Control of de-excitation to selected vibrational levels in the ground state of NaH molecule using two broadband ultrashort pulses

We show that the de-excitation to different vibrational levels of the ground state in NaH molecule can be controlled by using two delayed ultrashort pulses (4 fs Gaussian). A vibrational wave packet generated on the excited A¹Σ⁺ state by the first pulse is de-excited back to the ground state by a second pulse after a time delay. The cross-section for de-excitation of the wave packet to different vibrational levels of the ground electronic state can be controlled by controlling the delay time between the two pulses as well as by choosing a pulse duration much shorter than the vibrational period of the molecule, such that the de-excited wave packet remains localized in the Franck–Condon region of a particular vibrational level of the ground state. Hence, the de-excitation to a particular vibrational level can be enhanced by suppressing that in others. In spite of the large bandwidth of the pulse which includes nine vibrational levels of the upper state and five vibrational levels of the ground state, one can selectively de-excite the molecule to any one or two vibrational levels of the ground state by carefully choosing the delay time between the pulses and the pulse duration. We are designing the wave packet in the ground state by two short pulses and selectively distributing the population in one or two levels at various values of the delay time. In light molecules having small vibrational period, this selectivity in de-excitation to one or two vibrational levels in the ground state can be achieved only by using ultrashort (4 fs) pulses in the presence of which the localization of the wave packet in the Franck–Condon region of the vibrational levels are particularly possible. It has been shown that the de-excitation cross-section to a particular vibrational level oscillates with delay between the pulses which can be realized as a time-dependent quantum gate.     

基于主动锁相的二维电子光谱方法

二维电子光谱是探测复杂系统激发态相干动力学的重要工具,实现二维电子光谱测试的最大挑战是精确控制多束超短脉冲之间的相位差. 本综述回顾了利用主动相位管理方法实现二维电子光谱仪装置,主要包括干涉仪相位稳定、声光调制器进行频率标记和多光频梳等三类方法;结合四波混频、泵浦探测及完全共线等不同构型,能实现高时空分辨及量子跃迁通道选择的二维光谱检测. 超短脉冲技术与主动相位调控的结合实现二维电子光谱学方法,为研究激发态相干动力学提供新的机遇.     

A solitary wave of coherent excitonic polaritons in an extended chain of quantum dots

The propagation of ultrashort optical pulses in a chain of two-level two-electron quantum dots was studied theoretically. It was assumed that an excited state of an individual quantum dot can be transferred to the neighboring quantum dots, as is the case for a molecular exciton. As a result, optical-pulse motion is accompanied with a wave of polarization of quantum dots. It is shown that two types of steady-state circularly polarized solitary polaritonic waves can propagate along such chains; these are waves with exponentially and algebraically decaying leading and trailing edges.     

CALCULATION OF HIGHLY EXCITED VIBRATIONAL ENERGY LEVELS OF CH3CN MOLECULE BY NON-LINEAR QUANTUM THEORY

A three-parameter nonlinear dynamical model, i.e., the quantized discrete self-trapping equation, was used to calculate the highly excited CH stretching vibrational energy levels of liquid phase CH₃CN molecule in the electronic ground state up to n=7. The calculated results show that the experimental energy levels can be well described by the model.     

Optical control of the coherent dynamics of excitons in a semiconductor quantum well

The dynamics of the coherent superposition of exciton states in a semiconductor quantum well excited by the joint action of two successive light pulses with the time interval between them t ₁₂ has been theoretically studied. The dependences of the amplitude and initial phase of the quantum bits on t ₁₂ have been found. It has been shown that the time dependence of the Kerr rotation of the reflected probe pulse is determined not only by the dynamics of the excited state, but also by the optical properties of the heterostructure containing the quantum well. The dependence of the decay rate of the excited state on t ₁₂ has been predicted.     

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.     

