Femtosecond energy relaxation in suspended graphene: phonon-assisted spreading of quasiparticle distribution

Ultra-fast optical measurements of few-layer suspended graphene films grown by chemical vapor deposition were performed with femtosecond pump–probe spectroscopy. The relaxation processes were monitored in transient differential transmission (ΔT/T) after excitation at two different wavelengths of 350 and 680 nm. Intraband electron–electron scattering, electron–phonon scattering, interband Auger recombination and impact ionization were considered to contribute to ΔT/T. All these processes may play important roles in spreading the quasiparticle distribution in time scales up to 100 fs. Optical phonon emission and absorption by highly excited non-equilibrium electrons were identified from ΔT/T peaks in the wide spectral range. When the probe energy region was far from the pump energy, the energy dependence of the quasiparticle decay rate was found to be linear. Longer lifetimes were observed when the quasiparticle population was localized due to optical phonon emission or absorption.     

Ultrafast dynamics of surface electromagnetic waves in nanohole array on metallic film

We study the ultrafast dynamics of surface electromagnetic waves photogenerated on aluminum film perforated with subwavelength holes array by means of transient photomodulation with ∼100 fs time resolution. We observed a pronounced blueshift of the resonant transmission band that reveals the important role of plasma attenuation in the dynamics and that is inconsistent with plasmon–polariton mechanism of extraordinary transmission. The transient photomodulation spectra were successfully modeled within the Boltzmann equation approach for the electron–phonon relaxation dynamics, involving non-equilibrium hot electrons and quasi-equilibrium phonons.     

Morphology dependent ultrafast electron dynamics in ultrathin gold films

Ultrafast electron dynamics in 5 nm thick gold films have been investigated as a function of film morphology. The transient reflectivity data reveal a sub-100 fs rise time and a complex relaxation profile on the picosecond timescale. These data are discussed in terms of a modified two-temperature model of the electron dynamics accounting for the initial relaxation of the non-thermal population. The electron–phonon coupling may be sensitive to film morphology. The possible origin of this behaviour is discussed and results are placed in the context of enhanced photochemistry on thin metal films.     

The kinetics of low-temperature electron-phonon relaxation in a metallic film following instantaneous heating of the electrons

The theoretical analysis of experiments on pulsed laser irradiation of metallic films sputtered on insulating supports is usually based on semiphenomenological dynamical equations for the electron and phonon temperatures, an approach that ignores the nonuniformity and the nonthermal nature of the phonon distribution function. In this paper we discuss a microscopic model that describes the dynamics of the electron-phonon system in terms of kinetic equations for the electron and phonon distribution functions. Such a model provides a microscopic picture of the nonlinear energy relaxation of the electron-phonon system of a rapidly heated film. We find that in a relatively thick film the energy relaxation of electrons consists of three stages: the emission of nonequilibrium phonons by “hot” electrons, the thermalization of electrons and phonons due to phonon reabsorption, and finally the cooling of the thermalized electron-phonon system as a result of phonon exchange between film and substrate. In thin films, where there is no reabsorption of nonequilibrium phonons, the energy relaxation consists of only one stage, the first. The relaxation dynamics of an experimentally observable quantity, the phonon contribution to the electrical conductivity of the cooling film, is directly related to the dynamics of the electron temperature, which makes it possible to use the data of experiments on the relaxation of voltage across films to establish the electron-phonon and phonon-electron collision times and the average time of phonon escape from film to substrate. Zh. éksp. Teor. Fiz. 111, 2106–2133 (June 1997)     

Nonlinear optical absorption in Bi3TiNbO9 thin films using Z-scan?technique

Bi₃TiNbO₉ (BTN) thin films with layered perovskite structure were fabricated on fused silica by pulsed laser deposition. The XRD pattern revealed that the films are single-phase perovskite and highly (00l) textured. Their fundamental optical constants, such as band gap, linear refractive index, and linear absorption coefficient, were obtained by optical transmittance measurements. The dispersion relation of the refractive index vs. wavelength follows the single electronic oscillator model. The nonlinear optical absorption of the films was investigated by single beam Z-scan method at a wavelength of 800 nm with laser duration of 80 fs. We obtained the nonlinear absorption coefficient β=1.44×10⁻⁷ m/W. The results show that the BTN thin films are promising for applications in absorbing-type optical devices.     

