Controlling Fragmentation of the Acetylene Cation in the Vacuum Ultraviolet via Transient Molecular Alignment.

An open-loop control scheme of molecular fragmentation based on transient molecular alignment combined with single-photon ionization induced by a short-wavelength free electron laser (FEL) is demonstrated for the acetylene cation. Photoelectron spectra are recorded, complementing the ion yield measurements, to demonstrate that such control is the consequence of changes in the electronic response with molecular orientation relative to the ionizing field. We show that stable C2H2+ cations are mainly produced when the molecules are parallel or nearly parallel to the FEL polarization, while the hydrogen fragmentation channel (C2H2+ → C2H+ + H) predominates when the molecule is perpendicular to that direction, thus allowing one to distinguish between the two photochemical processes. The experimental findings are supported by state-of-the art theoretical calculations.

Direct observation of electron propagation and dielectric screening on the atomic length scale.

The propagation and transport of electrons in crystals is a fundamental process pertaining to the functioning of most electronic devices. Microscopic theories describe this phenomenon as being based on the motion of Bloch wave packets. These wave packets are superpositions of individual Bloch states with the group velocity determined by the dispersion of the electronic band structure near the central wavevector in momentum space. This concept has been verified experimentally in artificial superlattices by the observation of Bloch oscillations--periodic oscillations of electrons in real and momentum space. Here we present a direct observation of electron wave packet motion in a real-space and real-time experiment, on length and time scales shorter than the Bloch oscillation amplitude and period. We show that attosecond metrology (1 as = 10(-18) seconds) now enables quantitative insight into weakly disturbed electron wave packet propagation on the atomic length scale without being hampered by scattering effects, which inevitably occur over macroscopic propagation length scales. We use sub-femtosecond (less than 10(-15) seconds) extreme-ultraviolet light pulses to launch photoelectron wave packets inside a tungsten crystal that is covered by magnesium films of varied, well-defined thicknesses of a few ångströms. Probing the moment of arrival of the wave packets at the surface with attosecond precision reveals free-electron-like, ballistic propagation behaviour inside the magnesium adlayer--constituting the semi-classical limit of Bloch wave packet motion. Real-time access to electron transport through atomic layers and interfaces promises unprecedented insight into phenomena that may enable the scaling of electronic and photonic circuits to atomic dimensions. In addition, this experiment allows us to determine the penetration depth of electrical fields at optical frequencies at solid interfaces on the atomic scale.

Femtosecond all-optical synchronization of an X-ray free-electron laser.

Many advanced applications of X-ray free-electron lasers require pulse durations and time resolutions of only a few femtoseconds. To generate these pulses and to apply them in time-resolved experiments, synchronization techniques that can simultaneously lock all independent components, including all accelerator modules and all external optical lasers, to better than the delivered free-electron laser pulse duration, are needed. Here we achieve all-optical synchronization at the soft X-ray free-electron laser FLASH and demonstrate facility-wide timing to better than 30 fs r.m.s. for 90 fs X-ray photon pulses. Crucially, our analysis indicates that the performance of this optical synchronization is limited primarily by the free-electron laser pulse duration, and should naturally scale to the sub-10 femtosecond level with shorter X-ray pulses.

Coherent spectral enhancement of carrier-envelope-phase stable continua with dual-gas high harmonic generation.

Attosecond science is enabled by the ability to convert femtosecond near-infrared laser light into coherent harmonics in the extreme ultraviolet spectral range. While attosecond sources have been utilized in experiments that have not demanded high intensities, substantially higher photon flux would provide a natural link to the next significant experimental breakthrough. Numerical simulations of dual-gas high harmonic generation indicate that the output in the cutoff spectral region can be selectively enhanced without disturbing the single-atom gating mechanism. Here, we summarize the results of these simulations and present first experimental findings to support these predictions.

Attosecond time-resolved photoemission from core and valence states of magnesium.

We report on laser-assisted attosecond photoemission from single-crystalline magnesium. In strong contrast to the previously investigated transition metal tungsten, photoelectron wave packets originating from the localized core level and delocalized valence-band states are launched simultaneously from the solid within the experimental uncertainty of 20 as. This phenomenon is shown to be compatible with a heuristic model based on free-particle-like propagation of the electron wave packets generated inside the crystal by the attosecond excitation pulse and their subsequent interaction with the assisting laser field at the metal-vacuum interface.

Angle-resolved electron spectroscopy of laser-assisted Auger decay induced by a few-femtosecond x-ray pulse.

