Selective excitation of the molecular rotational wave packet by two time-delayed laser pulses

In this paper, we investigate the control of the molecular wave packet of a linear molecule by two femtosecond laser pulses. It is shown that the odd and the even rotational wave packets created by a single laser pulse can be selectively excited by accurately controlling the time delay of another laser pulse. By inserting the peak of the second laser pulse at the position of maximum or minimum value around quarter or three quarter rotational period of the slope curve with odd (or even) rotational wave packet contribution that is created by the first laser pulse, the odd rotational wave packet can be enhanced (or suppressed) while the even rotational wave packet is suppressed (or enhanced). As a result, the molecular alignments around quarter and three quarter rotational periods can be obtained. Moreover, it is also shown that by inserting the second laser pulse around the quarter or three quarter rotational periods, the changes in the maximum degree of the molecular alignment for the odd and the even rotational wave packet contributions are consistent with their corresponding slope curves at these positions.     

Temporal ghost imaging of a time object,dispersion cancelation,and nonlocal time lens with bi-photon state

We present a theory of temporal diffraction, temporal imaging of a bi-photon state, and temporal ghost imaging of a time object. By applying factional Fourier transform to the bi-photon wave packet propagating in space, we could obtain a theory that shows the physical origin of dispersion cancelation, temporal imaging, nonlocal effects of time lenses, and temporal ghost imaging. We introduce the temporal diffraction distance for bi-photon wave packet and show that the bi-photon wave packet behaves like a single wave packet whose temporal diffraction distance is determined by the coherent sum of the temporal diffraction distances for the signal and the idler beams. This property yields the well known dispersion cancelation, the recovery of original bi-photon wave packet in temporal imaging, and the nonlocal combination of two time lenses placed in different arms. We also propose a method for ghost imaging of an arbitrary time object.     

Molecular state reconstruction by nonlinear wave packet interferometry

We show that time- and phase-resolved two-color nonlinear wave packet interferometry can be used to reconstruct the probability amplitude of an optically prepared molecular wave packet without prior knowledge of the underlying potential surface. We analyze state reconstruction in pure- and mixed-state model systems excited by shaped laser pulses and propose nonlinear wave packet interferometry as a tool for identifying optimized wave packets in coherent control experiments.     

基片衍射对会聚激光驻波场中原子波包几率密度演化的影响

针对激光会聚铬原子沉积实验,运用标量衍射理论,通过数值模拟研究了基片衍射对会聚激光驻波场中原子波包几率密度演化的影响。结果显示基片衍射的影响会随激光中轴线与基片沉积表面距离b0的变化而变化。相对于非衍射情况,衍射效应会提高激光驻波场中会聚平面内原子波包几率密度分布的中心值,同时减小其半峰全宽。当参量b0=－0.2w0(w0为高斯光束的束腰半径)时,原子波包几率密度的会聚平面和基片沉积表面完全重合。此处,衍射时原子波包几率密度分布的中心值为1.26,其半峰全宽为5.62 nm,两者分别为非衍射时的1.1倍和0.94倍。     

Theoretical Study of the Influence of Femtosecond Laser Wavelength on the Evolution of a Double-Minimum Electronic Excited State Wave Packet for NaRb

Employing the two-state model and the time-dependent wave packet method, the influence of femtosecond laser wavelength on the evolution of the double-minimum electronic excited state wave packet is numerically investigated. For different laser wavelengths, evolutions of the double-minimum electronic excited state wave packet with time and internuclear distance are different. One can control the evolution of the wave packet by varying the laser wavelength appropriately, which will benefit the light manipulation of atomic and molecular processes. Furthermore, study of the dynamics of the NaRb molecule may yield clues to creating an ultracold molecule.     

PHOTON ACCELERATION DRIVEN BY AN INTENSE LASER PULSE

Interaction of a laser field with a plasma wave is studied by metric optics. Analysis shows that the frequency upshifting of the laser pulse results from the plasma density gradient. A laser beam can be thought of as a packet of photons moving in a plasma and thus the laser frequency upshifting is equivalent to photon acceleration. Examination of the three-dimensional motion equations shows that a laser beam diffraction occurs in the presence of a radial variation of the plasma density. It is argued that the focusing mechanism originating from the plasma wave can curb laser diffraction so that photons may be trapped in the plasma wave and accelerated continuously.     

Control the revisit time of the electron wave packet

Ionization of molecules by strong laser fields launches an electron wave packet. This electron wave packet, which can be driven back by the field to recollide with the parent ion, has been widely explored to probe the ultrafast nuclear dynamics. We numerically demonstrate the precise control of the temporal characteristic of the recolliding electron wave packet (REWP) by orthogonally polarized two-color fields. Through changing the relative phase of the two fields, the revisit time of REWP can be manipulated with a resolution of less than 200 attos, thus significantly improving the resolution of the well known molecular clock. This provides an efficient method for real-time observation of the ultrafast molecular dynamics with attosecond resolution.     

