Energy-gap dynamics of superconducting NbN thin films studied by time-resolved terahertz spectroscopy

Using time-domain terahertz spectroscopy we performed direct studies of the photoinduced suppression and recovery of the superconducting gap in a conventional BCS superconductor NbN. Both processes are found to be strongly temperature and excitation density dependent. The analysis of the data with the established phenomenological Rothwarf-Taylor model enabled us to determine the bare quasiparticle recombination rate, the Cooper pair-breaking rate and the electron-phonon coupling constant, λ=1.1±0.1, which is in excellent agreement with theoretical estimates.     

Surface plasmon dynamics in silver nanoparticles studied by femtosecond time-resolved photoemission

Multiphoton photoelectron spectroscopy reveals the multiple excitation of the surface plasmon in silver nanoparticles on graphite. Resonant excitation of the surface plasmon with 400 nm femtosecond radiation allows one to distinguish between photoemission from the nanoparticles and the substrate. Two different previously unobserved decay channels of the collective excitation have been identified, namely, decay into one or several single-particle excitations.     

Electron dynamics in supported metal nanoparticles: relaxation and charge transfer studied by time-resolved photoemission

Resonant excitation of the plasmon polariton in supported nanoparticles leads to a strong enhancement of the multiphoton photoemission yield and consequently, the total yield is dominated by the emission from the nanoparticles although they cover only a minor fraction of the surface. This allows investigation of the electron dynamics in supported nanoparticles, directly in the time domain. Here, Ag nanoparticles grown on graphite are used to demonstrate that the transient shape of the photoemission spectrum in time-resolved two-color multiphoton photoemission spectroscopy, reveals the electron relaxation within the nanoparticle, and the dynamic charge transfer between substrate and nanoparticle. The photoemission spectra map the transient electron energy distribution and exhibit a transient shift that is attributed to a dynamic charging of the nanoparticle. The comparison with model calculations comprising the full relaxation cascade in the nanoparticle and substrate, shows that the dynamic charge transfer accounts for almost half of the total deposited energy in the nanoparticle. PACS 78.67.Bf; 73.22.-f; 67.40.Fd; 78.47.+p     

Femtosecond electron and spin dynamics in Gd(0001) studied by time-resolved photoemission and magneto-optics

Femtosecond electron and spin dynamics of the Gd(0001) surface are investigated by time-resolved photoemission and second harmonic generation. Upon optical excitation the spin polarization of the surface state is reduced by half while its exchange splitting remains nearly unchanged. Electron-magnon interaction is proposed to facilitate electron-spin-flip scattering among spin-mixed surface and bulk states, which provides a mechanism for ultrafast demagnetization.     

Nonequilibrium magnetization dynamics of gadolinium studied by magnetic linear dichroism in time-resolved 4f core-level photoemission

The magnetic linear dichroism of the gadolinium 4f core level is studied in a time-resolved photoemission experiment employing laser pump- and synchrotron-radiation probe pulses. Upon optical excitation of the 5d6s valence electrons with femtosecond laser pulses, the magnetic order in the 4f spin system is reduced. Remarkably, the linear dichroism remains at 80% of the equilibrium contrast while the lattice temperature reaches the Curie temperature due to electron-phonon scattering. Contrasting itinerant ferromagnets, this shows that equilibration between the lattice and spin subsystems takes in Gd about 80 ps and is established in parallel with heat diffusion.     

Charge-carrier dynamics in polythiophene films studied by in-situ measurement of flash-photolysis time-resolved microwave conductivity (FP-TRMC) and transient optical spectroscopy (TOS)

An in-situ measurement system for flash-photolysis time-resolved microwave conductivity (FP-TRMC) and transient optical spectroscopy (TOS) has been developed to perform simultaneous measurements of photo-induced changes in conductivity and charge-carrier density in an organic thin film. The electric field in the resonant cavity designed for the present system was analysed by electrostatic simulation. Using the present system and the simulated electric field, the photoconductivity and transient absorption in a regioregular poly(3-hexyl thiophene) film were measured using one particular geometry under photon excitation energies of 6.39, 4.98, 3.48, and 2.34?eV. The dynamics of photogenerated charge carriers is discussed in terms of the excitation energy and incident photon intensity. The transient absorption spectrum induced by 3.48?eV light is presented and compared with the TRMC transient.     