Quantum-classical simulation of the photoisomerization during the transformation of ultrashort light pulses by a molecule

The dynamics of photoisomerization of a model molecule during its transformation of ultrashort (with a duration much shorter than the lifetime of the resonant excited electronic state) light pulses is simulated numerically. The two-level electronic subsystem of the molecule is described using the quantum theory, while the nuclear subsystem (taking into account the two isomeric states of the molecule) and the radiation field are described using the classical theory. The ranges of the carrier frequency, the peak intensity, and the durations of nπ sinusoidal pulses (n = 1–10) irradiation with which results in the photoisomerization of molecules of the type under study (for example, cyanine dyes) are determined from the analysis of solutions to self-consistent equations that describe the motion of the “isomerization oscillator” and the time evolution of the population amplitude of the resonant electronic state of the molecule. Each of these non-overlapping ranges corresponds to a particular value of n. Bifurcation values of the above parameters of the light pulse are boundaries of these ranges.     

反应物分子初始振动激发对O+HCl→OH+Cl反应的立体动力学性质的影响

在Peterson的高精度从头计算势能面上,运用准经典轨线方法讨论了反应物分子初始振动激发对O+HCl→OH+Cl反应的立体动力学性质的影响.反映两矢量k-j′相关的P(θr)函数的分布说明产物的转动角动量j′在垂直于反应物相对速度矢量k的方向上的排列取向程度随着初始反应物振动量子数的增加而增加;反映三矢量k-k′-j′相关的极角分布函数P(r)显示产物的转动角动量有比较弱的定向效应,且随着初始振动量子数的增加,这种弱的定向效应由沿Y轴负向变为沿Y轴正向.说明反应物分子的初始振动激发有利于增强产物分子的转动排列取向效应,但对产物分子P(r)分布的影响则不明显.     

Quantum computation with vibrationally excited polyatomic molecules: effects of rotation,level structure,and field gradients

Accurate rotation–vibration energy levels and transition dipoles of the molecule thiophosgene are used to model the execution of quantum gates with shaped laser pulses. Qubits are encoded in 2 ⁿ vibrational computing states on the ground electronic surface of the molecule. Computations are carried out by cycling amplitude between these computing states and a gateway state with a shaped laser pulse. The shaped pulse that performs the computation is represented by a physical model of a 128–1024 channel pulse shaper. Pulse shapes are optimized with a standard genetic algorithm, yielding experimentally realizable computing pulses. The robustness of optimization is studied as a function of the vibrational states selected, rotational level structure, additional vibrational levels not assigned to the computation, and compensation for laser power variation across a molecular ensemble.     

Quantum control over isomerization of spiropyran (model potential)

The dynamics of the isomerization of spiropyran was simulated based on the two-well model potential. The possibility of effective control over the transition using phase-modulated (chirp-modulated) laser femtosecond pulses was studied. The probability of transitions to the A and B forms from the excited S ₁ state was evaluated at 1: 5; i.e., the efficiency of the transition reached 80%. It is phase the modulation of vibrational packets (purely quantum effect) that makes it possible to effectively control the behavior of the system, but one-parameter quartic modulation seemed not sufficient for total control.     

Modeling of dual fluorescence kinetics for 9-anthryl-substituted oligothiophenes

Expressions for time-dependent level populations in four- and five-level molecular models are obtained for the case of radiative and nonradiative decay from an initially populated state corresponding to the highest energy of the molecule. The two lowest energy levels in the models are assigned to vibrational levels of a molecular subsystem in the ground state; the others, to levels of the molecule in the excited electronic state. Examples of applying the obtained expressions to establish the formation mechanism for dual fluorescence pulses that accompany the phototransfer of a H-bond proton and other conformational transformations of molecules are presented.     

Quantum state measurement using coherent transients

We present the principle and experimental demonstration of time resolved quantum state holography. The quantum state of an excited state interacting with an ultrashort chirped laser pulse is measured during this interaction. This has been obtained by manipulating coherent transients created by the interaction of femtosecond shaped pulses and rubidium atoms.     

