Resolving vibrational wave-packet dynamics of D2(+) using multicolor probe pulses

We demonstrate the generation and real-time observation of the vibrational wave packet of D(2)(+) by using a sub-10-fs extreme UV high-harmonic pump pulse and a three-color probe laser pulse whose wavelength ranges from near-IR to vacuum UV. This multicolor pump-probe scheme can provide us with a powerful experimental tool for investigating a variety of wave packets evolving with a time scale of ~20 fs.     

Spatial control of high-harmonic generation in hollow fibers

We demonstrate the control of high-harmonic generation in a hollow fiber by shaping the spatial structure of the generating laser pulse. We use a liquid-crystal-based two-dimensional spatial light modulator to control the spatial phase of the driver pulse. An evolutionary algorithm finds the spatial laser phase distribution that is optimal for reaching maximum total harmonic yield and for selectively enhancing the cutoff region of the spectrum. We show that enhacement of harmonic generation is related to coupling into a single fiber mode. Our results directly show that spatial properties of the laser are important parameters in fully controlling the high-harmonic spectrum. It is thus not possible to derive the controllability of the high-harmonic generation from the single-atom response only.     

Single attosecond pulse generation in the multicycle-driver regime by adding a weak second-harmonic field

We present a method of producing single attosecond pulses by high-harmonic generation with multicycle driver laser pulses. This can be achieved by tailoring the driving pulse so that attosecond pulses are produced only every full cycle of the oscillating laser field rather than every half-cycle. It is shown by classical and quantum-mechanical model calculations that even a minor addition (1%) of phase-locked second-harmonic light to the 800 nm fundamental driver pulse for high-harmonic generation leads to a major (15%) difference in the maximum kinetic energies of the recombining electrons in adjacent half-cycles.     

Phase-coherent frequency combs in the vacuum ultraviolet via high-harmonic generation inside a femtosecond enhancement cavity

We demonstrate the generation of phase-coherent frequency combs in the vacuum utraviolet spectral region. The output from a mode-locked laser is stabilized to a femtosecond enhancement cavity with a gas jet at the intracavity focus. The resulting high-peak power of the intracavity pulse enables efficient high-harmonic generation by utilizing the full repetition rate of the laser. Optical-heterodyne-based measurements reveal that the coherent frequency comb structure of the original laser is fully preserved in the high-harmonic generation process. These results open the door for precision frequency metrology at extreme ultraviolet wavelengths and permit the efficient generation of phase-coherent high-order harmonics using only a standard laser oscillator without active amplification of single pulses.     

氦原子在啁啾激光与中红外组合场中产生的单个阿秒脉冲

通过Crank Nicolson方法数值求解一维氦原子的含时Schrdinger方程,研究了啁啾激光与中红外激光形成组合场驱动氦原子发射高次谐波的特点.研究结果表明,在组合场驱动下,高次谐波平台区能得到很大的扩展,其截至位置得到大幅度扩展,对平台区不同阶次范围的高次谐波进行叠加均能得到单个的阿秒脉冲,最短可实现46 as的单个脉冲输出,经分析发现,中红外场的加入,不仅使高次谐波的平台得到扩展,而且提高了平台区前端的谐波强度.通过经典计算和对电离几率特点的讨论,解释了发生这种现象的原因.     

High harmonic XUV spectral phase interferometry for direct electric-field reconstruction

We demonstrate the first experimental complete temporal characterization of high-harmonic XUV pulses by spectral phase interferometry, with an all-optical setup. This method allows us to perform single-shot measurements of the harmonic temporal profile and phase, revealing a remarkable shot-to-shot stability. We characterize harmonics generated in argon by a 50 fs 800 nm laser pulse. The 11th harmonic is found to be 22 fs long with a negative chirp rate of -4.8 x 10(27) s(-2). This duration can be reduced to 13 fs by modulating the polarization of the generating laser. The technique is easy to implement and could be routinely used in femtosecond XUV pump-probe experiments with harmonics.     