Optical phonon dynamics of GaAs studied with time-resolved terahertz spectroscopy

We investigate the reflection near the reststrahlen band of the optical phonon in bulk GaAs in the time domain, using time-resolved terahertz spectroscopy. We find that the dynamics of the reflection measured for GaAs differs strongly from the reflection dynamics that would be expected for a TO phonon with a frequency-independent dephasing time.     

Partially wetting thin liquid films: structure and dynamics studied with coherent x rays

We studied the surface structure of thin liquid films vapor deposited on solid substrates in a partial wetting situation by means of coherent x-ray scattering. No dynamics has been observed showing the absence of capillary waves on liquid films partially wetting a substrate. Instead an exponential form of the height-height correlation function has been found pointing toward a solidlike behavior of the thin liquid films at large length scales. The exact surface structure and degree of replication with the substrate depend on the deposition rate of the molecules.     

Ultrafast structural dynamics studied by kilohertz time-resolved x-ray diffraction

Ultrashort multi-ke V x-ray pulses are generated by electron plasma produced by the irradiation of femtosecond pulses on metals. These sub-picosecond x-ray pulses have extended the field of x-ray spectroscopy into the femtosecond time domain. However, pulse-to-pulse instability and long data acquisition time restrict the application of ultrashort x-ray systems operating at low repetition rates. Here we report on the performance of a femtosecond laser plasma-induced hard x-ray source that operates at 1-k Hz repetition rate, and provides a flux of 2.0 × 1010 photons/s of Cu Kαradiation. Using this system for time-resolved x-ray diffraction experiments, we record in real time, the transient processes and structural changes induced by the interaction of 400-nm femtosecond pulse with the surface of a 200-nm thick Au(111) single crystal.     

Ultrafast dynamics of o-fluorophenol studied with femtosecond time-resolved photoelectron and photoion spectroscopy

The ultrafast dynamics of o-fluorophenol via the excited states has been studied by femtosecond time-resolved photoelectron imaging. The photoion and photoelectron spectra taken with a time delay between 267 nm pump laser and 800 nm probe laser provide a longer-lived S1 electronic state of about ns timescale. In comparison,the spectra obtained by exciting the S2 state with femtosecond laser pulses at 400 nm and ionizing with pulses at 800 nm suggest that the S2 state has an ultrashort lifetime about 102 fs and reflects the internal conversion dynamics of the S2 state to the S1 state.     

Lattice dynamics in two-photon-excited CdS studied by picosecond time-resolved X-ray diffraction

Lattice dynamics and radiative processes in single-crystal cadmium sulfide induced by two-photon excitation with a femtosecond laser are investigated. The development of lattice expansion is directly observed by picosecond time-resolved X-ray diffraction. The obtained lattice dynamics are explained on the basis of a thermally induced impulsive-strain model. The model calculation indicates that two- and more-photon absorption processes occur and that reflectivity rapidly increases under laser irradiation. In photoluminescence spectroscopy, the spectra for TW cm⁻² excitation are shifted to lower energy and show an additional shoulder at 2.35 eV. Furthermore, emission due to Fabry-Perot laser modes with self-formed cavities was observed under 11 TW cm⁻² excitation. The discrepancy between carrier densities deduced from the lattice expansion and the PL spectra indicates that the predominant process at a higher carrier density is not radiative recombination, but Auger recombination followed by lattice heating.     

