Time-dependent energy absorption changes during ultrafast lattice deformation

The ultrafast time-dependence of the energy absorption of covalent solids upon excitation with femtosecond laser pulses is theoretically analyzed. We use a microscopic theory to describe laser induced structural changes and their influence on the electronic properties. We show that from the time evolution of the energy absorbed by the system important information on the electronic and atomic structure during ultrafast phase transitions can be gained. Our results reflect how structural changes affect the capability of the system to absorb external energy.Comment: 7 pages RevTeX, 8 ps figures, submitted to Journal of Appl. Physic

Probing laser-driven structure formation at extreme scales in space and time

Irradiation of solid surfaces with high intensity, ultrashort laser pulses triggers a variety of secondary processes that can lead to the formation of transient and permanent structures over large range of length scales from mm down to the nano-range. One of the most prominent examples are LIPSS - Laser Induced Periodic Surface Structures. While LIPSS have been a scientific evergreen for of almost 60 years, experimental methods that combine ultrafast temporal with the required nm spatial resolution have become available only recently with the advent of short pulse, short wavelength free electron lasers. Here we discuss the current status and future perspectives in this field by exploiting the unique possibilities of these 4th-generation light sources to address by time-domain experimental techniques the fundamental LIPSS-question, namely why and how laser-irradiation can initiate the transition of a "chaotic" (rough) surface from an aperiodic into a periodic structure.Comment: 13 pages incl. 5 figure

Theory for the ultrafast ablation of graphite films

The physical mechanisms for damage formation in graphite films induced by femtosecond laser pulses are analyzed using a microscopic electronic theory. We describe the nonequilibrium dynamics of electrons and lattice by performing molecular dynamics simulations on time-dependent potential energy surfaces. We show that graphite has the unique property of exhibiting two distinct laser induced structural instabilities. For high absorbed energies (> 3.3 eV/atom) we find nonequilibrium melting followed by fast evaporation. For low intensities above the damage threshold (> 2.0 eV/atom) ablation occurs via removal of intact graphite sheets.Comment: 5 pages RevTeX, 3 PostScript figures, submitted to Phys. Re

Ablation of solids by femtosecond lasers: ablation mechanism and ablation thresholds for metals and dielectrics

The mechanism of ablation of solids by intense femtosecond laser pulses is described in an explicit analytical form. It is shown that at high intensities when the ionization of the target material is complete before the end of the pulse, the ablation mechanism is the same for both metals and dielectrics. The physics of this new ablation regime involves ion acceleration in the electrostatic field caused by charge separation created by energetic electrons escaping from the target. The formulae for ablation thresholds and ablation rates for metals and dielectrics, combining the laser and target parameters, are derived and compared to experimental data. The calculated dependence of the ablation thresholds on the pulse duration is in agreement with the experimental data in a femtosecond range, and it is linked to the dependence for nanosecond pulses.Comment: 27 pages incl.3 figs; presented at CLEO-Europe'2000 11-15 Sept.2000; papers QMD6 and CTuK11

Kikuchi ultrafast nanodiffraction in four-dimensional electron microscopy

Coherent atomic motions in materials can be revealed using time-resolved X-ray and electron Bragg diffraction. Because of the size of the beam used, typically on the micron scale, the detection of nanoscale propagating waves in extended structures hitherto has not been reported. For elastic waves of complex motions, Bragg intensities contain all polarizations and they are not straightforward to disentangle. Here, we introduce Kikuchi diffraction dynamics, using convergent-beam geometry in an ultrafast electron microscope, to selectively probe propagating transverse elastic waves with nanoscale resolution. It is shown that Kikuchi band shifts, which are sensitive only to the tilting of atomic planes, reveal the resonance oscillations, unit cell angular amplitudes, and the polarization directions. For silicon, the observed wave packet temporal envelope (resonance frequency of 33 GHz), the out-of-phase temporal behavior of Kikuchi's edges, and the magnitude of angular amplitude (0.3 mrad) and polarization [011] elucidate the nature of the motion: one that preserves the mass density (i.e., no compression or expansion) but leads to sliding of planes in the antisymmetric shear eigenmode of the elastic waveguide. As such, the method of Kikuchi diffraction dynamics, which is unique to electron imaging, can be used to characterize the atomic motions of propagating waves and their interactions with interfaces, defects, and grain boundaries at the nanoscale

Time-resolved diffraction with an optimized short pulse laser plasma X-ray source

We present a set-up for time-resolved X-ray diffraction based on a short pulse, laser-driven plasma X-ray source. The employed modular design provides high flexibility to adapt the set-up to the specific requirements (e.g. X-ray optics, sample environment) of particular applications. The configuration discussed here has been optimized towards high angular/momentum resolution and uses K$_{\alpha}$-radiation (4.51 keV) from a Ti wire-target in combination with a toroidally bent crystal for collection, monochromatization and focusing of the emitted radiation. $2\times 10^5$ Ti-K$_{\alpha1}$ photons per pulse with $10^{-4}$ relative bandwidth are delivered to the sample at 10 Hz repetition rate. This allows for high dynamic range ($10^4$) measurements of transient changes of the rocking curves of materials as for example induced by laser-triggered strain waves.Comment: 29 pages, 8 figure

Silicon clusters produced by femtosecond laser ablation: Non-thermal emission and gas-phase condensation

Neutral silicon clusters Si_n (up to n = 7) and their cations Si_n+ (up to n = 10) have been produced by femtosecond laser ablation of bulk silicon in vacuum and investigated using time-of-flight mass spectrometry. Two populations of the Si_n+ clusters with different velocity and abundance distributions in the ablation plume have been clearly distinguished. Possible mechanisms of cluster formation (Coulomb explosion, gas-phase condensation, phase explosion) are discussed

Short pulse laser-induced optical damage and fracto-emission of amorphous, diamond-like carbon

Short pulse laser damage and ablation of amorphous, diamond-like carbon films is investigated. Material removal is due to fracture of the film and ejection of large fragments, which exhibit a broadband emission of microsecond duration

Nonthermal fragmentation of C60

A theoretical study of the subpicosecond fragmentation of C60 clusters in response to ultrafast laser pulses is presented. We simulate the laser excitation and the consequent nonequilibrium relaxation dynamics of the electronic and nuclear degrees of freedom. The first stages of the nonequilibrium dynamics are dominated by a coherent breathing mode followed by the cold ejection of single C atoms, in contrast to the dimer emission which characterizes the thermal relaxation. We also determine the nonequilibrium damage thresholds as a function of the pulse duration.Comment: 5 pages, 4 figures, submitted to Chem. Phys. Let