Probing the hydrogen-bond network of water via time-resolved soft x-ray spectroscopy

We report time-resolved studies of hydrogen bonding in liquid H2O, in response to direct excitation of the O-H stretch mode at 3 mu m, probed via soft x-ray absorption spectroscopy at the oxygen K-edge. This approach employs a newly developed nanofluidic cell for transient soft x-ray spectroscopy in liquid phase. Distinct changes in the near-edge spectral region (XANES) are observed, and are indicative of a transient temperature rise of 10K following transient laser excitation and rapid thermalization of vibrational energy. The rapid heating occurs at constant volume and the associated increase in internal pressure, estimated to be 8MPa, is manifest by distinct spectral changes that differ from those induced by temperature alone. We conclude that the near-edge spectral shape of the oxygen K-edge is a sensitive probe of internal pressure, opening new possibilities for testing the validity of water models and providing new insight into the nature of hydrogen bonding in water

THz Pump and X-Ray Probe Development at LCLS

We report on measurements of broadband, intense, coherent transition radiation at terahertz frequencies, generated as the highly compressed electron bunches in Linear Coherent Light Source (LCLS) pass through a thin metal foil. The foil is inserted at 45{sup o} to the electron beam, 31 m downstream of the undulator. The THz emission passes downward through a diamond window to an optical table below the beamline. A fully compressed 350-pC bunch produces up to 0.5 mJ in a nearly half-cycle pulse of 50 fs FWHM with a spectrum peaking at 10 THz. We estimate a peak field at the focus of over 2.5 GV/m. A 20-fs Ti:sapphire laser oscillator has recently been installed for electro-optic measurements. We are developing plans to add an x-ray probe to this THz pump, by diffracting FEL x rays onto the table with a thin silicon crystal. The x rays would arrive with an adjustable time delay after the THz. This will provide a rapid start to user studies of materials excited by intense single-cycle pulses and will serve as a step toward a THz transport line for LCLS-II

Structure, Morphology and Optical Properties of Chiral N-(4-X-phenyl)-N-[1(S)-1-phenylethyl]thiourea, X= Cl, Br, and NO2

Three new enantiopure aryl-thioureas have been synthesized, N-(4-X-phenyl)-N-[1(S)-1-phenylethyl]thiourea, X= Cl, Br, and NO2 (compounds 1-3, respectively). Large single crystals of up to 0.5 cm3 were grown from methanol/ethanol solutions. Molecular structures were derived from X-ray diffraction studies and the crystal morphology was compared to calculations employing the Bravais-Friedel, Donnay-Harker model. Molecular packing was further studied with Hirshfeld surface calculations. Semi-empirical classical model calculations of refractive indices, optical rotation and the electro-optic effect were performed with OPTACT on the basis of experimentally determined refractive indices. Compound 3 (space group P 1 (No. 1)) was estimated to possess a large electro-optic coefficient r333 of approximately 30 pm/V, whereas 1 and 2 (space Group P 21 (No. 4) exhibit much smaller effects

Single-cycle terahertz pulses with \u3e0.2 V/Å field amplitudes via coherent transition radiation

We demonstrate terahertz pulses with field amplitudes exceeding 0.2 V/Å generated by coherent transition radiation. Femtosecond, relativistic electron bunches generated at the Linac Coherent Light Source are passed through a beryllium foil, and the emitted radiation is characterized as a function of the bunch duration and charge. Broadband pulses centered at a frequency of 10 THz with energies of 140 µJ are measured. These far-below- band gap pulses drive a nonlinear optical response in a silicon photodiode, with which we perform nonlinear autocorrelations that yield information regarding the terahertz temporal profile

Single-cycle Terahertz Pulses with >0.2 V/A Field Amplitudes via Coherent Transition Radiation

We demonstrate terahertz pulses with field amplitudes exceeding 0.2 V/{angstrom} generated by coherent transition radiation. Femtosecond, relativistic electron bunches generated at the Linac Coherent Light Source are passed through a beryllium foil, and the emitted radiation is characterized as a function of the bunch duration and charge. Broadband pulses centered at a frequency of 10 THz with energies of 140 {mu}J are measured. These far-below-bandgap pulses drive a nonlinear optical response in a silicon photodiode, with which we perform nonlinear autocorrelations that yield information regarding the terahertz temporal profile. Simulations of the spatiotemporal profile agree well with experimental results