Ultrafast ab Initio Quantum Chemistry Using Matrix Product States.

@article{Frahm2019UltrafastAI,
  title={Ultrafast ab Initio Quantum Chemistry Using Matrix Product States.},
  author={Lars-Hendrik Frahm and Daniela Pfannkuche},
  journal={Journal of chemical theory and computation},
  year={2019},
  volume={15 4},
  pages={
          2154-2165
        }
}
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… 

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References

SHOWING 1-10 OF 97 REFERENCES

Molcas 8: New capabilities for multiconfigurational quantum chemical calculations across the periodic table

The report includes the description of a computational machinery for nonlinear optical spectroscopy through an interface to the QM/MM package Cobramm.

Attosecond Electron Dynamics in Molecules.

This review will concentrate on the application of attosecond methods to the investigation of ultrafast processes in molecules, with emphasis in molecules of chemical and biological interest.

Electronic decoherence following photoionization: Full quantum-dynamical treatment of the influence of nuclear motion

Photoionization using attosecond pulses can lead to the formation of coherent superpositions of the electronic states of the parent ion. However, ultrafast electron ejection triggers not only

The density matrix renormalization group for ab initio quantum chemistry

During the past 15 years, the density matrix renormalization group (DMRG) has become increasingly important for ab initio quantum chemistry. Its underlying wavefunction ansatz, the matrix product

Quantum-information analysis of electronic states of different molecular structures

We have studied transition metal clusters from a quantum information theory perspective using the density-matrix renormalization group (DMRG) method. We demonstrate the competition between

Coupled Cluster Method with Single and Double Excitations Tailored by Matrix Product State Wave Functions.

A novel method for accurate "post-DMRG" treatment of dynamic correlation based on the tailored coupled cluster (CC) theory in which the DMRG method is responsible for the proper description of nondynamic correlation, whereas dynamic correlation is incorporated through the framework of the CC theory.

Multireference correlation in long molecules with the quadratic scaling density matrix renormalization group.

A local ab initio density matrix renormalization group algorithm is devised to describe multireference correlations in large systems and can obtain an exact characterization of correlation for long molecules that are extended in one of their spatial dimensions with a cost that scales only quadratically with the size of the system.

Multiconfiguration time-dependent Hartree-Fock treatment of electronic and nuclear dynamics in diatomic molecules

The multiconfiguration time-dependent Hartree-Fock (MCTDHF) method is formulated for treating the coupled electronic and nuclear dynamics of diatomic molecules without the Born-Oppenheimer

Charge migration and charge transfer in molecular systems

Important new insights into each of the elementary steps of charge transfer in liquids and nanoparticles, obtained from state-of-the-art ultrafast spectroscopy and/or theoretical methods, are summarized in this review.
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