Lorenzo Restaino, Deependra Jadoun, Markus Kowalewski
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引用次数: 4
Abstract
Linear off-resonant x-ray Raman techniques are capable of detecting the ultrafast electronic coherences generated when a photoexcited wave packet passes through a conical intersection. A hybrid femtosecond or attosecond probe pulse is employed to excite the system and stimulate the emission of the signal photon, where both fields are components of a hybrid pulse scheme. In this paper, we investigate how attosecond pulse trains, as provided by high-harmonic generation processes, perform as probe pulses in the framework of this spectroscopic technique, instead of single Gaussian pulses. We explore different combination schemes for the probe pulse as well as the impact of parameters of the pulse trains on the signals. Furthermore, we show how Raman selection rules and symmetry consideration affect the spectroscopic signal, and we discuss the importance of vibrational contributions to the overall signal. We use two different model systems, representing molecules of different symmetries, and quantum dynamics simulations to study the difference in the spectra. The results suggest that such pulse trains are well suited to capture the key features associated with the electronic coherence.
Structural Dynamics-UsCHEMISTRY, PHYSICALPHYSICS, ATOMIC, MOLECU-PHYSICS, ATOMIC, MOLECULAR & CHEMICAL
CiteScore
5.50
自引率
3.60%
发文量
24
审稿时长
16 weeks
期刊介绍:
Structural Dynamics focuses on the recent developments in experimental and theoretical methods and techniques that allow a visualization of the electronic and geometric structural changes in real time of chemical, biological, and condensed-matter systems. The community of scientists and engineers working on structural dynamics in such diverse systems often use similar instrumentation and methods.
The journal welcomes articles dealing with fundamental problems of electronic and structural dynamics that are tackled by new methods, such as:
Time-resolved X-ray and electron diffraction and scattering,
Coherent diffractive imaging,
Time-resolved X-ray spectroscopies (absorption, emission, resonant inelastic scattering, etc.),
Time-resolved electron energy loss spectroscopy (EELS) and electron microscopy,
Time-resolved photoelectron spectroscopies (UPS, XPS, ARPES, etc.),
Multidimensional spectroscopies in the infrared, the visible and the ultraviolet,
Nonlinear spectroscopies in the VUV, the soft and the hard X-ray domains,
Theory and computational methods and algorithms for the analysis and description of structuraldynamics and their associated experimental signals.
These new methods are enabled by new instrumentation, such as:
X-ray free electron lasers, which provide flux, coherence, and time resolution,
New sources of ultrashort electron pulses,
New sources of ultrashort vacuum ultraviolet (VUV) to hard X-ray pulses, such as high-harmonic generation (HHG) sources or plasma-based sources,
New sources of ultrashort infrared and terahertz (THz) radiation,
New detectors for X-rays and electrons,
New sample handling and delivery schemes,
New computational capabilities.