Visualizing ultrafast chemical dynamics with X-rays

Sension, Roseanne J.

doi:10.1073/pnas.2017806117

Cited by 4 publications

(4 citation statements)

References 16 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Time-resolved X-ray spectroscopies have extended chemical selectivity into the time domain for investigations, for example, of short-lived transient species in chemical reactions (Chergui, 2015;Zhang & Gaffney, 2015;Chergui & Collet, 2017;Kraus et al, 2018) and energy-relaxation pathways in biological systems (Kinschel et al, 2020;Sension, 2020;Bacellar & Chergui, 2022). The advent of high harmonic generation (HHG) sources and free-electron lasers (FELs), which deliver energy-tunable ultrashort pulses, has been exploited to investigate ultrafast dynamics by means of a pump-probe approach (Arrell et al, 2017;Bergmann et al, 2021).…”

Section: Introductionmentioning

confidence: 99%

A sub-100 nm thickness flat jet for extreme ultraviolet to soft X-ray absorption spectroscopy

De Angelis,

Longetti,

Bonano

et al. 2024

J Synchrotron Radiat

View full text Add to dashboard Cite

Experimental characterization of the structural, electronic and dynamic properties of dilute systems in aqueous solvents, such as nanoparticles, molecules and proteins, are nowadays an open challenge. X-ray absorption spectroscopy (XAS) is probably one of the most established approaches to this aim as it is element-specific. However, typical dilute systems of interest are often composed of light elements that require extreme-ultraviolet to soft X-ray photons. In this spectral regime, water and other solvents are rather opaque, thus demanding radical reduction of the solvent volume and removal of the liquid to minimize background absorption. Here, we present an experimental endstation designed to operate a liquid flat jet of sub-micrometre thickness in a vacuum environment compatible with extreme ultraviolet/soft XAS measurements in transmission geometry. The apparatus developed can be easily connected to synchrotron and free-electron-laser user-facility beamlines dedicated to XAS experiments. The conditions for stable generation and control of the liquid flat jet are analyzed and discussed. Preliminary soft XAS measurements on some test solutions are shown.

show abstract

Section: Introductionmentioning

confidence: 99%

A sub-100 nm thickness flat jet for extreme ultraviolet to soft X-ray absorption spectroscopy

De Angelis,

Longetti,

Bonano

et al. 2024

J Synchrotron Radiat

View full text Add to dashboard Cite

show abstract

“…X-ray spectroscopy is a powerful tool for studies of non-equilibrium processes, with a time resolution down to femtoseconds, through the combination of laser pumps and ultrafast X-ray sources. 1,2 The X-ray probe is element specific and does not interfere with the optical pump due to the large difference in wavelength.…”

Section: Introductionmentioning

confidence: 99%

Sensitivity of Kβ mainline X-ray emission to structural dynamics in iron photosensitizer

Rogvall

Singh

Vacher

et al. 2023

Phys. Chem. Chem. Phys.

View full text Add to dashboard Cite

show abstract

“…Unfortunately, UV–visible transient absorption spectra can be ambiguous to interpret and do not typically provide a direct link to molecular structure. As a consequence, while time scales can be exquisitely well defined using UV–visible transient absorption spectroscopy, the connection to electronic and structural dynamics is often less clear. − Ultrafast X-ray spectroscopies offer an element-specific probe of these dynamics, helping to refine assignments and thus providing new understanding of the structural transformations that occur following photoexcitation. − In this paper, we use ultrafast X-ray absorption at the Co K-edge and ultrafast X-ray emission in the Kβ 1,3 and valence-to-core regions to probe the excited state dynamics of two cobalamin compounds and use the results to obtain insights into the excited state dynamics.…”

Section: Introductionmentioning

confidence: 99%

Watching Excited State Dynamics with Optical and X-ray Probes: The Excited State Dynamics of Aquocobalamin and Hydroxocobalamin

Sension,

McClain,

Lamb

et al. 2023

J. Am. Chem. Soc.

Self Cite

View full text Add to dashboard Cite

Femtosecond time-resolved X-ray absorption (XANES) at the Co K-edge, X-ray emission (XES) in the Co Kβ and valence-to-core regions, and broadband UV–vis transient absorption are combined to probe the femtosecond to picosecond sequential atomic and electronic dynamics following photoexcitation of two vitamin B12 compounds, hydroxocobalamin and aquocobalamin. Polarized XANES difference spectra allow identification of sequential structural evolution involving first the equatorial and then the axial ligands, with the latter showing rapid coherent bond elongation to the outer turning point of the excited state potential followed by recoil to a relaxed excited state structure. Time-resolved XES, especially in the valence-to-core region, along with polarized optical transient absorption suggests that the recoil results in the formation of a metal-centered excited state with a lifetime of 2–5 ps. This combination of methods provides a uniquely powerful tool to probe the electronic and structural dynamics of photoactive transition-metal complexes and will be applicable to a wide variety of systems.

show abstract

Visualizing ultrafast chemical dynamics with X-rays

Cited by 4 publications

References 16 publications

A sub-100 nm thickness flat jet for extreme ultraviolet to soft X-ray absorption spectroscopy

A sub-100 nm thickness flat jet for extreme ultraviolet to soft X-ray absorption spectroscopy

Sensitivity of Kβ mainline X-ray emission to structural dynamics in iron photosensitizer

Watching Excited State Dynamics with Optical and X-ray Probes: The Excited State Dynamics of Aquocobalamin and Hydroxocobalamin

Contact Info

Product

Resources

About