scholarly journals Probing electronic and vibrational dynamics in molecules by time-resolved photoelectron, Auger-electron, and X-ray photon scattering spectroscopy

2015 ◽  
Vol 177 ◽  
pp. 405-428 ◽  
Author(s):  
Kochise Bennett ◽  
Markus Kowalewski ◽  
Shaul Mukamel

We present a unified description for time-resolved electron and photon scattering spectroscopies from molecules prepared in nonstationary states. Signals are expressed in terms of superoperator Green's functions and a systematic procedure for treating various degrees of freedom consistently at different levels of theory is developed. The standard Fermi Golden Rule expressions for photoelectron spectra, which are limited to broad, slowly-varying signals, are obtained as a limiting case of our more general theory that applies to broader parameter regimes.

2021 ◽  
Vol 6 (1) ◽  
Author(s):  
E. Paris ◽  
C. W. Nicholson ◽  
S. Johnston ◽  
Y. Tseng ◽  
M. Rumo ◽  
...  

AbstractInvestigations of magnetically ordered phases on the femtosecond timescale have provided significant insights into the influence of charge and lattice degrees of freedom on the magnetic sub-system. However, short-range magnetic correlations occurring in the absence of long-range order, for example in spin-frustrated systems, are inaccessible to many ultrafast techniques. Here, we show how time-resolved resonant inelastic X-ray scattering (trRIXS) is capable of probing such short-ranged magnetic dynamics in a charge-transfer insulator through the detection of a Zhang–Rice singlet exciton. Utilizing trRIXS measurements at the O K-edge, and in combination with model calculations, we probe the short-range spin correlations in the frustrated spin chain material CuGeO3 following photo-excitation, revealing a strong coupling between the local lattice and spin sub-systems.


Science ◽  
2020 ◽  
Vol 367 (6474) ◽  
pp. 186-189 ◽  
Author(s):  
Jayadev Vijayan ◽  
Pimonpan Sompet ◽  
Guillaume Salomon ◽  
Joannis Koepsell ◽  
Sarah Hirthe ◽  
...  

Elementary particles carry several quantum numbers, such as charge and spin. However, in an ensemble of strongly interacting particles, the emerging degrees of freedom can fundamentally differ from those of the individual constituents. For example, one-dimensional systems are described by independent quasiparticles carrying either spin (spinon) or charge (holon). Here, we report on the dynamical deconfinement of spin and charge excitations in real space after the removal of a particle in Fermi-Hubbard chains of ultracold atoms. Using space- and time-resolved quantum gas microscopy, we tracked the evolution of the excitations through their signatures in spin and charge correlations. By evaluating multipoint correlators, we quantified the spatial separation of the excitations in the context of fractionalization into single spinons and holons at finite temperatures.


2020 ◽  
Vol 11 (1) ◽  
Author(s):  
Federico S. Gnesotto ◽  
Grzegorz Gradziuk ◽  
Pierre Ronceray ◽  
Chase P. Broedersz

Abstract Time-lapse microscopy imaging provides direct access to the dynamics of soft and living systems. At mesoscopic scales, such microscopy experiments reveal intrinsic thermal and non-equilibrium fluctuations. These fluctuations, together with measurement noise, pose a challenge for the dynamical analysis of these Brownian movies. Traditionally, methods to analyze such experimental data rely on tracking embedded or endogenous probes. However, it is in general unclear, especially in complex many-body systems, which degrees of freedom are the most informative about their non-equilibrium nature. Here, we introduce an alternative, tracking-free approach that overcomes these difficulties via an unsupervised analysis of the Brownian movie. We develop a dimensional reduction scheme selecting a basis of modes based on dissipation. Subsequently, we learn the non-equilibrium dynamics, thereby estimating the entropy production rate and time-resolved force maps. After benchmarking our method against a minimal model, we illustrate its broader applicability with an example inspired by active biopolymer gels.


2019 ◽  
Vol 9 (1) ◽  
Author(s):  
Weifang Lu ◽  
Abebe T. Tarekegne ◽  
Yiyu Ou ◽  
Satoshi Kamiyama ◽  
Haiyan Ou

Abstract A comprehensive study of surface passivation effect on porous fluorescent silicon carbide (SiC) was carried out to elucidate the luminescence properties by temperature dependent photoluminescence (PL) measurement. The porous structures were prepared using an anodic oxidation etching method and passivated by atomic layer deposited (ALD) Al2O3 films. An impressive enhancement of PL intensity was observed in porous SiC with ALD Al2O3, especially at low temperatures. At temperatures below 150 K, two prominent PL emission peaks located at 517 nm and 650 nm were observed. The broad emission peak at 517 nm was attributed to originate from the surface states in the porous structures, which was supported by X-ray photoelectron spectra characterization. The emission peak at 650 nm is due to donor-acceptor-pairs (DAP) recombination via nitrogen donors and boron-related double D-centers in fluorescent SiC substrates. The results of the present work suggest that the ALD Al2O3 films can effectively suppress the non-radiative recombination for the porous structures on fluorescent SiC. In addition, we provide the evidence based on the low-temperature time-resolved PL that the mechanism behind the PL emission in porous structures is mainly related to the transitions via surface states.


Author(s):  
Yuanqin Xia ◽  
Yang Zhao ◽  
Sheng Zhang ◽  
Ping He ◽  
Zhiwei Dong ◽  
...  

2019 ◽  
Vol 30 (9) ◽  
pp. 4185-4201
Author(s):  
Daniel Klatt ◽  
Michael Proff ◽  
Robert Hruschka

Purpose The present work aims to investigate the capabilities of accurately predicting the six-degrees-of-freedom (6DoF) trajectory and the flight behavior of a flare-stabilized projectile using computational fluid dynamics (CFD) and rigid body dynamics (RBD) methods. Design/methodology/approach Two different approaches are compared for calculating the trajectory. First, the complete matrix of static and dynamic aerodynamic coefficients for the projectile is determined using static and dynamic CFD methods. This discrete database and the data extracted from free-flight experiments are used to simulate flight trajectories with an in-house developed 6DoF solver. Second, the trajectories are simulated solving the 6DoF motion equations directly coupled with time resolved CFD methods. Findings Virtual fly-out simulations using RBD/CFD coupled simulation methods well reproduce the motion behavior shown by the experimental free-flight data. However, using the discrete database of aerodynamic coefficients derived from CFD simulations shows a slightly different flight behavior. Originality/value A discrepancy between CFD 6DoF/RBD simulations and results obtained by the MATLAB 6DoF-solver based on discrete CFD data matrices is shown. It is assumed that not all dynamic effects on the aerodynamics of the projectile are captured by the determination of the force and moment coefficients with CFD simulations based on the classical aerodynamic coefficient decomposition.


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