Publications de Seonghoon Choi

High-order geometric integrators for nonadiabatic molecular quantum dynamics and their applications to explore conical intersections

Accurate simulations of molecular quantum dynamics are crucial for understanding numerous natural processes and experimental results. Yet, such high-accuracy simulations are challenging even for relatively simple systems where the Born-Oppenheimer approxim ...

EPFL2022

How important are the residual nonadiabatic couplings for an accurate simulation of nonadiabatic quantum dynamics in a quasidiabatic representation?

Jiri Vanicek, Seonghoon Choi

Diabatization of the molecular Hamiltonian is a standard approach to remove the singularities of nonadiabatic couplings at conical intersections of adiabatic potential energy surfaces. In general, it is impossible to eliminate the nonadiabatic couplings en ...

2021

High-order geometric integrators for representation-free Ehrenfest dynamics

Jiri Vanicek, Seonghoon Choi

Ehrenfest dynamics is a useful approximation for ab initio mixed quantum-classical molecular dynamics that can treat electronically nonadiabatic effects. Although a severe approximation to the exact solution of the molecular time-dependent Schrödinger equa ...

2021

Semiclassical Approach to Photophysics Beyond Kasha’s Rule and Vibronic Spectroscopy Beyond the Condon Approximation. The Case of Azulene

Jacques-Edouard Moser, Marius Wehrle, Jiri Vanicek, Tomas Zimmermann, Julien Roulet, Antonio Prlj, Tomislav Begusic, Seonghoon Choi, Zhan Tong Zhang, George Cameron Fish

Azulene is a prototypical molecule with ananomalousfluorescence from the second excited electronic state,thus violating Kasha’s rule, and with an emission spectrum thatcannot be understood within the Condon approximation. To betterunderstand the photophysi ...

2020

Which form of the molecular Hamiltonian is the most suitable for simulating the nonadiabatic quantum dynamics at a conical intersection?

Jiri Vanicek, Seonghoon Choi

Choosing an appropriate representation of the molecular Hamiltonian is one of the challenges faced by simulations of the nonadiabatic quantum dynamics around a conical intersection. The adiabatic, exact quasidiabatic, and strictly diabatic representations ...

2020

A time-reversible integrator for the time-dependent Schrödinger equation on an adaptive grid

Jiri Vanicek, Seonghoon Choi

One of the most accurate methods for solving the time-dependent Schrödinger equation uses a combination of the dynamic Fourier method with the split-operator algorithm on a tensor-product grid. To reduce the number of required grid points, we let the grid ...

2019

Efficient geometric integrators for nonadiabatic quantum dynamics. II. The diabatic representation

Jiri Vanicek, Julien Roulet, Seonghoon Choi

Exact nonadiabatic quantum evolution preserves many geometric properties of the molecular Hilbert space. In the first paper of this series ["Paper I," S. Choi and J. Vaníček, J. Chem. Phys. 150, 204112 (2019)], we presented numerical integrators of arbitra ...

2019

Efficient geometric integrators for nonadiabatic quantum dynamics. I. The adiabatic representation

Jiri Vanicek, Seonghoon Choi

Geometric integrators of the Schrödinger equation conserve exactly many invariants of the exact solution. Among these integrators, the split-operator algorithm is explicit and easy to implement but, unfortunately, is restricted to systems whose Hamiltonian ...

2019