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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…

Chemical Physics · Physics 2015-09-02 Konstantin E. Dorfman , Kochise Bennett , Shaul Mukamel

Natively, atomic and molecular processes develop in a sub-femtosecond time scale. In order to, for instance, track and capture the electron motion in that scale we need suitable `probes'. Attosecond pulses configure the most appropriate…

The success of non-linear optics relies largely on pulse-to-pulse consistency. In contrast, covariance based techniques used in photoionization electron spectroscopy and mass spectrometry have shown that wealth of information can be…

The correlated behavior of electrons determines the structure and optical properties of molecules, semiconductor and other systems. Valuable information on these correlations is provided by measuring the response to femtosecond laser…

Mesoscale and Nanoscale Physics · Physics 2009-11-13 Shaul Mukamel , Rafal Oszwaldowski , Lijun Yang

Streaking of photoelectrons has long been used for the temporal characterization of attosecond extreme ultraviolet pulses. When the time-resolved photoelectrons originate from a coherent superposition of electronic states, they carry an…

Chemical Physics · Physics 2016-07-27 Markus Kowalewski , Kochise Bennett , Jérémy R. Rouxel , Shaul Mukamel

We propose a scheme for sensing of an oscillating field in systems with large inhomogeneous broadening and driving field variation by applying sequences of phased, adiabatic, chirped pulses. The latter act as a double filter for dynamical…

Quantum Physics · Physics 2020-08-12 Genko T. Genov , Yachel Ben-Shalom , Fedor Jelezko , Alex Retzker , Nir Bar-Gill

State-of-the-art attosecond metrology deals with the detection and characterization of photon pulses with typical energies up to the hundreds of eV and time resolution of several tens of attoseconds. Such short pulses are used for example…

Instrumentation and Detectors · Physics 2015-06-04 Andreas Ipp , Jörg Evers , Christoph H. Keitel , Karen Z. Hatsagortsyan

Conical intersections (CoIn) dominate the pathways and outcomes of virtually all photophysical and photochemical molecular processes. Despite extensive experimental and theoretical effort, CoIns have not been directly observed yet and the…

Chemical Physics · Physics 2015-11-16 Markus Kowalewski , Kochise Bennett , Konstantin E. Dorfman , Shaul Mukamel

We present a novel approach to transient Raman spectroscopy, which combines stochastic probe pulses and a covariance-based detection to measure stimulated Raman signals in alpha-quartz. A coherent broadband pump is used to simultaneously…

Photoelectron interferometry with femto- and atto-second light pulses is a powerful probe of the fast electron wavepacket dynamics, albeit it has practical limitations on the energy resolution. We show that one can simultaneously obtain…

Atomic Physics · Physics 2022-02-24 A. Plunkett , M. A. Alarcon , J. K. Wood , C. H. Greene , A. Sandhu

Excited-state vibrational dynamics in molecules can be studied by an electronically off-resonant Raman process induced by a probe pulse with variable delay with respect to an actinic pulse. We establish the connection between several…

Chemical Physics · Physics 2013-09-27 Konstantin E. Dorfman , Benjamin P. Fingerhut , Shaul Mukamel

Coherent Raman scattering provides highly sensitive vibrational analysis through nonlinear light-matter interactions. However, its application to metal interfaces has remained challenging because the intrinsically large non-resonant…

Two trains of light pulses at periods that are equally shifted from the harmonics of a missing fundamental, are combined in a nonlinear crystal. As a result of a noncollinear phase matched second order nonlinear generation, a new train of…

Other Condensed Matter · Physics 2016-08-16 Xavier Vidal , Pablo Balenzuela , Javier M. Buldú , Jordi Martorell , Jordi García-Ojalvo

We simulate the transient absorption of attosecond pulses of infrared-laser-dressed atoms by considering a three-level system with the adiabatic approximation. The delay-dependent interference features are investigated from the perspective…

Atomic Physics · Physics 2015-09-23 Wenpu Dong , Yongqiang Li , Xiaowei Wang , Jianmin Yuan , Zengxiu Zhao

Tracking the coupled motion of electrons and nuclei on their intrinsic timescales is essential to understanding and controlling photochemical transformations. While attosecond techniques have provided unprecedented insight into electronic…

Realistic attosecond wave packets have complex profiles that, in dispersive conditions, rapidly broaden or split into multiple components. Such behaviors are encoded in sharp features of the wave packet spectral phase. Here, we exploit the…

Attosecond streaking, as a measurement technique, was originally conceived as a means to characterize attosecond light pulses, which is a good approximation if the relevant transition matrix elements are approximately constant within the…

Atomic Physics · Physics 2015-05-19 Vladislav S. Yakovlev , Justin Gagnon , Nicholas Karpowicz , Ferenc Krausz

The basic properties of atoms, molecules and solids are governed by electron dynamics which take place on extremely short time scales. To measure and control these dynamics therefore requires ultrafast sources of radiation combined with…

Atomic Physics · Physics 2008-02-27 J. Mauritsson , P. Johnsson , E. Gustafsson , M. Swoboda , T. Ruchon , A. LHuillier , K. J. Schafer

Many recent experimental ultrafast spectroscopy studies have hinted at non-adiabatic dynamics indicating the existence of conical intersections, but their direct observation remains a challenge. The rapid change of the energy gap between…

Chemical Physics · Physics 2021-05-05 Deependra Jadoun , Mahesh Gudem , Markus Kowalewski

Attosecond science has been transforming our understanding of electron dynamics in atoms, molecules and solids. However, to date almost all of the attoscience experiments have been based on spectroscopic measurements because attosecond…

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