Extreme Ultraviolet Reflection Spectroscopy of Lanthanides and Actinides Using a High Harmonic Generation Light Source.

Absorption spectroscopy probing transitions from shallow-core d and f orbitals in lanthanides and actinides reveals information about bonding and the electronic structure in compounds containing these elements. However, spectroscopy in this photon energy range is challenging because of the limited availability of light sources and extremely short penetration depths. In this work, we address these challenges using a tabletop extreme ultraviolet (XUV), ultrafast, laser-driven, high harmonic generation light source, which generates femtosecond pulses in the 40-140 eV range.

Hard x-ray - optical four-wave mixing using a split-and-delay line.

New, hard x-ray free electron lasers (FEL) produce intense femtosecond-to-attosecond pulses at angstrom wavelengths, giving access to the fundamental spatial and temporal scales of matter. These revolutionary light sources open the door to applying the suite of nonlinear, optical spectroscopy methods at hard x-ray photon energies. Nonlinear spectroscopy with hard x-rays can allow for measuring the coherence properties of short wavelength excitations with atomic specificity and for understanding how high energy excitations couple to other degrees of freedom in atomic, molecular or condensed-phase systems.

Tracking Thermal Decomposition Chemistry in Secondary Solid Explosives with X-ray Diffraction.

We present an approach for measuring thermal decomposition kinetics in crystalline solids using X-ray diffraction to track the loss of crystallinity that accompanies condensed phase decomposition chemistry. We apply this method to systems for which extracting thermodynamic parameters has been historically difficult: organic molecular crystals that thermally decompose below their melting points, such as solid explosives. To demonstrate this method, we measured the rate of solid, thermal decomposition versus temperature in three different secondary solid explosives and the sugar fructose.

Measuring an ultrashort, ultraviolet pulse in a slowly responding, absorbing medium.

Frequency-resolved optical gating (FROG) is a common technique for measuring ultrashort laser pulses using an instantaneous, nonlinear-optical interaction as a fast time-gate to measure the pulse intensity and phase. But at high frequencies, materials are often absorbing and it is not always possible to find a medium with a fast nonlinear-optical response. Here we show that an ultrashort, ultraviolet (UV) pulse can be measured in a strongly absorbing medium, using the absorption as the nonlinear-optical time-gate.

Encoding the complete electric field of an ultraviolet ultrashort laser pulse in a near-infrared nonlinear-optical signal.

We introduce a variation on the cross-correlation frequency-resolved optical gating (XFROG) technique that uses a near-infrared (NIR) nonlinear-optical signal to characterize pulses in the ultraviolet (UV). Using a transient-grating XFROG beam geometry, we create a grating using two copies of the unknown UV pulse and diffract a NIR reference pulse from it. We show that, by varying the delay between the UV pulses creating the grating, the UV pulse intensity-and-phase information can be encoded into a NIR signal.

Induced ferroelectric phases in SrTiO by a nanocomposite approach.

Inducing new phases in thick films via vertical lattice strain is one of the critical advantages of vertically aligned nanocomposites (VANs). In SrTiO (STO), the ground state is ferroelastic, and the ferroelectricity in STO is suppressed by the orthorhombic transition. Here, we explore whether vertical lattice strain in three-dimensional VANs can be used to induce new ferroelectric phases in SrTiO:MgO (STO:MgO) VAN thin films.

Insight into the Chemistry of PETN Under Shock Compression Through Ultrafast Broadband Mid-Infrared Absorption Spectroscopy.

Thin films of pentaerythritol tetranitrate (PETN) were shock compressed using the laser driven shock apparatus at Los Alamos National Laboratory (LANL). Two spectroscopic probes were available to this apparatus: visible white light transient absorption spectroscopy (VIS) from 400 to 700 nm and mid-infrared transient absorption spectroscopy (MIR) from 1150 to 3800 cm. Important PETN vibrational modes are the symmetric and antisymmetric NO stretches at 1280 and 1650 cm, respectively, as well as CH stretches at ∼2900 cm.

Parallel replica dynamics simulations of reactions in shock compressed liquid benzene.

