相关论文: Core-hole Coherent Spectroscopy in Molecules
In quantum systems, coherent superpositions of electronic states evolve on ultrafast timescales (few femtosecond to attosecond, 1 as = 0.001 fs = 10^{-18} s), leading to a time dependent charge density. Here we exploit the first attosecond…
We introduce and demonstrate a new approach to measuring coherent electron wave packets using high-harmonic spectroscopy. By preparing a molecule in a coherent superposition of electronic states, we show that electronic coherence opens…
In recent years, ultrafast pump-probe spectroscopy has provided insightful information about nonequilibrium dynamics of excitations in materials. In a typical experiment of time-resolved x-ray absorption spectroscopy, the systems are…
We propose an imaging technique to follow core-hole wave-packet oscillations in the nitrogen molecule. In this scheme, an attosecond x-ray pulse core-ionizes the nitrogen molecule and a subsequent attosecond x-ray pulse probes the evolution…
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…
We study the core hole-electron correlation in coherently coupled molecules by energy dispersive near edge X-ray absorption fine-structure spectroscopy. In a transient phase, which exists during the transition between two bulk arrangements,…
Quantum coherence between electronic states of a photoionized molecule and the resulting process of ultrafast electron-hole migration have been put forward as a possible quantum mechanism of charge-directed reactivity governing the…
Coherent superposition of electronic states, created by ionizing a molecule, can initiate ultrafast dynamics of the electron density. Correlation between nuclear and electron motions, however, typically dissipates the electronic coherence…
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…
Optical excitation and control of excitonic wavepackets in organic molecules is the basis to energy conversion processes. To gain insights into such processes, it is essential to establish the relationship between the coherence timescales…
We propose a protocol to probe the ultrafast evolution and dephasing of coherent electronic excitation in molecules in the time domain by the intrinsic streaking field generated by the molecule itself. Coherent electronic motion in 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…
A deep understanding of molecular photo-transformations is challenging because of the complex interaction between the configurations of electrons and nuclei. An initial optical excitation dissipates energy into electronic and structural…
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…
We propose an approach to probe coherent spin-state dynamics of molecules using circularly polarized hard x-ray pulses. For the dynamically aligned nitric oxide molecules in a coherent superposition spin-orbit coupled electronic state that…
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…
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…
The capability of generating two intense, femtosecond x-ray pulses with controlled time delay opens the possibility of performing time-resolved experiments for x-ray induced phenomena. We have applied this capability to study the…
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…
We develop a large scale quantum master equation approach to describe dynamical processes of practical open quantum systems driven by both coherent and stochastic interactions by including more than one thousand true states of the systems,…