Dynamics of laser-induced desorption from dielectric surfaces on a sub-picosecond timescale

The impact of ultra-short laser pulses induces intensity-dependent non-equilibrium processes in the surface region of dielectric targets, resulting in desorption of surface constituents. We report time-resolved studies on particle ejection from CaF₂ and BaF₂ targets.Pump-probe time-of-flight mass spectrometry (ToF MS) was used to measure the particle yields as a function of the delay time between pairs of sub-damage threshold laser pulses, thus obtaining the temporal dynamics of the laser-excited charged particle emission.In a correlative manner, the positive ion, electron and negative ion desorption yields dependence on the pump-probe delay time reveal a coherence peak around zero delay (similar to a two-pulse autocorrelation), accounting for the increase of the ion yield with laser intensity. Additionally, the measurements reveal a delayed peaks at ∼900 fs (BaF₂) and ∼300 fs (CaF₂). For comparison, we present time-resolved studies on electron emission from aluminum targets with pump and probe pulses below the damage threshold. The measurements show, again, the autocorrelation peak in the coherence region and an additional increase in the electron yield when the pulses are several picoseconds apart.The autocorrelation could also stand for the dephasing time of the electronic coherence, while the delayed peaks may reveal for the time needed for the collisional energy to be transferred to the lattice. The pump pulse induces a new unstable phase, which is further destabilized by the probe pulse.A corresponding qualitative picture for temporal dynamics of femtosecond (fs) laser-induced particle emission is proposed.     

Theoretical strength of 2D hexagonal crystals: application to bubble raft indentation

By means of lattice and molecular dynamics we study the theoretical strength of homogeneously strained, defect-free 2D crystals whose atoms interact via pair potentials with short- and longer-ranged interactions, respectively. We calculate the instability surface, i.e. the boundary in the 3D homogeneous strain space (ε _xx ,?ε _yy ,?ε _xy ), at which the first vanishing of the frequency of a vibrational mode occurs, taking into account all 2(N???1)?+?3 modes of a 2D periodic system of N atoms. We also compute the strain energies of the crystal on the instability surface, thus defining the most dangerous direction(s) of strain where the critical energy density is small. A theory is developed to incorporate the effect of loading device–sample interactions in the lattice instability criterion. The results are applied to the model problem of bubble raft indentation. We analyse the distribution of the unstable phonon modes in the first Brillouin zone as a function of the loading parameter, and discuss the post-critical behaviour of the lattice in the presence of strain gradients as in nano-indentation experiments.     

Strong decay to equilibrium in one-dimensional random spin systems

We consider a spin system on a lattice with finite-range, possibly unbounded random interactions. We show that for such systems the Glauber dynamics cannot decay to equilibrium exponentially fast inL ₂ even at high temperatures. Additionally, for one-dimensional systems with unbounded random couplings we prove that with probability one the corresponding Glauber dynamics has a fast (subexponential) decay to equilibrium in the uniform norm, provided that the distribution of random couplings satisfies some exponential bound.     

Analysis of the crystal lattice instability for cage–cluster systems using the superatom model

We have investigated the lattice dynamics for a number of rare-earth hexaborides based on the superatom model within which the boron octahedron is substituted by one superatom with a mass equal to the mass of six boron atoms. Phenomenological models have been constructed for the acoustic and lowenergy optical phonon modes in RB₆ (R = La, Gd, Tb, Dy) compounds. Using DyB₆ as an example, we have studied the anomalous softening of longitudinal acoustic phonons in several crystallographic directions, an effect that is also typical of GdB₆ and TbB₆. The softening of the acoustic branches is shown to be achieved through the introduction of negative interatomic force constants between rare-earth ions. We discuss the structural instability of hexaborides based on 4f elements, the role of valence instability in the lattice dynamics, and the influence of the number of f electrons on the degree of softening of phonon modes.     

