Dynamical analysis of the effect of elliptically polarized laser pulses on molecular alignment and orientation

In this Letter, we study the molecular alignment and orientation driven by two elliptically polarized laser pulses.It is shown that the field-free molecular alignment can be achieved in a three-dimensional(3D) case, while the field-free molecular orientation is only along the x and y directions, and that the field-free alignment and orientation along different axes are related to the populations of the rotational states. It is demonstrated that changing the elliptic parameter is efficient for controlling both in-pulse and post-pulse molecular alignment and orientation. The delay time also has an influence on the field-free molecular alignment and orientation.     

Optical control of the rotational angular momentum of a molecular Rydberg wave packet

An intuitive scheme for controlling the rotational quantum state of a Rydberg molecule is demonstrated experimentally. We determine the accumulated phase difference between the various components of a molecular electron wave packet, and then employ a sequence of phase-locked optical pulses to selectively enhance or depopulate specific rotational states. The angular momentum composition of the resulting wave packet, and the efficiency of the control scheme, is determined by calculating the multipulse response of the time-dependent Rydberg populations.     

Cs(6 ~2D_(5/2))与H_2反应生成的CsH分子的转动和振动态分布

利用激光泵浦-探测技术,在样品池条件下,研究了Cs(6D5/2)态与H2反应生成的CsH分子基电子态的转动和振动的量子态分布。在Cs-H2混合蒸气中,脉冲激光双光子激发Cs(6D5/2)态,另一台调频脉冲激光器扫描CsHX1Σ+(v″,J″)→A1Σ+(v′,J′=J″±1)吸收线,发现CsH分子只有v″=0和1上的振动带上有布居而不布居在v″1的振动带上。v″=0和1上的转动带分布呈现单峰结构,其峰值位于J″=6～8处,转动带分布轮廓与池温下的统计分布接近。转动Boltzmann温度分别为(458±20)K(对v″=1)和(447±18)K(对v″=0),得到的CsH分子的转动温度稍低于池温。从转动态分布得到v″=1与v″=0上布居数之比约为0.897,从而计算出CsH基电子态上的平均转动能ER和平均振动能EV,有效能减去平均振转能得到平均平动能ET。CsH分子3种能量的相对比值fT∶fV∶     

Field-free molecular orientation induced by combined femtosecond single- and dual-color laser pulses：The role of delay time and quantum interference

The coherent control of field-free molecular orientation of CO with combined femtosecond single- and dual-color laser pulses has been theoretically studied. The effect of the delay time between the femtosecond single- and dual-color laser pulses is discussed, and the physical mechanism of the enhancement of molecular orientation with pre-alignment of the molecule is investigated. It is found that the basic mechanism is based on the creation of a rotational wave packet by the femtosecond single-color laser pulse. Furthermore, we investigate the interference between multiple rotational excitation pathways following pre-alignment with femtosecond single-color laser pulse. It is shown that such interference can lead to an enhancement of the orientation of CO molecule by a factor of 1.6.     

Carbon Monoxide Triplet Rydberg Series in the f Complex Region

Using a multistep state-selective excitation scheme, fluorescence-dip spectra of carbon monoxide have been recorded in the energy region between 106 100 and 112 200 cm(-1). Prominent groups of bands were tentatively identified as transitions into the 6f em leader10f (v=0) and 9psigma em leader11psigma (v=0) triplet Rydberg series. For the f complex states, molecular constants have been calculated. The triplet f levels show an unusually large rotational constant and are located at higher energies than their singlet counterparts. Copyright 2001 Academic Press.     

CO_2在与高振动激发NaH碰撞中的量子态分辨能量再分配

利用简并受激超拉曼泵浦激发NaH基态到高位振动态(ν″=14,J″=20)。研究了NaH(14,20)与CO_2(00°0)间的振转能量转移。利用吸收系数和瞬时Doppler线宽,得到不同池温下NaH(14,20)分子密度,测量CO_2(00°0,J)与NaH高振动态碰撞前后的瞬时泛频激光感应荧光谱线的相对强度,确定了CO_2(00°0,J=2~80)的初生态布居,它们呈现双指数转动分布。拟合实验数据得到两个转动温度T_(rot)=(650±80)和(1 531±150)K。较冷的分布约占CO_2(00°0)的79%,它是由弹性或弱非弹性碰撞产生的,因而CO_2只有很小的转动激发。另有21%的CO_2(00°0)较大地增加了转动能,故有较热的转动温度。对碰撞产生的CO_2(00°0,J)进行高分辨率瞬时泛频荧光谱线的轮廓测量,得到各转动态平移能的改变。对于CO_2(00°0,J=56~80),转移能从582cm~(-1)(对于J=60)增加到2 973cm~(-1)(对于J=80)。探测转动态布居数的改变,得到各转动态的产生速率系数k_(app)~J之和为(7.2±1.8)×10~(-10) cm~3·mol~(-1)·s~(-1),而平均倒空速率系数〈kdep〉=(6.9±1.7)×10~(-10)cm~3·mol~(-1)·s~(-1)。     

Field-Free Molecular Orientation Generated from Cyclic Rotational States by Using Two Trains of Half-Cycle Pulses

We show that two trains of half-cycle pulses （HCPs） with different amplitudes irradiating alternately on polar molecules can achieve a remarkable enhancement of field-free orientation compared with the case of an equal amplitude HCPs train for the same pulse separation. optimal adjustment of the population distribution on This kind of orientation enhancements is mainly due to an every field-free angular momentum eigenstate, in which the populations on the undesired states of high angular momenta are effectively suppressed, and the populations on the desired states of low angular momenta are correspondingly promoted.     

