X-ray scattering signatures of early-time accelerations in iodine dissociation

Gabalski, Ian; Ware, Matthew; Bucksbaum, P. H.

doi:10.1088/1361-6455/abc22a

Cited by 3 publications

(4 citation statements)

References 24 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…along the pump-probe delay axis τ . Molecular vibrations and dissociations are mapped to sparse and easily interpreted features in the FRXS representation 26,32,41 . Vibrations appear as horizontal lines centered at the vibrational frequency, with the phase of these lines giving information about the equilibrium bond distance of the vibration 41 .…”

Section: B Frequency-resolved Analysismentioning

confidence: 99%

“…Dissociations appear as slanted lines in the FRXS power spectrum |S(Q, ν)| 2 where the radial dissociation velocity v corresponds to the slope of the line: 26 ν = Qv. The phase of these dissociation lines gives information about the dissociation time shift 27,41 and the initial period of acceleration 32 .…”

Section: B Frequency-resolved Analysismentioning

confidence: 99%

“…TRXS is a well-proven technique for the measurement of the evolution of molecular structure in photochemical reactions [26][27][28][29][30][31][32][33][34][35][36][37][38] . In gas-phase TRXS experiments, a hard X-ray pulse probes the electron charge density distribution surrounding the nuclei following molecular photoexcitation.…”

Section: Introductionmentioning

confidence: 99%

“…Time-domain analysis can distinguish between types of vibrational motion, quantify timescales of this motion, and support and validate calculations of molecular dynamics 30,33,39 . Frequencyresolved X-ray scattering (FRXS) provides an alternate view of TRXS data that facilitates the measurement of vibrational frequencies, dissociation velocities, and nuclear acceleration 26,27,32,40,41 . We employ both timeand frequency-domain techniques to extract information about the nuclear motion of UV-photoexcited CS 2 .…”

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

Transient vibration and product formation of photoexcited CS2 measured by time-resolved x-ray scattering

Gabalski

Sere

Acheson

et al. 2022

The Journal of Chemical Physics

Self Cite

View full text Add to dashboard Cite

We have observed details of the internal motion and dissociation channels in photoexcited carbon disulfide (CS2) using time-resolved X-ray scattering (TRXS). Photoexcitation of gas-phase CS2 with a 200 nm laser pulse launches oscillatory bending and stretching motion leading to dissociation of atomic sulfur in under a picosecond. During the first 300 fs following excitation we observe significant changes in the vibrational frequency as well as some dissociation of the C-S bond leading to atomic sulfur in the both 1D and 3P states. Beyond 1400 fs the dissociation is consistent with primarily 3P atomic sulfur dissociation. This channel-resolved measurement of the dissociation time is based on our analysis of the time-windowed dissociation radial velocity distribution, which is measured using the temporal Fourier transform of the TRXS data aided by a Hough transform that extracts the slopes of linear features in an image. The relative strength of the two dissociation channels reflects both their branching ratio and differences in the spread of their dissociation times. Measuring the time-resolved dissociation radial velocity distribution aids the resolution of discrepancies between models for dissociation proposed by prior photoelectron spectroscopy work.

show abstract

Section: B Frequency-resolved Analysismentioning

confidence: 99%

Section: B Frequency-resolved Analysismentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

Transient vibration and product formation of photoexcited CS2 measured by time-resolved x-ray scattering

Gabalski

Sere

Acheson

et al. 2022

The Journal of Chemical Physics

Self Cite

View full text Add to dashboard Cite

show abstract

Time-resolved X-ray Scattering of Excited State Structure and Dynamics

Yong,

Kirrander,

Weber

2023

Structural Dynamics With X-Ray and Electron Scattering

View full text Add to dashboard Cite

Ultrafast gas-phase X-ray scattering using X-ray free-electron lasers (XFELs) has enabled the measurement of molecular structures and dynamics in excited states with atomic spatial and femtosecond time resolution. This chapter reviews important recent advances in the X-ray scattering of excited states. In particular, details will be given of additional observables such as the orientation of optical transition dipoles within the molecular frame, the excited state molecular electron densities, and rate constants for chemical kinetics. In excited states, the structures of medium sized molecules (up to eight non-hydrogenic atoms) have been determined with high precision in the non-hydrogenic atom–atom distances. Effects arising from the redistribution of electron density upon optical excitation are observed and confirmed by high-level calculations, allowing for the observation of ultrafast excited state charge transfer reactions. Fragmentation of molecules is readily observed, and is identifiable from a characteristic decrease in the X-ray scattering signal at small scattering angles. Furthermore, the structures of transient radical fragments have been measured.

show abstract

A comparative review of time-resolved x-ray and electron scattering to probe structural dynamics

Lee,

Oang,

Kim

et al. 2024

Structural Dynamics

View full text Add to dashboard Cite

The structure of molecules, particularly the dynamic changes in structure, plays an essential role in understanding physical and chemical phenomena. Time-resolved (TR) scattering techniques serve as crucial experimental tools for studying structural dynamics, offering direct sensitivity to molecular structures through scattering signals. Over the past decade, the advent of x-ray free-electron lasers (XFELs) and mega-electron-volt ultrafast electron diffraction (MeV-UED) facilities has ushered TR scattering experiments into a new era, garnering significant attention. In this review, we delve into the basic principles of TR scattering experiments, especially focusing on those that employ x-rays and electrons. We highlight the variations in experimental conditions when employing x-rays vs electrons and discuss their complementarity. Additionally, cutting-edge XFELs and MeV-UED facilities for TR x-ray and electron scattering experiments and the experiments performed at those facilities are reviewed. As new facilities are constructed and existing ones undergo upgrades, the landscape for TR x-ray and electron scattering experiments is poised for further expansion. Through this review, we aim to facilitate the effective utilization of these emerging opportunities, assisting researchers in delving deeper into the intricate dynamics of molecular structures.

show abstract

X-ray scattering signatures of early-time accelerations in iodine dissociation

Cited by 3 publications

References 24 publications

Transient vibration and product formation of photoexcited CS2 measured by time-resolved x-ray scattering

Transient vibration and product formation of photoexcited CS2 measured by time-resolved x-ray scattering

Time-resolved X-ray Scattering of Excited State Structure and Dynamics

A comparative review of time-resolved x-ray and electron scattering to probe structural dynamics

Contact Info

Product

Resources

About