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We report the plasma pressure reached inside the central plasma column of a sheared-flow-stabilized Z-pinch using Thomson scattering measurements. Building on previously reported experimental results and the analysis methods established for the high temperature and moderate density plasmas generated on the FuZE device, we show evidence of a central plasma region with higher electron temperature and density, which is consistent with a pinch behavior. Elevated electron temperatures up to 2.25 ± 0.8 keV and densities up to (4.9 ± 0.2) × 10 17 cm − 3 are observed to temporally coincide with the fusion neutron production from the plasma. Reconstructed plasma pressure profiles highlight the presence of a several millimeter-wide column with elevated pressure whose location varies shot-to-shot. The plasma pressure rises as neutron production from the deuterium plasma increases, reaching a peak value of 2.6 kBar. This peak value is consistent with a radially force-balanced pinch equilibrium model based on the measured ∼320 kA pinch current. Complete datasets were obtained at two axial locations, 10 and 20 cm axial position from the tip of the central electrode, which corroborate the estimated neutron source axial lengths. [ABSTRACT FROM AUTHOR]

The sheared-flow-stabilized Z pinch concept has been studied extensively and is able to produce fusion-relevant plasma parameters along with neutron production over several microseconds. We present here elevated electron temperature results spatially and temporally coincident with the plasma neutron source. An optical Thomson scattering apparatus designed for the FuZE device measures temperatures in the range of 1-3 keV on the axis of the device, 20 cm downstream of the nose cone. The 17-fiber system measures the radial profiles of the electron temperature. Scanning the laser time with respect to the neutron pulse time over a series of discharges allows the reconstruction of the T_{e} temporal response, confirming that the electron temperature peaks simultaneously with the neutron output, as well as the pinch current and inductive voltage generated within the plasma. Comparison to spectroscopic ion temperature measurements suggests a plasma in thermal equilibrium. The elevated T_{e} confirms the presence of a plasma assembled on axis, and indicates limited radiative losses, demonstrating a basis for scaling this device toward net gain fusion conditions.

Quantifying charge delocalization associated with short-lived photoexcited states of molecular complexes in solution remains experimentally challenging, requiring local element specific femtosecond experimental probes of time-evolving electron transfer. In this study, we quantify the evolving valence hole charge distribution in the photoexcited charge transfer state of a prototypical mixed valence bimetallic iron-ruthenium complex, [(CN) 5 Fe II CNRu III (NH 3 ) 5 ] - , in water by combining femtosecond X-ray spectroscopy measurements with time-dependent density functional theory calculations of the excited-state dynamics. We estimate the valence hole charge that accumulated at the Fe atom to be 0.6 ± 0.2, resulting from excited-state metal-to-metal charge transfer, on an ∼60 fs time scale. Our combined experimental and computational approach provides a spectroscopic ruler for quantifying excited-state valency in solvated complexes.

Excited-state intramolecular proton transfer (ESIPT) is a fundamental chemical process with several applications. Ultrafast ESIPT involves coupled electronic and atomic motions and has been primarily studied using femtosecond optical spectroscopy. X-ray spectroscopy is particularly useful because it is element-specific and enables direct, individual probes of the proton-donating and -accepting atoms. Herein, we report a computational study to resolve the ESIPT in 10-hydroxybenzo[ h ]quinoline (HBQ), an intramolecularly hydrogen bonded compound. We use linear-response time-dependent density functional theory (LR-TDDFT) combined with ab initio molecular dynamics (AIMD) and time-resolved X-ray absorption spectroscopy (XAS) computations to track the ultrafast excited-state dynamics. Our results reveal clear X-ray spectral signatures of coupled electronic and atomic motions during and following ESIPT at the oxygen and nitrogen K-edge, paving the way for future experiments at X-ray free electron lasers.