Coupled-cavity passively Q-switched two-Stokes microchip laser

Experimental and theoretical studies of the coupled-cavity diode-pumped Nd:YAG/Cr:YAG microchip lasers with intracavity Raman conversion of laser pulses in a Ba(NO₃)₂ crystal into two Stokes pulses have been made. Two lasers with a different cavity length have been investigated. The minimal pulse durations at the 2nd Stokes wavelength were ??100 ps in the short-cavity laser at pulse energy of 5???J, and the pulse repetition rate reached 20?C24?kHz. The laser and Stokes pulse dynamics, as well as the spatial intensity distribution of the laser and the 1st Stokes beams at the output mirror have been recorded. A model describing such coupled-cavity microchip Raman lasers has been developed. The numerically simulated laser and Stokes pulse dynamics, and the calculated pulse energy, duration, and repetition rate are in good agreement with the experimental data.     

Effect of phonon spectrum heating on the formation of laser-induced electron plasma in wide-gap insulators

The effect of lattice heating by laser pulses on the dynamics of electron plasma generation in transparent solids has been theoretically studied. Several ways of taking into account the contribution of the phonon spectrum heating to the electron avalanche dynamics, depending on the type of the effective (with respect to the field energy transfer to electrons) phonons and laser pulse duration, have been proposed. A comparative analysis of the results of Monte Carlo computation of electron gas heating in the laser pulse field, which were obtained for cold and heated lattices, has been performed. It is shown that the consideration of the effect of lattice heating on the probabilities of electron-phonon and electron-phonon-photon scattering leads to an increase in the avalanche rate, which is more pronounced at longer wavelengths of the incident radiation and under longer laser pulses. Some qualitative features of the redistribution of the energy, absorbed during a pulse, between the electron plasma and lattice are revealed, which suggest initiation of irreversible microscopic changes in the insulator. In particular, the ratio R of the energy accumulated in the electron subsystem to the excess (with respect to the initial equilibrium state) energy in the phonon subsystem has been calculated for different initial lattice temperatures. It is shown that this ratio increases with a decrease in the laser wavelength in the computation scheme with lattice heating disregarded and decreases at all pulse durations when the lattice heating is taken into account.     

A priori theory of incommensurate behavior in Rb2ZnCl4

We have performed a study of the potential energy, normal modes, static relaxation, and molecular dynamics of Rb₂ZnCl₄ using ab initio Gordon-Kim interionic potentials for intermolecular and interionic potentials. We find that the Pnam–Pna2₁ transition in this, and almost certainly many isomorphous systems, is entropy driven and shows no soft mode behavior. This is shown to arise from the presence in this system of a large equipotential volume of phase space between the Pnam and the tripled Pna2₁ low temperature structure. This region arises from a major lattice instability involving large rotations and displacements and having approximately six-fold screw symmetry along the a axis. This concealed imperfect symmetry which we call latent symmetry is the basic cause of the existence of a near-tripled incommensurate phase over a range of 113 K (302 K–189 K) between the Pnam and Pna2₁ phases. In this region the helicity is incommensurate with the lattice, being largely determined by the relief of intrahelical stresses. In addition, we have demonstrated by molecular dynamics that the ZnCl₄ ^2- tetrahedra are orientationally disorderd, but, despite this, the helical instability remains. These findings are also related to anomalies in the observed Raman spectra and to X-ray data which confirm the presence of dynamically correlated disorder.     

Ultrafast structural dynamics of perovskite superlattices

Femtosecond x-ray diffraction provides direct insight into the ultrafast reversible lattice dynamics of materials with a perovskite structure. Superlattice (SL) structures consisting of a sequence of nanometer-thick layer pairs allow for optically inducing a tailored stress profile that drives the lattice motions and for limiting the influence of strain propagation on the observed dynamics. We demonstrate this concept in a series of diffraction experiments with femtosecond time resolution, giving detailed information on the ultrafast lattice dynamics of ferroelectric and ferromagnetic superlattices. Anharmonically coupled lattice motions in a SrRuO₃/PbZr_0.2Ti_0.8O₃ (SRO/PZT) SL lead to a switch-off of the electric polarizations on a time scale of the order of 1 ps. Ultrafast magnetostriction of photoexcited SRO layers is demonstrated in a SRO/SrTiO₃ (STO) SL.     

