Gigahertz-repetition-rate, narrowband-deep-ultraviolet light source for minimization of acquisition time in high-resolution angle-resolved photoemission spectroscopy.

Ultrahigh-repetition-rate (1.1 GHz), deep-ultraviolet coherent light at 208.8 nm is generated by applying an external Fabry-Pérot cavity for repetition-rate multiplication to the fourth harmonics of a 10-ps, mode-locked Ti:sapphire laser. Its small pulse energy minimizes the unwanted space charge effect, while its high repetition rate drastically reduces the acquisition time in high-energy resolution angle-resolved photoemission spectroscopy using hemispherical electron analyzers. The absence of the space charge effect in the photoemission spectrum near the Fermi edge of polycrystalline Au at 8 K demonstrates this idea.

Ring and unimodal angular-frequency distribution of THz emission from two-color femtosecond plasma spark.

We study angular and frequency-angular distributions of the terahertz (THz) emission of the low-frequency region (0.3-3 THz) from a two-color femtosecond plasma spark experimentally and in three-dimensional numerical simulations. We investigate the dependence of the angular shapes of the THz radiation on focusing conditions and pulse durations by using two laser facilities (pulse durations 35 and 150 fs) for different focusing geometries. Our experiments and simulations show that decrease in the numerical aperture from NA ≈0.2 to NA ≈0.02 results simultaneously in (I) squeezing of the THz angular distribution and (II) formation of the bright conical emission in the THz range. The moderate focusing NA ≈0.05, which forms the relatively narrow unimodal THz angular distribution, is identified as optimal in terms of angular divergence. Numerical simulations with carrier wave resolved show that bright THz ring structures appear at the frequencies ≥2 THz for longer focuses (NA ≈0.02), while for optimal focusing conditions NA ≈0.05 the conical emission develops at THz frequencies higher than 10 THz.

Observation of excitonic N-body bound states: polyexcitons in diamond.

We have found a series of resonances associated with the bound state (polyexcitons, PE(N)s) of N excitons up to N=6 in the emission spectra of diamond under two-photon excitation at around 10 K. Time-resolved spectra show a stepwise formation of PE(N)s with smaller to larger N, as well as a successive decay from larger to smaller N. At higher excitation levels, the transformation of PE(N)s into a condensed phase of electron-hole droplets occurs. The binding energies of the PE(N)s, normalized to the exciton Rydberg energy, agree well with those of silicon, suggesting the universality of the phenomena.

High-power, narrow-band, high-repetition-rate, 5.9 eV coherent light source using passive optical cavity for laser-based angle-resolved photoelectron spectroscopy.

We demonstrate a scheme for efficient generation of a 5.9 eV coherent light source with an average power of 23 mW, 0.34 meV linewidth, and 73 MHz repetition rate from a Ti: sapphire picosecond mode-locked laser with an output power of 1 W. Second-harmonic light is generated in a passive optical cavity by a BiB(3)O(6) crystal with a conversion efficiency as high as 67%. By focusing the second-harmonic light transmitted from the cavity into a ß-BaB(2)O(4) crystal, we obtain fourth-harmonic light at 5.9 eV. This light source offers stable operation for at least a week. We discuss the suitability of the laser light source for high-resolution angle-resolved photoelectron spectroscopy by comparing it with other sources (synchrotron radiation facilities and gas discharge lamp).

Control of magnetic dipole terahertz radiation by cavity-based phase modulation.

Although it is well accepted that the ultrafast manipulation of spins or magnetization in solid promises potential applications in coherent terahertz (THz) radiation source, spintronics and quantum information processing, their performance is significantly limited by the weak coupling between radiation field and magnetic dipole oscillation. For such 'weak' magnetic system, we propose an effective and simple route based on the cavity-based phase modulation technique towards the efficient energy extraction, demonstrated via controlling the magnetic dipole THz radiation generated in the nonlinear Raman process from antiferromagnetic (AFM) NiO. An asymmetric coupled Fabry-Pérot (FP) cavity is constituted by simply placing a metallic planar mirror in the vicinity of a NiO slab. The energy-extraction (THz radiation) can be effectively manipulated by changing the NiO-mirror distance to modulate the phase relation between the magnetic wave and the induced magnetization in NiO. The distinct radiation control can be observed and the experiments are well explained by numerically analyzing the radiation dynamics that highlights the role of phase modulation during the radiation process.

Effect of surface plasmon resonance on the optical activity of chiral metal nanogratings.

We examine the mechanism responsible for the optical activity of a two-dimensional array of gold nanostructures with no mirror symmetry on a dielectric substrate. Measurements with different incident angles, polarizations and sample orientations allow us to reveal that observed polarization effect is enhanced by surface plasmon resonance. By performing numerical simulation with rigorous diffraction theory we also show that the grating chirality can be described in terms of the non-coplanarity of the electric field vectors at the front (air-metal) and back (substrate-metal) sides of the grating layer.

Terahertz wave polarization rotation with double layered metal grating of complimentary chiral patterns.

