飞秒激光场中OCS分子的里德堡态激发

本文研究了800nm飞秒强激光场下OCS分子的里德堡态激发过程. 实验不仅观测到强激光场中的中性母体分子的里德堡态激发,而且观测到大量的中性里德堡态碎片. 我们测量了里德堡态激发产率随激光强度及椭偏率的变化,并与强场电离解离进行了比较. 分析表明,飞秒激光场下中性里德堡态碎片的产生与强场多次电离密切相关. 此外,我们还讨论了中性里德堡态碎片对激光椭偏率依赖的内在原因.     

Correlation of momenta of electrons and the nucleus in atoms

The process of resonant multiphoton ionization of a hydrogen atom in the ground 1s state is studied by direct numerical integration of the nonstationary Schrödinger equation for a quantum system in an electromagnetic field. The dependence of photoionization probability on the radiation intensity is found to be nonmonotonic. It is established that the minima of ionization correspond to multiphoton resonances between the ground state and one of the excited (Rydberg) atomic states perturbed by the laser field. It is shown that ionization is suppressed due to rearrangement of Rydberg states in a strong electromagnetic field and is accompanied by efficient Raman Λ transitions, which connect a set of closely lying Rydberg states via the continuum.     

Field ionization process of Eu 4f~76snp Rydberg states

The field ionization process of the Eu 4f76 snp Rydberg states, converging to the first ionization limit, 4f76s9S4, is systematically investigated. The spectra of the Eu 4f76 snp Rydberg states are populated with three-step laser excitation, and detected by electric field ionization(EFI) method. Two different kinds of the EFI pulses are applied after laser excitation to observe the possible impacts on the EFI process. The exact EFI ionization thresholds for the 4f76 snp Rydberg states can be determined by observing the corresponding EFI spectra. In particular, some structures above the EFI threshold are found in the EFI spectra, which may be interpreted as the effect from black body radiation(BBR). Finally, the scaling law of the EFI threshold for the Eu 4f76 snp Rydberg states with the effective quantum number is built.     

Intense interactions of molecules with a short-wavelength electromagnetic radiation field: II. Resonance scattering of radiation and fluorescence

Within the framework of the nonadiabatic approach developed in the preceding paper, the resonance scattering, resonance Raman scattering, and resonance fluorescence are studied in detail for diatomic and triatomic molecules, and polyatomic symmetric and antisymmetric top molecules, which interact with the field of short-wavelength radiation with a wavelength λ ≥ Å and an intensity up to 10¹⁴ W/cm². The coherent excitations of high-lying Rydberg and autoionizing states are taken into account. Analytical expressions for calculating the tensors and cross sections of the above processes are derived.     

Rydberg excitation of neutral nitric oxide molecules in strong UV and near-IR laser fields

Rydberg state excitations of neutral nitric oxide molecules are studied in strong ultraviolet(UV) and near-infra-red(IR) laser fields using a linear time-of-flight(TOF) mass spectrometer with the pulsed electronic field ionization method.The yield of Rydberg molecules is measured as a function of laser intensity and ellipticity,and the results in UV laser fields are compared with those in near-IR laser fields.The present study provides the first experimental evidence of neutral Rydberg molecules surviving in a strong laser field.The results indicate that a rescattering-after-tunneling process is the main contribution to the formation of Rydberg molecules in strong near-IR laser fields,while multi-photon excitation may play an important role in the strong UV laser fields.     

Local blockade of Rydberg excitation in an ultracold gas

In the laser excitation of ultracold atoms to Rydberg states, we observe a dramatic suppression caused by van der Waals interactions. This behavior is interpreted as a local excitation blockade: Rydberg atoms strongly inhibit excitation of their neighbors. We measure suppression, relative to isolated atom excitation, by up to a factor of 6.4. The dependences of this suppression on both laser irradiance and atomic density are in good agreement with a mean-field model. These results are an important step towards using ultracold Rydberg atoms in quantum information processing.     

Lifetimes of Rydberg states of Eu atoms

The radiative lifetimes of the Eu 4f76snp(8PJ or10PJ)Rydberg states with J=5/2 and 11/2 are investigated with a combination of multi-step laser excitation and pulsed electric field ionization,from which their dependence on the effective principal quantum number is observed.The lifetimes of 21 states are reported along with an evaluation of their experimental uncertainty.The influence of blackbody radiation,due to the oven temperature,on the lifetime of the higher-n states is detected.The non-hydrogen behavior of the investigated states is also observed.     