Two-dimensional dynamics of metal nanoparticles on the surface of thin polymer films studied with coherent X rays

X-ray photon-correlation spectroscopy is used to measure the dynamic structure factor f(q,tau) of gold particles moving on the surface of thin polymer films. Above the glass transition of the polymer the peculiar form f(q,tau) approximately exp[-(Gamma tau)(alpha)] is found with 0.7 < alpha < 1.5, depending on sample age and temperature. The relaxation rates Gamma scale linearly with q, excluding a simple Brownian diffusive motion. This type of behavior, already observed in aging bulk soft matter systems, is explained by a power law distribution of particle velocities due to ballistic motion.     

Theory of dynamics of electron wave packets in time-resolved two-photon photoemission via image states

Time-resolved two-photon photoemission (TR2PPE) from the Cu(100) surface is investigated by the Keldysh Green function method in order to analyze ultrafast dynamics of an electron wave packet in the image states of the surface. By numerical analysis, the quantum beats in the TR2PPE spectrum due to interference among the image states are reproduced, and the motion of the electron wave packet in front of the surface is demonstrated. It is discussed on the basis of the obtained results as to how the motion of the electron wave packet is evaluated from the TR2PPE spectrum.     

Magnetic properties of thin epitaxial films investigated by spin-polarized photoemission

The surface sensitivity of the spin-polarized photoemission experiment was exploited to study two-dimensional magnetism. The magnetization of thin films of Fe, Co, and V in the monolayer (ML) range, grown on Cu(001) and Ag(001) single crystals, was measured as a function of perpendicularly applied field and temperature. Bcc Fe films and fcc Fe and Co films exhibit ferromagnetism down to the single monolayer range, while no evidence for ferromagnetism is found for V on Ag(001). All Co films are magnetized in plane and have a Curie temperature far above room temperature. A thickness dependence of the anisotropy and Curie temperature is observed for the two phases of Fe. Remanent magnetization perpendicular to the surface is found at 30 K for fcc Fe films thicker than 2 ML and for bcc Fe between 3 and 4 ML. The magnetic effects caused by coating and by interdiffusion are discussed in the light of measurements of Cu/Fe/Cu sandwiches and of overlayers obtained by simultaneous evaporation of Fe and Cu. The fcc Fe films are shown to be suitable for thermomagnetic writing.     

Quasi-molecular angle dependence of photoemission from thin films of polystyrene

Angle-resolved photoelectron spectra from thin films of randomly oriented polystyrene show a pronounced angular dependence of the emission for several peaks derived from benzene molecular orbitals in the valence band region. The analysis yields a clear molecular behaviour for the angular distribution of the uppermost π-band (1e_1g) which can be described by a β parameter of β = 0.6 for hν = 31 eV. These results support, for polystyrene, the notion of weak intermolecular interaction in a randomly oriented “condensed gas”.     

Magnetization dynamics in thin films and multilayers

The behavior of spin waves is influenced by essentially all the parameters which characterize a magnetic material – exchange interactions, anisotropy, surface effects, dipolar interactions, phase transitions and imperfections. Thus measurements of spin wave frequencies can give important information on characterizing different magnetic materials and structures. In this paper we outline the major results and calculational methods for long-wavelength spin waves in thin films and multilayers. While the primary attention is on ferromagnet-based structures, long-wavelength spin waves in antiferromagnets are also discussed. We indicate how particular measurements of spin wave frequencies can be used to extract the fundamental parameters of the different structures.     

Internal photoemission and plasmon gain in solid and thin films of Al

Weak features in the electron spectrum of Al excited by bremsstrahlung radiation from a Cu anode have been studied using a recently developed multidetector. A feature at ～1410 eV which has been identified as the Al 2p internal photoelectron line was found to have an intensity 4.2 × 10^?3 times that of the Al KL_2,3L_2,3:¹D₂ Auger line, in agreement with a simple theoretical treatment. The identification of this feature is confirmed by the observation of an ～67% decrease in its intensity in spectra obtained from clean Al films in the thickness range 3.1–34.0 nm. The intensity of a plasmon gain peak at ～1404 eV is found to be independent of thickness for films of thickness greater than 7.5 nm.