Phonon heat transport in gallium arsenide

The lifetimes of quantum excitations are directly related to the electron and phonon energy linewidths of a particular scattering event. Using the versatile double time thermodynamic Green’s function approach based on many-body theory, an ab-initio formulation of relaxation times of various contributing processes has been investigated with newer understanding in terms of the linewidths of electrons and phonons. The energy linewidth is found to be an extremely sensitive quantity in the transport phenomena of crystalline solids as a collection of large number of scattering processes, namely, boundary scattering, impurity scattering, multiphonon scattering, interference scattering, electron–phonon processes and resonance scattering. The lattice thermal conductivities of three samples of GaAs have been analysed on the basis of modified Callaway model and a fairly good agreement between theory and experimental observations has been reported.     

Highly oriented La2/3Ca1/3MnO3 films grown on silicon-on-insulator substrates by pulsed laser deposition

High quality La_2/3Ca_1/3MnO₄(LCMO) thin films have been deposited on silicon-on-insulator (SOI) substrates only buffered by yt tria-stabilized zirconia (YSZ) by using the pulsed laser deposition (PLD) technique. The results obtained from X-ray diffraction (XRD), reflection high energy electron diffraction (RHEED), scanning electron microscopy (SEM) and magnetization investigations indicate that the LCMO films are highly oriented both in-plane and out-of-plane. The Curie temperature T _c is close to 260 K and the insulator–metal (I–M) transition appears around 220 K. The conducting mechanism at low temperatures is dominated by the electron–magnon scattering. A tensile stress from the film–substrate lattice mismatch results in magnetic ‘easy axes’ in the film plane and the magnetic anisotropy energy increases with cooling. A maximum magnetoresistance (MR) is observed near 190 K, with the external magnetic field either parallel or vertical to the LCMO film plane. Moreover, the large intrinsic high-field magnetoresistance (HFMR) and the very small extrinsic low-field magnetoresistance (LFMR) again reveal that the LCMO films on SOI substrates are highly oriented thin films of good crystallinity.     

Intervalley scattering in GaAs: ab initio calculation of the effective parameters for Monte Carlo simulations

Interactions between excited electrons and short-wavelength (intervalley) phonons in GaAs are studied using density functional theory for the conduction bands, and density functional perturbation theory for phonon frequencies and matrix elements of the electron–phonon interaction. We have calculated the deformation potentials (DPs) and the average intervalley scattering time 〈τ〉. The integration of the scattering probabilities over all possible final states in the Brillouin zone has been performed without any ad hoc assumption about the behavior of the electron–phonon matrix elements nor the topology of the conduction band. For transitions from the L point to Γ valley (within the first conduction band), we find 〈τ〉_L to be 1.5 ps at 300 K, in good agreement with time-resolved photoluminescence experiment. We discuss the difference between our calculated DPs, and effective parameters used in Monte Carlo simulations of optical and transport properties of semiconductors. The latter are based on Conwell’s model, in which electron–phonon interaction is described by one single constant and a parabolic model is used for conduction bands. We deduce the effective DP from our 〈τ〉, and compare it to our calculated DPs. We conclude that only effective DPs obtained from a full calculation of 〈τ〉 are relevant parameters for Monte Carlo simulations. PACS 71.10-w; 72.10.Di; 71.55.Eq     

Optical properties and ultrafast electron dynamics in gold–silver alloy and core–shell nanoparticles

Silver and gold are the two most popular metals used for many nanoparticle applications, such as surface enhanced Raman scattering or surface enhanced fluorescence, in which the local field enhancement associated with the excitation of the localized surface-plasmon–polariton resonance (SPR) is exploited. Therefore, tunability of the SPR over a wide energy range is required. For this purpose we have investigated core–shell nanoparticles composed of gold and silver with different shell thicknesses as well as the impact of alloying on these nanoparticles due to a tempering process. The nanoparticles were prepared by subsequent deposition of Au and Ag atoms or vice versa on quartz substrates followed by diffusion and nucleation. Their linear extinction spectra were measured as a function of shell thickness and annealing temperature. It turned out that different gold shell thicknesses on silver cores allow a tuning of the SPR position from 2.79 to 2.05 eV, but interestingly without a significant change on the extinction amplitude. Heating of core–shell nanoparticles up to only 540 K leads to the formation of alloy nanoparticles, accompanied by a back shift of the SPR to 2.60 eV. Calculations performed in quasi-static approximation describe the experimental results quite well and prove the structural assignments of the samples. In additional experiments, we applied the well-established persistent spectral hole burning technique to the alloy nanoparticles in order to determine the ultrafast dephasing time T ₂. We obtained a dephasing time of T ₂=(8.1±1.6) fs, in good agreement with the dephasing time of T _2,∞=8.9 fs, which is already included in the dielectric function of the bulk.     