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.     

强场中NO分子回归谱的长程散射矩阵的理论研究

采用半经典散射矩阵方法研究外磁场中高里德伯态双原子分子在能量范围为77010—77050cm^-1的回归谱.通过引进模型势简化强磁场中NO分子的高里德伯电子的势函数,找出其在核转动量子数分别为N=1,3,5的三个通道中的闭合轨道,重点分析了强磁场中NO分子的长程散射矩阵元实部的傅里叶变换谱与闭合轨道之间的一一对应关系.     

分子里德伯态的电子能级结构——一些小分子及分子离子的里德伯能级结构

本文在独立电子近似的基础上,利用多重散射自洽场理论方法,计算了He₂,H₂等分子和He₂⁺分子离子的里德伯能级结构。根据分子的电子组态极限,确定了各里德伯系列初始态的主量子数,阐明了这些分子和分子离子里德伯能级结构的变化规律。理论计算的结果同已有的实验数据符合良好,从而为超越独立电子近似的计算打下了基础。     

Intense interactions of molecules with a short-wavelength electromagnetic radiation field: I. The fundamentals of the nonadiabatic theory

The intense interactions between short-wavelength (SW) electromagnetic radiation with a wavelength λ ≥ 1 Å and intensity up to 10¹⁴ W/cm² and simple and polyatomic molecules are studied with the coherent excitations of high-lying Rydberg and autoionizing states taken into account. The Hamiltonian of a system “molecule + SW radiation” is obtained by using the methods of quantum electrodynamics. Conditions for the applicability of the dipole approximation to describe the interactions of molecules with radiation of the UV, VUV, XUV, and soft X-ray range are found. The fundamentals of the theory of resonance scattering of SW radiation from diatomic, triatomic, and symmetric-and asymmetric-top polyatomic molecules are outlined.     

Ionization and stabilization of atoms in a high-intensity,low-frequency laser field

The dynamics of a model silver atom in the strong radiation field of a Ti:sapphire laser is studied in the Keldysh parameter regions γ ⩾ 1 and γ ⩽ 1. It is found that in the entire range of Keldysh parameter variations, along with ionization, the efficient excitation of Rydberg states of the atom with principal quantum numbers n = 6−14 is observed. A Rydberg wavepacket appearing in this case proved stable with respect to ionization; i.e., the atomic system in strong low-frequency electromagnetic fields becomes stable with respect to ionization. The physical reasons behind the stabilization are discussed.     

Efficient production of Rydberg positronium

We demonstrate experimentally the production of Rydberg positronium (Ps) atoms in a two-step process, comprising incoherent laser excitation, first to the 2(3)P state and then to states with principal quantum numbers ranging from 10 to 25. We find that excitation of 2(3)P atoms to Rydberg levels occurs very efficiently (~90%) and that the ~25% overall efficiency of the production of Rydberg atoms is determined almost entirely by the spectral overlap of the primary excitation laser and the Doppler broadened width of the 1 (3)S-2(3)P transition. The observed efficiency of Rydberg Ps production can be explained if stimulated emission back to the 2P states is suppressed, for example, by intermixing of the Rydberg state Stark sublevels. The efficient production of long-lived Rydberg Ps in a high magnetic field may make it possible to perform direct measurements of the gravitational free fall of Ps.     

The positronium atom as a benchmark for Rydberg excitation experiments in atomic physics

Positronium is a hydrogen-like pure leptonic atom that has gained great attention in basic physics for its role in antimatter studies, in quantum electrodynamics tests and in material science. Positronium spectroscopy is also an interesting research field, especially in the again unexplored region of Rydberg states, where motional effects turns out of overwhelming importance in determining the level structure, at variance with the usual Rydberg atomic spectroscopy. In this paper we present a simple theory of optical excitation of positronium high-n levels in strong magnetic fields, and determine the conditions for obtaining saturation of the transitions. It is shown that positronium atom can be an atomic physics benchmark for laser excitation experiments on Rydberg states in magnetic environments.     

Rovibrational-state-selected photoionization of acetylene by the two-color IR+VUV scheme: observation of rotationally resolved Rydberg transitions

We have demonstrated a rovibrational-state-selected photoionization experiment using an IR laser and high-resolution VUV-synchrotron radiation. The VUV photoionization of acetylene [C2H2(Xtilde; (1)Sigma(+)(g);nu(3)=1,J(')=8 or 10)] prepared by IR excitation reveals three strong autoionizing Rydberg series converging to C2H+2(Xtilde; (2)Pi(u);nu(+)(3)=1) with little ion background interference. Rotational transitions resolved for the Rydberg states provide an estimate of approximately 1.8 ps for their lifetimes. This experiment opens the way for state-selective photoionization studies of polyatomic molecules using VUV-synchrotron radiation.     

