相关论文: Time-dependent coupled cluster theory for ultrafas…
The power spectrum of an optical field can be acquired without a spectrally resolving detector by means of Fourier-transform spectrometry, based on measuring the temporal autocorrelation of the optical field. Analogously, we here perform…
Standard optical pump-probe methods analyze a system's temporal response to a laser pulse within sub-femtoseconds to several nanoseconds, constrained by the optical delay line's length. While resistance is a sensitive detector in various…
Stimulated Rayleigh scattering of pump and probe light pulses of close carrier frequencies is considered. A nonzero time delay between the two pulses is shown to give rise to amplification of the delayed (probe) pulse accompanied by…
We present the first successful application of the coupled cluster approach to simulate the X-ray absorption (XA) spectrum of liquid water. The system size limitations of standard coupled cluster theory are overcome by employing a newly…
We propose a novel method that uses the oscillation of an atomic excited wave packet observed through a pump-probe technique to accurately determine the zero time delay between a pair of ultrashort laser pulses. This physically-based…
We present a time-dependent perturbative approach adapted to the treatment of intense pulsed interactions. We show there is a freedom in choosing secular terms and use it to optimize the accuracy of the approximation. We apply this…
In order to explore the effects of high levels of electron correlation on the real-time coupled cluster formalism and algorithmic behavior, we introduce a time-dependent implementation of the CC3 singles, doubles and approximate triples…
We investigate how the quantum control of a two-level system (TLS) coupled to photons can modify and tune the TLS's photon absorption spectrum. Tuning and controlling the emission and the absorption is of much interest e.g.\ for the…
We present a general analysis for the interaction of a probe laser radiation with a coherently prepared molecular Raman medium. We describe a general formalism which includes dispersive effects, such as group velocity and group velocity…
The linear optical absorption spectra of three isomers of planar boron cluster B$_{13}$ are calculated using time-dependent spin-polarized density functional approach. The geometries of these cluster are optimized at the B3LYP/6-311+G*…
A novel polarization-modulation transient method has been developed for studying fast anisotropic relaxation in electronic excited states of polyatomic and biologically relevant molecules under excitation with femtosecond laser pulses. The…
The phase transition present in the linear-chain and square-lattice cases of the transverse Ising model is examined. The extended coupled cluster method (ECCM) can describe both sides of the phase transition with a unified approach. The…
This study investigates the propagation of an ultrafast laser pulse through a liquid medium. A femtosecond laser oscillator with a pulse duration of less than 8 fs is used. By conducting experiments with coumarin and fluorescein dyes in…
The origin of the coherences in two-dimensional spectroscopy of photosynthetic complexes remains disputed. Recently it has been shown that in the ultrashort-pulse limit, oscillations in a frequency-integrated pump-probe signal correspond…
We simulate the transient absorption of attosecond pulses of infrared-laser-dressed atoms by considering a three-level system with the adiabatic approximation. The delay-dependent interference features are investigated from the perspective…
We report on the observation, characterization, and control of the electron dynamics in ionized argon atoms. We utilized an intense mid-infrared (MIR) pulse to create a coherent superposition of the spin-orbit split ground state of the ion.…
Optical pump-probe spectroscopy is a powerful tool to directly probe the carrier dynamics in materials down to sub-femtosecond resolution. To perform such measurement, while keeping the pump induced perturbation to the sample as small as…
The electronic structure of atomic quantum systems and their dynamical interaction with light is reflected in transition dipole matrix elements coupling the system's energy eigenstates. In this work, we measure phase shifts of the…
The dynamics of excitonic energy transfer in molecular complexes triggered by interaction with laser pulses offers a unique window into the underlying physical processes. The absorbed energy moves through the network of interlinked pigments…
We show that the third-order optical response of disordered linear J-aggregates can be calculated by considering only a limited number of transitions between (multi-) exciton states. We calculate the pump-probe absorption spectrum resulting…