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A structural transition in an atomic indium wire on a silicon substrate proceeds as fast as the indium atom vibrations and is facilitated by strong In–Si interface bonds. Speedy surface structure shifts Ultrafast diffraction techniques enable us to observe laser-induced structural changes at the atomic scale and with high temporal resolution. A decade of such experiments has indicated that structural changes on surfaces are several orders of magnitude slower than changes in bulk materials, raising the question of whether there is a fundamental limit for low-dimensional systems. Tim Frigge et al. apply laser excitation to a one-dimensional wire of indium atoms on a silicon surface and find that structural changes take place on femtosecond timescales. This short timescale is made possible by electronic coupling to the underlying surface and indicates that structural changes at the surface can, in principle, be as fast as in the bulk material. The findings point to a new method for controlling the dynamic structural responses of solids to laser excitation. Transient control over the atomic potential-energy landscapes of solids could lead to new states of matter and to quantum control of nuclear motion on the timescale of lattice vibrations. Recently developed ultrafast time-resolved diffraction techniques 1 combine ultrafast temporal manipulation with atomic-scale spatial resolution and femtosecond temporal resolution. These advances have enabled investigations of photo-induced structural changes in bulk solids that often occur on timescales as short as a few hundred femtoseconds 2 , 3 , 4 , 5 , 6 . In contrast, experiments at surfaces and on single atomic layers such as graphene report timescales of structural changes that are orders of magnitude longer 7 , 8 , 9 . This raises the question of whether the structural response of low-dimensional materials to femtosecond laser excitation is, in general, limited. Here we show that a photo-induced transition from the low- to high-symmetry state of a charge density wave in atomic indium (In) wires supported by a silicon (Si) surface takes place within 350 femtoseconds. The optical excitation breaks and creates In–In bonds, leading to the non-thermal excitation of soft phonon modes, and drives the structural transition in the limit of critically damped nuclear motion through coupling of these soft phonon modes to a manifold of surface and interface phonons that arise from the symmetry breaking at the silicon surface. This finding demonstrates that carefully tuned electronic excitations can create non-equilibrium potential energy surfaces that drive structural dynamics at interfaces in the quantum limit (that is, in a regime in which the nuclear motion is directed and deterministic) 8 . This technique could potentially be used to tune the dynamic response of a solid to optical excitation, and has widespread potential application, for example in ultrafast detectors 10 , 11 .

Electron-phonon coupling processes determine electronic transport properties of materials and are responsible for the transfer of electronic excess energy to the lattice. With decreasing device dimensions an understanding of these processes in nanoscale materials is becoming increasingly important. Here we use time-resolved electron diffraction to directly study energy relaxation in thin bismuth films after optical excitation. Precise measurements of the transient Debye-Waller-effect for various film thicknesses and over an extended range of excitation fluences allow to separate different contributions to the incoherent lattice response. While phonon softening in the electronically excited state is responsible for an immediate increase of the r.m.s. atomic displacement within a few hundred fs, 'ordinary' electron-phonon coupling leads to subsequent heating of the material on a few ps time-scale. The data reveal distinct changes in the energy transfer dynamics which becomes faster for stronger excitation and smaller film thickness, respectively. The latter effect is attributed to a cross-interfacial coupling of excited electrons to phonons in the substrate.

Using ultrafast, time-resolved, 1.54 angstrom x-ray diffraction, thermal and ultrafast nonthermal melting of germanium, involving passage through non-equilibrium extreme states of matter, was observed. Such ultrafast, optical-pump, x-ray diffraction probe measurements provide a way to study many other transient processes in physics, chemistry, and biology, including direct observation of the atomic motion by which many solid-state processes and chemical and biochemical reactions take place.

The lattice response of a Bi(111) surface upon impulsive femtosecond laser excitation is studied with time-resolved reflection high-energy electron diffraction. We employ a Debye–Waller analysis at large momentum transfer of 9.3 Å−1 ≤ Δ k ≤ 21.8 Å−1 in order to study the lattice excitation dynamics of the Bi surface under conditions of weak optical excitation up to 2 mJ/cm2 incident pump fluence. The observed time constants τint of decay of diffraction spot intensity depend on the momentum transfer Δk and range from 5 to 12 ps. This large variation of τint is caused by the nonlinearity of the exponential function in the Debye–Waller factor and has to be taken into account for an intensity drop ΔI > 0.2. An analysis of more than 20 diffraction spots with a large variation in Δk gave a consistent value for the time constant τT of vibrational excitation of the surface lattice of 12 ± 1 ps independent on the excitation density. We found no evidence for a deviation from an isotropic Debye–Waller effect and conclude that the primary laser excitation leads to thermal lattice excitation, i.e., heating of the Bi surface.

Strong optical irradiation of indium atomic wires on a Si(111) surface causes the nonthermal structural transition from the (8 × 2) reconstructed ground state to an excited (4 × 1) state. The immediate recovery of the system to the ground state is hindered by an energy barrier for the collective motion of the indium atoms along the reaction coordinate from the (4 × 1) to the (8 × 2) state. This metastable, supercooled state can only recover through nucleation of the ground state at defects like adsorbates or step edges. Subsequently, a recovery front propagates with constant velocity across the surface and the (8 × 2) ground state is reinstated. In a combined femtosecond electron diffraction and photoelectron emission microscopy study, we determined—based on the step morphology—a velocity of this recovery front of ∼100 m/s.

Ultrafast reflection high-energy electron diffraction is employed to follow the lattice excitation of a Bi(111) surface upon irradiation with a femtosecond laser pulse. The thermal motion of the atoms is analyzed through the Debye–Waller effect. While the Bi bulk is heated on time scales of 2 to 4 ps, we observe that the excitation of vibrational motion of the surface atoms occurs much slower with a time constant of 12 ps. This transient nonequilibrium situation is attributed to the weak coupling between bulk and surface phonon modes which hampers the energy flow between the two subsystems. From the absence of a fast component in the transient diffraction intensity, it is in addition concluded that truncated bulk phonon modes are absent at the surface.

Ultrafast high energy electron diffraction in reflection geometry is employed to study the structural dynamics of self-organized Germanium hut-, dome-, and relaxed clusters on Si(001) upon femtosecond laser excitation. Utilizing the difference in size and strain state the response of hut- and dome clusters can be distinguished by a transient spot profile analysis. Surface diffraction from {105}-type facets provide exclusive information on hut clusters. A pixel-by-pixel analysis of the dynamics of the entire diffraction pattern gives time constants of 40, 160, and 390 ps, which are assigned to the cooling time constants for hut-, dome-, and relaxed clusters.

The photoinduced structural dynamics of the atomic wire system on the Si(111)-In surface has been studied by ultrafast electron diffraction in reflection geometry. Upon intense fs-laser excitation, this system can be driven in around 1 ps from the insulating (8×2) reconstructed low temperature phase to a metastable metallic (4×1) reconstructed high temperature phase. Subsequent to the structural transition, the surface heats up on a 6 times slower timescale as determined from a transient Debye-Waller analysis of the diffraction spots. From a comparison with the structural response of the high temperature (4×1) phase, we conclude that electron-phonon coupling is responsible for the slow energy transfer from the excited electron system to the lattice. The significant difference in timescales is evidence that the photoinduced structural transition is non-thermally driven.

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.

With the combination of high resolution low energy electron diffraction and a bending sample technique we have simultaneously studied surface stress and surface structure during adsorption and desorption of antimony on the Si(111) surface. During desorption, several surface reconstructions with significantly different effects on the stress signal evolve. The surface stress of all observed structures has been obtained.