Structure retrieval in liquid-phase electron scattering

Yang, Jie; Nunes, João; Ledbetter, Kathryn; Biasin, Elisa; Centurion, Martin; Chen, Zhijiang; Cordones, Amy A.; Crissman, Christopher; DePonte, Daniel P.; Glenzer, S. H.; Lin, Ming-Fu; Mo, Mianzhen; Rankine, Conor D.; Shen, Xiaozhe; Wolf, Thomas; Wang, Xijie

doi:10.1039/d0cp06045c

Cited by 15 publications

(13 citation statements)

References 39 publications

(50 reference statements)

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“…The 1 st O-O peak position between the simulated H 2 O and UED D 2 O data is nearly the same and the hydrogen bond (~1.8 A) for D 2 O is relatively larger than that of simulated H 2 O; these two features are consistent with earlier reports [16]. As expected the peak positions were fairly insensitive to thickness for the thinner regions [15,17,18]. For sheet thickness above one MFP, the effect of multiple scattering is apparent.…”

supporting

confidence: 89%

“…12 shows the charge pair distribution function as described by Yang. 15 In the 1st Born approximation, the angle averaged electron scattering intensity I ( Q ) for a liquid is given bywhere Z u is the charge of particle labelled u and P uv ( r⃑ ) is the probability distribution of pairs uv at separation r⃑ . The CPDF is defined to include all possible pairings of charged particles, nuclear and electron.The CPDF can then be calculated from the measured scattered intensity by sine transform.…”

Section: Resultsmentioning

confidence: 99%

“…Figure 12 shows the charge pair distribution function as described by Yang. [15] In the 1 st Born approximation, the angle averaged electron scattering intensity I(Q) for a liquid is given by There is a shift in peak amplitude for the second O-O peak at 4.5A that may be due to a temperature decrease. [19] We expect positions measured further from the nozzle will be increasingly lower temperature due to evaporative cooling.…”

Section: Figmentioning

confidence: 99%

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Sub-micron thick liquid sheets produced by isotropically etched glass nozzles

Crissman

Chen

et al. 2022

Lab Chip

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supporting

confidence: 89%

Section: Resultsmentioning

confidence: 99%

Section: Figmentioning

confidence: 99%

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Sub-micron thick liquid sheets produced by isotropically etched glass nozzles

Crissman

Chen

et al. 2022

Lab Chip

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“…In a recent paper, we have proposed a charge-pair-distribution-function (CPDF) that can be obtained directly from the raw patterns with neither atomic form factors nor background removal 36 .…”

Section: G2 and Temperature Extractionmentioning

confidence: 99%

Direct observation of ultrafast hydrogen bond strengthening in liquid water

Yang

Dettori

Nunes

et al. 2021

Nature

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Water is one of the most important, yet least understood, liquids in nature. Many anomalous properties of liquid water originate from its well-connected hydrogen bond network 1 , including unusually efficient vibrational energy redistribution and relaxation 2 . An accurate description of the ultrafast vibrational motion of water molecules is essential for understanding the nature of hydrogen bonds and many solution-phase chemical reactions. Most existing knowledge of vibrational relaxation in water is built upon ultrafast spectroscopy experiments 2-7 . However, these experiments cannot directly resolve the motion of the atomic positions and require difficult translation of spectral dynamics into hydrogen bond dynamics. Here we measured the ultrafast structural response to the excitation of the OH stretching vibration in liquid water with femtosecond temporal and atomic spatial resolution using liquid ultrafast electron scattering. We observed a transient hydrogen bond contraction of roughly 0.04 Å on a timescale of 80 femtoseconds, followed by a thermalization on a timescale of ~1 picosecond. Molecular dynamics simulations reveal the need to treat the distribution of the shared proton in the hydrogen bond quantum mechanically to capture the structural dynamics on the femtosecond timescales. Our experiment and simulations unveiled the intermolecular character of the water vibration preceding the relaxation of the OH stretch.The vibrational spectroscopy of water has critically contributed to our understanding of the dynamics of hydrogen bond (HB) reorganization and energy redistribution in liquid water. It is

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“…The implementation of radio-frequency mega-electron volt (MeV) ultrafast electron diffraction in combination with sub-micron thick liquid sheet jets have proven to be successful in determining the structure of water and other solvents 25,26 , and the dissociation process of aqueous I 3 -. 27 However, the elastic scattering cross-section ( el ) of 1 -100-MeV electrons in water is comparable to that of 300-keV electrons owing the plateau behaviour experienced by  el at high kinetic energies 28 .…”

Section: Introductionmentioning

confidence: 99%

A plastic feedthrough suitable for high-voltage DC femtosecond electron diffractometers

Gicala

Petruk

Rivas

et al. 2021

Review of Scientific Instruments

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Highly energetic ultrashort electron bunches have the potential to reveal the ultrafast structural dynamics in relatively thicker in-liquid samples. However, direct current (DC) voltages higher than 100 kV are exponentially difficult to attain as surface and vacuum breakdown become an important problem as the electric field increases. One of the most demanding components in the design of a high-energy electrostatic ultrafast electron source is the high voltage feedthrough (HVFT), which must keep the electron gun from discharging against ground. Electrical discharges can cause irreversible component damage while voltage instabilities render the instrument inoperative. We report the design, manufacturing, and conditioning process for a new HVFT that utilizes ultra-high molecular weight polyethylene (UHMWPE) as the insulating material. Our HVFT is highly customizable, inexpensive, and has proven to be effective in high voltage applications. After a couple of weeks of gas and voltage conditioning, we achieved a maximum voltage of 180 kV with a progressively improved vacuum level of 1.8 × 10 -8 Torr.

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Structure retrieval in liquid-phase electron scattering

Abstract: A novel analysis method for the direct retrieval of the real-space distribution of charged particle pairs from liquid-phase electron scattering.

Cited by 15 publications

References 39 publications

Sub-micron thick liquid sheets produced by isotropically etched glass nozzles

Sub-micron thick liquid sheets produced by isotropically etched glass nozzles

Direct observation of ultrafast hydrogen bond strengthening in liquid water

A plastic feedthrough suitable for high-voltage DC femtosecond electron diffractometers

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