相关论文: Multidimensional X-Ray Spectroscopy of Valence and…
Expressions for the two-dimensional Stimulated x-ray Raman Spectroscopy (2D-SXRS) signal obtained using attosecond x-ray pulses are derived. The 1D- and 2D-SXRS signals are calculated for trans-N-methyl acetamide (NMA) with broad bandwidth…
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…
We propose two dimensional x-ray coherent correlation spectroscopy (2DXCS) for the study of interactions between core-electron and valence transitions. This technique might find experimental applications in the future when very high…
Nonstationary molecular states which contain electronic coherences can be impulsively created and manipulated by using recently-developed ultrashort optical and X-ray pulses via photoexcitation, photoionization and Auger processes. We…
We present an approach for initiating and tracing ultra-fast electron dynamics in core-excited atoms, molecules and solids. The approach is based on stimulated resonant inelastic x-ray scattering induced by a single, chirped, broadband…
The attosecond, time-resolved X-ray double-quantum-coherence (XDQC) four wave mixing signals of formamide at the nitrogen and oxygen K-edges are simulated using restricted excitation window time-dependent density functional theory…
Bound state, valence electronic excitation spectra of N_2 are probed by nonresonant inelastic x-ray and electron scattering. Within the usual theoretical treatments, dynamical structure factors derived from the two probes should be…
We present an ab initio study of neutral core and valence electronic excitations in {\alpha}-Al2O3 by solving the Bethe-Salpeter equation (BSE) of many-body perturbation theory within an all-electron framework. Calculated spectra at the Al…
Intense few-to-sub-femtosecond soft x-ray pulses can produce neutral, two-site excited double-core-hole states by promoting two core electrons to the same unoccupied molecular orbital. We theoretically investigate double nitrogen K-edge…
Using a model Hamiltonian, we discuss how we could interpret data obtained from transition metal $K$-edge resonant inelastic x-ray scattering (RIXS) experiments. By analyzing the creation of valence excitations from the screening of the…
Photophysical and photochemical processes are ruled by the interplay between transient vibrational and electronic degrees of freedom, which are ultimately determined by the multidimensional potential energy surfaces (PESs). Differences…
Correlation-function expressions are derived for the coherent nonlinear response of molecules to three resonant ultrafast pulses in the x-ray regime. The ability to create two-core-hole states with controlled attosecond timing in…
Time-dependent equation-of-motion coupled cluster (TD-EOM-CC) is used to simulate impulsive stimulated x-ray Raman scattering (ISXRS) of ultrashort laser pulses by neon, carbon monoxide, pyrrole, and p-aminophenol. The TD-EOM-CC equations…
We present a microscopic theory of resonant soft x-ray scattering (RSXS) that accounts for the delocalized character of valence electrons. Unlike past approaches defined in terms of form factors for atoms or clusters, we develop a…
We present a theoretical study of temporal, spectral, and spatial reshaping of intense, ultrafast x-ray pulses propagating through a resonant medium. Our calculations are based on the solution of a 3D time-dependent Schr\"odinger-Maxwell…
We have observed the signatures of valence electron rearrangement in photoexcited ammonia using ultrafast hard X-ray scattering. Time-resolved X-ray scattering is a powerful tool for imaging structural dynamics in molecules because of the…
Polarization dependence has historically seen extensive use in x-ray spectroscopy to determine magnetic and local geometric properties, but more broadly as a way to gain extra sensitivity to electronic structure at the level of individual…
We investigate mixed-valence oxide Co$_3$O$_4$ using Co $2p3d$ resonant inelastic X-ray scattering (RIXS). By setting resonant edges at Co$^{2+}$ and Co$^{3+}$ ions, the $dd$ excitations on the two Co sites are probed selectively, providing…
The temporal dynamics of stimulated emission is studied, with the particular emphasis on stimulated emission induced by x-ray pulses interacting with nuclei. In typical nuclear forward scattering experiments, the short incident x-ray pulse…
We develop the theory for shallow-core to valence excitations when the multiplet spread is larger than the core-hole attraction, e.g., if the core and valence orbitals have the same principal quantum number. This results in a cross-over…