Two-color (x-ray+infrared) electron spectroscopy is used for investigating laser-assisted KLL Auger decay following 1s photoionization of atomic Ne with few-femtosecond x-ray pulses from the Linac Coherent Light Source. In an angle-resolved experiment, the overall width of the laser-modified Auger-electron spectrum and its structure change significantly as a function of the emission angle. The spectra are characterized by a strong intensity variation of the sidebands revealing a gross structure. This variation is caused, as predicted by theory, by the interference of electrons emitted at different times within the duration of one optical cycle of the infrared dressing laser, which almost coincides with the lifetime of the Ne 1s vacancy.

Clocking the melting transition of charge and lattice order in 1T-TaS2 with ultrafast extreme-ultraviolet angle-resolved photoemission spectroscopy.

We use time- and angle-resolved photoemission spectroscopy with sub-30-fs extreme-ultraviolet pulses to map the time- and momentum-dependent electronic structure of photoexcited 1T-TaS(2). This compound is a two-dimensional Mott insulator with charge-density wave ordering. Charge order, evidenced by splitting between occupied subbands at the Brillouin zone boundary, melts well before the lattice responds. This challenges the view of a charge-density wave caused by electron-phonon coupling and Fermi-surface nesting alone, and suggests that electronic correlations play a key role in driving charge order.

A flexible apparatus for attosecond photoelectron spectroscopy of solids and surfaces.

We describe an apparatus for attosecond photoelectron spectroscopy of solids and surfaces, which combines the generation of isolated attosecond extreme-ultraviolet (XUV) laser pulses by high harmonic generation in gases with time-resolved photoelectron detection and surface science techniques in an ultrahigh vacuum environment. This versatile setup provides isolated attosecond pulses with photon energies of up to 140 eV and few-cycle near infrared pulses for studying ultrafast electron dynamics in a large variety of surfaces and interfaces. The samples can be prepared and characterized on an atomic scale in a dedicated flexible surface science end station. The extensive possibilities offered by this apparatus are demonstrated by applying attosecond XUV pulses with a central photon energy of ∼125 eV in an attosecond streaking experiment of a xenon multilayer grown on a Re(0001) substrate.

Delay in photoemission.

Photoemission from atoms is assumed to occur instantly in response to incident radiation and provides the basis for setting the zero of time in clocking atomic-scale electron motion. We used attosecond metrology to reveal a delay of 21 +/- 5 attoseconds in the emission of electrons liberated from the 2p orbitals of neon atoms with respect to those released from the 2s orbital by the same 100-electron volt light pulse. Small differences in the timing of photoemission from different quantum states provide a probe for modeling many-electron dynamics. Theoretical models refined with the help of attosecond timing metrology may provide insight into electron correlations and allow the setting of the zero of time in atomic-scale chronoscopy with a precision of a few attoseconds.

X-ray diffuse scattering measurements of nucleation dynamics at femtosecond resolution.

Femtosecond time-resolved small and wide angle x-ray diffuse scattering techniques are applied to investigate the ultrafast nucleation processes that occur during the ablation process in semiconducting materials. Following intense optical excitation, a transient liquid state of high compressibility characterized by large-amplitude density fluctuations is observed and the buildup of these fluctuations is measured in real time. Small-angle scattering measurements reveal snapshots of the spontaneous nucleation of nanoscale voids within a metastable liquid and support theoretical predictions of the ablation process.

Attosecond spectroscopy in condensed matter.

Comprehensive knowledge of the dynamic behaviour of electrons in condensed-matter systems is pertinent to the development of many modern technologies, such as semiconductor and molecular electronics, optoelectronics, information processing and photovoltaics. Yet it remains challenging to probe electronic processes, many of which take place in the attosecond (1 as = 10(-18) s) regime. In contrast, atomic motion occurs on the femtosecond (1 fs = 10(-15) s) timescale and has been mapped in solids in real time using femtosecond X-ray sources. Here we extend the attosecond techniques previously used to study isolated atoms in the gas phase to observe electron motion in condensed-matter systems and on surfaces in real time. We demonstrate our ability to obtain direct time-domain access to charge dynamics with attosecond resolution by probing photoelectron emission from single-crystal tungsten. Our data reveal a delay of approximately 100 attoseconds between the emission of photoelectrons that originate from localized core states of the metal, and those that are freed from delocalized conduction-band states. These results illustrate that attosecond metrology constitutes a powerful tool for exploring not only gas-phase systems, but also fundamental electronic processes occurring on the attosecond timescale in condensed-matter systems and on surfaces.

Attosecond control and measurement: lightwave electronics.