Soft-x-ray wavelength shift induced by ionization effects in a capillary

Coherent soft x rays are produced by high-harmonic generation in a capillary filled with Ar gas. We demonstrate that the tuning of the harmonic wavelengths with intensity and chirp arises from changes in the Ar ionization level. Control over the tuning can be achieved either by changing the average intensity of the laser pulse or by varying the quadratic spectral phase of the laser pulse. We observe an ionization-dependent blueshift of the fundamental wavelength that is directly imprinted on the harmonic wavelengths. The harmonic tuning is shown to depend on nonlinear spectral shifts of the fundamental laser pulse that are due to the plasma created by ionization, rather than directly on any chirp imposed on the fundamental wavelength.     

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

Using a model of high-harmonic generation that couples a fully quantum calculation with a semiclassical 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.     

Gouy phase shift for few-cycle laser pulses

We measured for the first time the influence of the Gouy effect on focused few-cycle laser pulses. The carrier-envelope phase is shown to undergo a smooth variation over a few Rayleigh distances. This result is of critical importance for any application of ultrashort laser pulses, including high-harmonic and attosecond pulse generation, as well as phase-dependent effects.     

Control of laser high-harmonic generation with counterpropagating light

Relatively weak counterpropagating light is shown to disrupt the emission of laser high-harmonic generation. Harmonic orders ranging from the teens to the low thirties produced by a 30-femtosecond pulse in a narrow argon jet are "shut down" with a contrast as high as 2 orders of magnitude by a chirped 1-picosecond counterpropagating laser pulse (60 times less intense). Alternatively, under poor phase-matching conditions, the counterpropagating light boosts harmonic production by similar contrast through quasiphase matching where out-of-phase emission is suppressed.     

Single-pass high-harmonic generation at 20.8 MHz repetition rate

We report on single-pass high-harmonic generation (HHG) with amplified driving laser pulses at a repetition rate of 20.8?MHz. An Yb:YAG Innoslab amplifier system provides 35?fs pulses with 20?W average power at 1030?nm after external pulse compression. Following tight focusing into a xenon gas jet, we observe the generation of high-harmonic radiation of up to the seventeenth order. Our results show that state-of-the-art amplifier systems have become a promising alternative to cavity-assisted HHG for applications that require high repetition rates, such as frequency comb spectroscopy in the extreme UV.     

Single attosecond pulse generation with intense mid-infrared elliptically polarized laser pulses

We have studied theoretically high-harmonic-order and single attosecond pulse generation with elliptically polarized laser pulses at wavelengths ranging from the visible to the mid-infrared. Results of ab initio simulations of the time-dependent Schr?dinger equation show that the ellipticity dependence of the high-harmonic signal intensifies with increasing wavelength of the driving pulse and saturates in the mid-infrared. The isolation of single attosecond pulses using the polarization gating method in the mid-infrared is due to an effective suppression of side pulses as compared with an operation at Ti:sapphire wavelengths.     

Ionization phase-match gating for wavelength-tunable isolated attosecond pulse generation

High-order harmonic emission can be confined to the leading edge of an 800 nm driver laser pulse under moderately intense focusing conditions (7×10¹⁴ W/cm²) (Pfeifer et al. in Opt. Express 15:17120, 2007). Here, the experimentally observed curtailment of harmonic production on the leading edge of the driver pulse is shown to be controlled by an ionization-induced phase-matching condition. The transient plasma density inherent to the process of high-harmonic generation terminates the harmonic emission by an ultrafast loss of phase matching on the leading edge of the laser pulse. The analysis is supported by a reconstruction of the in situ intensity envelope of the driver pulse with attosecond temporal resolution, performed by measurements of the carrier-envelope phase dependence of individual half-cycle harmonic cutoffs. The method opens the way to wavelength-tunable isolated attosecond pulse generation.     

Implementation of the direct locking method for long-term carrier-envelope-phase stabilization of a grating-based kHz femtosecond laser

We have stabilized the carrier-envelope phase (CEP) of amplified femtosecond laser pulses from a grating-based chirped-pulse amplification femtosecond laser by the direct locking method. Long-term CEP stabilization in the oscillator was achieved by employing a double-feedback loop to control both the pumping power and the cavity dispersion. Large CEP drift, induced during amplification, was compensated by adjusting the grating separation in the pulse compressor, and the CEP stabilization was maintained for four hours with a phase jitter of about 180 mrad. After pulse compression to 5.5-fs pulses in a filamentation pulse compressor, CEP-stabilized laser pulses were applied for high-harmonic generation to confirm the CEP stabilization.     

