Seeded stimulated X-ray emission at 5.9 keV.

X-ray free-electron lasers (XFELs) provide intense pulses that can generate stimulated X-ray emission, a phenomenon that has been observed and studied in materials ranging from neon to copper. Two schemes have been employed: amplified spontaneous emission (ASE) and seeded stimulated emission (SSE), where a second color XFEL pulse provides the seed. Both phenomena are currently explored for coherent X-ray laser sources and spectroscopy. Here, we report measurements of ASE and SSE of the 5.9 keV Mn Kα1 fluorescence line from a 3.9 molar NaMnO4 solution, pumped with 7 femtosecond FWHM XFEL pulses at 6.6 keV. We observed ASE at a pump pulse intensity of 1.7 × 1019 W/cm2, consistent with earlier findings. We observed SSE at dramatically reduced pump pulse intensities down to 1.1 × 1017 W/cm2. These intensities are well within the range of many existing XFEL instruments, which supports the experimental feasibility of SSE as a tool to generate coherent X-ray pulses, spectroscopic studies of transition metal complexes, and other applications.

Generation of intense phase-stable femtosecond hard X-ray pulse pairs.

Coherent nonlinear spectroscopies and imaging in the X-ray domain provide direct insight into the coupled motions of electrons and nuclei with resolution on the electronic length scale and timescale. The experimental realization of such techniques will strongly benefit from access to intense, coherent pairs of femtosecond X-ray pulses. We have observed phase-stable X-ray pulse pairs containing more than 3 × 107 photons at 5.9 keV (2.1 Å) with ∼1 fs duration and 2 to 5 fs separation. The highly directional pulse pairs are manifested by interference fringes in the superfluorescent and seeded stimulated manganese Kα emission induced by an X-ray free-electron laser. The fringes constitute the time-frequency X-ray analog of Young's double-slit interference, allowing for frequency domain X-ray measurements with attosecond time resolution.

Shortening X-Ray Pulse Duration via Saturable Absorption.

To shorten the duration of x-ray pulses, we present a nonlinear optical technique using atoms with core-hole vacancies (core-hole atoms) generated by inner-shell photoionization. The weak Coulomb screening in the core-hole atoms results in decreased absorption at photon energies immediately above the absorption edge. By employing this phenomenon, referred to as saturable absorption, we successfully reduce the duration of x-ray free-electron laser pulses (photon energy: 9.000 keV, duration: 6-7 fs, fluence: 2.0-3.5×10^{5} J/cm^{2}) by ∼35%. This finding that core-hole atoms are applicable to nonlinear x-ray optics is an essential stepping stone for extending nonlinear technologies commonplace at optical wavelengths to the hard x-ray region.

Avalanche parametric conversion and white spectrum generation from infrared femtosecond pulses in glasses.

The observation of discrete lines in the white spectrum at the initial stage of filamentation of powerful femtosecond laser pulses, propagating in silica glasses, as well as the filamentation without plasma channels observed in the experiments in air, pushed us to look for other nonlinear mechanisms for describing these effects. In this paper, we present a new parametric conversion mechanism for asymmetric spectrum broadening of femtosecond laser pulses towards higher frequencies in isotropic media. This mechanism includes cascade generation with THz spectral shift for solids and GHz shift for gases. The process works simultaneously with the four-photon parametric wave mixing. The theoretical model proposed agrees well with the experimental data.

Ultrafast ellipsometric pump-probe diagnostic of liquid metal surface with chirped continuum probe pulses.

We describe our ellipsometric pump-probe experiment to study materials at extreme conditions. To demonstrate the performance, liquid bismuth surface is pumped by intense 25 fs pulse and subsequent evolution of non-equilibrium bismuth plasma is probed by chirped continuum pulse. The shift in the origin-time at continuum spectral component is precisely corrected by comparing chirp behavior estimated from induced phase modulation (IPM) in fused silica to one from liquid bismuth reflectivity measurement. From IPM measurements, it was found that the time resolution of a chirped pulse depends on group delay dispersion at corresponding continuum spectral components. Moreover, due to explicit relation between time and frequency of a chirped probe pulse, pump induced rapid changes are projected onto different probe wavelengths. Using these properties, we investigated polarization dependent reflection dynamics of non-equilibrium bismuth plasma with sub-100 fs temporal resolution and a broader wavelength response. These ultrafast measurements will be useful to study exotic phase transitions at extreme states of matter.

Atomic inner-shell laser at 1.5-ångström wavelength pumped by an X-ray free-electron laser.

Since the invention of the first lasers in the visible-light region, research has aimed to produce short-wavelength lasers that generate coherent X-rays; the shorter the wavelength, the better the imaging resolution of the laser and the shorter the pulse duration, leading to better temporal resolution in probe measurements. Recently, free-electron lasers based on self-amplified spontaneous emission have made it possible to generate a hard-X-ray laser (that is, the photon energy is of the order of ten kiloelectronvolts) in an ångström-wavelength regime, enabling advances in fields from ultrafast X-ray spectrosopy to X-ray quantum optics. An atomic laser based on neon atoms and pumped by a soft-X-ray (that is, a photon energy of less than one kiloelectronvolt) free-electron laser has been achieved at a wavelength of 14 nanometres. Here, we use a copper target and report a hard-X-ray inner-shell atomic laser operating at a wavelength of 1.5 ångströms. X-ray free-electron laser pulses with an intensity of about 10(19) watts per square centimetre tuned to the copper K-absorption edge produced sufficient population inversion to generate strong amplified spontaneous emission on the copper Kα lines. Furthermore, we operated the X-ray free-electron laser source in a two-colour mode, with one colour tuned for pumping and the other for the seed (starting) light for the laser.

