# 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…

## 18 Citations

### Large-Scale Quantum Dynamics with Matrix Product States.

- PhysicsJournal of chemical theory and computation
- 2019

The time-dependent density matrix renormalization group (TD-DMRG) is employed which parametrizes the time- dependent wave function as a matrix product state and leads to a set of coupled equations that can be integrated exactly.

### Time-dependent density matrix renormalization group quantum dynamics for realistic chemical systems.

- PhysicsThe Journal of chemical physics
- 2019

Two typical chemical systems of internal conversion and singlet fission are investigated and a comparison shows that the tDMRG methods can describe the full quantum dynamics in large chemical systems accurately and efficiently.

### Accurate and efficient description of interacting carriers in quantum nanostructures by selected configuration interaction and perturbation theory

- Physics
- 2020

We present a method to calculate many-body states of interacting carriers in million atom quantum nanostructures based on atomistic tight-binding calculations and a combination of iterative selection…

### Electron Dynamics with the Time-Dependent Density Matrix Renormalization Group.

- PhysicsJournal of chemical theory and computation
- 2021

This work simulates the electron dynamics in molecular systems with the time-dependent density matrix renormalization group (TD-DMRG) algorithm and shows that by parametrizing the wave function as a matrix product state, it can accurately simulate the dynamics of systems.

### The density matrix renormalization group in chemistry and molecular physics: Recent developments and new challenges.

- Chemistry, PhysicsThe Journal of chemical physics
- 2020

The method is presented following its historical development, starting from its original formulation up to its most recent applications, and emerging new fields of applications of DMRG are explored, such as its time-dependent formulation and the application to vibrational spectroscopy.

### Time dependent adaptive configuration interaction applied to attosecond charge migration.

- PhysicsThe Journal of chemical physics
- 2019

TD-ACI is shown to be a valuable benchmark theory for electron dynamics, and it represents an important step toward accurate and affordable TD multireference methods.

### Functional Tensor-Train Chebyshev Method for Multidimensional Quantum Dynamics Simulations.

- Chemistry, PhysicsJournal of chemical theory and computation
- 2021

The functional tensor-train Chebyshev (FTTC) method is introduced for rigorous nuclear quantum dynamics simulations and its capabilities are demonstrated as applied to simulations of proton quantum dynamics in a 50-dimensional model of hydrogen-bonded DNA base pairs.

### Chebyshev matrix product states with canonical orthogonalization for spectral functions of strongly correlated systems

- Physics
- 2021

We propose a method to calculate the spectral functions of strongly correlated systems by Chebyshev expansion in the framework of matrix product states coupled with canonical orthogonalization…

### Numerical assessment for accuracy and GPU acceleration of TD-DMRG time evolution schemes.

- Computer ScienceThe Journal of chemical physics
- 2020

This paper comparatively studies the accuracy of three time evolution schemes in the TD-DMRG, the global propagation and compression method with the Runge-Kutta algorithm, the time dependent variational principle based methods with the matrix unfolding algorithm, and with the projector-splitting algorithm by performing benchmarks on the exciton dynamics of the Fenna-Matthews-Olson complex.

### Transcorrelated density matrix renormalization group.

- PhysicsThe Journal of chemical physics
- 2020

The transcorrelated Density Matrix Renormalization Group (tcDMRG) theory is introduced for the efficient approximation of the energy for strongly correlated systems and provides a generally powerful approach toward the dynamic correlation problem of DMRG.

## References

SHOWING 1-10 OF 97 REFERENCES

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

- ChemistryJ. Comput. Chem.
- 2016

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.

- Chemistry, PhysicsChemical reviews
- 2017

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.

### CheMPS2: A free open-source spin-adapted implementation of the density matrix renormalization group for ab initio quantum chemistry

- PhysicsComput. Phys. Commun.
- 2014

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

- Physics
- 2017

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

- Chemistry
- 2014

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

- Chemistry, Physics
- 2011

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.

- PhysicsThe journal of physical chemistry letters
- 2016

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.

- PhysicsThe Journal of chemical physics
- 2006

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

- Chemistry, Physics
- 2011

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

- Physics, ChemistryStructural dynamics
- 2017

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.