Hybrid quantum dynamics based on the augmented correlated Gaussian wavepacket
- 1Department of Chemistry and Biochemistry
- 2University of South Carolina
Abstract
The nuclear quantum effects, including tunneling, zero-point energy and wavefunction delocalization, are increasingly recognized as relevant to reactivity, charge and energy transfer, and other properties of large molecular systems, including those in nano-scale and biological environments. In the presence of active dynamic quantum modes, however, application of the numerically exact quantum methods becomes unfeasible beyond a handful of atoms, while classical and semiclassical description can be very inaccurate, and the error is hard to quantify. Thus, theoretical approaches capable of accurately describing the quantum system on one side, and efficiently accounting for the environment on the other, remain an active area of method development. In this work, we present a hybrid approach combining basis representation of the active quantum modes correlated at the functional level with a “mean-field” version of the variational Gaussian wavepacket referred to as Augmented Correlated Gaussian (ACG) dynamics. This allows one to include the effects of the environmental modes on the system within quadratic scaling of the wavefunction with the system size. The method is demonstrated on a double well system coupled to a chain of harmonic oscillators capturing the tunneling dynamics. The ACG scalability is demonstrated by simulating the quantum vibrational densities of states of a five-dimensional molecular model of a hydrogen atom adsorbed on a graphene flake, incorporating anharmonicitiy into the CH stretch.
Related
- Calculating strongly correlated ground states from the non-Markovian dissipative dynamics of Gaussian fermions
- Random Gaussian Augmented Matrix Product States
- Fully Automated Wannier Disentanglement via Projectability Selection in Gaussian and Augmented Plane-Wave Frameworks
- Wavepacket Approach for Spin Transport in Zigzag Spin Chain
- Pinning of a High-Energy Wavepacket by a Single Impurity
BibTeX
@misc{botti2026hybrid,
title = {{Hybrid quantum dynamics based on the augmented correlated Gaussian wavepacket}},
author = {Giacomo Botti and Sophya Garashchuk},
howpublished = {ChemRxiv},
year = {2026},
month = sep,
doi = {10.26434/chemrxiv.15009705/v1},
url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009705/v1},
note = {CC BY},
}
RIS
TY - UNPB
TI - Hybrid quantum dynamics based on the augmented correlated Gaussian wavepacket
AU - Giacomo Botti
AU - Sophya Garashchuk
PY - 2026
DA - 2026/09/30
PB - ChemRxiv
DO - 10.26434/chemrxiv.15009705/v1
UR - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009705/v1
AB - The nuclear quantum effects, including tunneling, zero-point energy and wavefunction delocalization, are increasingly recognized as relevant to reactivity, charge and energy transfer, and other properties of large molecular systems, including those in nano-scale and biological environments. In the presence of active dynamic quantum modes, however, application of the numerically exact quantum methods becomes unfeasible beyond a handful of atoms, while classical and semiclassical description can be very inaccurate, and the error is hard to quantify. Thus, theoretical approaches capable of accurately describing the quantum system on one side, and efficiently accounting for the environment on the other, remain an active area of method development. In this work, we present a hybrid approach combining basis representation of the active quantum modes correlated at the functional level with a “mean-field” version of the variational Gaussian wavepacket referred to as Augmented Correlated Gaussian (ACG) dynamics. This allows one to include the effects of the environmental modes on the system within quadratic scaling of the wavefunction with the system size. The method is demonstrated on a double well system coupled to a chain of harmonic oscillators capturing the tunneling dynamics. The ACG scalability is demonstrated by simulating the quantum vibrational densities of states of a five-dimensional molecular model of a hydrogen atom adsorbed on a graphene flake, incorporating anharmonicitiy into the CH stretch.
ER -