13 May 2020 ∗ corresponding author:
[email protected] 1 I. INTRODUCTION Modeling the static and dynamical properties of molecular systems relies routinely on the Born{Oppenheimer (BO) approximation [1, 2] which separates the time-independent Schr¨odingerequation into the electronic and nuclear parts, motivated by the large mass dif- ference between the two subsystem components.