Autocorrelation Function of Hydrogen Atoms in Magnetic Fields

The autocorrelation function is an important quantity that can reflect the dynamical properties of the Rydberg wave packet and can be measured in experiments. Applying time-dependent perturbation theory and rotating wave approximation, we derive the autocorrelation function of the double-pulse laser describing the evolution of a Rydberg wave packet of hydrogen atoms in magnetic fields. The resulting expression is written as a sum of the modified Caussian terms. Each Caussian term comes from a parent semiclassical closed orbit. It provides a direct explanation and experimentally controllable measurement scheme, which allows us therefore to recognize the closed orbit and to determine its returning time in high precision.     

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.     

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.     

Observation of inner electron ionization from radial rydberg wave packets in two-electron atoms

We have observed multiphoton ionization of the 5s core electron from a 5snd radial Rydberg wave packet of Sr atoms using a short optical pulse. When the outer nd electron is at its outer turning point the inner 5s electron is removed from the atom, and the outer electron is left in a Sr+ Rydberg state, but when the outer electron is at the inner turning point this does not occur. Analysis of the final Sr+ Rydberg states shows that the two electrons interact as the inner electron leaves, so that the outer electron is not simply projected onto the Sr+ Rydberg states.     

Coupling of electron orbital motion with rotation in the high Rydberg states of BH

We have applied optical-optical-optical triple resonance spectroscopy to resolve a system of high Rydberg states in BH that serves quantitatively to characterize a fundamental example of electron-orbital-cation core rotational coupling. The third-color ionization-detected absorption spectrum originating from the photoselected 3s B1Sigma+ Rydberg state with vibrational and total angular momentum quantum numbers, v'=1 and N'=0 consists entirely of vibrationally autoionizing resonances for which final N=1 that converge in series to the BH+v+=1 rotational limits, N+=0, 1, and 2. For series with l=1 converging to N+=0 and 2, Rydberg orbital and rotational angular momenta couple to systematically perturb level energies and distribute lifetime in a well-isolated two-channel rotronic interaction that spans hundreds of wave numbers.     

Control of diabatic versus adiabatic field dissociation in a heavy Rydberg system

A novel phenomenon is observed in the dynamics of laser-prepared coherent wave packets, bound by the Coulombic 1/r potential of an ion-pair system. After exciting weakly bound (approximately 3 meV) H(+)(-) wave packets in a Stark field, and permitting them to evolve in time, control of field dissociation via adiabatic and diabatic routes is demonstrated by applying delayed pulsed-electric fields, involving a zero-field crossing. Control manifests itself through the production of ions from each pathway at a different instant in time. This phenomenon is applied to map the oscillatory behavior of an angular momentum wave packet in a heavy Rydberg system. The characteristic frequencies of the observed Stark oscillations verify predicted mass-scaling laws for heavy Rydberg systems.     

一般幂指数中心势作用下的波包回归和部分回归

利用WKB近似和自关联函数方法,我们研究了一般幂指数中心势V(r)=γrk (-20)作用下波包的回归和部分回归.对于排斥势(γ>0, k>0), 势是一长程势,量子化能级结构中只有一个量子数,波包的回归结构和一维幂指数势的情况类似.这一结果表明能级结构相同的体系具有相同的波包回归结构.对于吸引势,能级结构中有两个量子数, 当 k取不同的值时,波包的回归结构不同.对于库仑吸引势,波包回归和部分回归出现;但是对于其它的k值, 经过一段时间后,波包出现坍塌.本文的研究对于探讨里德堡原子和分子中电子运动的经典极限提供了一个新的方法.     

一般幂指数中心势作用下的波包回归和部分回归

利用WKB近似和自关联函数方法,我们研究了一般幂指数中心势V(r)=rk (-20)作用下波包的回归和部分回归。对于排斥势(>0, k>0), 势是一长程势,量子化能级结构中只有一个量子数,波包的回归结构和一维幂指数势的情况类似。这一结果表明能级结构相同的体系具有相同的波包回归结构。 对于吸引势,能级结构中有两个量子数, 当 k取不同的值时,波包的回归结构不同。对于库仑吸引势,波包回归和部分回归出现; 但是对于其它的k值, 经过一段时间后,波包出现坍塌。本文的研究对于探讨里德堡原子和分子中电子运动的经典极限提供了一个新的方法。     

Navigating localized wave packets in phase space

The ability to localize and to steer Rydberg wave packets in phase space using tailored sequences of half-cycle pulses is demonstrated. Classical phase-space portraits are used to explain the method and to illustrate the level of control that can be achieved. This is confirmed experimentally by positioning a phase-space-localized wave packet at the center of a stable island or navigating it around its periphery. This work provides a valuable starting point for further engineering of electronic wave functions.     