Electrons emit light, carry electric current, and bind atoms together to form molecules. Insight into and control of their atomic-scale motion are the key to understanding the functioning of biological systems, developing efficient sources of x-ray light, and speeding up electronics. Capturing and steering this electron motion require attosecond resolution and control, respectively (1 attosecond = 10(-18) seconds). A recent revolution in technology has afforded these capabilities: Controlled light waves can steer electrons inside and around atoms, marking the birth of lightwave electronics. Isolated attosecond pulses, well reproduced and fully characterized, demonstrate the power of the new technology. Controlled few-cycle light waves and synchronized attosecond pulses constitute its key tools. We review the current state of lightwave electronics and highlight some future directions.

Carrier-density-dependent lattice stability in InSb.

The ultrafast decay of the x-ray diffraction intensity following laser excitation of an InSb crystal has been utilized to observe carrier dependent changes in the potential energy surface. For the first time, an abrupt carrier dependent onset for potential energy surface softening and the appearance of accelerated atomic disordering for a very high average carrier density have been observed. Inertial dynamics dominate the early stages of crystal disordering for a wide range of carrier densities between the onset of crystal softening and the appearance of accelerated atomic disordering.

Ultrafast bond softening in bismuth: mapping a solid's interatomic potential with X-rays.

Intense femtosecond laser excitation can produce transient states of matter that would otherwise be inaccessible to laboratory investigation. At high excitation densities, the interatomic forces that bind solids and determine many of their properties can be substantially altered. Here, we present the detailed mapping of the carrier density-dependent interatomic potential of bismuth approaching a solid-solid phase transition. Our experiments combine stroboscopic techniques that use a high-brightness linear electron accelerator-based x-ray source with pulse-by-pulse timing reconstruction for femtosecond resolution, allowing quantitative characterization of the interatomic potential energy surface of the highly excited solid.

Generation and propagation of a picosecond acoustic pulse at a buried interface: time-resolved x-ray diffraction measurements.

We report on the propagation of coherent acoustic wave packets in (001) surface oriented Al0.3Ga0.7As/GaAs heterostructure, generated through localized femtosecond photoexcitation of the GaAs. Transient structural changes in both the substrate and film are measured with picosecond time-resolved x-ray diffraction. The data indicate an elastic response consisting of unipolar compression pulses of a few hundred picosecond duration traveling along [001] and [001] directions that are produced by predominately impulsive stress. The transmission and reflection of the strain pulses are in agreement with an acoustic mismatch model of the heterostructure and free-space interfaces.

Observation of structural anisotropy and the onset of liquidlike motion during the nonthermal melting of InSb.

The melting dynamics of laser excited InSb have been studied with femtosecond x-ray diffraction. These measurements observe the delayed onset of diffusive atomic motion, signaling the appearance of liquidlike dynamics. They also demonstrate that the root-mean-squared displacement in the [111] direction increases faster than in the [110] direction after the first 500 fs. This structural anisotropy indicates that the initially generated fluid differs significantly from the equilibrium liquid.

Clocking femtosecond X rays.

Linear-accelerator-based sources will revolutionize ultrafast x-ray science due to their unprecedented brightness and short pulse duration. However, time-resolved studies at the resolution of the x-ray pulse duration are hampered by the inability to precisely synchronize an external laser to the accelerator. At the Sub-Picosecond Pulse Source at the Stanford Linear-Accelerator Center we solved this problem by measuring the arrival time of each high energy electron bunch with electro-optic sampling. This measurement indirectly determined the arrival time of each x-ray pulse relative to an external pump laser pulse with a time resolution of better than 60 fs rms.

Atomic-scale visualization of inertial dynamics.

The motion of atoms on interatomic potential energy surfaces is fundamental to the dynamics of liquids and solids. An accelerator-based source of femtosecond x-ray pulses allowed us to follow directly atomic displacements on an optically modified energy landscape, leading eventually to the transition from crystalline solid to disordered liquid. We show that, to first order in time, the dynamics are inertial, and we place constraints on the shape and curvature of the transition-state potential energy surface. Our measurements point toward analogies between this nonequilibrium phase transition and the short-time dynamics intrinsic to equilibrium liquids.

Adaptive dispersion compensation for remote fiber delivery of near-infrared femtosecond pulses.

We report on remote delivery of 25-pJ broadband near-infrared femtosecond light pulses from a Ti:sapphire laser through 150 m of single-mode optical fiber. Pulse distortion caused by dispersion is overcome with precompensation by adaptive pulse shaping techniques, while nonlinearities are mitigated by use of an SF10 glass rod for the final stage of pulse compression. A near-transform-limited pulse duration of 130 fs was measured after the final compression.