Table-top kHz hard X-ray source with ultrashort pulse duration for time-resolved X-ray diffraction

The interaction of ultrashort laser pulses with solid state targets is studied concerning the production of short X-ray pulses with photon energies up to about 10 keV. The influence of various parameters such as pulse energy, repetition rate of the laser system, focusing conditions, the application of prepulses, and the chirp of the laser pulses on the efficiency of this highly nonlinear process is examined. In order to increase the X-ray flux, the laser pulse energy is increased by a 2nd multipass amplifier from 750 μJ to 5 mJ. By applying up to 4 mJ of the pulse energy a X-ray flux of 4×10¹⁰ Fe K _α photons/s or 2.75×10¹⁰ Cu K _α photons/s are generated. The energy conversion efficiency is therefore calculated to η _Fe≈1.4×10⁻⁵ and η _Cu≈1.0×10⁻⁵. The X-ray source size is determined to 15×25 μm². By focusing the produced X-rays using a toroidally bent crystal a quasi-monochromatic X-ray point source with a diameter of 56 μm×70μm is produced containing ≈10⁴ Fe K _α1 photons/s which permits the investigation of lattice dynamics on a picosecond or even sub-picosecond time scale. The lattice movement of a GaAs(111) crystal is shown as a typical application.     

Extended modes and energy dynamics in two-dimensional lattices with correlated disorder

We study the nature of the vibrational modes in a two-dimensional harmonic lattice with long-range correlated random masses, with power-law spectral density S(k)∼1/k^α. We obtain numerically the scale invariance of the fluctuations of the relative participation number and the local density of states. We find signatures of extended vibrational modes when α>α_c and α_c depends on the magnitude of disorder. In order to confirm this claim, we also study the time evolution of an initially localized perturbation of the lattice. We show that the second moment of the spatial distribution of the energy displays a ballistic regime when α>α_c, in agreement with the occurrence of extended vibrational modes.     

Calculation of the lattice dynamical properties of Ge

The lattice dynamical properties of Ge are studied employing a frozen phonon approach within an ab initio density-functional pseudopotential formalism. Using the atomic number, atomic mass, and crystal structure as the only input information, we calculate phonon frequencies and mode Grüneisen parameters at Γ and X and the third-order anharmonic parameter for the zone center optical mode. The results are in excellent agreement with available experimental data. An analysis of various energy contributions to the TA (X) mode shows that the proper inclusion of the exchange-correlation energy is crucial for accurate microscopic studies of lattice dynamics.     

High-repetition-rate Nd:YVO4 slab laser with a 1-D top-hat output beam

A high-repetition-rate electro-optic Q-switched Nd:YVO₄ slab laser is demonstrated in this paper. The Nd:YVO₄ slab inside the compact resonator is end-pumped by a 2-bar laser diode stack. The output beam with one dimension (1-D) top-hat intensity distribution at both near field and far field is generated. Continuous wave (CW) output of 13 5 W is obtained under the total pump power of 50 W. At the repetition rate of 40 kHz, the energy per pulse is 0.32 mJ with its pulse width of 26.3 ns. At 20 kHz, we have achieved the maximum pulse energy of 0.56 mJ and 56 kW peak power with 10 ns pulse width.     

Electron-lattice interaction and the CDW state of 1T-TiSe2

The electronic band structure in the CDW state (superlattice structure) of 1T-TiSe₂ is calculated on the basis of the band-type Jahn-Teller model by extending our theory of lattice instability in the normal phase. A strong coupling between the hole-band (Se p states) around the Λ point and the electron-bands (Ti d states) around the Λ points is caused by the electron-lattice interaction. Reflecting such a strong coupling remarkable changes appear in the dispersion curves near the Fermi energy and the largest CDW gap is obtained to be 0.2 eV. We have also calculated a change of the density of states near the Fermi energy due to the superlattice formation. The result is consistent with that observed by angle-integrated photoemmision by Margaritondo et al. It is also shown that the magnitude of the lattice distortion observed at low temperatures can be explained in a way consistent with the lattice dynamics in the normal phase.     

Muon spin rotation in heavy-electron pauli-limit superconductors

The formalism for analyzing the magnetic field distribution in the vortex lattice of Pauli-limit heavy-electron superconductors is applied to the evaluation of the vortex lattice static linewidth relevant to the muon spin rotation (??SR) experiment. Based on the Ginzburg-Landau expansion for the superconductor free energy, we study the evolution with respect to the external field of the static linewidth both in the limit of independent vortices (low magnetic field) with a variational expression for the order parameter and in the near H _c2 ^P (T) regime with an extension of the Abrikosov analysis to Pauli-limit superconductors. We conclude that in the Ginzburg-Landau regime in the Pauli-limit, anomalous variations of the static linewidth with the applied field are predicted as a result of the superconductor spin response around a vortex core that dominates the usual charge-response screening supercurrents. We propose the effect as a benchmark for studying new puzzling vortex lattice properties recently observed in CeCoIn₅.     