Molecular photodetachment microscopy

The photodetachment microscopy technique, which was originally used with atomic negative ions, is now applied to a molecular anion. The interferograms of several rotational thresholds corresponding to transitions from OH- X (1)Sigma(+) v=0 states to OH X (2)Pi(3/2,1/2) v=0 states have been recorded. No effect due to the 1/r(2) dipolar potential of the neutral molecule appears. Using a double-pass scheme of the laser on the negative ion beam, we measure the energy of the first few detachment thresholds with improved accuracy. The new recommended value of the electron affinity of 16OH is 14,740.996(13) cm(-1), or 1.827 650 3(17) eV.     

硝基甲烷与硝基乙烷266 nm光解动力学

利用单光子激光诱导荧光技术，在硝基甲烷与硝基乙烷气相条件下266 nm光解过程中，对初生态的解离产物OH进行了测量．结果表明，两个解离过程中产生的初生态OH都没有振动激发．硝基甲烷光解过程中产生的OH的转动分布可以用玻尔兹曼温度简单的表示，相对于自旋轨道分裂的2|3=2与2|1=2两个态，其转动温度分别为2045§150与1923§150 K．硝基乙烷光解过程中产生的OH不是简单的玻尔兹曼分布，因此不能用玻尔兹曼温度来描述，这一结果 意味着硝基甲烷与硝基乙烷在生成OH的过程中经历了不同的解离过程．硝基甲烷     

Blackbody-radiation-assisted laser cooling of molecular ions

The translational motion of molecular ions can be effectively cooled sympathetically to temperatures below 100 mK in ion traps through Coulomb interactions with laser-cooled atomic ions. The distribution of internal rovibrational states, however, gets in thermal equilibrium with the typically much higher temperature of the environment within tens of seconds. We consider a concept for rotational cooling of such internally hot, but translationally cold, heteronuclear diatomic molecular ions. The scheme relies on a combination of optical pumping from a few specific rotational levels into a "dark state" with redistribution of rotational populations mediated by blackbody radiation.     

Active manipulation of the selective alignment by two laser pulses

This paper solves numerically the full time-dependent Schrdinger equation based on the rigid rotor model, and proposes a novel strategy to determine the optimal time delay of the two laser pulses to manipulate the molecular selective alignment. The results illustrate that the molecular alignment generated by the first pulse can be suppressed or enhanced selectively, the relative populations of even and odd rotational states in the final rotational wave packet can be manipulated selectively by precisely inserting the peak of the second laser pulse at the time when the slope for the alignment parameter by the first laser locates a local maximum for the even rotational states and a local minimum for the odds, and vice versa. The selective alignment can be further optimised by selecting the intensity ratio of the two laser pulses on the condition that the total laser intensity and pulse duration are kept constant.     

基于ab initio的BD~+离子激光冷却理论研究

基于相关一致基组aug-cc-pV5Z,采用内收缩多参考组态相互作用方法计算了BD~+离子两个最低解离极限B~+(~1Sg)+D(~2Sg)和B+(~3Pu)+D(~2Sg)对应的5个Λ—S态(X~2Σ~+,A~2Π,B~2Σ+,a~4Π和b~4Σ~+)的势能曲线和跃迁偶极矩.根据计算结果,求解核运动的径向薛定谔方程得到相应电子态的振-转光谱常数、Franck-Condon(F-C)因子和振动能级辐射寿命.其中A~2Π—X~2Σ~+的F-C因子(f_(00)=0.923)、辐射寿命(τ=235 ns)满足激光直接冷却的条件.因此,我们基于分子转动跃迁提出了一个可实现Doppler激光冷却的光循环方案:A~2Π_(1/2)(υ′=0)—X~2Σ+(υ′′=0,1),其中υ′=0中包含2个转动能级,υ′′=0和υ′′=1中分别包含6个和4个转动能级.根据方案,模拟了激光冷却过程中的分子布居数动力学变化过程,并计算了初速度为100 m/s的BD~+,历经5.4 ms散射1150个光子可减速到4.6 m/s、温度为13 mK.     

Photodissociation and rotational coherence

The rotational coherence of an ensemble of photodissociation fragments is studied in the absence of collisions. Formulas for quantum orientation correlation functions are obtained for the case when parent molecules and their fragments are asymmetric tops and the predissociation time is much shorter than the characteristic time of rotational reorientation. It is shown that photodissociation does not affect periods of a rotational echo, but the structure of the echo pulses (their shape and width) depends substantially on the features of rotational excitation of photofragments upon photodissociation.     