Charge-carrier dynamics in single-wall carbon nanotube bundles: a time-domain study

We present a real-time investigation of ultra-fast carrier dynamics in single-wall carbon nanotube bundles using femtosecond time-resolved photoelectron spectroscopy. The experiments allow us to study the processes governing the sub-picosecond and the picosecond dynamics of non-equilibrium charge carriers. On the sub-picosecond time scale the dynamics are dominated by ultra-fast electron–electron scattering processes, which lead to internal thermalization of the laser-excited electron gas. We find that quasiparticle lifetimes decrease strongly as a function of their energy up to 2.38 eV above the Fermi level – the highest energy studied experimentally. The subsequent cooling of the laser-heated electron gas to the lattice temperature by electron–phonon interaction occurs on the picosecond time scale and allows us to determine the electron–phonon mass-enhancement parameter λ. The latter is found to be over an order of magnitude smaller if compared, for example, with that of a good conductor such as copper. Received: 4 March 2002 / Accepted: 7 March 2002 / Published online: 3 June 2002     

Ultra-fast dynamics of coherent lattice and spin excitations at the Gd(0001) surface

The Gd(0001) surface is investigated by pump–probe experiments using femtosecond laser pulses at 740–860 nm wavelength. Employing optical second-harmonic generation, spin and lattice dynamics are separated through the symmetry of optical field contributions that are even and odd with respect to magnetization reversal. A coherent phonon–magnon mode at a frequency of 3 THz that is excited through the exchange-split surface state is observed in the time domain. A magneto-elastic phonon–magnon interaction based on spin–orbit coupling is weak for Gd and a modulation of the exchange interaction mediated by the lattice vibration is proposed as a microscopic interaction mechanism of this coupled mode. In parallel, electron–electron and electron–phonon interactions and their magnetic counterparts lead to incoherent dynamics of the electron, lattice, and spin subsystems. Variation of the optical wavelength shows that for longer wavelengths up to 860 nm the coherent mode dominates, while for shorter ones (≥740 nm) incoherent contributions prevail. This dependence indicates that selective depopulation of the occupied surface state component drives the coherent excitation. However, temperature-dependent studies show that the oscillation amplitude of even and odd contributions scales with the spin polarization of the surface state, suggesting that the spin dependence of the ion potentials contributes as well. Furthermore, the frequency of the coherent mode presents a blue shift with a delay of 0.17 THz/ps that saturates at the static frequency of the respective bulk phonon. This behavior is a consequence of equilibration of the screened ion potential at the surface subsequent to the intense laser excitation. PACS 78.47.+p; 63.22.+m; 63.20.Ls; 75.30.Ds     

Preparation and optical properties of sol–gel neodymium-doped germania/γ-glycidoxypropyltrimethoxysilane organic–inorganic hybrid thin films

Germania/γ-glycidoxypropyltrimethoxysilane organic–inorganic hybrid spin-coating thin films doped with neodymium ions are prepared by a sol–gel technique and a spin-coating process. Acid-catalyzed solutions of γ-glycidoxypropyltrimethoxysilane mixed with germanium isopropoxide are used as matrix precursors. Thermal gravimetric analysis, UV–visible spectroscopy, and Fourier transform infrared spectroscopy are used to study the structural and optical properties of the hybrid thin films. The results indicate that films that are crack-free and have a high transparency in the visible and near-infrared range can be obtained; a strong UV absorption region at short wavelength ∼200 nm, accompanied with a shoulder peaked at ∼240 nm, due to the neutral oxygen monovacancy defects, is also identified. Upconversion emission properties of the transparent dried gel and the thin films heated at different heat treatment temperatures and doped with different neodymium ion concentrations are studied; a relatively strong room-temperature yellow to violet upconversion emission at 397 nm (⁴ D _3/2→⁴ I _13/2) is observed under a xenon lamp excitation with yellow light at the wavelength of 580 nm (⁴ I _9/2→⁴ G _5/2). The effect of Nd³⁺ doping concentration and heat treatment temperature on upconversion emission of the thin films is also studied. The mechanism of the upconversion is proposed. PACS 81.05.Kf; 81.20.Fw; 78.55.Hx     

Comparative Analysis of Temperature-dependent .Raman Spectra of GaN and GaN/Mg Films

The Raman spectra of unintentionally doped gallium nitride (GaN) and Mg-doped GaN films were investigated and compared at room temperature and low temperature. The differences of E₂ and A₁(LO) mode in two samples are discussed. Stress relaxation is observed in Mg-doped GaN, and it is suggested that Mg-induced misfit dislocation and electron–phonon interaction are the possible origins. A peak at 247 cm⁻¹ is observed in both the Raman spectra of GaN and Mg-doped GaN. Temperature-dependent Raman scattering experiment of Mg-doped GaN shows the frequency and intensity changes of this peak with temperature. This peak is attributed to the defect-induced vibrational mode. Translated from Chinese Journal of Semiconductors, 2005, 26(4) (in Chinese)     

