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Coherence among rotational ion channels during photoionization is exploited to control the anisotropy of the resulting photoelectron angular distributions at specific photoelectron energies. The strategy refers to a robust and single…

化学物理 · 物理学 2019-09-11 R. Chamakhi , M. Telmini , O. Atabek , E. Charron

Non-adiabatic dynamics and conical intersections play a central role in the chemistry of most polyatomic molecules, ranging from isomerization to heterocyclic ring opening and avoided photo-damage of DNA. Studying the underpinning…

化学物理 · 物理学 2024-11-07 S. Severino , K. M. Ziems , M. Reduzzi , A. Summers , H. -W. Sun , Y. -H. Chien , S. Gräfe , J. Biegert

Time-resolved photoelectron spectra are proposed for the measurement of classical information recorded in the quantum phases of a molecular rotational wave packet. Taking Li2 as a prototypical system, we show that an interference arises…

量子物理 · 物理学 2007-05-23 Eric Charron , Maurice Raoult

X-ray four-wave mixing signals generated in the $k_1 + k_2 - k_3$ phase-matching direction are simulated for N1s transitions in para-nitroanline and two-ring hydrocarbons disubstituted with an amine and a nitroso groups. The two-dimensional…

原子物理 · 物理学 2008-11-20 Igor V. Schweigert , Shaul Mukamel

We explore the novel capabilities offered by attosecond extreme ultraviolet and x-ray pulses that can be now generated by free-electron lasers and high-harmonics generation sources for probing photon-induced electron dynamics in molecules.…

量子物理 · 物理学 2023-02-15 Marvin Reuner , Daria Popova-Gorelova

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…

介观与纳米尺度物理 · 物理学 2009-11-13 Shaul Mukamel , Rafal Oszwaldowski , Lijun Yang

Photoinduced quantum dynamics in molecules have hierarchical temporal structures with different energy scales that are associated with electron and nuclear motions. Femtosecond-to-attosecond transient absorption spectroscopy (TAS) using…

We have recorded the coherent diffraction images of individual xenon clusters with intense extreme ultraviolet pulses to elucidate the influence of light-induced electronic changes on the diffraction pattern. Using the FLASH free-electron…

The detection of electron motion and electronic wavepacket dynamics is one of the core goals of attosecond science. Recently, choosing the nitric oxide (NO) molecule as an example, we have introduced and demonstrated a new experimental…

原子与分子团簇 · 物理学 2015-04-17 Song Bin Zhang , Denitsa Baykusheva , Peter M. Kraus , Hans Jakob Wörner , Nina Rohringer

We investigate the creation of double K-shell holes in N2 molecules via sequential absorption of two photons on a timescale shorter than the core-hole lifetime by using intense x-ray pulses from the Linac Coherent Light Source free electron…

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…

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…

The coupling of electronic and nuclear motion in polyatomic molecules is at the heart of attochemistry. The molecular properties, transient structures and reaction mechanism of these many-body quantum objects are defined on the level of…

We show that the complete photoemission dynamics in situations of electron-ion entanglement can be retrieved from photoelectron spectral measurements without information on the ion. To this end, we develop an energy-time analysis of the…

Numerical simulations are presented to validate the possible use of cutting-edge attosecond time- resolved photoelectron spectroscopy to observe in real time the creation of an electronic wavepacket and subsequent electronic motion in a…

原子与分子团簇 · 物理学 2015-06-22 Aurelie Perveaux , David Lauvergnat , Fabien Gatti , Gabor Halasz , Agnes Vibok , Benjamin Lasorne

We explore the effects of correlation on the ground-state energies and on photoionization dynamics in atomic Be and Ne. We apply the time-dependent restricted-active-space self-consistent-field method for several excitation schemes and…

原子物理 · 物理学 2019-03-27 Juan J. Omiste , Lars Bojer Madsen

Imaging changes in molecular geometries on their natural femtosecond timescale with sub-Angstrom spatial precision is one of the critical challenges in the chemical sciences, since the nuclear geometry changes determine the molecular…

Split-pulse x-ray photon correlation spectroscopy has been proposed as one of the unique capabilities made possible with the x-ray free electron lasers. It enables characterization of atomic scale structural dynamics that dictates the…

仪器与探测器 · 物理学 2020-05-06 Yanwen Sun , Mike Dunne , Paul Fuoss , Taito Osaka , Aymeric Robert , Mark Sutton , Makina Yabashi , Diling Zhu

We employ the R-matrix with time-dependence method to study attosecond angular streaking of F$^-$. Using this negative ion, free of long-range Coulomb interactions, we elucidate the role of short-range electron correlation effects in an…

原子物理 · 物理学 2020-05-20 G. S. J. Armstrong , D. D. A. Clarke , J. Benda , A. C. Brown , H. W. van der Hart

Exchange correlation plays an important role in double-ionization of complex atoms by ultrashort laser pulse. In this work, we investigate two-photon double inner-shell electron ionization of neon induced by an attosecond extreme…

原子物理 · 物理学 2019-06-05 Jianpeng Liu , Yongqiang Li , Jianmin Yuan