Selective preparation of ground state wave-packets: a theoretical analysis of femtosecond pump-dump-probe experiments on the potassium dimer

We present simulations on pump-dump-probe experiments performed on the potassium dimer. The interaction of two time-delayed laser pulses prepares vibrational wave packets in the electronic ground state. The quantum calculations reveal to what extent it is possible to prepare a ground state superposition of states with high versus low vibrational quantum numbers by changing the pump-dump delay time. It is shown that transient signals may exhibit interference effects which are due to characteristics of ground state wave-packets composed of two components showing different vibrational dynamics. In this way the signals are able to yield information about vibrational overtone motion. Received 27 September 2000 and Received in final form 21 November 2000     

CALCULATIONS OF STRETCHING VIBRATIONAL ENERGY LEVELS OF THE CH3I MOLECULE BY A NONLINEAR MODEL

A nonlinear model, i.e. the quantized discrete self-trapping equation, is applied to calculate the highly excited CH stretching vibrational energy levels of the CH₃I molecule in the liquid phase at the electronic ground state up to n=8. The obtained results agree well with the experimental data and with those obtained from local mode model calculations. We note that the dominant feature of the methyl CH stretching vibrational energy levels of the CH₃I molecule is a pattern of local mode pairs. When n≥7, all the vibrational energy of the CH₃ group can nearly be localized on a single CH bond.     

Spectral phase and amplitude interferometry for direct electric-field reconstruction

An extension of the well-known technique for spectral phase interferometry for direct electric-field reconstruction (SPIDER) has been developed that permits the reconstruction of the spectral amplitude and the spectral phase of ultrashort laser pulses from the acquisition of only one spectrum. Temporal intensity and temporal phase can therefore easily be retrieved. The characterization of pulses from a Ti:sapphire oscillator by use of an extended SPIDER is discussed. Advantages and drawbacks of the modified technique are also discussed.     

Mid-infrared electric field characterization using a visible charge-coupled-device-based spectrometer

We characterize ultrashort mid-infrared pulses through upconversion by using the stretched pulses obtained from the uncompressed output of a chirped-pulse amplifier. The power spectrum thus translated into the visible region can be readily measured with a standard silicon CCD camera-based spectrometer. The spectral phase is also characterized by a variant of zero-added-phase spectral phase interferometry for direct electric field reconstruction. This is a general method that provides a multiplex advantage over conventional infrared detector array-based methods.     

Local mode vibrations of water

Classical trajectory calculations on a realistic potential for the stretching vibrations of the water molecule are used to demonstrate the existence of stable local vibrational modes, which occur in degenerate pairs. The proportion of phase space occupied by such modes increases with increasing energy, with a clearly characterized (0, 2) local state in a local quantum number assignment. It is argued that quantum mechanical corrections will lead to a local mode splitting which is predicted to decrease in magnitude along any given stretching vibrational progression, and to be larger for a given quantum state of D₂O than for H₂O.     

Scheme for n phase gates operation and one-step preparation of highly entangled cluster state

In the system with superconducting quantum interference devices (SQUIDs) in a cavity, we propose a scheme for simultaneous implementing n phase gates and one step preparing the highly entangled cluster states based on the two-channel Raman interaction. In our scheme, the system is independent to the photon number of the cavity field, the cavity field can be initially in an arbitrary state, which is convenient for the experimental operation. The n phase gates operation and the cluster state generation are realized by using only the two lower flux states of the SQUID and the excited state would not be excited so that the influence of the decoherence due to spontaneous emission of the SQUID’s levels is possible to minimize. More importantly, the operation time of the phase gates is independent of the number n of the qubits. Finally, the experimental feasibility is also discussed in detail.     

Controlling vibrational excitation with shaped mid-IR pulses

We report selective population of the excited vibrational levels of the T(1u) CO-stretching mode in W(CO)(6) using phase-tailored, femtosecond mid-IR (5.2 microm, 1923 cm(-1)) pulses. An evolutionary algorithm was used to optimize specific vibrational populations. Stimulated emission peaks, indicative of population inversion, could be induced. Systematic truncation of each optimized pulse allowed for increased understanding of the excitation mechanism. The pulses and techniques developed herein will have broad applications in controlling ground state chemistry and enhancing vibrational spectroscopies.     

Control of motional states of a trapped ion

We propose a scheme to drive the vibrational motion of a trapped ion to an arbitrary quantum state from the vacuum state. In the scheme the ion is excited by a sequence of laser pulses tuned to the respective lower vibrational sidebands. Finally, the system evolves into a pure state given by the product of the ground electronic state with the desired vibrational state.