Control of femtosecond filamentation by field-free revivals of molecular alignment

We show that the filamentation dynamics of a femtosecond laser probe pulse can be readily controlled by properly matching it to the quantum revivals of pre-aligned molecules prepared through impulsive rotational Raman excitation with an advancing ultrashort pump pulse. Several features of the filamentation process including supercontinuum generation, the length of the plasma channel generated in the wake of the filament, the associated secondary radiations and the multiple filamentation pattern are all easily modified by tuning the cross phase modulation induced by the field-free revivals of molecular alignment, through the delay between the pump and the probe pulses. We show that molecular alignment can also be used to generate conical waves with extremely short intensity spike called shocked X-waves and to further tune the frequency of a few-cycle laser pulse in the wake of a self-guided intense filament.     

Spectral modulation of third-harmonic generation by molecular alignment and preformed plasma

We demonstrate spectral modulation of third-harmonic generation from molecular alignment effects. The third harmonic spectrum is broadened or narrowed under different influences of cross-phase modulations originating from various molecular alignment revivals. Furthermore, the spectrum and spatial distribution of the generated third harmonic pulse change dramatically in the presence of a preformed plasma. Under the influence of a preformed plasma, a narrower third harmonic spectrum is observed, and the conical third-harmonic pulse increases while the axial part decreases. The investigation provides an effective method to modulate the spectral characteristic and spatial distribution of third-harmonic generation from intense femtosecond filament.     

Information content of high harmonics generated from aligned molecules

We derive an expression for the harmonic signal from nonadiabatically aligned molecules that accounts for both electronic and rotational motions. We identify a single approximation, which converts the expression into a physically transparent and computationally convenient form. Our analytical result gives explicitly the time dependence of the harmonic spectra, thus explaining the observations of a class of recent experiments. Moreover, it points to new opportunities for generating insights into the structure and dynamics of molecular systems through harmonic generation experiments from aligned molecules. This includes information regarding the rotational and electronic dynamics of isolated systems, as well as regarding the decoherence and relaxation in molecules subject to a dissipative environment.     

Dynamic properties of angle-dependent high-order harmonic generation from coherently rotating molecules

High-order harmonic generation from coherently rotating N2 and O2 molecules has been observed for different alignment angles in a pump and probe experiment using femtosecond laser pulses. The results obtained are in excellent agreement with those calculated using a recently developed theory, which represent the characteristic properties predicted for angle-dependent harmonic generation. It is shown that polarization geometry and alignment distribution play essential roles in potential applications to probe electronic structure and dynamics of molecular systems.     

Field-free alignment of molecules observed with high-order harmonic generation

High-order harmonic generation is demonstrated to provide a sensitive way for an extensive study of dynamic processes in the field-free alignment of strong-field-induced molecular rotational wave packets. The time-dependent harmonic signal observed from field-free-aligned N2, O2, and CO2 has been found to include two sets of beat frequency for pairs of coherently populated rotational states. One of them is the well-known frequency component characterizing the field-free alignment of molecules, and the other is ascribed to the beat that arises from coherence embedded in the wave packet. We discuss the effect of each frequency component on the revival signal observed with the harmonic generation.     

Phase-matched high harmonic generation for the study of rotational coherence molecular dynamics

We report the observation of periodic modulations in the high order harmonic radiation from diatomic molecules in a semi-infinitive gas cell when a preceding femtosecond laser beam, which is off-axis to the high-harmonic generation beam, modifies the phase-matching condition through the field-free alignment of the molecules. The observed modulations of the high harmonic radiation versus the time delay between the pulses result from periodic changes in the nonlinear refractive index associated with rotational Raman coherence. This opens up a new potential technique for studying rotational coherence dynamics in the ground states of molecules.     

Vortex revivals with trapped light

We predict that vortex dipoles nested in light beams trapped in graded-index media can undergo closed Berry trajectories, yielding periodic vortex annihilations and revivals along the light-propagation direction. The vortex revivals from vortex-free wave fronts are mediated by Freund stationary point bundles that carry the necessary Poincaré-Hopf indices. Vortex spiraling and spontaneous generation of circular-edge dislocations are also found to occur.     

High-order harmonic transient grating spectroscopy in a molecular jet

We study high-order harmonic generation in excited media using a four-wave-mixing-like configuration. We analyze the spatial profile of high harmonics emitted by a grating of rotationally excited molecules as a function of the pump-probe delay. We demonstrate a dramatic improvement in the contrast of the diffracted signal relative to the total high harmonic signal. This allows us to observe subtle effects in the rotational wave packet excitation such as the pump-intensity dependence of the wave packet dynamics. High harmonic transient grating spectroscopy can be extended to all forms of molecular excitation and to weak resonant excitation.     

Phase control of rotational wave packets and quantum information

Lasers can create rotational wave packets in gas-phase molecules which periodically revive as field-free, aligned distributions. We control the wave packet evolution with relatively weak laser pulses at fractional revivals which modify the phase between wave packet components. We demonstrate two phase control effects in oxygen: coherently switching revivals off and on, and doubling the revival frequency. When viewed as a quantum logic system, these effects correspond to a Hadamard and a T operation.     

空气中等离子光栅诱导探测光丝三次谐波辐射放大的实验研究

对探测光丝的不同位置与等离子光栅相互作用和探测光丝作用到等离子光栅不同位置引起三次谐波的增强进行了实验研究.研究发现,探测光丝的三次谐波信号强度对于探测光丝不同位置与等离子光栅相互作用和等离子光栅内部钳制的激光强度具有极强的依赖关系.与等离子光栅相互作用,三次谐波信号与等离子光栅基波信号的相位匹配与否是解释探测光丝三次谐波信号强度变化的关键.控制探测光丝以小角度与等离子光栅相互作用是实现探测光丝三次谐波信号有效放大的最佳途径.     

