Related papers: Extracting Coupling-Mode Spectral Densities with T…
We theoretically investigate an electron transfer (ET) process in a dissipative environment by means of two-dimensional (2D) correlation spectroscopy. We extend the reduced hierarchy equations of motion approach to include both overdamped…
We introduce a quantum information analysis of vibrational wave functions to understand complex vibrational spectra of molecules with strong anharmonic couplings and vibrational resonances. For this purpose, we define one- and two-modal…
Vibrational coherences in ultrafast pump-probe (PP) and 2D electronic spectroscopy (2DES) provide insight into the excited state dynamics of molecules. Femtosecond coherence spectra (FCS) and 2D beat maps yield information about…
In this study, we explore the potential of machine learning for modeling molecular electronic spectral intensities as a continuous function in a given wavelength range. Since presently available chemical space datasets provide excitation…
Real-time probing of electrons can uncover intricate relaxation mechanisms and many-body interactions hidden in strongly correlated materials. While experimenters have used ultrafast optical pump-probe methods in bulk materials, laser…
Two-dimensional (2D) vibrational spectroscopy is a powerful means of investigating the structure and dynamics of complex molecules in condensed phases. However, even in theory, analysis of 2D spectra resulting from complex inter- and…
We describe a practical procedure for extracting the spatial structure and the growth rates of slow eigenmodes of a spatially extended system, using a unique experimental capability both to impose and to perturb desired initial states. The…
The recently suggested possibility that weak vibronic transitions can be excitonically enhanced in light-harvesting complexes is studied in detail. A vibronic exciton dimer model which includes ground state vibrations is investigated using…
In the regime of strong coupling between molecular excitons and confined optical modes, the intra-molecular degrees of freedom are profoundly affected, leading to a reduced vibrational dressing of polaritons compared to bare electronically…
The observed prevalence of oscillatory signals in the spectroscopy of biological light-harvesting complexes at ambient temperatures has led to a search for mechanisms supporting coherent transport through larger molecules in noisy…
We present a theory that efficiently describes the quantum dynamics of an electronic excitation that is coupled to a continuous, highly structured phonon environment. Based on a stochastic approach to non-Markovian open quantum systems, we…
Ultrashort non-resonant electromagnetic pulses applied to effective one-electron systems may operate on the electronic state as a position or momentum translation operator. As derived here, extension to many-body correlated systems exposes…
We develop a detailed theoretical model of photo-induced proton-coupled electron transfer (PPCET) processes, which are at the basis of solar energy harvesting in biological systems and photovoltaic materials. Our model enables to analyze…
We extend density matrix embedding theory to periodic systems, resulting in an electronic band structure method for solid-state materials. The electron correlation can be captured by means of a local impurity model using various choices of…
We perform a beat-frequency-resolved analysis for two-dimensional electronic spectroscopy using a high-speed and stable 2D electronic spectrometer and few-cycle visible laser pulses to disentangle the vibrational coherences in an artificial…
How atoms and electrons in a molecule move during a chemical reaction and how rapidly energy is transferred to or from the surroundings can be studied with flashes of laser light. However, despite prolonged efforts to develop various…
The presence of solvent tunes many properties of a molecule, such as its ground and excited state geometry, dipole moment, excitation energy, and absorption spectrum. Because the energy of the system will vary depending on the solvent…
Cavity dressing of molecular vibrational dynamics expands the role of characteristic vibrations as spectroscopic markers of underlying ultrafast dynamics. Interacting vibrational modes exhibit a pronounced excited state delocalization due…
Coherent spin resonance methods, such as nuclear magnetic resonance and electron spin resonance spectroscopy, have led to spectrally highly sensitive, non-invasive quantum imaging techniques. Here, we propose a pump-probe spin resonance…
Two-dimensional electronic spectroscopy (2DES) can be implemented with different geometries, e.g., BOXCARS, collinear and pump-probe geometries. The pump-probe geometry has its advantage of overlapping only two beams and reducing phase…