Out-of-Plane Longitudinal Sound Speed Determination in GaS by Broadband Time-Domain Brillouin Scattering.

Two-dimensional semiconducting gallium sulfide (GaS) has garnered notable interest for its distinct structural and optical properties, which position it as a promising candidate material for various applications ranging from photodetection and photovoltaics to nonlinear frequency conversion. In this work, we determined the out-of-plane longitudinal sound velocity, , via impulsive time-domain femtosecond broadband Brillouin scattering measurements performed on a single flake-like GaS crystal. We obtained a value (3140 ± 20) m/s, which yields an out-of-plane compressive elastic constant, = (38.

Determining the Out-of-Plane Longitudinal Sound Speed in GeS by Broadband Time-Domain Brillouin Scattering.

Over the past decade, two-dimensional (2D) layered semiconducting materials, with their distinctive structures and unique physicochemical properties, have attracted attention for potential applications in photonics and optoelectronics. In this study, we utilized time-domain broadband Brillouin scattering on a single germanium monosulfide (GeS) crystal to determine the out-of-plane longitudinal sound speed, evaluated at = (4035 ± 200) m/s. The reported results demonstrate the effectiveness of this nondestructive, all-optical technique for measuring the elastic properties in fragile 2D layered materials and provide the value of the out-of-plane compressive elastic constant, = (69 ± 7) GPa.

Solvent effects on the intramolecular charge transfer excited state of 3CzClIPN: a broadband transient absorption study.

The prediction of solvent properties using molecular probes often relies on correlating steady-state absorption and fluorescence measurements, as well as determining absorption maxima and/or Stokes shifts. In this study, we employ femtosecond broadband transient absorption (fs-bb-TA) spectroscopy to investigate the spectroscopic behaviour of the intramolecular charge transfer (ICT) excited state of 3CzClIPN (2,4,6-tri(9-carbazol-9-yl)-5-chloroisophthalonitrile), a representative ICT organic molecule, in both aromatic and non-aromatic solvents. Unlike observations in non-aromatic media, fs-bb-TA spectra of 3CzClIPN in aromatic solvents exhibit enhanced spectral broadening that strongly correlates with the solvent's polarity.

Robust fully controlled nanometer liquid layers for high resolution liquid-cell electron microscopy.

Liquid cell electron microscopy (LCEM) has long suffered from irreproducibility and its inability to confer high-quality images over a wide field of view. LCEM demands the encapsulation of the sample between two ultrathin membranes (windows). In the vacuum environment of the electron microscope, the windows bulge, drastically reducing the achievable resolution and the usable viewing region.

N-oleoylethanolamide treatment of lymphoblasts deficient in Tafazzin improves cell growth and mitochondrial morphology and dynamics.

Barth syndrome (BTHS) is caused by mutations in the TAZ gene encoding the cardiolipin remodeling enzyme, Tafazzin. The study objective was to quantitatively examine growth characteristics and mitochondrial morphology of transformed lymphoblast cell lines derived from five patients with BTHS relative to five healthy controls, as well as the therapeutic potential of oleoylethanolamide (OEA) and linoleoylethanolamide (LEA). These bioactive lipids both activate PPARα, which may be therapeutic.

High-Performance Mid-IR to Deep-UV van der Waals Photodetectors Capable of Local Spectroscopy at Room Temperature.

The ability to perform broadband optical spectroscopy with subdiffraction-limit resolution is highly sought-after for a wide range of critical applications. However, sophisticated near-field techniques are currently required to achieve this goal. We bypass this challenge by demonstrating an extremely broadband photodetector based on a two-dimensional (2D) van der Waals heterostructure that is sensitive to light across over a decade in energy from the mid-infrared (MIR) to deep-ultraviolet (DUV) at room temperature.

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

Highly energetic ultrashort electron bunches have the potential to reveal the ultrafast structural dynamics in relatively thicker in-liquid samples. However, direct current 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.

Static and dynamic scavenging of ammoniated electrons by nitromethane.

We studied the time-resolved scavenging efficiency of nitromethane for transient electron species in liquid ammonia, at a temperature of 298 K. UV excitation of iodide ions produced fully solvated electrons, as well as transient (I, e-) and (counterion, e-) pairs, the overall concentration of which was monitored by NIR absorption with subpicosecond time resolution. After the UV pulse, the solution absorbance decays almost completely in a few hundreds of picoseconds due to geminate electron-iodine atom recombination and a competitive annihilation channel involving the scavenger.

