The controlled excitation of forbidden transitions in the two-photon spectrum of strontium by using collisions and electric fields

We present experimental results involving controlled configuration mixing in two-photon spectroscopy of highly-excited states by exploiting a weak external electric field and collisions. The method has allowed new extensions to high members of the two-photon forbidden J = 3 odd-parity 5snf ¹F₃ and the J = 0, even-parity 5sns ¹S₀ Rydberg series of neutral strontium to be observed. We achieve resonant two-photon transverse excitation of a high density atomic jet by using a narrow bandwidth tunable dye laser in a heat pipe setup with sensitive ionization detection. Experimental term values are extended for the 5sns ¹S₀ series up to n = 46. By suitable exploitation of the composition and pressure of the buffer gases in conjunction with the electric field strength in the excitation region and the exciting laser beam intensity we have also extended observations up to n = 44 for the 5snf ¹F₃ series and up to n = 46 for the 5snp ¹P₁ series. Our results demonstrate a novel and remarkably simple experimental method to access high Rydberg states to which transitions are forbidden from the ground state by parity and other selection rules.     

Atomic jet with ionization detection for laser spectroscopy of Rydberg atoms under collisions and fields

An efficient atomic jet setup offering many unprecedented advantages over a conventional heat pipe setup used in multi-photon spectroscopy, mainly of alkaline-earth metals, has been constructed by a scheme in which the sample material is encapsulated in a disposable cartridge oven located inside a thermally stabilised heat-pipe and is made to effuse in to a row of atomic beams merging to form a jet target. This novel scheme combines the advantages of both high density atomic beam with convenient geometry for orthogonal excitation and high sensitive ionisation detection capabilities of thermionic diodes, besides eliminating several problems inherent in the usual heat-pipe operation. Out of various designs, typical results are presented for a linear heat-pipe with vertical atomic jet used in two-photon spectroscopy of highly excited states of Sr I. Controlled excitations of both Rydberg and non-Rydberg states, which cannot otherwise be accessed from the ground state due to parity and spectroscopic selection rules, have been achieved by employing a weak electric field complimented by collisions. The atomic jet setup is also found very useful for the study of collisional broadening and shift of excited states and time evolution of Rydberg atoms. PACS 32.80.Rm     

Two-color three-photon excitation studies of thallium Rydberg states

We present new data on the even-parity Rydberg states of atomic thallium using two-step three-photon laser excitation technique in conjunction with a thermionic diode ion detector. Atoms are excited from the 6p ²P_1/2 ground state to the 7p ²P_1/2 intermediate state via two-photon excitation and subsequently promoted to the high lying ns ² S_1/2 and nd ²D_3/2 Rydberg states. The first ionization potential of thallium is determined as 49,266.66(1) cm^-1 using data for the ns ² S_1/2 (25 ≤ n ≤ 54) and nd ²D_3/2 (24 ≤ n ≤ 65) Rydberg series. This value is believed to be more accurate because the contribution due to the hyperfine structure splitting of the 7p ²P_1/2 state (0.07185 cm^-1) is much smaller as compared to that of the 6p ²P_1/2 ground state (0.711 cm^-1).     

Investigation of the 6p 2(3 P 0)n p Rydberg series of bismuth by multiphoton excitation

Rydberg states of the odd-parity series 6p ²(³ p ₀)n p of BiI are excited by a three-photon process. A two-photon dissociation of Bi₂ into excited atomic states followed by a one-photon absorption leads to highly excited atomic Rydberg states up ton = 32. States of the even-parity Rydberg series 6p ²(³ p ₀)nsJ=1/2,ndJ=3/2 andndJ=5/2 are also observed. In order to avoid the background caused by ionization of the bismuth molecules we performed a two-color excitation with pulsed dye lasers. With this experiment the 6p ²(³ p ₀)npJ=3/2 Rydberg series could be resolved up ton=75. The increasing quantum defect of this series is due to a perturbing state close to the first ionization limit. By a MQDT analysis we obtain the energy of the perturbing state and a value of 58,761.68±0.1 cm^?1 for the first ionization limit of atomic bismuth.     