Probe of high-order harmonic generation in a hollow waveguide geometry using counterpropagating light

We use counterpropagating light to directly observe the coherent buildup of high harmonic generation in a hollow waveguide geometry. We measure, for the first time, coherence lengths for high photon energies that cannot be phase matched using conventional approaches. We also probe the transition through phase matching, the ionization level at which different harmonic orders are generated, and the change in the coherence length as the driving laser is depleted. These results directly prescribe the optimal structures or pulse trains required for implementing quasiphase matching.     

Quantum carpets: efficiently probing fractional revivals in position-dependent mass systems

Position-dependent-mass systems are of great importance in many physical situations,such as the transport of charge carriers in semiconductors with non-uniform composition and in the theory of many-body interactions in condensed matter.Here we investigate,numerically and analytically,the phenomenon of fractional revivals in such systems,which is a generic characteristic manifested by the wave-packet evolution in bounded Hamiltonian systems.Identifying the fractional revivals using specific probe...     

Evidence of high harmonics from echo-enabled harmonic generation for seeding x-ray free electron lasers

Echo-enabled harmonic generation free electron lasers hold great promise for the generation of fully coherent radiation in x-ray wavelengths. Here we report the first evidence of high harmonics from the echo-enabled harmonic generation technique in the realistic scenario where the laser energy modulation is comparable to the beam slice energy spread. In this experiment, coherent radiation at the seventh harmonic of the second seed laser is generated when the energy modulation amplitude is about 2-3 times the slice energy spread. The experiment confirms the underlying physics of echo-enabled harmonic generation and may have a strong impact on emerging seeded x-ray free electron lasers that are capable of generating laserlike x rays which will advance many areas of science.     

Coherent x-ray Raman spectroscopy: a nonlinear local probe for electronic excitations

Nonlinear x-ray four-wave mixing experiments are becoming feasible due to rapid advances in high harmonic generation and synchrotron radiation coherent x-ray sources. By tuning the difference of two x-ray frequencies across the valence excitations, it is possible to probe the entire manifold of molecular electronic excitations. We show that the wave vector and frequency profiles of this x-ray analogue of coherent Raman spectroscopy provide an excellent real-space probe that carries most valuable structural and dynamical information, not available from spontaneous Raman techniques.     

Enhanced harmonic generation from expanding clusters

We report controlled enhancement of optical third harmonic generation (THG) from hydrodynamically expanding clusters of approximately 6x10(5) noble-gas atoms several hundred femtoseconds following ionization and heating by ultrashort pump pulses. This resonant enhancement is more pronounced for orthogonal than for parallel pump-probe polarizations, a consequence of faster cluster expansion along the pump polarization. Simulations show that the nonlinear susceptibility chi(3) of the individual clusters and the coherence length of the clustered plasma medium are optimized nearly simultaneously as the clusters expand, and both contribute to the observed THG enhancement. This dual enhancement mechanism may be scalable to relativistic probe intensity and to generation of high-order harmonics in the soft-x-ray regime.     

相干叠加态高次谐波发射的时间行为分析

本文研究了一维模型分子离子(初态为基态和一个激发束缚态叠加的相干态)在超强超短激光脉冲作用下的谐波发射谱.我们发现在高次谐波谱平台区域出现了周期性的结构变化.我们利用小波变换对谐波谱进行了暂态时间频率分析,结果表明该谐波结构产生的原因是由电离电子返回母离子时与不同束缚态复合而产生的谐波光脉冲之间相干叠加.同时采用半经典计算,对所得到的计算结果进行了分析,验证了我们的结论.     

Classical aspects of Raman excited rotational revivals

The rotational coherence of Raman excited quantum wavepackets is shown to correspond to angular realignment of a classical ensemble of quantized rotors, a picture that provides an intuitive explanation for the existence and chirp shapes of four distinct partial revivals in the optical refractive index, at fractions of the full recurrence period. Evidence from the chirp shapes, of classical orientational alignment by the laser pulse (in an angle-action sense) is supported by an approximate analytically soluble quantum mechanical model.     

High order harmonic generation from solid targets: Towards intense attosecond pulses

Experiments and computer simulations on high order harmonic generation (HOHG) from steep plasma gradients using intense femtosecond laser pulses are presented. The importance of the plasma scale length for the efficiency of HOHG is demonstrated. By changing the pump intensity and the target parameters the regime of HOHG can be switched from non-relativistic to relativistic. Simulations show that attosecond pulses should already be present in our experiments in both interaction regimes. Two-color driven harmonic generation is shown to provide a highly efficient way of attosecond pulse production.     

原子在红外激光场中产生高次谐波及阿秒脉冲随波长的变化规律

利用强场近似理论,研究了在长波红外激光场(波长800—2000 nm)驱动下氢原子产生的高次谐波,分析了在截止位置附近高次谐波的转换效率随激光波长的变化规律.发现在截止位置附近原子发射高次谐波的转换效率比平台区域的转换效率低,但获得的阿秒脉冲的宽度会随波长的增大而缩短. 关键词： 强场近似 高次谐波 阿秒脉冲     

Polarization of multiple rotational Raman sidebands from hydrogen gas by delayed four-wave Raman mixing in the femtosecond regime

We demonstrate delayed four-wave Raman mixing in hydrogen gas and discuss the polarization of multiple rotational Raman radiation in the sub-100-fs regime. The mechanism of sideband generation through the interaction between a probe pulse and coherence of molecular motions induced by a pump pulse in hydrogen is revealed. One can artificially control the ellipticity of the polarization of the rotational Raman sidebands by changing the pump pulse polarization.