Enhancement of high-harmonic generation by laser-induced cluster vibration

Sharp periodic enhancement of high-harmonic generation synchronized to prepulse-induced cluster vibration is observed. Tenfold enhancement of high-harmonic-generation efficiency is achieved by optimal selection of the prepulse-pump delay. This strong correlation between high-harmonic generation and cluster vibration also provides a new tool for studying the vibrational dynamics of nanometer atomic clusters.     

Phase matching, quasi-phase matching, and pulse compression in a single waveguide for enhanced high-harmonic generation

We demonstrate, for the first time to our knowledge, that the efficient region of high-harmonic generation can be shifted from lower to higher photon energies by combining phase matching, quasi-phase matching, and pulse compression in a single gas-filled waveguide. An intrawaveguide pulse compression process that works through a combination of ionization-induced refraction and guiding shortens the laser pulse as it propagates through an Ar-filled waveguide. This leads to enhanced harmonic emission at high photon energies near 95 eV while it reduces emission at low photon energies near 45 eV. The waveguide geometry also mitigates ionization-induced refraction, allowing Ar gas with high effective nonlinear susceptibility to be used.     

Carrier-envelope offset phase control: A novel concept for absolute optical frequency measurement and ultrashort pulse generation

The shortest pulses periodically emitted directly from a mode-locked Ti:sapphire laser are approaching the two-optical-cycle range. In this region, the phase of the optical carrier with respect to the pulse envelope becomes important in nonlinear optical processes such as high-harmonic generation. Because there are no locking mechanisms between envelope and carrier inside a laser, their relative phase offset experiences random fluctuations. Here, we propose several novel methods to measure and to stabilize this carrier-envelope offset (CEO) phase with sub-femtosecond uncertainty. The stabilization methods are an important prerequisite for attosecond pulse generation schemes. Short and highly periodic pulses of a two-cycle laser correspond to an extremely wide frequency comb of equally spaced lines, which can be used for absolute frequency measurements. Using the proposed phase-measurement methods, it will be possible to phase-coherently link any unknown optical frequency within the comb spectrum to a primary microwave standard. Experimental studies using a sub-6-fs Ti:sapphire laser suggesting the feasibility of carrier-envelope phase control are presented. Received: 19 August 1999 / Published online: 8 September 1999     

Influence of the intensity gradient upon HHG from free electrons scattered by an intense laser beam

When an electron is scattered by a tightly focused laser beam in vacuum, the intensity gradient is a critical factor to influence the electron dynamics. In this paper, we have further investigated its influence upon the electron high-harmonic generation (HHG) by treating the spacial gradient of the laser intensity as a ponderomotive potential. Based upon perturbative quantum electrodynamics calculations, it has been found that the main effect of the intensity gradient is the broadening of the originally line HHG spectra. A one-to-one relationship can be built between the beam width and the corresponding line width. Hence, this finding may provide us a promising way to measure the beam width of intense lasers in experiments. In addition, for a laser pulse, we have also studied the different influences from transverse and longitudinal intensity gradients upon HHG.     

Controlling the spectral shape of coherent soft X-rays

We demonstrate the generation of arbitrarily shaped spectra of coherent soft X-ray radiation by adaptive control of the driving laser pulse. The selection of both narrow and wide spectral ranges as well as suppression of high-harmonic emission in a selected wavelength region is achieved. Feedback-controlled spectral engineering of coherent soft X-rays paves the way to shaping of soft X-ray pulses and coherent control of electron dynamics in the sub-femtosecond regime.     

Exact Timing of Returned Molecular Wavepacket

An ionizing wavepacket of electron will re-visit its parent molecular ion during photoionization by strong laser field. This scenario is associated with physical concepts such as molecular re-scattering/collision, interference, diffraction, molecular clock, and generation of XUV light via high-order harmonic generation. On the workbench of a reduced dimensionality model of molecular hydrogen ions irradiated by laser pulse of 0.01-10.0 a.u. intensities, one-cycle pulsewidth, and 800nm wavelength, by deploying a momentum operator on the time-dependent wavefunction of an ionizing wavepacket, we can determine, in a precise manner, the exact time instant for the re-visiting electron to come back to the cation position. The time value is 57.6% of an optical cycle of the exciting laser pulse. This result may be useful in attosecond pump-probe experiments or molecular clock applications.