Related papers: Non-Adiabatic Electronic and Vibrational Ring-Open…
Ultrafast laser excitation can create coherent superpositions of electronic states in molecules and trigger ultrafast flow of electron density on few- to sub-femtosecond time scales. While recent attosecond experiments have addressed…
The effect of nuclear dynamics and conical intersections on electronic coherences is investigated employing a two-state, two-mode linear vibronic coupling model. Exact quantum dynamical calculations are performed using the…
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 electronic but also nuclear dynamics---leading…
Time-resolved X-ray absorption spectroscopy is emerging as a uniquely powerful tool to probe coupled electronic-nuclear dynamics in photo-excited molecules. Theoretical studies to date have established that time-resolved X-ray absorption…
We study strong field molecular ionization using few- (four to ten) cycle laser pulses. Employing a supercontinuum light source, we are able to tune the optical laser wavelength (photon energy) over a range of about $\sim$200 nm (500 meV).…
We examine time-resolved X-ray diffraction from molecules in the gas phase which undergo nonadiabatic avoided-crossing dynamics involving strongly coupled electrons and nuclei. Several contributions to the signal are identified,…
Accurate description of nonadiabatic dynamics of molecules at metal surfaces involving electron transfer has been a longstanding challenge for theory. Here, we tackle this problem by first constructing high-dimensional neural network…
Following the changes in molecular structure throughout the entirety of a chemical reaction with atomic resolution is a long-term goal in femtochemistry. Although the development of a plethora of ultrafast technique has enabled detailed…
Photoelectron spectroscopy is a powerful method that provides insight into the quantum mechanical properties of a wide range of systems. The ionized electron wavefunction carries information on the structure of the bound orbital, the ionic…
We present a framework for simulating relaxation dynamics through a conical intersection of an open quantum system that combines methods to approximate the motion of degrees of freedom with disparate time and energy scales. In the vicinity…
Attosecond interferometry in a two-color field is central to attosecond metrology and spectroscopy. In this technique, a photoelectron wave packet is released when a single photon from an extreme ultraviolet comb is absorbed. The wave…
High harmonic light sources make it possible to access attosecond time-scales, thus opening up the prospect of manipulating electronic wave packets for steering molecular dynamics. However, two decades after the birth of attosecond physics,…
X-ray four-wave mixing signals generated in the $k_1 + k_2 - k_3$ phase-matching direction are simulated for N1s transitions in para-nitroanline and two-ring hydrocarbons disubstituted with an amine and a nitroso groups. The two-dimensional…
Coupling of nuclear and electronic degrees of freedom mediates energy flow in molecules after optical excitation. The associated coherent dynamics in polyatomic systems, however, remain experimentally unexplored. Here, we combined transient…
We report attosecond-scale probing of the laser-induced dynamics in molecules. We apply the method of high-harmonic spectroscopy, where laser-driven recolliding electrons on various trajec- tories record the motion of their parent ion.…
The geometric phase is a fundamental quantum mechanical phenomenon uniquely associated with conical intersections (CI) between potential energy surfaces and serves as a definitive signature of their presence. In this study, we propose a…
Many recent experimental ultrafast spectroscopy studies have hinted at non-adiabatic dynamics indicating the existence of conical intersections, but their direct observation remains a challenge. The rapid change of the energy gap between…
When the interaction between a molecular system and confined light modes in an optical or plasmonic cavity is strong enough to overcome the dissipative process, hybrid light-matter states (polaritons) become the fundamental excitations in…
The interplay of nuclear and electronic dynamics characterizes the multi-dimensional electronic spectra of various molecular and solid-state systems. Theoretically, the observable effect of such interplay can be accounted for by response…
Molecular dynamics with electronic friction (MDEF) approach can describe nonadiabatic effects accurately at metal surfaces in the weak nonadiabatic limit. That being said, MDEF treats nuclear motion classically, such that the nuclear…