Isotope shifts and hyperfine structure in calcium 4snp and 4snf F Rydberg states

Isotope shifts and hyperfine structure have been measured in 4snp ¹ P₁ and Rydberg states for all stable calcium isotopes and the radioisotope ⁴¹Ca using high-resolution laser spectroscopy. Triple-resonance excitation via Rydberg state was followed by photoionization with a CO₂ laser and mass selective ion detection. Isotope shifts for the even-mass isotopes have been analyzed to derive specific mass shift and field shift factors. The apparent isotope shifts for ⁴¹Ca and ⁴³Ca exhibit anomalous values that are n-dependent. This is interpreted in terms of hyperfine-induced fine-structure mixing, which becomes very pronounced when singlet-triplet fine-structure splitting is comparable to the hyperfine interaction energy. Measurements of fine-structure splittings for the predominant isotope ⁴⁰Ca have been used as input parameters for theoretical calculation of the perturbed hyperfine structure. Results obtained by diagonalizing the second-order hyperfine interaction matrices agree very well with experimentally observed spectra. These measurements allow the evaluation of highly selective and sensitive methods for the detection of the rare ⁴¹Ca isotope. Received 17 December 1999 and Received in final form 29 March 2000     

Extracting generalized multiphoton ionization cross-sections from nonperturbative time-dependent calculations: An application in positronium

Ab initio time-dependent (TD) calculations of the behavior of positronium (Ps) under strong subpicosecond laser pulses are presented. The results are compared with results in H through scaling. It is found that a substantial amount of the population can be found in excited states after the pulse. In the perturbative regime, generalized multiphoton ionization cross-sections are extracted from the results of the time-dependent calculations. The generalized cross-sections are used to predict the response of Ps to nanosecond laser pulses at wavelengths of current experimental interest. Beyond the application to Ps, the generality of the method for extracting generalized cross-sections from TD nonperturbative calculations is discussed. Received 8 June 1999     

铯原子nP_(3/2)(n=70—94)里德伯态的紫外单光子激发及量子亏损测量

基于成熟的光纤激光器、光纤放大器及高效激光频率转换技术,我们在实验中研制了一套瓦级输出的窄线宽连续波单频可调谐318.6 nm紫外激光系统,并在室温铯原子气室中实现了6S_(1/2)—nP_(3/2)(n=70—94)单光子跃迁里德伯激发.借助由铯原子6S_(1/2)(F=4)基态、6P_(3/2)(F′=5)激发态和nP_(3/2)(n=70—94)里德伯态构成的V型三能级系统,通过频率锁定于铯原子6S_(1/2)(F=4)—6P_(3/2)(F′=5)超精细跃迁的852.3 nm探测光束的吸收减弱信号获得了里德伯态的信息,并利用高精度波长计测量了铯原子nP_(3/2)(n=70—94)里德伯态的量子亏损值.经过与理论计算值的变化趋势进行对比,我们认为由于原子气室的里德伯屏蔽效应并不能完全屏蔽外部直流电场,铯原子气室内存在残余的直流电场,影响了对里德伯态的量子亏损值的实验测量.利用残余直流电场的Stark效应理论模型及其与有效主量子数n*的依赖关系,对铯原子里德伯态的量子亏损实验测量值进行了修正.修正后的铯原子nP_(3/2)(n=70—94)态量子亏损测量值为3.5591±0.0007,与理论计算值相吻合.     

里德伯电磁感应透明中的相位

本文在典型的里德伯电磁感应透明系统中研究弱探测场在相互作用原子系统中的传播特性,重点关注基于偶极阻塞效应的探测场相位的合作光学非线性行为.通过与探测场透射率和光子关联作对比,发现相位的光学响应具有新特性:共振和Autler-Townes劈裂条件下相位对入射场强和初始光子关联不敏感,而在两者之间的频率范围内相位响应具有非线性特征,尤其在经典光频率处最显著.此外,提高主量子数和原子密度都会促进相位的非线性效应.综上,与探测场透射率和光子关联一样,相位可以作为合作光学非线性的另一个标识来刻画非线性现象,对里德伯电磁感应透明研究是一个有力的补充.     