Laser diagnostics of the energy spectrum of Rydberg states of the lithium-7 atom

The spectra of excited lithium-7 atoms prepared in a magneto-optical trap are studied using a UV laser. The laser diagnostics of the energy of Rydberg atoms is developed based on measurements of the change in resonance fluorescence intensity of ultracold atoms as the exciting UV radiation frequency passes through the Rydberg transition frequency. The energies of various nS configurations are obtained in a broad range of the principal quantum number n from 38 to 165. The values of the quantum defect and ionization energy obtained in experiments and predicted theoretically are discussed.     

Ultrahigh frequency additional background radiation of the lower ionosphere during strong geomagnetic disturbances

In periods of high solar activity and the formation of geomagnetic storms, additional background incoherent ultrahigh frequency (UHF) radiation with decimeter to millimeter wavelengths in the high E and D layers of the Earth’s ionosphere is generated. This emission is produced by transitions between Rydberg states of atoms and molecules of atmospheric gases, which are excited by electrons and are surrounded by a neutral species of the medium. At present, there is no reliable information on the integrated intensity of UHF radiation in this wavelength range. This problem can be solved on knowledge of the dynamics of collisional and radiative quenching of Rydberg states and of the kinetics of their population in the lower ionosphere. An analysis of the available experimental data shows that the radiation is generated in an atmospheric layer located at altitudes between 50 and 110 km. The current theory is discussed and the ways of its further improvement connected with the development of more rigorous theoretical methods for describing the effect of neutral particles of medium on the collisional and radiative quenching dynamics, including the elementary processes with participation of the nitrogen and oxygen molecules, are suggested. For quantitatively estimates the influence of excited particles on the incoherent UHF radiation of the atmosphere, it is necessary carrying out of the preliminary calculations the potential energy surfaces and dynamics of nonadiabatic transitions between Rydberg states, construction the electronic wave functions, and determination the dipole moments of the allowed transitions and the emission line shapes. Obtained results can be included into the general kinetic scheme which defines of the UHF radiation intensity versus the density and temperature of the atmosphere. Accompanying its infrared (IR) radiation can be used to define of Rydberg states.     

Low-frequency strong-field ionization and excitation of hydrogen atom

The dynamics of hydrogen atom in the presence of a strong radiation field of the titanium-sapphire laser is studied for the Keldysh parameters γ ≥ 1 and γ ≤ 1. It is demonstrated that the ionization is supplemented with the effective population of the excited states with the principal quantum numbers n = 5–10 in the entire range of variation in the Keldysh parameter. The population of the excited Rydberg states can be interpreted as a consequence of the multiphoton resonance involving the initial 1s state and a group of excited states in the vicinity of the continuum boundary with the simultaneous repopulation of these states by Λ-type Raman transitions under the action of the laser field. The resulting coherent Rydberg packet appears to be stable with respect to ionization, so that the ionization of the atomic system in the presence of strong electromagnetic field is suppressed. Physical reasons for the stabilization are discussed. An interpretation of the effective population of the Rydberg states in the recent experiments on the ionization of atomic helium by the titanium-sapphire laser is proposed.     

Role of weak transitions in multiphoton excitation of molecules by IR laser radiation

Simultaneous excitation of a considerable part of molecules from many rotational levels of the ground state to higher vibrational states by IR laser radiation can be explained by considering weak transitions in a rotational band structure as it is shown at the example of SF₆ molecule. Very accurate compensation of anharmonicity in relatively wide spectral interval at comparatively low intensity of laser radiation can be explained on this basis. The considered scheme can be applied to the molecules of various symmetry with arbitrary anharmonicity.     

Sensitivity to anharmonicity of vibrational energy in a diatomic gasdynamic laser

A parameter for evaluating the sensitivity of quantum vibrational energy to anharmonicity in a diatomic gasdynamic laser is defined and calculated by considering the corresponding diatomic molecules as quantum anharmonic oscillators under an interatomic Morse potential. The variation of the above parameter in terms of the vibrational states and in terms of an involved anharmonic coefficient is discussed. In particular, the parameter in question at the classical limit is examined. Both weak and strong anharmonicities are discussed.