The study of the long-term evolution of slow chemical reactions is challenging because quantum-based reactive molecular dynamics simulation times are typically limited to hundreds of picoseconds. Here, the extended Lagrangian Born-Oppenheimer molecular dynamics formalism is used in conjunction with parallel replica dynamics to obtain an accurate tool to describe the long-term chemical dynamics of shock-compressed benzene. Langevin dynamics has been employed at different temperatures to calculate the first reaction times in liquid benzene at pressures and temperatures consistent with its unreacted Hugoniot.

Probing ultrafast shock-induced chemistry in liquids using broad-band mid-infrared absorption spectroscopy.

We probe shock-induced chemistry in two organic liquids by measuring broadband, midinfrared absorption in the 800-1400 cm frequency range. To test this new method and understand the signatures of chemical reactions in time resolved vibrational spectra, we compared liquid benzene shocked to unreactive conditions (shocked to a pressure of 18 GPa for a duration of 300 ps) to nitromethane under reactive conditions (25 GPa). We see clear signatures of shock-induced chemistry that are distinguishable from the pressure- and temperature-induced changes in vibrational mode shapes.

Tracking Ultrafast Photocurrents in the Weyl Semimetal TaAs Using THz Emission Spectroscopy.

We investigate polarization-dependent ultrafast photocurrents in the Weyl semimetal TaAs using terahertz (THz) emission spectroscopy. Our results reveal that highly directional, transient photocurrents are generated along the noncentrosymmetric c axis regardless of incident light polarization, while helicity-dependent photocurrents are excited within the ab plane. This is consistent with earlier static photocurrent experiments, and demonstrates on the basis of both the physical constraints imposed by symmetry and the temporal dynamics intrinsic to current generation and decay that optically induced photocurrents in TaAs are inherent to the underlying crystal symmetry of the transition metal monopnictide family of Weyl semimetals.

Kinetics of the γ-δ phase transition in energetic nitramine-octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine.

The solid, secondary explosive nitramine-octahydro-1,3,5,7-tetranitro-1,3,5,7 or HMX has four different stable polymorphs which have different molecular conformations, crystalline structures, and densities, making structural phase transitions between these nontrivial. Previous studies of the kinetics of the β-δ HMX structural transition found this to happen by a nucleation and growth mechanism, where growth was governed by the heat of fusion, or melting, even though the phase transition temperature is more than 100 K below the melting point. A theory known as virtual melting could easily justify this since the large volume difference in the two phases creates a strain at their interface that can lower the melting point to the phase transition temperature through a relaxation of the elastic energy.

Diffraction of ultrashort optical pulses from circularly symmetric binary phase gratings.

The complete spatiotemporal characterization of the diffracted field of ultrashort pulses after passing through circularly symmetric binary phase diffraction gratings is carried out. The complex field is registered at different planes behind the gratings with an ultrashort-pulse measurement technique called SEA TADPOLE. Numerical simulations based on scalar diffraction theory are compared with the measurements.

High-field transport in an electron-hole plasma: transition from ballistic to drift motion.

The time evolution of high-field carrier transport in bulk GaAs is studied with intense femtosecond THz pulses. While ballistic transport of electrons occurs in an n-type sample, a transition from ballistic to driftlike motion is observed in an electron-hole plasma. This onset of friction is due to the holes, which are heated by THz absorption.

Complete single-shot measurement of arbitrary nanosecond laser pulses in time.

For essentially all applications, laser pulses must avoid variations in their intensity and phase within a pulse and from pulse to pulse. Currently available devices work very well for both long (>10ns) and short (<100ps) pulses. But intermediate (~ns) pulses remain difficult to measure and, not surprisingly, are the least stable.

Measuring extremely complex pulses with time-bandwidth products exceeding 65,000 using multiple-delay crossed-beam spectral interferometry.

We measure the complete electric field of extremely complex ultrafast waveforms using the simple linear-optical, interferometric pulse-measurement technique, MUD TADPOLE. The waveforms were measured with ~40 fs temporal resolution over a temporal range of ~3.5 ns and had time-bandwidth products exceeding 65,000.

Basic diffraction phenomena in time domain.

