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

Bennett, Kochise; Kowalewski, Markus; Mukamel, Shaul

doi:10.1039/c4fd00178h

Cited by 22 publications

(51 citation statements)

References 54 publications

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“…The nuclear ensemble approach (NEA) can be explored to simulate different steady and time-resolved spectroscopic techniques, including inhomogeneous broadening. [391][392] Usually, working as a post-processing of the dynamics results, the nuclear ensembles have been applied for simulations of a large variety of time-resolved spectra, including twodimensional, differential transmission, 393 photoelectron, 24,217,325,[389][390][394][395][396][397] ultrafast Auger, 24,398 and X-ray photo-scattering 24 spectroscopies. These developments and applications have been based on a broad range of approximations and electronic structure methods, from simple estimates of transition probabilities 24,325,387,395,[399][400][401] to involved modeling of transition moments.…”

Section: Spectroscopic Simulations Based On Na-mqc Dynamicsmentioning

confidence: 99%

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Recent Advances and Perspectives on Nonadiabatic Mixed Quantum–Classical Dynamics

2018

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Nonadiabatic mixed quantum-classical (NA-MQC) dynamics methods form a class of computational theoretical approaches in quantum chemistry tailored to investigate the time evolution of nonadiabatic phenomena in molecules and supramolecular assemblies. NA-MQC is characterized by a partition of the molecular system into two subsystems: one to be treated quantum mechanically (usually but not restricted to electrons) and another to be dealt with classically (nuclei). The two subsystems are connected through nonadiabatic couplings terms to enforce self-consistency. A local approximation underlies the classical subsystem, implying that direct dynamics can be simulated, without needing precomputed potential energy surfaces. The NA-MQC split allows reducing computational costs, enabling the treatment of realistic molecular systems in diverse fields. Starting from the three most well-established methods-mean-field Ehrenfest, trajectory surface hopping, and multiple spawning-this review focuses on the NA-MQC dynamics methods and programs developed in the last 10 years. It stresses the relations between approaches and their domains of application. The electronic structure methods most commonly used together with NA-MQC dynamics are reviewed as well. The accuracy and precision of NA-MQC simulations are critically discussed, and general guidelines to choose an adequate method for each application are delivered.

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Section: Spectroscopic Simulations Based On Na-mqc Dynamicsmentioning

confidence: 99%

“…423 An excellent general discussion on the use of ensembles to compute time-resolved photoelectron, Auger-electron, and X-ray photon scattering spectroscopy can be found in Ref. 24 .…”

Section: Pump-probe Spectrummentioning

confidence: 99%

Recent Advances and Perspectives on Nonadiabatic Mixed Quantum–Classical Dynamics

2018

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“…These incoherent detection modes are more versatile and often more convenient [71]. Electron spectroscopies, including time-resolved photoelectron spectroscopy (TRPES) and Auger probing following x-ray pulse sequences should be extremely valuable [72][73][74]78]. Electron rather than photon detection is more sensitive in many cases.…”

Section: Discussion and Summarymentioning

confidence: 99%

Multidimensional resonant nonlinear spectroscopy with coherent broadband x-ray pulses

et al. 2016

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New x-ray free electron laser (XFEL) and high harmonic generation (HHG) light sources are capable of generating short and intense pulses that make x-ray nonlinear spectroscopy possible. Multidimensional spectroscopic techniques, which have long been used in the nuclear magnetic resonance, infrared, and optical regimes to probe the electronic structure and nuclear dynamics of molecules by sequences of short pulses with variable delays, can thus be extended to the attosecond x-ray regime. This opens up the possibility of probing core-electronic structure and couplings, the real-time tracking of impulsively created valence-electronic wavepackets and electronic coherences, and monitoring ultrafast processes such as nonadiabatic electron-nuclear dynamics near conical-intersection crossings. We survey various possible types of multidimensional x-ray spectroscopy techniques and demonstrate the novel information they can provide about molecules.

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“…X-ray signals allow one to probe valence excitations rather than vibrations. Furthermore, both the initial preparation and/or the preparation process can then be the product of an X-ray scattering, photoionization, or Auger process (as recently discussed in [24,40]) in addition to an X-ray pulse E 1 centered at t 1 interacts with the system and after another delay T 2 = t 2 − t 1 the second pulse E 2 centered at t 2 yields the two-dimensional spectra as a function of the two time delays. The corresponding diagrams are given in Fig.…”

Section: Discussionmentioning

confidence: 99%

Detecting electronic coherence by multidimensional broadband stimulated x-ray Raman signals

2015

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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 propose several stimulated-Raman detection schemes that can monitor the phase-sensitive electronic and nuclear dynamics. Three detection protocols of an X-ray broadband probe are compared -frequency dispersed transmission, integrated photon number change, and total pulse energy change. In addition each can be either linear or quadratic in the X-ray probe intensity. These various signals offer different gating windows into the molecular response which is described by correlation functions of electronic polarizabilities.Off-resonant and resonant signals are compared. * kdorfman@uci.edu 1 arXiv:1506.08226v1 [physics.chem-ph]

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

Cited by 22 publications

References 54 publications

Recent Advances and Perspectives on Nonadiabatic Mixed Quantum–Classical Dynamics

Recent Advances and Perspectives on Nonadiabatic Mixed Quantum–Classical Dynamics

Multidimensional resonant nonlinear spectroscopy with coherent broadband x-ray pulses

Detecting electronic coherence by multidimensional broadband stimulated x-ray Raman signals

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