It is well known that the solvent plays a critical role in ultrafast electron-transfer reactions. However, solvent reorganization occurs on multiple length scales, and selectively measuring short-range solute-solvent interactions at the atomic level with femtosecond time resolution remains a challenge. Here we report femtosecond X-ray scattering and emission measurements following photoinduced charge-transfer excitation in a mixed-valence bimetallic (Fe ii Ru iii ) complex in water, and their interpretation using non-equilibrium molecular dynamics simulations. Combined experimental and computational analysis reveals that the charge-transfer excited state has a lifetime of 62 fs and that coherent translational motions of the first solvation shell are coupled to the back electron transfer. Our molecular dynamics simulations identify that the observed coherent translational motions arise from hydrogen bonding changes between the solute and nearby water molecules upon photoexcitation, and have an amplitude of tenths of ångströms, 120-200 cm -1 frequency and ~100 fs relaxation time. This study provides an atomistic view of coherent solvent reorganization mediating ultrafast intramolecular electron transfer.

We demonstrate the existence of a strictly non-adiabatic control pathway in deprotonation of the acetylene dication. This pathway is identified experimentally by measuring a kinetic energy shift in an ion coincidence experiment. We use a time dependent Schrödinger equation simulation to identify which properties most strongly affect our control. We find that resonant control around conical intersections is limited by the speed of non-adiabatic dynamics.

We have studied strong-field enhanced dissociative ionization of D 2 O in 40 fs, 800 nm laser pulses with focused intensities of <1-3 × 10 15 W/cm 2 by resolving the charged fragment momenta with respect to the laser polarization. We that observe dication dissociation into OD + /D + dominates when the polarization is out of the plane of the molecule, whereas trication dissociation into O + /D + /D + is strongly dominant when the polarization is aligned along the D-D axis. Dication dissociation into O/D + /D + and O + /D 2 is not seen nor is there any significant fragmentation into multiple ions when the laser is polarized along the C + is not seen nor is there any significant fragmentation into multiple ions when the laser is polarized along the C 2v symmetry axis of the molecule. Even below the saturation intensity for OD + /D + , the O + /D + channel has higher yield. By analyzing how the laser field is oriented within the molecular frame for both channels, we show that enhanced ionization is driving the triply charged three body breakup but is not active for the doubly charged two body breakup. We conclude that laser-induced distortion of the molecular potential suppresses multiple ionization along the C + channel has higher yield. By analyzing how the laser field is oriented within the molecular frame for both channels, we show that enhanced ionization is driving the triply charged three body breakup but is not active for the doubly charged two body breakup. We conclude that laser-induced distortion of the molecular potential suppresses multiple ionization along the C 2v axis but enhances ionization along the D-D direction.

Ultrafast proton migration and isomerization are key processes for acetylene and its ions. However, the mechanism for ultrafast isomerization of acetylene [HCCH] 2+ to vinylidene [H 2 CC] 2+ dication remains nebulous. Theoretical studies show a large potential barrier ( > 2 eV) for isomerization on low-lying dicationic states, implying picosecond or longer isomerization timescales. However, a recent experiment at a femtosecond X-ray free-electron laser suggests sub-100 fs isomerization. Here we address this contradiction with a complete theoretical study of the dynamics of acetylene dication produced by Auger decay after X-ray photoionization of the carbon atom K shell. We find no sub-100 fs isomerization, while reproducing the salient features of the time-resolved Coulomb imaging experiment. This work resolves the seeming contradiction between experiment and theory and also calls for careful interpretation of structural information from the widely applied Coulomb momentum imaging method.The timescale of isomerization in molecules involving ultrafast migration of constituent atoms is difficult to measure. Here the authors report that sub-100 fs isomerization time on acetylene dication in lower electronic states is not possible and point to misinterpretation of recent experimental results.

Conical intersections (CIs) between molecular potential energy surfaces with non-vanishing non-adiabatic couplings generally occur in any molecule consisting of at least three atoms. They play a fundamental role in describing the molecular dynamics beyond the Born-Oppenheimer approximation and have been used to understand a large variety of effects, from photofragmentation and isomerization to more exotic applications such as exciton fission in semiconductors. However, few studies have used the features of a CI as a tool for coherent control. Here we demonstrate two modes of control around a conical intersection. The first uses a continuous light field to control the population on the two intersecting electronic states in the vicinity of a CI. The second uses a pulsed light field to control wavepackets that are subjected to the geometric phase shift in transit around a CI. This second technique is likely to be useful for studying the role of nuclear dynamics in electronic coherence phenomena.