Ultrafast ab Initio Quantum Chemistry Using Matrix Product States

Journal of Chemical Theory and Computation
Lars-Hendrik Frahm, Daniela Pfannkuche

Abstract

Ultrafast dynamics in chemical systems provide a unique access to fundamental processes at the molecular scale. A proper description of such systems is often very challenging because of the quantum nature of the problem. The concept of matrix product states (MPS), however, has proven its performance in describing such correlated quantum systems in recent years for a wide range of applications. In this work, we continue the development of the MPS approach to study ultrafast electron dynamics in quantum chemical systems. The method combines time evolution schemes, such as fourth-order Runge-Kutta and Krylov space time evolution, with MPS, in order to solve the time-dependent Schrödinger equation efficiently. This allows for describing electron dynamics in molecules on a full configurational interaction (CI) level for a few femtoseconds after excitation. As a benchmark, we compare MPS-based calculations to full CI calculations for a chain of hydrogen atoms and for the water molecule. Krylov space time evolution is in particular suited for the MPS approach, as it provides a wide range of opportunities to be adjusted to the reduced MPS dimension case. Finally, we apply the MPS approach to describe charge migration effects in iodoace...Continue Reading

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Citations

Jan 17, 2020·The Journal of Chemical Physics·Weitang LiZhigang Shuai
Nov 11, 2019·The Journal of Chemical Physics·Jeffrey B Schriber, Francesco A Evangelista
Nov 4, 2020·The Journal of Chemical Physics·Alberto Baiardi, Markus Reiher
May 28, 2021·Journal of Chemical Theory and Computation·Alberto Baiardi
May 9, 2019·Journal of Chemical Theory and Computation·Alberto Baiardi, Markus Reiher
Sep 23, 2021·The Journal of Physical Chemistry Letters·Tong JiangZhigang Shuai
Dec 14, 2021·Journal of Chemical Theory and Computation·Micheline B SoleyVictor S Batista
Dec 30, 2021·Journal of Chemical Theory and Computation·Vladislav Kochetov, Sergey I Bokarev

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