相关论文: Resolving Competing Conical Intersection Pathways:…
Ongoing developments in ultrafast X-ray sources offer powerful new means of probing the com- plex non-adiabatically coupled structural and electronic dynamics of photoexcited molecules. These non-Born-Oppenheimer effects are governed by…
Time-resolved coincidence imaging of photoelectrons and photoions represents the most complete experimental measurement of ultrafast excited state dynamics, a multi-dimensional measurement for a multi-dimensional problem. Here we present…
X-ray spectroscopy has been a key method to determine ground and excited state properties of quantum materials with atomic specificity. Now, new x-ray facilities are opening the door to the study of pump-probe x-ray spectroscopy -…
Conical intersections play a pivotal role in excited-state quantum dynamics. Capturing transient molecular structures near conical intersections remains challenging due to the rapid timescales and subtle structural changes involved. We…
We assess the performance of different protocols for simulating excited-state X-ray absorption spectra. We consider three different protocols based on equation-of-motion coupled-cluster singles and doubles, two of them combined with the…
Time-resolved X-ray Emission/Absorption Spectroscopy (Tr-XES/XAS) is an informative experimental tool sensitive to electronic dynamics in materials, widely exploited in diverse research fields. Typically, Tr-XES/XAS requires X-ray pulses…
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…
Time-resolved X-ray absorption spectroscopy (TR-XAS), based on laser-pump/X-ray probe method, is powerful in capturing the change of geometrical and electronic structure of the absorbing atom upon excitation. TR-XAS data analysis is…
Non-adiabatic dynamics and conical intersections play a central role in the chemistry of most polyatomic molecules, ranging from isomerization to heterocyclic ring opening and avoided photo-damage of DNA. Studying the underpinning…
Conical intersections (CoIn) dominate the pathways and outcomes of virtually all photophysical and photochemical molecular processes. Despite extensive experimental and theoretical effort, CoIns have not been directly observed yet and the…
The electronic excitation occurring on adsorbates at ultrafast time scales from optical lasers that initiate surface chemical reactions is still an open question. Here, we report the ultrafast temporal evolution of X-ray absorption…
Conical intersections between electronic states often dictate the chemistry of photoexcited molecules. Recently developed sources of ultrashort extreme ultraviolet (XUV) pulses tuned to element-specific transitions in molecules allow for…
Transient X-ray absorption techniques can measure ultrafast dynamics of the elemental edges in a material or multiple layer junction, giving them immense potential for deconvoluting concurrent processes. However, the interpretation of the…
Conical intersections constitute the conceptual bedrock of our working understanding of ultrafast, nonadiabatic processes within photochemistry (and photophysics). Accurate calculation of potential energy surfaces within the vicinity of…
We show that time-resolved x-ray scattering from molecules prepared in a superposition of electronic states moving through an avoided crossing has new features not found in diffraction from the corresponding classical mixed state.…
Modern X-ray spectroscopy has proven itself as a robust tool for probing the electronic structure of atoms in complex environments. Despite working on energy scales that are much larger than those corresponding to nuclear motions, taking…
Conical intersections serve as critical gateways in photochemical reactions, enabling rapid nonradiative transitions between potential energy surfaces that underpin fundamental processes such as photosynthesis or vision. Their calculation…
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…
Conical intersections between electronic potential energy surfaces are paradigmatic for the study of non-adiabatic processes in the excited states of large molecules. However, since the corresponding dynamics occurs on a femtosecond…
Time-resolved x-ray scattering (TRXS) measures internuclear separations in a molecule following laser-induced photoexcitation. The molecular dynamics induced by the excitation laser may lie on one or several bound or dissociative electronic…