紫外光解动力学DNCO+hv→D+NCO: 两个竞争解离通道

本文利用D原子里德堡态时间飞行谱研究了DNCO分子在波长200∽235 nm范围的光解动力学. 实验测量了产物的平动能分布和空间角分布. 在210∽235 nm光解离下,观测到接近统计分布和各向同性的产物,该产物有可能来自从S₁势能面内转换到S₀势能面,然后在S₀势能面上解离. 在更短的解离波长下,除了统计分布的产物,另外一种分布的产物出现在高平动能的地方,具有很高的各向异性,该产物来自从S₁势能面上的直接解离. 相比较HNCO的解离结果,DNCO直接解离通道出现在更高的激发能量. 通过对NCO产物内能态的归属,发现NCO产物主要是弯曲振动激发和适当的伸缩振动激}.     

超高碰撞能23.84 kJ/mol下反应F+D2→DF+D的交叉分子束研究

本文搭建了一套新的实验设备,首次将氢原子里德堡态标记的飞行时间谱技术与激光爆破束源技术相结合,进行超高碰撞能下化学反应的动力学研究. 初步进行了F+D₂→DF+D在超高碰撞能23.84 kJ/mol下的实验研究. 在研究中应用了两种类型束源：一类是通过激光爆破过程产生的高能F原子束源,另一类是通过液氮冷却脉冲阀而产生的D₂束源. 实验中探测了反应产物振动态分辨的微分散射截面. 结果显示,大部分反应产物DF主要呈现侧向和后向散射分布,而产物DF(v''=4)则主要分布在前向. 对前向散射产物DF(v''=4)的动力学来源进行了讨论.     

中性原子量子计算研究进展

相互作用可控、相干时间较长的中性单原子体系具备在1 mm2的面积上提供成千上万个量子比特的规模化集成的优势,是进行量子模拟、实现量子计算的有力候选者.近几年中性单原子体系在实验上取得了快速的发展,完成了包括50个单原子的确定性装载、二维和三维阵列中单个原子的寻址和操控、量子比特相干时间的延长、基于里德伯态的两比特量子门的实现和原子态的高效读出等,这些工作极大地推动了该体系在量子模拟和量子计算方面的应用.本文综述了该体系在量子计算方面的研究进展,并介绍了我们在其中所做的两个贡献:一是实现了"魔幻强度光阱",克服了光阱中原子退相干的首要因素,将原子相干时间提高了百倍,使得相干时间与比特操作时间的比值高达105;二是利用异核原子共振频率的差异建立了低串扰的异核单原子体系,并利用里德伯阻塞效应首次实现了异核两原子的量子受控非门和量子纠缠,将量子计算的实验研究拓展至异核领域.最后,分析了中性单原子体系在量子模拟和量子计算方面进一步发展面临的挑战与瓶颈.     

利用自电离探测技术研究Sm原子Rydberg态光谱

采用孤立实激发与自电离探测技术相结合的方法对Sm原子偶宇称高激发态进行了系统研究.按照不同的自电离通道将所测数据进行了分类和比较,并进行了详细讨论.不仅报道了许多收敛于不同电离限的Rydberg态的能级位置和跃迁的相对强度等信息,而且还把处于同一能域内的Rydberg态和价态进行了辨识.另外,不但提供了一种有效识别不同类型的高激发态的鉴别技术,而且还对处于41800 cm^-1到43800 cm^-1能域内的Rydberg态和价态的光谱特性进行了详细分析和讨论. 关键词： 自电离探测 Rydberg态 Sm原子     

Electronic states of neutral and ionized tetrahydrofuran studied by VUV spectroscopy and ab initio calculations

The electronic spectroscopy of isolated tetrahydrofuran (THF) in the gas phase has been investigated using high-resolution photoabsorption spectroscopy in the 5.8–10.6 eV with absolute cross-section measurements derived. In addition, an electron energy loss spectrum was recorded at 100 eV and 10° over the 5–11.4 eV range. The He(I) photoelectron spectrum was also collected to quantify ionisation energies in the 9–16.1 eV spectral region. These experiments are supported by the first high-level ab initio calculations performed on the excited states of the neutral molecule and on the ground state of the positive ion. The excellent agreement between the theoretical results and the measurements allows us to solve several discrepancies concerning the electronic state spectroscopy of THF. The present work reconsiders the question of the lowest energy conformers of the molecule and its population distribution at room temperature. Electronic supplementary material  Supplementary Online Material