Attosecond time-scale intra-atomic phase matching of high harmonic generation

Includes bibliographical references (page 5461).Using a model of high-harmonic generation that couples a fully quantum calculation with a semi-classical electron trajectory picture, we show that a new type of phase matching is possible when an atom is driven by an optimal optical waveform. For an optimized laser pulse shape, strong constructive interference is obtained in the frequency domain between emissions from different electron trajectories, thereby selectively enhancing a particular harmonic order. This work demonstrates that coherent control in the strong-field regime is possible by adjusting the peaks of a laser field on an attosecond time scale

Adaptive pulse compression for transform-limited 15-fs high-energy pulse generation

Includes bibliographical references (page 589).We demonstrate the use of a deformable-mirror pulse shaper, combined with an evolutionary optimization algorithm, to correct high-order residual phase aberrations in a 1-mJ, 1-kHz, 15-fs laser amplifier. Frequency resolved optical gating measurements reveal that the output pulse duration of 15.2 fs is within our measurement error of the theoretical transform limit. This technique significantly reduces the pulse duration and the temporal prepulse energy of the pulse while increasing the peak intensity by 26%. It is demonstrated, for what is believed to be the first time, that the problem of pedestals in laser amplifiers can be addressed by spectral-domain correction

Absolute determination of the wavelength and spectrum of an extreme-ultraviolet beam by a Young's double-slit measurement

Includes bibliographical references (page 709).The interference pattern produced by irradiation of a pair of pinholes with a beam contains information on both the spatial and the temporal coherence properties of the beam, as well as its power spectrum. We demonstrate experimentally for what is believed to be the first time that the spectrum of an extreme-ultraviolet (EUV) beam can be obtained from a measurement of the interference pattern produced by a pinhole pair. This approach offers a convenient method of making absolute wavelength and relative spectral intensity calibrations in the EUV

Nonresonant control of multimode molecular wave packets at room temperature

Includes bibliographical references (pages 033001-4).We demonstrate the creation and measurement of shaped multimode vibrational wave packets with overtone and combination mode excitation in CCl4. Excitation of wave packets through nonresonant impulsive stimulated Raman scattering allows for coherent control of molecular vibrations without passing through an electronic resonance. This technique is therefore very general and can be implemented in a large class of molecular gases and liquids at STP, which were previously inaccessible because their resonances are in the VUV

Generation of broadband VUV light using third-order cascaded processes

Includes bibliographical references (pages 013601-4).We report the first demonstration of broadband VUV light generation through cascaded nonlinear wave mixing in a gas. Using a hollow-fiber geometry to achieve broad-bandwidth phase-matching, frequency conversion of ultrashort-pulse Ti:sapphire laser pulses from the visible into the deep UV around 200 and160 nm is achieved. A new type of quasi-phase-matching is also observed in the VUV for the first time. Conversion using cascaded processes exhibits higher efficiencies, shorter pulse durations, and broader bandwidths than other schemes for generating light in the deep UV, and will enable many applications in science and technology

Generation of broadband VUV light using third-order cascaded processes

Includes bibliographical references (pages 013601-4).We report the first demonstration of broadband VUV light generation through cascaded nonlinear wave mixing in a gas. Using a hollow-fiber geometry to achieve broad-bandwidth phase-matching, frequency conversion of ultrashort-pulse Ti:sapphire laser pulses from the visible into the deep UV around 200 and160 nm is achieved. A new type of quasi-phase-matching is also observed in the VUV for the first time. Conversion using cascaded processes exhibits higher efficiencies, shorter pulse durations, and broader bandwidths than other schemes for generating light in the deep UV, and will enable many applications in science and technology

Ptychographic hyperspectral spectromicroscopy with an extreme ultraviolet high harmonic comb

We demonstrate a new scheme of spectromicroscopy in the extreme ultraviolet (EUV) spectral range, where the spectral response of the sample at different wavelengths is imaged simultaneously. It is enabled by applying ptychographical information multiplexing (PIM) to a tabletop EUV source based on high harmonic generation, where four spectrally narrow harmonics near 30 nm form a spectral comb structure. Extending PIM from previously demonstrated visible wavelengths to the EUV/X-ray wavelengths promises much higher spatial resolution and more powerful spectral contrast mechanism, making PIM an attractive spectromicroscopy method in both the microscopy and the spectroscopy aspects. Besides the sample, the multicolor EUV beam is also imaged in situ, making our method a powerful beam characterization technique. No hardware is used to separate or narrow down the wavelengths, leading to efficient use of the EUV radiation

Two-center Interferences in Photoionization of Dissociating H2+_2^+ Molecule

We analyze two-center interference effects in the yields of ionization of a dissociating hydrogen molecular ion by an ultrashort VUV laser pulse. To this end, we performed numerical simulations of the time-dependent Schr\"odinger equation for a H$_2^+$ model ion interacting with two time-delayed laser pulses. The scenario considered corresponds to a pump-probe scheme, in which the first (pump) pulse excites the molecular ion to the first excited dissociative state and the second (probe) pulse ionizes the electron as the ion dissociates. The results of our numerical simulations for the ionization yield as a function of the time delay between the two pulses exhibit characteristic oscillations due to interferences between the partial electron waves emerging from the two protons in the dissociating hydrogen molecular ion. We show that the photon energy of the pump pulse should be in resonance with the $\sigma_g - \sigma_u$ transition and the pump pulse duration should not exceed 5 fs in order to generate a well confined nuclear wavepacket. The spreading of the nuclear wavepacket during the dissociation is found to cause a decrease of the amplitudes of the oscillations as the time delay increases. We develop an analytical model to fit the oscillations and show how dynamic information about the nuclear wavepacket, namely velocity, mean internuclear distance and spreading, can be retrieved from the oscillations. The predictions of the analytical model are tested well against the results of our numerical simulations

Phase-matching conditions for nonlinear frequency conversion by use of aligned molecular gases

Includes bibliographical references (page 348).Transient birefringence can be induced in a gas of anisotropic molecules by an intense polarized laser pulse. We propose to use this birefringence to phase match nonlinear optical frequency-conversion processes. The conditions for anisotropic phase matching are derived, and experimental conditions required for phase-matched third-harmonic generation in a gas-filled hollow-core fiber are presented. We show that these conditions are experimentally feasible over a significant parameter range, making possible a new type of nonlinear optics