Efficient coherent population transfer among three states in NO molecules by Stark-Chirped rapid adiabatic passage

We present the experimental demonstration of a novel, efficient, and selective technique to prepare population inversion. The technique is an extension of Stark-chirped rapid adiabatic passage (SCRAP), i.e., SCRAP among three states. In this process a Lambda-type quantum system is driven by two laser pulses, the pump and Stokes pulses, which are appropriately detuned from transition frequencies. A third laser pulse induces a dynamic Stark shift in the upper energy level, and the timing of all three pulses is controlled in order to prepare population inversion between the two lower states in the Lambda-type level scheme. Our data on population transfer in nitric oxide (NO) molecules clearly show that SCRAP among three states provides an advantageous alternative to such techniques as stimulated Raman adiabatic passage.     

Rotational and vibrational excitation of sputtered diatomic molecules

The rotational and vibrational level population distributions of ground and electronically excited states of several homonuclear and heteronuclear molecules are calculated for direct ejection, association, and associative ionization mechanisms of molecule sputtering. The cascade properties, formation mechanism, initial atom separation, and axis orientation to the surface are clearly reflected in the sputtered molecule distributions. In general, extensive non-Boltzmann rotational and vibrational distributions are predicted. The probability that an atom pair survives the ejection, for typical sputtering parameters, is high; approximately 50% for homonuclear molecules to near 100% for hydrides. The predictions are compared with experimental optical emission spectra in the accompanying paper.     

Optical control of the quantum-state distribution of vibrational wave packets using trains of phase-locked pulses

An intuitive scheme for controlling the quantum state composition of one-coordinate molecular wave packets is developed. The accumulated phase difference between the various components of the molecular wave packet is determined, and then a sequence of phase-locked optical pulses is employed to selectively enhance or depopulate specific vibrational states, or sets of vibrational states. The quantum state composition of the resulting wave packet, and the efficiency of the control scheme, is determined by calculating the multi-pulse response of the time-dependent vibrational state populations.     

Normal modes of a probe field in the pulsed regime of electromagnetically induced transparency in a Λ-scheme of degenerate quantum transitions

The effect of separation of linearly polarized short probe pulses of electromagnetically induced transparency in the field of linearly polarized coupling radiation is modeled numerically. It is shown that the input-probe pulses polarized parallel or perpendicular to the input-probe field propagate in the medium without changing the state of their polarization. If the input-probe radiation is weak compared to the coupling radiation, then the probe field inside the medium is the sum of two independently propagating linearly polarized normal modes, which are excited by the projections of the input-probe pulse onto the direction of polarization of the coupling radiation and onto the perpendicular direction, respectively. The normal modes have the same phase velocities, but different velocities of their real envelopes. This circumstance leads to the rotation of the plane of polarization of the total probe field at short distances and to its separation into two pulses with mutually perpendicular directions of polarization at long distances. At a high intensity of the probe radiation, the input-probe pulse decays into pulses the planes of polarization of which are not mutually perpendicular. Under these conditions, it is impossible to represent the probe radiation as a sum of normal modes. The modeling is performed in the scheme of degenerate quantum transitions between states of levels ³ P ₀, ³ P ₁ ⁰, and ³ P ₂ of isotope ²⁰⁸Pb taking into account the Doppler broadening of spectral lines.     

Round-Robin Differential Phase Shift with Heralded Single-Photon Source

Round-robin differential phase shift(RRDPS) is a novel quantum key distribution protocol which can bound information leakage without monitoring signal disturbance. In this work, to decrease the effect of the vacuum component in a weak coherent pulses source, we employ a practical decoy-state scheme with heralded singlephoton source for the RRDPS protocol and analyze the performance of this method. In this scheme, only two decoy states are needed and the yields of single-photon state and multi-photon states, as well as the bit error rates of each photon states, can be estimated. The final key rate of this scheme is bounded and simulated over transmission distance. The results show that the two-decoy-state method with heralded single-photon source performs better than the two-decoy-state method with weak coherent pulses.     

Lifetime Measurements of the DΠ State of HfS and the bΠ1 State of HfO

Lifetime measurements of individual rotational levels in excited states of hafnium oxide and hafnium sulfide have been performed using population probing by resonant two-photon ionization in a molecular beam. For the b³Π₁ state of HfO rotational levels in the vibrational level v=0 were found to have lifetimes in the region 650-700 ns. For the D¹Π state of HfS rotational level lifetimes in the vibrational levels v=0 and v=1 were determined to be around 240 ns. The technique used here provides very accurate results and the uncertainty in the reported values is only about 2%. Possible sources of errors are examined. The absorption oscillator strengths from the ground state are calculated.     

Cyclic State Orientation of Polar Molecules Produced by a Train of Half-Cycle Pulse Clusters of a Long Repetition Period

Using a variational method, we derive the optimal population distribution of angular momentum eigenstates for any given population range in a rotational wavepacket within the field-free cyclic state orientation framework. Correspondingly, we devise a train of half-cycle pulse clusters to purposively make the structure of the computed wavepacket approach the optimal population distribution, so that we can now utilize much more powerful means to realize an ideal orientation goal.