We propose and demonstrate polarization rotation of a terahertz (THz) electromagnetic wave by using two-dimensional gratings consisting of two displaced layers of gold film with complimentary chiral patterns with four-fold symmetry. We develop a time domain THz polarimetry method with three wire grid polarizers and distinguish optical activity from optical anisotropy. We obtain the isotropic polarization rotation of a terahertz wave free from the birefringence of the structures. Results indicate the possibility of controlling THz polarization with artificial chiral structures fabricated with thin metal films.

Study of orthoexciton-to-paraexciton conversion in Cu(2)O by excitonic Lyman spectroscopy.

Using time-resolved 1s-2p excitonic Lyman spectroscopy, we study the orthoexciton-to-paraexciton transfer, following the creation of a high density population of ultracold 1s orthoexcitons by resonant two-photon excitation with femtosecond pulses. An observed fast exciton-density dependent conversion rate is attributed to spin exchange between pairs of orthoexcitons. Implication of these results on the feasibility of Bose-Einstein condensation of paraexcitons in Cu(2)O is discussed.

Efficient two-photon light amplification by a coherent biexciton wave.

A reversible coupling between photon pair states and a long-lived, highly coherent biexciton wave in CuCl allows efficient phase-sensitive two-photon amplification or attenuation of ultrashort light pulses. We demonstrate a gain of 350 cm(-1) for a pump intensity of 1 MW/cm(2), nearly 2 orders of magnitude higher than that achievable with conventional parametric crystal amplifiers. We develop a theoretical model that describes this new type of parametric converter where the light pump is replaced by a coherent biexciton wave and show that it is well suited for the generation of entangled photons and the squeezing of an optical beam with ultrafast time gating.

Electron-hole droplet formation in direct-gap semiconductors observed by mid-infrared pump-probe spectroscopy.

Mid-infrared pump-probe measurements with subpicosecond time resolution reveal the existence of a metastable condensed phase of the electron-hole ensemble in a direct-gap semiconductor CuCl. High-density electrons and holes are directly created in a low-temperature state by the resonant femtosecond excitation of excitons above the Mott transition density. Strong metallic reflection with a plasma frequency Planck's over 2pi(omega)p approximately 0.5 eV builds up within 0.3 ps. Within a few picoseconds, the mid-infrared reflection spectrum is transformed from metalliclike into colloidlike. The observed resonance feature at Planck's over 2pi(omega)p/sqrt[3] allows us to obtain the carrier density in the metastable electron-hole droplets of 2x10(20) cm(-3).

Ultrafast optical nonlinearity in the quasi-one-dimensional mott insulator Sr2CuO3

We report strong instantaneous photoinduced absorption in the quasi-one-dimensional Mott insulator Sr2CuO3 in the IR spectral region. The observed photoinduced absorption is to an even-parity two-photon state that occurs immediately above the absorption edge. Theoretical calculation based on a two-band extended Hubbard model explains the experimental features and indicates that the strong two-photon absorption is due to a very large dipole coupling between nearly degenerate one- and two-photon states. Room temperature picosecond recovery of the optical transparency suggests the strong potential of Sr2CuO3 for all-optical switching.

Ultrafast spin dynamics and critical behavior in half-metallic ferromagnet: Sr2FeMoO6

Ultrafast spin dynamics in ferromagnetic half-metallic compound Sr2FeMoO6 is investigated by pump-probe measurements of the magneto-optical Kerr effect. The half-metallic nature of this material gives rise to anomalous thermal insulation between spins and electrons and allows us to pursue the spin dynamics from a few to several hundred picoseconds after the optical excitation. The optically detected magnetization dynamics clearly shows the crossover from microscopic photoinduced demagnetization to macroscopic critical behavior with universal power law divergence of relaxation time for a wide dynamical critical region.

Spherical cavity-mode laser with self-organized CuCl microspheres.

We report lasing of exciton-polaritons in semiconductor microspheres with spherical cavity modes under subpicosecond ultraviolet laser excitation at low temperature. Small bulk crystals of CuCl are melted and formed into fused microspheres with diameters ranging from a few to several tens of micrometers. The threshold for lasing is 1nJ/pulse, which corresponds to 10(9) photons/pulse. We found that the biexciton-to-longitudinal-exciton transition is responsible for the lasing.

Polarization dependent quantum beats of homogeneously broadened excitons.

The polarization dependence of quantum beats from the A-exciton and the B-exciton in a GaN sample of exceptional quality is studied with four-wave mixing experiments. When changing the incident polarizations from collinear to crossed linear, a pi-phase shift of the beats is observed while the decay rate remains unchanged. This confirms previous theoretical predictions.

Polymer microdisk and microring lasers.

Dye-doped polymer microlasers have been fabricated by photolithography and self-assembly. Microdisk lasers 5 to 30 microm in diameter were photolithographically patterned on thin planar polymer waveguides. We formed polymer microring lasers on thinned silica fibers by dipping the fibers in polymers and allowing the polymer droplets to cure.