Saturable absorption of intense hard X-rays in iron.

In 1913, Maurice de Broglie discovered the presence of X-ray absorption bands of silver and bromine in photographic emulsion. Over the following century, X-ray absorption spectroscopy was established as a standard basis for element analysis, and further applied to advanced investigation of the structures and electronic states of complex materials. Here we show the first observation of an X-ray-induced change of absorption spectra of the iron K-edge for 7.1-keV ultra-brilliant X-ray free-electron laser pulses with an extreme intensity of 10(20) W cm(-2). The highly excited state yields a shift of the absorption edge and an increase of transparency by a factor of 10 with an improvement of the phase front of the transmitted X-rays. This finding, the saturable absorption of hard X-rays, opens a promising path for future innovations of X-ray science by enabling novel attosecond active optics, such as lasing and dynamical spatiotemporal control of X-rays.

Study of the thermo-optical constants of Yb doped Y2O3, Lu2O3 and Sc2O3 ceramic materials.

Thermally induced depolarization and thermal lens of three Konoshima Chemical Co. laser-ceramics samples Yb(3+):Lu(2)O(3)(C(Yb) ≈ 1.8 at.%), Yb(3+):Y(2)O(3)(C(Yb) ≈ 1.8 at.%), and Yb(3+):Sc(2)O(3) (C(Yb) ≈ 2.5 at.%) were measured in experiment at different pump power. The results allowed us to estimate the thermal conductivity of the investigated ceramic samples and compare their thermo-optical properties. The thermo-optical constants P and Q and its sign measured for these materials at the first time.

Strong compression of a magnetic field with a laser-accelerated foil.

We demonstrate the generation of high magnetic fields for condensed matter research using a high-power laser system. A cavity in which a seed magnetic field is applied is compressed by a kJ ns laser pulse. The time history of the compressed magnetic field is monitored by observing the Faraday effect rotation of polarization of a probe pulse in a glass fiber. To maintain a low-temperature condition in the final high-field region, we put a high-resistance foil around the final compression area. If we assume the length of the compression region is equal to the laser spot size, a magnetic field of more than 800 T is observed by Faraday rotation. Because of the large mass of the compression foil, this high magnetic field is sustained during almost 2 ns. During compression, a rarefaction wave from the backside of the accelerated foil and expanding material from the inner protection foil affect the magnetic field compression history, but the final compressed magnetic field strength agrees with the ratio between the initial sample area and the compressed cavity area.

Ultra-fast switching of light by absorption saturation in vacuum ultra-violet region.

Advances in free electron lasers producing high energy photons [Nat. Photonics 2(9), 555-559 (2008)] are expected to open up a new science of nonlinear optics of high energy photons. Specifically, lasers of photon energy higher than the plasma frequency of a metal can show new interaction features because they can penetrate deeply into metals without strong reflection. Here we show the observation of ultra-fast switching of vacuum ultra-violet (VUV) light caused by saturable absorption of a solid metal target. A strong gating is observed at energy fluences above 6J/cm2 at wavelength of 51 nm with tin metal thin layers. The ratio of the transmission at high intensity to low intensity is typically greater than 100:1. This means we can design new nonlinear photonic devices such as auto-correlator and pulse slicer for the VUV region.

Detection of hydrodynamic expansion in ultrashort pulse laser ellipsometric pump-probe experiments.

In ultrashort-pulse laser interaction with solid target materials, the target rapidly heats, melts, evaporates, and begins to expand as a vapor or plasma. The onset of hydrodynamic expansion following surface evaporation is a switching point, where the dominant physics changes from temperature dependence of the solid dielectric function to refraction by the dense vapor cloud. We propose and demonstrate a method to analyze reflection data to identify this onset of target expansion. We use two of the Stokes parameters obtained from ellipsometric pump-probe measurements to determine a dielectric function with an assumption of no expansion. We use this dielectric function to predict the full set of reflectivity measurements. If there is a sharply defined target interface, this method reproduces the experimental data. When the plasma expansion is no longer negligible, the prediction deviates from the experimental measurements. This comparison shows when the plasma expansion is no longer negligible.

Ultrashort-pulse laser ellipsometric pump-probe experiments on gold targets.

Ultrashort-pulse laser pump-probe ellipsometry has been performed on gold targets at intensities 2 x 10(12)-5 x 10(13) W/cm(2). We measured time-resolved p- and s-polarized reflectivity (r(p) and r(s)) and the s-p phase difference (delta). When plotted as Y=[2|r(s)||r(p)|sin((delta)]/(|r(s)|(2)+|r(p)|(2)) versus X=|r(p)|(2)/|r(s)|(2), the experimental data follow approximately the same curve in X-Y space, even for different pump intensities. Although the input energy density is about 40 eV/atom and the plasma expansion is rapid (up to 10 km/sec), our data are consistent with a partially transparent blowoff having an atomic polarizability (-1.75+0.2i)x 10(-24) cm(3). We attribute this behavior to recombination in the expanding plasma. The Saha equation predicts recombination and formation of negative ions and a low density of free electrons in the low-density vapor, and solutions of the Maxwell equations approximately reproduce the data.