Photoionization of the aqueous phase: clusters, droplets and liquid jets

Signorell, Ruth; Winter, Bernd

doi:10.1039/d2cp00164k

Cited by 28 publications

(44 citation statements)

References 132 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“… 9 , 14 − 23 Unfortunately, a major challenge that has been hampering the development of UV LJ-PES for aqueous solutions is a lack of consensus on the precise effect of inelastic scattering of low kinetic energy electrons in liquid water on peak shapes and positions. 24 − 30 …”

mentioning

confidence: 99%

“…Liquid-jet PES (LJ-PES) is now an active research field involving a growing number of research groups around the world. − Nonetheless, the requirement for relatively high concentrations of solute to obtain adequate signal-to-noise ratio after subtracting the photoelectron spectrum of water has excluded most X-ray LJ-PES studies of aqueous solutions of organic molecules because organic molecules tend to be only weakly soluble . A solution to this problem is to use resonance-enhanced PES with ultraviolet (UV) light pulses. ,− Unfortunately, a major challenge that has been hampering the development of UV LJ-PES for aqueous solutions is a lack of consensus on the precise effect of inelastic scattering of low kinetic energy electrons in liquid water on peak shapes and positions. − …”

mentioning

confidence: 99%

See 1 more Smart Citation

Accurate Vertical Ionization Energy of Water and Retrieval of True Ultraviolet Photoelectron Spectra of Aqueous Solutions

Scholz

Fortune

Tau

et al. 2022

J. Phys. Chem. Lett.

View full text Add to dashboard Cite

Ultraviolet (UV) photoelectron spectroscopy provides a direct way of measuring valence electronic structure; however, its application to aqueous solutions has been hampered by a lack of quantitative understanding of how inelastic scattering of low-energy (<5 eV) electrons in liquid water distorts the measured electron kinetic energy distributions. Here, we present an efficient and widely applicable method for retrieving true UV photoelectron spectra of aqueous solutions. Our method combines Monte Carlo simulations of electron scattering and spectral inversion, with molecular dynamics simulations of depth profiles of organic solutes in aqueous solution. Its application is demonstrated for both liquid water, and aqueous solutions of phenol and phenolate, which are ubiquitous biologically relevant structural motifs.

show abstract

mentioning

confidence: 99%

mentioning

confidence: 99%

Accurate Vertical Ionization Energy of Water and Retrieval of True Ultraviolet Photoelectron Spectra of Aqueous Solutions

Scholz

Fortune

Tau

et al. 2022

J. Phys. Chem. Lett.

View full text Add to dashboard Cite

show abstract

“…Among these are typically large biomolecules, clusters and nanoparticles, 237,238 areosols, and systems at the boundary of condensed phases. Recent activity is on the study of liquids, in particular water and solutions, like droplets or liquid jets, 239,240 or surfactant layer structure at liquid–vapor interface. 241…”

Section: Laboratory Frame Padsmentioning

confidence: 99%

Trends in angle-resolved molecular photoelectron spectroscopy

Dowek

Decleva

2022

Phys. Chem. Chem. Phys.

View full text Add to dashboard Cite

show abstract

“…(a) Two typical cases in comparing the electron attenuation length (EAL) and inelastic mean free path (IMFP) for incident electrons from the liquid surface (upper) to the bulk (bottom), adapted from ref . (b) Variances of the EAL and IMFP values against the electron energy [Suzuki, et al (2014), Shinotsuka, et al (2017), Thümer, et al (2013), Garcia-Molina, et al (2017), Nguyen-Truong et al (2018), Signorell (2022)] …”

Section: Introductionmentioning

confidence: 99%

“…Knowlegdes of electron collisions in liquid can be learnt from recent progress in liquid-beam photoelectron spectroscopy. − As shown in Figure (a), the electron attenuation length (EAL, the distance at which the flux of electrons maintaining the initial kinetic energy diminishes by a factor of 1/e) could be smaller than or nearly equal to the inelastic mean free path (IMFP, the average distance between consecutive inelastic scattering events), which is determined with the elastic scattering events . The EAL and IMFP values in the aqueous liquid are plotted in Figure (b), where the EAL values are mimicked with the photoelectron trajectories. − In general, EAL approximately equals IMFP when the initial (incident) electron energy is more than 10 2 eV, and IMFP > EAL for the low-energy electrons.…”

Section: Introductionmentioning

confidence: 99%

Electron Impact with the Liquid–Vapor Interface

Chen¹,

Li²,

Hu³

et al. 2022

Acc. Chem. Res.

View full text Add to dashboard Cite

Metrics & MoreArticle Recommendations CONSPECTUS: Reaction dynamics in the liquid−vapor interface is one of the crucial physical sciences but is still starving for in-depth exploration. It is challenging to selectively detect the interfacial species or the yields of chemical reaction therein, meanwhile shielding or reducing the interference from the vapor and liquid bulk. Mass spectrometry is a straightforward method but is also frustrated in such a selective detection. Using a liquid microjet in combination with a pulsed electron beam, a linear time-of-flight mass spectrometer, and a quadrupole mass filter, we recently innovated time-delayed mass spectrometry for investigations of the liquid−vapor interface. In this Account, we illustrate how this unique method succeeds in disentangling different sources, i.e., the vapor and liquid−vapor interface, of the ionic yields of the electron impacts with a liquid beam of alcohol in vacuum. These achievements are basically attributed to the application of an onion-peeling strategy in the ion detection. Concretely, the microsecond time scale of molecular volatilization can be resolved well by tuning the delay time between the nanosecond pulses of incident electron bunch and ion attractor. First, the specific orientation of the interfacial molecule, i.e., a well-known fact about the hydrophobic hydrocarbon groups pointing outside the liquid surface of alcohol, is validated again. More importantly, the dynamic features of time-delayed mass spectra, in particular, for the ionic yields from the liquid−vapor interface, are rationalized explicitly. Moreover, we demonstrate evidence of in situ molecular dimers in the liquid−vapor interface of 1-propanol. As the first example of electron-induced reaction in the liquid−vapor interface, dimethyl ether can be synthesized in the liquid methanol interface due to local interfacial acidification by high-energy electron impacts. On the contrary, the low energy electron can lead to local basicity through dissociative electron attachment (DEA).Besides the primary low-energy electrons, the low-energy secondary and inelastically scattered electrons in the higher-energy impacts of the primary electrons can also participate in the DEA process. In contrast to the gas-or solid-phase DEAs, that in the liquid− vapor interface shows distinct differences in both the types and efficiencies of anionic products. With these and efforts in the future, we develop a molecular-level understanding of how the chemical reactions happen in the liquid−vapor interface.

show abstract

Photoionization of the aqueous phase: clusters, droplets and liquid jets

Abstract: This perspective article reviews specific challenges associated with photoemission spectroscopy of bulk liquid water, aqueous solutions, water droplets and water clusters. The main focus lies on retrieving accurate energetics and...

Cited by 28 publications

References 132 publications

Accurate Vertical Ionization Energy of Water and Retrieval of True Ultraviolet Photoelectron Spectra of Aqueous Solutions

Accurate Vertical Ionization Energy of Water and Retrieval of True Ultraviolet Photoelectron Spectra of Aqueous Solutions

Trends in angle-resolved molecular photoelectron spectroscopy

Electron Impact with the Liquid–Vapor Interface

Contact Info

Product

Resources

About