Ionisation of Rydberg hydrogen atom near a metal surface by short pulse laser

In the ionisation of Rydberg hydrogen atoms near a metal surface,the electron will escape from the nucleus and arrive at the detector in a time sequence.This probability flux train relies on the initial electron wave packet irradiated by the laser pulse.For simplicity,the laser pulse is usually simplified to a delta function in energy domain,resulting in a sharp initial arrival time with an exponentially decaying tail at the detector.Actually and semiclassically,the initial outgoing wave should be modeled as an ensemble of trajectories propagating away from the atomic core in all directions with a range of launch times and a range of energies.In this case,each pulse in the pulse train is averaged out rather than a sharp profile.We examine how energy and time averaging of the electron wave packet affects the resolution of escaping electron pulses and study the energy dependence of the arrival time for each pulse in the ionisation train.An optimization condition for the laser pulse shape to generate narrow ionisation electron pulse in the train is obtained.The ionisation rates with various excitation energy are calculated also,which show the excitation to higher N Rydberg states will narrow the electron pulse as well.     

Calculation of thermal effects in the photodesorption of NO from NiO(100)

The influence of temperature in the photodesorption of NO from a NiO(100)-surface is studied with a two-dimensional quantum wave packet approach. The complete process including laser-induced excitation and subsequent relaxation is treated explicitly from first principles. The electronic quenching caused by the interaction of the excited adsorbate–substrate system with electron–hole-pairs in the surface is treated with the surrogate Hamiltonian approach. We have implemented a parallelization scheme of the wave packet propagation based on a one-dimensional data decomposition to perform simulations in a reasonable computing time. The results are compared with mixed quantum-classical simulations and with experimental measurements. Both desorption yield and mean velocity of the desorbing molecules were enhanced with increasing temperature. The calculated rotational temperatures are consistent with experimental results. PACS  79.20.La; 68.43.Tj     

Quantum phase retrieval of a Rydberg wave packet using a half-cycle pulse

A terahertz half-cycle pulse was used to retrieve information stored as quantum phase in an N-state Rydberg atom data register. The register was prepared as a wave packet with one state phase reversed from the others (the "marked bit"). A half-cycle pulse then drove a significant portion of the electron probability into the flipped state via multimode interference.     

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.     

Excitation of Rydberg states of atoms and diatomic molecules by short laser impulses

Excitation of multilevel Rydberg states (atoms and diatomic molecules) is studied under an intense time-periodic perturbation that is instantaneously turned on and off. For a one-quantum excitation from a lower lying state, general expressions for the Laplace images of the population amplitudes of Rydberg states are obtained with regard to their decay characteristics. It is shown that the problem considered is reduced to the determination of the positions and widths of the energy levels of a quantum system in the field of monochromatic laser radiation of the same frequency and intensity as that in a pulse mode. To determine these quantities, an integral formulation is proposed for the eigenvalue problem for energies that is relatively simply solved with regard to the effect of the ionic core and its complex vibration-rotation structure on diatomic molecules. The specific features of the excitation of Rydberg states and the behavior of Rydberg wave packets are studied depending on the intensity and duration of laser radiation. A quantum phenomenon of rotational orientation of electron-excited diatomic molecules is considered.     

Demonstration of turnstiles as a chaotic ionization mechanism in Rydberg atoms

We present an experimental and theoretical study of the chaotic ionization of quasi-one-dimensional potassium Rydberg wave packets via a classical phase-space turnstile mechanism. Turnstiles form a general transport mechanism for numerous chaotic systems, and this study explicitly illuminates their relevance to atomic ionization. We create time-dependent Rydberg wave packets, subject them to alternating applied electric-field pulses, and measure the electron survival probability. Ionization depends not only on the initial electron energy, but also on the classical phase-space position of the electron with respect to the turnstile--that part of the electron packet inside the turnstile ionizes after the applied ionization sequence, while that part outside the turnstile does not. The survival data thus encode information on the shape and location of the turnstile, in good agreement with theoretical predictions.     

Electric field controlled, pulsed autoionization in two electron wave packets

In this paper, control of the evolution of a two electron wave packet through the application of a static electric field is demonstrated. Specifically, application of a small electric field is used to produce pulsed autoionization events, the timing of which can be controlled on a picosecond time scale. The technique is demonstrated by exciting calcium atoms using a short-pulsed laser to the 4p(3/2)19d doubly excited state, which is energy degenerate with the 4p(1/2)nk stark states. Evolution of the resultant wave packet is monitored through the application of a second short laser pulse, which stimulates the atoms to emit a photon producing singly excited Rydberg states which are detected using field ionization.     

Modulation of third-harmonic generation conversion in the presence of a rotational wave packet

We report a modulation of third-harmonic generation (THG) owing to a rotational coherence in CO(2). The variation in conversion efficiency is mostly attributed to the dependence of chi(3)(tau) on the molecular alignment. THG via type I processes mainly depends on chi(3)(tau), while type II processes are influenced by the wave packet owing to both chi(3)(tau) and Delta k(tau). Observation of the generated third harmonic also shows significant changes of the polarization state owing to the birefringence induced by the rotational wave packet. Numerical modeling shows good qualitative agreement with the experimental data.     

NeICl体系振动预解离的含时黄金规则近似处理

在相互作用绘景中运用含时黄金规则波包近似方法，对ＮｅＩＣｌ体系的振动预解离进行计算。这里的波包传播法消除了全量子方法中需要长的传播时间的困难，又由于采用了相互作用绘景，可以选取大的时间传播步长，只需很少的传播步数即可得到解高寿命及终产物的转动态分布。     

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.     

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.