Transferability of Slater–Koster parameters

In this work, we present a method of improving the transferability of the Slater–Koster Tight-Binding (SK-TB) parameters given in [Handbook of the Band Structure of Elemental Solids, Plenum Press, New York, 1986] to describe the electronic properties at other lattice constants and structures. First of all, we express the Hamiltonian and on-site atom parameters as a function of distance. We validate our method by calculating the electronic structure for various lattice constants for Nb and Mo (bcc) and for Cu and Au (fcc) and we find good agreement with the APW results. Furthermore, we transfer successfully the SK-TB parameters of the bcc to the fcc structure of Nb and Mo and vice versa for Cu and Au. Moreover, we apply a uniform shift V_o, which equates the sum of SK-TB eigenvalues to the APW total energy for the available volumes. We find that V_o presents a smooth volume dependence. Finally, using the volume dependence of V_o and the SK-TB theory we calculate the total energy for every lattice constant.     

Theoretical study of CuxAg1−xI alloys

We have performed first-principles calculations using full potential linearized augmented plane wave (FP-LAPW) method within density functional theory (DFT) to investigate the fundamental properties of Cu_xAg_1−xI alloys. We used both GGA96 [J.P. Perdew, K. Burke, M. Ernzerhof, Phys. Rev. Lett. 77 (1996) 3865.] and EVGGA [E. Engel, S.H. Vosko, Phys. Rev. B. 47 (1993) 13164.] generalized gradient approximations of the exchange-correlation energy that are based on the optimization of total energy and corresponding potential. Quantities such as lattice constants, bulk modulus, band gap, density of occupied states and effective mass were calculated as a function of copper molar fraction x. These parameters were found to depend non-linearly on alloy composition x, except the lattice parameter, which follows Vegard's law. The microscopic origins of the gap bowing were explained using the approach of Zunger and co-workers; we have concluded that the band-gap energy bowing was mainly caused by the chemical charge-transfer effect and the volume deformation , while the structural relaxation contribute to the gap bowing parameter at smaller magnitude. The calculated phase diagram shows a broad miscibility gap for this alloy with a high critical temperature.     

The <Emphasis Type="Italic">η</Emphasis>′ meson from lattice QCD

We study the flavour-singlet pseudoscalar mesons from first principles using lattice QCD. With N _f=2 flavours of light quarks, this is the so-called η ₂ meson and we discuss the phenomenological status of this meson. Using maximally twisted-mass lattice QCD, we extract the mass of the η ₂ meson at two values of the lattice spacing for lighter quarks than previously discussed in the literature. We are able to estimate the mass value in the limit of light quarks with their physical masses.     

A Wilson-Yukawa Model with undoubled chiral fermions in 2D

We consider the fermion mass spectrum in the strong coupling vortex phase (VXS) of a lattice fermion-scalar model with a global U(1)_L × U(1)_R, in two dimensions, in the context of a recently proposed two-cutoff lattice formulation. The fermion doublers are made massive by a strong Wilson-Yukawa coupling, but in contrast with the standard formulation of these type of models, in which the light fermion spectrum was found to be vector-like, we find massless fermions with chiral quantum numbers at finite lattice spacing. When the global symmetry is gauged, this model is expected to give rise to a lattice chiral gauge theory.     

Low-energy ion scattering by monatomic films

The angular and energy distributions of Cs⁺ and Xe⁺ ions scattered by monatomic crystalline films have been calculated via the molecular dynamics method in the scope of the multiparticle interaction mechanism. The calculated dependences of scattered heavy ions with a low initial energy E ₀ = 40 eV on the atomic mass, crystal lattice type, interatomic distance, and binding energy of the film atoms are discussed and compared with the experiment. The presented data can be used to predict the physical properties of a surface covered with a monatomic layer of foreign atoms during experimental surface studies based on the backscattering of ions with low initial energies.