Ultrafast time-resolved optical spectroscopy has revealed new classes of physical, chemical and biological reactions, in which directed, deterministic motions of atoms have a key role. This contrasts with the random, diffusive motion of atoms across activation barriers that typically determines kinetic rates on slower timescales. An example of these new processes is the ultrafast melting of semiconductors, which is believed to arise from a strong modification of the inter-atomic forces owing to laser-induced promotion of a large fraction (10% or more) of the valence electrons to the conduction band. The atoms immediately begin to move and rapidly gain sufficient kinetic energy to induce melting--much faster than the several picoseconds required to convert the electronic energy into thermal motions. Here we present measurements of the characteristic melting time of InSb with a recently developed technique of ultrafast time-resolved X-ray diffraction that, in contrast to optical spectroscopy, provides a direct probe of the changing atomic structure. The data establish unambiguously a loss of long-range order up to 900 A inside the crystal, with time constants as short as 350 femtoseconds. This ability to obtain the quantitative structural characterization of non-thermal processes should find widespread application in the study of ultrafast dynamics in other physical, chemical and biological systems.

The study of phase-transition dynamics in solids beyond a time-averaged kinetic description requires direct measurement of the changes in the atomic configuration along the physical pathways leading to the new phase. The timescale of interest is in the range 10(-14) to 10(-12) s. Until recently, only optical techniques were capable of providing adequate time resolution, albeit with indirect sensitivity to structural arrangement. Ultrafast laser-induced changes of long-range order have recently been directly established for some materials using time-resolved X-ray diffraction. However, the measurement of the atomic displacements within the unit cell, as well as their relationship with the stability limit of a structural phase, has to date remained obscure. Here we report time-resolved X-ray diffraction measurements of the coherent atomic displacement of the lattice atoms in photoexcited bismuth close to a phase transition. Excitation of large-amplitude coherent optical phonons gives rise to a periodic modulation of the X-ray diffraction efficiency. Stronger excitation corresponding to atomic displacements exceeding 10 per cent of the nearest-neighbour distance-near the Lindemann limit-leads to a subsequent loss of long-range order, which is most probably due to melting of the material.

The control of light-matter interaction at the quantum level usually requires coherent laser fields. But already an exchange of virtual photons with the electromagnetic vacuum field alone can lead to quantum coherences, which subsequently suppress spontaneous emission. We demonstrate such spontaneously generated coherences (SGC) in a large ensemble of nuclei operating in the x-ray regime, resonantly coupled to a common cavity environment. The observed SGC originates from two fundamentally different mechanisms related to cooperative emission and magnetically controlled anisotropy of the cavity vacuum. This approach opens new perspectives for quantum control, quantum state engineering and simulation of quantum many-body physics in an essentially decoherence-free setting.

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We investigate ultrafast (fs) electron dynamics in a liquid hydrogen sample, isochorically and volumetrically heated to a moderately coupled plasma state. Thomson scattering measurements using 91.8 eV photons from the free-electron laser in Hamburg (FLASH at DESY) show that the hydrogen plasma has been driven to a nonthermal state with an electron temperature of 13 eV and an ion temperature below 0.1 eV, while the free-electron density is 2:8 Â 10 20 cm À3 . For dense plasmas, our experimental data strongly support a nonequilibrium kinetics model that uses impact ionization cross sections based on classical free-electron collisions. The investigation of warm dense matter (WDM) is one of the grand challenges of contemporary physics [1]. WDM is a plasma state characterized by moderate-tostrong interparticle coupling which takes place at freeelectron temperatures of several eV and free-electron densities around solid density [1]. It is present in many physical environments, such as planetary interiors [2,3], gravitationally collapsing protostellar disks, laser matter interaction and particularly during the implosion of an inertial confinement fusion capsule [4]. While in the astrophysical context WDM exists under stable conditions, in the laboratory it is achieved only as a transient state bridging condensed matter and hot plasma regimes. Here, we report on the first investigation of the nonequilibrium transition of hydrogen from a liquid to a moderately coupled plasma on the fs time scale, induced by highly intense soft-x-ray irradiation. This is an important step towards the investigation of strongly-coupled plasmas which are within reach of current light sources such as the Linac Coherent Light Source (LCLS). Our measurement enables unprecedented direct tests of nonequilibrium statistical models beyond mean field theories in a regime where collision and relaxation processes are dominant [5][6][7].The use of x-ray scattering for the investigation of dense, strongly-coupled plasmas was successfully demonstrated in the past decade [5,[7][8][9][10][11]. This technique is the x-ray analog of optical Thomson scattering (TS) [12] and enables the experimental determination of plasma parameters in dense systems where optical light cannot penetrate. While previous experiments were carried out using highenergy laser facilities, the advent of soft-and hard-x-ray free-electron lasers (FELs) makes ultrashort high brightness beams available for this type of research [13,14]. This Letter reports on ultrafast heating of liquid hydrogen and TS measurement of dense plasma parameters using softx-ray FEL radiation. For the first time, nonequilibrium distributions are observed and the underlying relaxation dynamics are compared with kinetic models showing electron relaxation times in the order of 20 fs, thus, shorter than the pulse duration.The scattering taking place is collective TS, which is characterized by a spectrally blue and red shifted response due to collective electron motion, plasmons, and nearly elastic scattering due t...

