Phase-matched nonlinear wave-mixing processes in XUV region with multicolor lasers.

We report here experimental results of perturbative nonlinear optical wave-mixing processes in the extreme ultraviolet region by using two-color and three-color laser fields. Besides the usual odd-harmonic spectrum of high harmonic generation, new spectral components are observed when multiple incommensurate lasers (one driving plus one or two control field) interact with neutral krypton gas. To demonstrate the wave-mixing process underlying such an observation, we first couple the driving field with either the signal or the idler field of an optical parametric amplifier in the gaseous ensemble to generate certain mixing frequencies. The two control fields are then simultaneously combined with the driving field to produce broad and distinguishable mixing peaks that clearly reveal the contribution of each control laser. Finally, the variation of the intensity of the mixing waves with the intensity of each control field, the gas density, and the relative focus position is examined for signatures of phase-matched generation of the mixing fields in this spectral region.

Cascaded four-wave mixing in the XUV region.

We present a detailed study of the wave-mixing process in the extreme ultraviolet (XUV) region (around 30 nm) by using two collinear multiple-cycle laser pulses with incommensurate frequencies (wavelengths 1400 and 800 nm). The experimental data provide evidence for the coherent accumulation of wave-mixing fields and a high third-order response of the medium in this spectral range. We show that the time evolution of the mixing fields can be used to study the coherence dynamics of the free-electron wave packet with a lifetime of 200-750 fs.

Coherent diffractive imaging microscope with a high-order harmonic source.

We report the generation of highly coherent extreme ultraviolet sources with wavelengths around 30 and 10 nm by phase-matched high-order harmonic generation (HHG) in a gas cell filled with argon and helium, respectively. We then perform coherent diffractive imaging (CDI) by using a focused narrow-bandwidth HHG source with wavelength around 30 nm as an illumination beam for two kinds of samples. The first is a transmission sample and the second is a absorption sample. In addition, we report the successful reconstruction of a complex absorption sample using a tabletop high-harmonic source. This will open the path to the realization of a compact soft x-ray microscope to investigate biological samples such as membrane proteins.

Phase-matched generation of highly coherent radiation in water window region.

Highly coherent extreme ultraviolet radiation around the water window region (~4.4 nm) is generated in a semi-infinitive helium gas cell using infrared pulses of wavelength 1300 nm, energy 2.5 mJ, duration 40 fs, and repetition rate 1 kHz. The pressure-squared dependence of the intensity and the almost-perfect Gaussian profile and low divergence of the high harmonic source indicate a phase-matched generation process. The spatial coherence of the source is studied using Young's double-slit measurements.

Ultrafast transient grating spectroscopy in silicon quantum dots.

Transient grating spectroscopy detects directly the relaxation of the excited carriers rather than time-resolved photoluminescence and thus it is particularly desired for the indirect semiconductors such as silicon quantum dots. We investigate ultrafast carrier dynamics in silicon quantum dots embedded in silicon oxide matrix using femtosecond transient grating spectroscopy. Two ultrafast decay components are observed with decay time of 800 fs and 4 ps at various detection wavelengths, which are attributed to the transverse optical and transverse acoustic phonon assisted relaxation. Photoexcited electrons and holes are effectively trapped into the localized states on the surface of the silicon quantum dots where electrons and holes have a slow recombination in the time scale of microseconds.

Coherent and collimated blue light generated by four-wave mixing in Rb vapour.

We investigate frequency up-conversion of low power cw resonant radiation in Rb vapour as a function of various experimental parameters. We present evidence that the process of four wave mixing is responsible for unidirectional blue light generation and that the phase matching conditions along a light-induced waveguide determine the direction and divergence of the blue light. Velocity-selective excitation to the 5D level via step-wise and two-photon processes results in a Doppler-free dependence on the frequency detuning of the applied laser fields from the respective dipole-allowed transitions. Possible schemes for ultraviolet generation are discussed.

Steep atomic dispersion induced by velocity-selective optical pumping.

We demonstrate a method of preparation of broadband sign-reversible dispersion in alkali vapour based on velocity-selective optical pumping. The refractive index in Rb vapour has been measured using a heterodyne method. The magnitudes of the normal and anomalous dispersion, which are almost constant over a spectral region of approximately 40 MHz, can lead to a reduced (V(g) approximately c/230) or negative (V(g) approximately -c/27) group velocity of light.

Spectrally resolved femtosecond two-color three-pulse photon echoes: study of ground and excited state dynamics in molecules.

We report the use of spectrally resolved femtosecond two-color three-pulse photon echoes as a potentially powerful multidimensional technique for studying vibrational and electronic dynamics in complex molecules. The wavelengths of the pump and probe laser pulses are found to have a dramatic effect on the spectrum of the photon echo signal and can be chosen to select different sets of energy levels in the vibrational manifold, allowing a study of the dynamics and vibrational splitting in either the ground or the excited state. The technique is applied to studies of the dynamics of vibrational electronic states in the dye molecule Rhodamine 101 in methanol.