Trapping a Photoelectron behind a Repulsive Coulomb Barrier in Solution.

Multiply charged anions (MCAs) display unique photophysics and solvent-stabilizing effects. Well-known aqueous species such as SO and PO experience spontaneous electron detachment or charge-separation fragmentation in the gas phase owing to the strong Coulomb repulsion arising from the excess of negative charge. Thus, anions often present low photodetachment thresholds and the ability to quickly eject electrons into the solvent via charge-transfer-to-solvent (CTTS) states.

High flow rate nanofluidics for in-liquid electron microscopy and diffraction.

We introduce a nanofluidic platform that can be used to carry out femtosecond electron diffraction (FED) and transmission electron microscopy (TEM) measurements in liquid samples or in-liquid specimens, respectively. The nanofluidic cell (NFC) system presented herein has been designed to withstand high sample refreshing rates (over one kilohertz), a prerequisite to succeed with FED experiments in our lab. Short beam paths, below 1 μm, in combination with ultrathin membranes (less than 100 nm thick) are necessary conditions for in-liquid FED and TEM studies due to the strongly interacting nature of electrons.

An aligned octahedral core in a nanocage: synthesis, plasmonic, and catalytic properties.

Plasmonic metal nanostructures with complex morphologies provide an important route to tunable optical responses and local electric field enhancement at the nanoscale for a variety of applications including sensing, imaging, and catalysis. Here we report a high-concentration synthesis of gold core-cage nanoparticles with a tethered and structurally aligned octahedral core and examine their plasmonic and catalytic properties. The obtained nanostructures exhibit a double band extinction in the visible-near infrared range and a large area electric field enhancement due to the unique structural features, as demonstrated using finite difference time domain (FDTD) simulations and confirmed experimentally using surface enhanced Raman scattering (SERS) tests.

Shaped cathodes for the production of ultra-short multi-electron pulses.

An electrostatic electron source design capable of producing sub-20 femtoseconds (rms) multi-electron pulses is presented. The photoelectron gun concept builds upon geometrical electric field enhancement at the cathode surface. Particle tracer simulations indicate the generation of extremely short bunches even beyond 40 cm of propagation.

Cold ablation driven by localized forces in alkali halides.

Laser ablation has been widely used for a variety of applications. Since the mechanisms for ablation are strongly dependent on the photoexcitation level, so called cold material processing has relied on the use of high-peak-power laser fluences for which nonthermal processes become dominant; often reaching the universal threshold for plasma formation of ~1 J cm(-2) in most solids. Here we show single-shot time-resolved femtosecond electron diffraction, femtosecond optical reflectivity and ion detection experiments to study the evolution of the ablation process that follows femtosecond 400 nm laser excitation in crystalline sodium chloride, caesium iodide and potassium iodide.

Mapping molecular motions leading to charge delocalization with ultrabright electrons.

Ultrafast processes can now be studied with the combined atomic spatial resolution of diffraction methods and the temporal resolution of femtosecond optical spectroscopy by using femtosecond pulses of electrons or hard X-rays as structural probes. However, it is challenging to apply these methods to organic materials, which have weak scattering centres, thermal lability, and poor heat conduction. These characteristics mean that the source needs to be extremely bright to enable us to obtain high-quality diffraction data before cumulative heating effects from the laser excitation either degrade the sample or mask the structural dynamics.

Full characterization of RF compressed femtosecond electron pulses using ponderomotive scattering.

High bunch charge, femtosecond, electron pulses were generated using a 95 kV electron gun with an S-band RF rebunching cavity. Laser ponderomotive scattering in a counter-propagating beam geometry is shown to provide high sensitivity with the prerequisite spatial and temporal resolution to fully characterize, in situ, both the temporal profile of the electron pulses and RF time timing jitter. With the current beam parameters, we determined a temporal Instrument Response Function (IRF) of 430 fs FWHM.

Snapshots of cooperative atomic motions in the optical suppression of charge density waves.

Macroscopic quantum phenomena such as high-temperature superconductivity, colossal magnetoresistance, ferrimagnetism and ferromagnetism arise from a delicate balance of different interactions among electrons, phonons and spins on the nanoscale. The study of the interplay among these various degrees of freedom in strongly coupled electron-lattice systems is thus crucial to their understanding and for optimizing their properties. Charge-density-wave (CDW) materials, with their inherent modulation of the electron density and associated periodic lattice distortion, represent ideal model systems for the study of such highly cooperative phenomena.

