On the divergence of time-dependent perturbation theory applied to laser-induced molecular transitions

  title={On the divergence of time-dependent perturbation theory applied to laser-induced molecular transitions},
  author={Klaus Renziehausen and Philipp Marquetand and Volker Engel},
  journal={Journal of Physics B: Atomic, Molecular and Optical Physics},
Population transfer between electronic molecular states can be effectively induced via the interaction with shaped laser pulses. Regarding a numerical example, it is demonstrated that perturbation theory, as is often applied in numerical simulations of field-matter interactions, might lead to divergences. The occurring error accumulating in the norm of the wavefunction can be decomposed into two contributions. The first one is a small numerical error, which is controllable by minimization of… 
7 Citations

Quantum diffusion wave-function approach to two-dimensional vibronic spectroscopy.

The wave-packet approach, besides being an alternative technique to calculate the spectra, offers an intuitive insight into the dissipation dynamics and its relation to the 2D vibronic spectra.

Extended quantum jump description of vibronic two-dimensional spectroscopy.

Two-dimensional (2D) vibronic spectra are calculated for a model system involving two electronic molecular states and the influence of dissipation and dephasing is characterized using a wave function based method.

Fragment momentum distributions obtained from coupled electron-nuclear dynamics.

It is shown that a simultaneous excitation of two different electronic states results in further interferences which are related to electronic wave-packet dynamics on the attosecond time-scale and are modified by the electronic degree-of-freedom.

Numerical method for nonlinear optical spectroscopies: Ultrafast ultrafast spectroscopy.

A novel numerical method, called Ultrafast Ultrafast (UF2) spectroscopy, for calculating the nth-order wavepackets required for calculating n-wave mixing signals, and it is demonstrated that it is computationally more efficient than other methods in a wide range of use cases.

Two-dimensional vibronic spectroscopy of molecular predissociation

We calculate two-dimensional (2D) spectra reflecting the time-dependent electronic predissociation of a diatomic molecule. The laser-excited electronic state is coupled non-adiabatically to a

Author index with titles (volume 42)

  • Medicine
  • 2009
The PDF file provided contains web links to all articles in this volume and is intended to be a springboard for further research.

Two-dimensional vibronic spectroscopy of coherent wave-packet motion.

Two-dimensional spectroscopic signals obtained from femtosecond pulse interactions with diatomic molecules are theoretically studied and various pulse sequences are discussed which yield information about vibrational level structure and phase relationships in different electronic states.



Non-perturbative wave-packet calculations of time-resolved four-wave-mixing signals

Abstract.We extend a method proposed by Seidner et al. [J. Chem. Phys. 103, 3998 (1995)] to extract directional terms from a time-dependent molecular polarization to obtain time-resolved

Wave packet dynamics in different electronic states investigated by femtosecond time-resolved four-wave-mixing spectroscopy

Abstract.This paper reviews results on wave packet dynamics investigated by means of femtosecond time-resolved four-wave-mixing (FWM) spectroscopy. First, it is shown that by making use of the

Efficient calculation of time- and frequency-resolved four-wave-mixing signals.

Alternative methods for the calculation of four-wave-mixing signals are reviewed, in which the relevant laser pulses are incorporated into the system Hamiltonian and the driven system dynamics is simulated numerically exactly.


A general nonperturbative approach to calculate femtosecond pump‐probe (PP) signals is proposed, which treats both the intramolecular couplings and the field‐matter interaction (numerically) exactly.

Ground state vibrational wave‐packet and recovery dynamics studied by time‐resolved CARS and pump‐CARS spectroscopy

Recent experiments on gaseous iodine and β-carotene are analyzed within a wave-packet description of femtosecond-time resolved four-wave mixing spectroscopy. Employing the same formalism, two

Theory of multiphoton processes

My aim in this book has been to give an account of the theoretical methods of analysis of multiphoton processes in atomic physics. In this account I have emphasized systematic methods as opposed to

Principles of Nonlinear Optical Spectroscopy

1. Introduction 2. Quantum Dynamics in Hilbert Space 3. The Density Operator and Quantum Dynamics in Liouville Space 4. Quantum Electrodynamics, Optical Polarization, and Nonlinear Spectroscopy 5.

Properties of wave packets deduced from quantum control fitness landscapes

We demonstrate the versatility of shaped femtosecond dump pulses for the investigation of molecular quantum systems. Model calculations show that population is most efficiently transferred by shaped