Extracting the phase distribution of the electron wave packet ionized by an elliptically polarized laser pulse

We use an interferometic scheme to extract the phase distribution of the electron wave packet from above-threshold ionization in elliptically polarized laser fields. In this scheme, an electron wave packet released from a circularly polarized laser pulse acts as a reference wave and interferes with the electron wave packet ionized by a time-delayed counter-rotating elliptically polarized laser field. The generated vortex-shaped interference pattern in the photoelectron momentum distribution enables us to extract the phase distribution of the electron wave packet in the elliptically polarized laser pulse with high precision. By artificially screening the ionic potential at different ranges when solving the time-dependent Schördinger equation, we find that the angle-dependent phase distribution of the electron wave packet in the elliptically polarized laser field shows an obvious angular shift as compared to the strong-field approximation, whose value is the same as the attoclock shift. We also show that the amplitude of the angle-dependent phase distribution is sensitive to the ellipticity of the laser pulse, providing an alternative way to precisely calibrate the laser ellipticity in the attoclock measurement.     

Theoretical study of the influence of intense femtosecond laser field on the evolution of the wave packet and the population of NaRb molecule

Employing the two-state model and the time-dependent wave packet method, we have investigated the influences of the parameters of the intense femtosecond laser field on the evolution of the wave packet, as well as the population of ground and double-minimum electronic states of the NaRb molecule. For the different laser wavelengths, the evolution of the wave packet of 6{ }^1\Sigma ^ + state with time and internuclear distance is different, and the different laser intensity brings different influences on the population of the electronic states of the NaRb molecule. One can control the evolutions of wave packet and the population in each state by varying the laser parameters appropriately, which will be a benefit for the light manipulation of atomic and molecular processes.     

Molecular dynamics driven by ultrashort laser pulses: Interference effects due to rescattering

A time-dependent Schrödinger equation is integrated numerically to investigate the dynamics of a model molecular system driven by a high-intensity ultrashort laser pulse. Two-dimensional photoelectron momentum distributions are analyzed. Highly nonmonotonic electron angular distributions are obtained that cannot be explained by diffraction in the double-well potential of a molecular ion. The nonmonotonicity is also demonstrated for atomic ionization and is attributed to the interference that occurs between components of an electron wave packet after its rescattering from the parent ion. An analytical model explaining the observed effects is developed.     

Coherent control of rotational wave-packet dynamics via fractional revivals

We show (i) how the evolution of a wave packet created from an initial thermal ensemble can be controlled by manipulating interferences during the wave packet's fractional revivals and (ii) how the wave-packet evolution can be mapped onto the dynamics of a few-state system, where the number of states is determined by the amount of information one wants to track about the wave packet in the phase space. We illustrate our approach by (i) switching off and on field-free molecular axis alignment induced by a strong laser pulse and (ii) converting alignment into field-free orientation, starting with rotationally cold or hot systems.     

Selective Alignment of D2 Induced by Two Ultrashort Laser Pulses

通过求解D₂分子在飞秒激光场中的含时薛定谔方程,研究了室温下D₂分子在超快飞秒激光驱动下的的转动波包动力学. 选择用第一束超短飞秒脉冲与温度为300 K的D₂分子系综相互作用产生一个相干转动波包,用第二束超短飞秒脉冲在波包的1/4和3/4恢复周期选择操纵D₂分子取向. 研究结果表明,通过选择两束超短飞秒脉冲的延迟时间,可以有效控制D₂分子转动波包中奇偶态的相对布居,从而选择性的控制D₂分子取向.     

Spatial control of recollision wave packets with attosecond precision

We propose orthogonally polarized two-color laser pulses to steer tunneling electrons with attosecond precision around the ion core. We numerically demonstrate that the angles of birth and recollision, the recollision energy, and the temporal structure of the recolliding wave packet can be controlled without stabilization of the carrier-envelope phase of the laser, and that the wave packet's properties can be described by classical relations for a point charge. This establishes unique mapping between parameters of the laser field and attributes of the recolliding wave packet. The method is capable of probing ionic wave packet dynamics with attosecond resolution from an adjustable direction and might be used as an alternative to aligning molecules. Shaping the properties of the recollision wave packet by controlling the laser field may also provide new routes for improvement of attosecond pulse generation via high harmonic radiation.     