Laser drilling of high aspect ratio holes in copper with femtosecond,picosecond and nanosecond pulses

Deep laser holes were drilled in copper sheets using various pulse lengths and environments. By recording the intensity on a photodiode placed under the sample while drilling the holes, we obtained the number of pulses to drill through the sheet as a function of pulse length and energy. The entrance diameter of the holes was successfully predicted using a Gaussian approximation and a material removal fluence threshold of 0.39 J/cm² for a pulse length of 150 fs. From cross sections of the holes, the morphology of the inside walls was observed and shows an increase in the amount of molten material with pulse length. A transition pulse length is defined as the point at which the laser affected material goes from being mainly vaporized to mainly melted. This transition occurs near ∼10 ps, which corresponds approximately to the electron–phonon relaxation time for copper. PACS 62.20.Mk; 62.25.+g; 79.20.Ds     

Surface plasmon resonance response of Au–WO3?x composite films

Surface plasmon resonance of metal–dielectric composite thin films formed by noble metal nanoparticles embedded in a dielectric matrix offers a high degree of flexibility and enables many applications such as surface enhanced spectroscopes, and biological and chemical sensing. In this article, Au–WO_3−x composite films of various Au contents and thicknesses were prepared by the pulsed laser deposition technique, and their SPR responses were measured in the Kreschmann geometry, using a polarized light beam at 640 nm wavelength. Theoretical calculation of SPR responses based on the Bruggeman or Maxwell–Garnett model with the MacLeod general characteristic matrix method is in obvious discrepancy with experimental measurements but it is able to predict the trend in term of the dependence of SPR responses on Au content and thickness of the Au–WO_3−x films. The SPR responses of the Au–WO_3−x films when exposed to NO gas molecules were measured and the preliminary results indicated that gas sensing using the SPR responses of metal–dielectric composite films is feasible.     

Phase transformation of nanostructured titanium dioxide thin films grown by sol–gel method

Nanostructured TiO₂ thin films were deposited on quartz glass at room temperature by sol–gel dip coating method. The effects of annealing temperature between 200^∘C to 1100^∘C were investigated on the structural, morphological, and optical properties of these films. The X-ray diffraction results showed that nanostructured TiO₂ thin film annealed at between 200^∘C to 600^∘C was amorphous transformed into the anatase phase at 700^∘C, and further into rutile phase at 1000^∘C. The crystallite size of TiO₂ thin films was increased with increasing annealing temperature. From atomic force microscopy images it was confirmed that the microstructure of annealed thin films changed from column to nubbly. Besides, surface roughness of the thin films increases from 1.82 to 5.20 nm, and at the same time, average grain size as well grows up from about 39 to 313 nm with increase of the annealing temperature. The transmittance of the thin films annealed at 1000 and 1100^∘C was reduced significantly in the wavelength range of about 300–700 nm due to the change of crystallite phase. Refractive index and optical high dielectric constant of the n-TiO₂ thin films were increased with increasing annealing temperature, and the film thickness and the optical band gap of nanostructured TiO₂ thin films were decreased.     

The study of optical characteristic of ZnSe nanocrystal

Nanocrystal ZnSe material was prepared in a triethylamine solvent using the modified solvothermal method in which potassium borohydride, a reducing reagent, is employed. Compared with the bulk ZnSe, the steady absorption edge and photoluminescence peak of nanocrystal ZnSe shift toward high energy. With the decrease of nanoparticle size, the probability of inelastic collision between electron and nanoparticle surface increases, which results in the enhancement of the intensity of electron–phonon coupling and the decrease of electron–phonon scattering time. In the lower temperature range (13–100 K), the transition probability between singlet state and triple state rapidly increases with the increase in temperature. With the further increase in temperature (100–292 K), the radiative recombination between singlet state and ground state is dominant. The competitive non-radiative recombination between singlet state and triple state is suppressed, therefore, the radiation decay time of singlet state changes slightly. PACS 78.55.Et; 73.61.Tm; 78.47.+p; 78.90.+t     

Precise determination of?optical properties of?pentacene thin films grown on various substrates: Gauss–Lorentz model with effective medium approach

Spectroscopic ellipsometry measurements are performed on thin pentacene films grown on glass, SiO₂, and n-Si substrates. The Gauss–Lorentz oscillator model is shown to be effective in modeling the π–π ^∗ transitions found in organic compounds. The effective medium approximation that considers the surface roughness of the films, which can be significant in case of pentacene, is also shown to be a key factor in precisely determining their dielectric functions. The proposed method reveals that there are some quantitative differences in the optical properties of the pentacene films prepared on different substrates.