Saturable absorption is a phenomenon readily seen in the optical and infrared wavelengths. It has never been observed in core-electron transitions owing to the short lifetime of the excited states involved and the high intensities of the soft X-rays needed. We report saturable absorption of an L-shell transition in aluminium using record intensities over 10 16 W cm −2 at a photon energy of 92 eV. From a consideration of the relevant timescales, we infer that immediately after the X-rays have passed, the sample is in an exotic state where all of the aluminium atoms have an L-shell hole, and the valence band has approximately a 9 eV temperature, whereas the atoms are still on their crystallographic positions. Subsequently, Auger decay heats the material to the warm dense matter regime, at around 25 eV temperatures. The method is an ideal candidate to study homogeneous warm dense matter, highly relevant to planetary science, astrophysics and inertial confinement fusion. Saturable absorption, the decrease in the absorption of light with increasing intensity, is a well-known effect in the visible and near-visible region of the electromagnetic spectrum 1 , and is a widely exploited phenomenon in laser technology. Although there are many ways to induce this effect, in the simplest two-level system it will occur when the population of the lower, absorbing level is severely depleted, which requires light intensities sufficiently high to overcome relaxation from the upper level. Here, we report on the production of saturable absorption of a metal in the soft X-ray regime by the creation of highly uniform warm dense conditions, a regime that is of great interest in high-pressure science 2,3 , the geophysics of large planets 4,5 , astrophysics 6 , plasma production and inertial confinement fusion 7 . Furthermore, the process by which the saturation of the absorption occurs will lead, after the X-ray pulse, to the storage of about 100 eV per atom, which in turn evolves to a warm dense state. This manner of creation is unique as it requires intense, subpicosecond, soft X-rays. As such, it has not hitherto been observed in this region of the spectrum, owing both to the lack of high-intensity sources, and the rapid recombination times associated with such high photon energies. However, with the advent of new fourth-generation X-ray light sources, including the free-electron laser in Hamburg 8 (FLASH), soft X-ray intensities that have previously remained the province of high-power optical lasers can now be produced. Experiments at such high intensities using gas jets have already exhibited novel absorption phenomena 9 , and the possibility of irradiating solid samples with intense soft and hard X-rays has aroused interest as a possible means of producing warm dense matter (WDM) at known atomic densities 10,11 .We present the first measurements of the absorption coefficient of solid samples subject to subpicosecond soft X-ray pulses with intensities up to and in excess of 10 16 W cm −2 , two orders of magnitude higher than could ...

The displacive phase transition in SrTiO3 was investigated by means of x-ray diffraction. We used 4.5 keV photons thus probing only a very thin region near the surface. In the low temperature phase the lattice parameters evolve substantially different than in bulk material. We also investigated the phase transition under the influence of an epitaxial coating with YBaCu2O7 and found the nature of the phase transition changed. The near-surface region behaves like an epitaxial thin SrTiO3 film.

The generation of femtosecond Kalpha x rays from laser-irradiated plasmas is studied with a view to optimizing photon number and pulse duration. Using analytical and numerical models of hot electron generation and subsequent transport in a range of materials, it is shown that an optimum laser intensity I(opt) = 7x10(9)Z4.4 exists for maximum Kalpha yield. Furthermore, it is demonstrated that bulk targets are unsuitable for generating sub-ps x-ray pulses: instead, design criteria are proposed for achieving Kalpha pulse durations