Using a recently developed technique (SEA TADPOLE) for easily measuring the complete spatiotemporal electric field of light pulses with micrometer spatial and femtosecond temporal resolution, we directly demonstrate the formation of theo-called boundary diffraction wave and Arago's spot after an aperture, as well as the superluminal propagation of the spot. Our spatiotemporally resolved measurements beautifully confirm the time-domain treatment of diffraction. Also they prove very useful for modern physical optics, especially in micro- and meso-optics, and also significantly aid in the understanding of diffraction phenomena in general.

Measuring temporally complex ultrashort pulses using multiple-delay crossed-beam spectral interferometry.

We introduce a spectral-interferometry (SI) technique for measuring the complete intensity and phase of relatively long and very complex ultrashort pulses. Ordinarily, such a method would require a high-resolution spectrometer, but our method overcomes this need. It involves making multiple measurements using SI (in its SEA TADPOLE variation) at numerous delays, measuring many temporal pulselets within the pulse, and concatenating the resulting pulselets.

Evolution of the frequency chirp of Gaussian pulses and beams when passing through a pulse compressor.

The evolution of the frequency chirp of a laser pulse inside a classical pulse compressor is very different for plane waves and Gaussian beams, although after propagating through the last (4th) dispersive element, the two models give the same results. In this paper, we have analyzed the evolution of the frequency chirp of Gaussian pulses and beams using a method which directly obtains the spectral phase acquired by the compressor. We found the spatiotemporal couplings in the phase to be the fundamental reason for the difference in the frequency chirp acquired by a Gaussian beam and a plane wave.

Direct spatiotemporal measurements of accelerating ultrashort Bessel-type light bullets.

We measure the spatiotemporal field of ultrashort pulses with complex spatiotemporal profiles using the linear-optical, interferometric pulse-measurement technique SEA TADPOLE. Accelerating and decelerating ultrashort, localized, nonspreading Bessel-X wavepackets were generated from a approximately 27 fs duration Ti:Sapphire oscillator pulse using a combination of an axicon and a convex or concave lens. The wavefields are measured with approximately 5 microm spatial and approximately 15 fs temporal resolutions.

Measuring the spatiotemporal field of ultrashort Bessel-X pulses.

We present direct measurements of the spatiotemporal electric field of an ultrashort Bessel-X pulse generated using a conical lens (axicon). These measurements were made using the linear-optical interferometric technique SEA TADPOLE, which has micrometer spatial resolution and femtosecond temporal resolution. From our measurements, both the superluminal velocity of the Bessel pulse and the propagation invariance of the central spot are apparent.

Propagation dependence of chirp in Gaussian pulses and beams due to angular dispersion.

The chirp acquired by a Gaussian ultrashort pulse due to angular dispersion, unlike that of plane waves, increases nonlinearly with propagation distance and eventually asymptotes to a constant. However, this interesting result has never been directly measured. In this Letter, we use two-dimensional spectral interferometry to measure the propagation dependence of the chirp for Gaussian ultrashort pulses and beams with angular dispersion.

Measuring the spatiotemporal electric field of tightly focused ultrashort pulses with sub-micron spatial resolution.

We demonstrate a powerful and practical spectral interferometer with near-field scanning microscopy (NSOM) probes for measuring the spatiotemporal electric field of tightly focused ultrashort pulses with high spatial and spectral resolution. Our measurements involved numerical apertures as high as 0.44 and yielded the spatiotemporal field at and around the foci produced by two microscope objectives and several different lenses.

Directly measuring the spatio-temporal electric field of focusing ultrashort pulses.

We present the first technique for directly measuring (without assumptions) the spatio-temporal intensity and phase of a train of ultrashort pulses at and near a focus. Our method uses an experimentally simple and high-spectral resolution variant of spectral interferometry (SEA TADPOLE). To illustrate our technique, we measured the spatio-temporal electric field in and around the foci of several different types of lenses.

Crossed-beam spectral interferometry: a simple, high-spectral-resolution method for completely characterizing complex ultrashort pulses in real time.

We present a high-spectral-resolution and experimentally simple version of spectral interferometry using optical fibers and crossed beams, which we call SEA TADPOLE. Rather than using collinear unknown and reference pulses separated in time to yield spectral fringes-and reduced spectral resolution-as in current versions, we use time-coincident pulses crossed at a small angle to generate spatial fringes. This allows the extraction of the spectral phase with the full spectrometer resolution, which allows the measurement of much longer and more complex pulses.