'Making the molecular movie': first frames.

Recent advances in high-intensity electron and X-ray pulsed sources now make it possible to directly observe atomic motions as they occur in barrier-crossing processes. These rare events require the structural dynamics to be triggered by femtosecond excitation pulses that prepare the system above the barrier or access new potential energy surfaces that drive the structural changes. In general, the sampling process modifies the system such that the structural probes should ideally have sufficient intensity to fully resolve structures near the single-shot limit for a given time point.

Electronic acceleration of atomic motions and disordering in bismuth.

The development of X-ray and electron diffraction methods with ultrahigh time resolution has made it possible to map directly, at the atomic level, structural changes in solids induced by laser excitation. This has resulted in unprecedented insights into the lattice dynamics of solids undergoing phase transitions. In aluminium, for example, femtosecond optical excitation hardly affects the potential energy surface of the lattice; instead, melting of the material is governed by the transfer of thermal energy between the excited electrons and the initially cold lattice.

The formation of warm dense matter: experimental evidence for electronic bond hardening in gold.

Under strong optical excitation conditions, it is possible to create highly nonequilibrium states of matter. The nuclear response is determined by the rate of energy transfer from the excited electrons to the nuclei and the instantaneous effect of change in electron distribution on the interatomic potential energy landscape. We used femtosecond electron diffraction to follow the structural evolution of strongly excited gold under these transient electronic conditions.

Is ammonia a better solvent than water for contact ion pairs?

The existence of a charge-transfer-to-solvent process when a KI contact ion pair (CIP) dissolved in supercritical water (SCW) is excited by UV light was confirmed by use of electronic structure calculations applied to molecular dynamics trajectories. We observed similar behavior with fluid density as that found for the KI-CIP in supercritical ammonia (SCA); nevertheless, there are some distinct features in the two supercritical solvents. First, the effect of the solvent field due to the molecules lying beyond the first solvation shell is very different in SCW compared with that observed in SCA; in SCW it actually has a destabilizing effect over the ground and excited states.

Grating enhanced ponderomotive scattering for visualization and full characterization of femtosecond electron pulses.

Real time views of atomic motion can be achieved using electron pulses as structural probes. The requisite time resolution requires knowledge of both the electron pulse duration and the exact timing of the excitation pulse and the electron probe to within 10 - 100 fs accuracy. By using an intensity grating to enhance the pondermotive force, we are now able to fully characterize electron pulses and to confirm many body simulations with laser pulse energies on the microjoule level.

Electronically driven structure changes of Si captured by femtosecond electron diffraction.

The excitation of a high density of carriers in semiconductors can induce an order-to-disorder phase transition due to changes in the potential-energy landscape of the lattice. We report the first direct resolution of the structural details of this phenomenon in freestanding films of polycrystalline and (001)-oriented crystalline Si, using 200-fs electron pulses. At excitation levels greater than approximately 6% of the valence electron density, the crystalline structure of the lattice is lost in <500 fs, a time scale indicative of an electronically driven phase transition.

Development of the charge-transfer-to-solvent process with increasing solvent fluid density: the effect of ion pairing.

The study of the UV spectroscopic behaviour of alkali metal iodides dissolved in supercritical ammonia showed that two absorbing species contributed to the UV absorption of the solutions. The two species differed in the type of interaction of iodide with the cation, i.e.

Influence of ion pairing on the UV-spectral behavior of KI dissolved in supercritical NH3: from vapor phase to condensed liquid.

The UV-spectroscopic behavior of KI dissolved in supercritical ammonia enabled us to identify two species that contribute to the optical absorption depending on the fluid density rho1 and the temperature T. At low rho1 and high T, contact ion pairs (CIPs) prevail, while at high density of ammonia, solvent separated ion pairs (SSIPs) and free iodide ions dominate the optical absorption of the solute. The features of the electron excitation process depend on the state of the K+ I- species present.

Solvent triggered change of the electron excitation route of KI in supercritical NH3.

The UV-spectroscopic behavior of KI contact ion pairs (CIPs) dissolved in supercritical NH3 was studied combining classical molecular dynamics simulations with electronic structure calculations, and the results show that an abrupt change of the photoexcitation route of KI CIPs occurs at very low solvent densities. Few NH3 solvating molecules are required to hamper the well-known photoinduced intramolecular electron (e-) transfer observed in isolated ion pairs of alkali metal halides in the vapor drawing the e- to solvent cavities leading to a charge-transfer-to-solvent process.