Soft X-ray-Driven Femtosecond Molecular Dynamics

Gagnon, Etienne; Ranitovic, Predrag; Tong, Xiao-Min; Cocke, C. L.; Murnane, Margaret M.; Kapteyn, Henry C.; Sandhu, Arvinder

doi:10.1126/science.1144920

Cited by 194 publications

(149 citation statements)

References 29 publications

(27 reference statements)

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“…As can be seen, both potentials are nearly identical in the vicinity of the energy minimum, thus suggesting that a Morse description of core-hole states for which standard CASSCF-MRCI calculations are not so easy to perform is accurate enough. For the ground state of the neutral and the cation, as well as for the lowest excited (valence) states of the cation, our calculated potential energy curves are in very good agreement with the ones previously reported in the literature 7,60,65,114,120,[126][127][128][129][130][131][132][133][134][135][136][137][138][139][140] .…”

Section: Inclusion Of the Nuclear Motionsupporting

confidence: 79%

Vibrational branching ratios in the photoelectron spectra of N2 and CO: interference and diffraction effects

Plésiat

Decleva

Martín

2012

Phys. Chem. Chem. Phys.

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Esta es la versión de autor del artículo publicado en: This is an author produced version of a paper published in: We present a detailed account of existing theoretical methods specially designed to provide vibrationally resolved photoionization cross sections of simple molecules within the Born-Oppenheimer approximation, with emphasis on newly developed methods based on density functional theory. The performance of these methods is shown for the case of N 2 and CO photoionization. Particular attention is paid to the region of high photon energies, where the electron wavelength is comparable to the bond length and, therefore, two-center interferences and diffraction are expected to occur. As shown in a recent work [Canton et al., Proc. Natl. Acad. Sci., 2011, 108, 73027306], the main experimental difficulty, which is to extract the relatively small diffraction features from the rapidly decreasing cross section, can be easily overcome by determining ratios of vibrationally resolved photoelectron spectra and existing theoretical calculations. From these ratios, one can thus get direct information about the molecular geometry. In this work, results obtained in a wide range of photon energies and for many different molecular orbitals of N 2 and CO are discussed and compared with the available experimental measurements. From this comparison, limitations and further possible improvements of the existing theoretical methods are discussed. The new results presented in the manuscript confirm that the conclusions reported in the above reference are of general validity.

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Section: Inclusion Of the Nuclear Motionsupporting

confidence: 79%

Vibrational branching ratios in the photoelectron spectra of N2 and CO: interference and diffraction effects

Plésiat

Decleva

Martín

2012

Phys. Chem. Chem. Phys.

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“…This spectrum is used in the following to further confirm that the PECs involved in the nuclear motion have been identified correctly (compare Refs. [23,24] for a similar approach). As in the ion spectra, a clear signal is visible at E QB ≈ 0.1 eV.…”

Section: Photoelectronsmentioning

confidence: 99%

Probing calculatedO2+potential-energy curves with an XUV-IR pump-probe experiment

et al. 2015

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We study dissociative photoionization of molecular oxygen in a kinematically complete XUV-IR pump-probe experiment. Detecting charged fragments and photoelectrons in coincidence using a reaction microscope, we observe a pump-probe delay-dependent yield of very low energetic O + ions which oscillates with a period of 40 fs. This feature is caused by a time-dependent vibrational wave packet in the potential of the binding O 2 + (a 4 u ) state, which is probed by resonant absorption of a single infrared photon to the weakly repulsive O 2 + (f 4 g ) state. By quantitative comparison of the experimental kinetic-energy-release (KER) and quantum-beat (QB) spectra with the results of a coupled-channel simulation, we are able to discriminate between the calculated adiabatic O + 2 potential-energy curves ( (2012)]. In general, we find a good agreement between experimental and simulated KER and QB spectra. However, we could not reproduce all features of the experimental data with these PECs. In contrast, adjusting a Morse potential to the experimental data, most features of the experimental spectra are well reproduced by our simulation. By comparing this Morse potential to theoretically predicted PECs, we demonstrate the sensitivity of our experimental method to small changes in the shape of the binding potential.

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“…In recent years, tremendous progress has been made in the study of molecular nuclear dynamics induced by strongfield ionization [7][8][9] and valence photoabsorption [10][11][12][13]. These studies consist of a wide variety of time-resolved experiments, in which the pump or/and the probe is a strongfield optical laser.…”

Section: Introductionmentioning

confidence: 99%

Ultrafast x-ray-induced nuclear dynamics in diatomic molecules using femtosecond x-ray-pump–x-ray-probe spectroscopy

et al. 2016

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The capability of generating two intense, femtosecond x-ray pulses with a controlled time delay opens the possibility of performing time-resolved experiments for x-ray-induced phenomena. We have applied this capability to study the photoinduced dynamics in diatomic molecules. In molecules composed of low-Z elements, K-shell ionization creates a core-hole state in which the main decay mode is an Auger process involving two electrons in the valence shell. After Auger decay, the nuclear wave packets of the transient two-valence-hole states continue evolving on the femtosecond time scale, leading either to separated atomic ions or long-lived quasibound states. By using an x-ray pump and an x-ray probe pulse tuned above the K-shell ionization threshold of the nitrogen molecule, we are able to observe ion dissociation in progress by measuring the time-dependent kinetic energy releases of different breakup channels. We simulated the measurements on N 2 with a molecular dynamics model that accounts for K-shell ionization, Auger decay, and the time evolution of the nuclear wave packets. In addition to explaining the time-dependent feature in the measured kinetic energy release distributions from the dissociative states, the simulation also reveals the contributions of quasibound states.

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Soft X-ray-Driven Femtosecond Molecular Dynamics

Cited by 194 publications

References 29 publications

Vibrational branching ratios in the photoelectron spectra of N2 and CO: interference and diffraction effects

Vibrational branching ratios in the photoelectron spectra of N2 and CO: interference and diffraction effects

Probing calculatedO2+potential-energy curves with an XUV-IR pump-probe experiment

Ultrafast x-ray-induced nuclear dynamics in diatomic molecules using femtosecond x-ray-pump–x-ray-probe spectroscopy

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