High-intensity molecular harmonic generation without ionization

We theoretically investigate high-order harmonic generation from H + 2 in an infrared laser field.Our numerical simulations show that a highly efficient plateau structure exists in the molecular harmonic spectrum.Under the action of the infrared laser pulse,the bound electronic wave packet in a potential well has enough time to tunnel through the effective potential barrier,which is formed by the molecular potential and the infrared laser field,and then recombine with the neighboring nucleus emitting a harmonic photon.During the entire dynamic process,because the wave packet is mainly located in the effective potential,the diffusion effect is of no significance,and thus a highly efficient harmonic plateau can be achieved.Specifically,the cut-off frequency of the plateau is linearly scaled with the peak amplitude of the infrared laser electric field,which may open another route to examine the internuclear distance of the molecule.Furthermore,one may detect the molecular bond lengths using the harmonic plateau.     

Controlling vibrational wave packet motion with intense modulated laser fields

Intense, nonresonant laser fields produce Stark shifts that strongly modify the potential energy surfaces of a molecule. A vibrational wave packet can be guided by this Stark shift if the laser field is appropriately modulated during the wave packet motion. We modulated a 70 fs laser pulse with a period on the time scale of the vibrational motion (approximately 10 fs) by mixing the signal and idler of an optical parametric amplifier. We used ionization of H2 or D2 to launch a vibrational wave packet on the ground state of H2(+) or D2(+). If the laser intensity was high as the wave packet reached its outer turning point, the Stark shift allowed the molecule to dissociate through bond softening. On the other hand, if the field was small at this critical time, little dissociation was measured. By changing the modulation period, we achieved control of the dissociation yield with a contrast of 90%.     

Formation of ground-state vibrational wave packets in intense ultrashort laser pulses

The formation of coherent vibrational wave packets in the electronic ground state of neutral molecules in intense ultrashort laser pulses and their subsequent detection by means of recently developed pump-probe experiments are discussed. The wave packet formation is due to the pronounced dependence of the strong-field ionization rate on the internuclear distance. This leads to a deformation of the initial wave function due to an internuclear-distance dependent depletion. The phenomenon is demonstrated with a time-dependent wave packet study for molecular hydrogen.     

Quantum state reconstruction of a rotational wave packet created by a nonresonant intense femtosecond laser field

We have experimentally determined the amplitudes and phases of a rotational wave packet in an adiabatically cooled benzene molecule, created by a nonresonant intense femtosecond laser field. In this wave-packet reconstruction, the initial wave packet is further interfered by a replica of the first laser pulse, and the resultant modulation in population is observed in a state-resolved manner. Though several states with different nuclear-spin modifications are populated in the initial condition, a single wave packet created from one of them (with J=0) is specifically reconstructed. Phase shifts characteristic of stepwise Raman excitation beyond the perturbative regime are experimentally identified.     

Atom-optics holograms

The temporal evolution of atomic wave packets interacting with object and reference electromagnetic waves is investigated, and an analytical solution for the off-resonant density matrix is presented. It is shown that, under certain physical conditions, the diffraction of an ultracold atomic beam by an inhomogeneous laser field can be interpreted as if the beam passes through a three-dimensional hologram. We show that high diffraction efficiencies can be realized if one restricts the extent of the atomic hologram in the time domain rather than in space. The hologram, thus, can work in a pulsed regime pumping atoms from the beam or from the initial wave packet into the reconstructed matter wave. The suggested regime is well compatible with the Raman cooling methods and the recent realization of an atom laser, which are capable of repeatedly reproducing coherent, or almost coherent, atomic wave packets necessary for the actual implementation of the reading beam. It is found that the diffraction efficiency of such a hologram may reach 100% and is determined by the duration of laser pulses. On this basis, a new method for the reconstruction of the object image with matter waves is offered. The latter may have useful practical applications, ranging from atom lithography, to the manufacturing of microstructures, and quantum microfabrication.     

矩形弹子球中的量子波包分析(英文)

利用波包分析量子力学体系的动力学行为在研究经典和量子的对应关系方面越来越成为一个非常重要的方法.利用高斯波包分析方法,我们计算了矩形弹子球体系的自关联函数,自关联函数的峰和经典周期轨道的周期符合的很好,这表明经典周期轨道的周期可以通过含时的量子波包方法产生.我们还讨论了矩形弹子球的波包回归和波包的部分回归,计算结果表明在每一个回归时间,波包出现精确的回归.对于动量为零的波包,初始位置在弹子球内部的特殊对称点处,出现一些时间比较短的附加的回归.     

Multiphoton stimulated bremsstrahlung for broad (in the momentum representation) electron wave packets in an ultrashort laser pulse field

We consider features of absorption and emission of external laser field quanta by a broad (in the momentum representation) electron wave packet during its scattering from a potential center. Various scattering modes for the electron wave packet in a high-intensity laser field are analyzed using perturbation theory of potential energy. It is found that the absorption of laser field energy by an electron is substantially more effective as compared to the case of a plane wave. The important role of a number of interference effects associated with the large width of the initial electron momentum distribution is demonstrated.