The break of L-S coupling and the double Stark resonance in the spectrum of 36P → 37P two-photon transition in Rydberg atoms of sodium

New results are presented of an experimental investigation of the spectrum of 36P → 37P two-photon microwave transition in Rydberg atoms of sodium in a constant electric field. Depending on the conditions of excitation of the initial 36P state (the constant electric field is switched on either before or after the exciting laser pulse) and polarization of laser radiation, a strong variation is observed of the amplitudes of individual two-photon transitions between the fine-structure Stark components of the 36P and 37P states. This effect is an analog of the Paschen-Back effect in a strong magnetic field and is due to the break of L-S coupling and to the variation of the wave functions of Rydberg electrons in an electric field. It is also found that the break of L-S coupling affects considerably the shape of double Stark resonance arising upon intersection of the virtual intermediate level of two-photon transition with the real intermediate 37S level.     

Continuous wave field ionization laser spectroscopy

A new technique is described which allows Doppler-free, isotope-selective excitation of atoms by continuous wave laser radiation and continuous ionization of the atoms by an electric field. The atoms are excited to high Rydberg states in an electric-field-free region of a collimated atomic beam. Because the lifetimes of Rydberg atoms are long they can reach a spatially separated region of the atomic beam where they are ionized by a continuous electric field with a probability of unity. In the case of lithium we obtained a 10³ times larger ion signal by field ionization of Rydberg atoms than by direct photoionization from low excited states.     

Three-photon resonance enhanced excitation spectrum of atomic thallium

We present first measurements on the resonance enhanced three-photon excitation in thallium, using a Nd:YAG laser pumped dye laser in conjunction with a thermionic diode ion detector. The even-parity 6s²ns²S_1/2 (15 ? n ? 31) and nd ²D_5/2 (13 ? n ? 42) Rydberg states have been observed. The measured level energies reveal a dynamic shift from the photoabsorption values, which is decreasing with increasing n, while the asymmetry in the line profile is observed to be increasing with increasing n. In addition, an autoionising level (sp²⁴P_3/2) adjacent to the ionization threshold has been observed and quantitatively analyzed using the Fano’s photoionization cross-section relation for an isolated autoionising resonance.     

Three photon resonant ionization in atomic potassium via S,P, D and F series Rydberg states

Single colour three photon resonant ionization (2 + 1) is observed in atomic potassium vapour in a heat pipe oven using an excimer laser pumped dye laser. Using wavelengths between 570 nm and 603 nm various²S and²D Rydberg states are populated by two photon excitation. Third photon of the same wavelength ionizes the atoms. Rydberg states up ton ⋍ 50 are observed. Electric field as low as 1 V/cm causes extensive Stark mixing of the states. This results in progressively higher three photon ionization signals via the perturbed²P and²F Rydberg states. The three photon ionization process is studied using both linearly and circularly polarized incident light. The experiment shows qualitatively that the²P Rydberg states are perturbed primarily by the²D states in the prescence of an external electric field and to a much smaller extent by²S states. This is also explained theoretically by calculating the Stark mixing coefficients under the Bates and Daamgard (1949) approximation. Implication for a similar effect in other alkali elements is discussed.     

Electric field induced hyperfine level-crossings in (nD)Cs at two-step laser excitation: Experiment and theory

The pure electric field level-crossing of m_F Zeeman sublevels of hyperfine F levels at two-step laser excitation is described theoretically and studied experimentally for the nD_3/2 states in Cs with n = 7, 9 and 10, by applying a diode laser in the first 6S_1/2 → 6P_3/2 step and a diode or dye laser for the second 6P_3/2 → nD_3/2 step. Level-crossing resonance signals are observed in the nD_3/2 → 6P_1/2 fluorescence. A theoretical model is presented to describe quantitatively the resonance signals by correlation analysis of the optical Bloch equations in the case when an atom simultaneously interacts with two laser fields in the presence of an external dc electric field. The simulations describe well the experimental signals. The tensor polarizabilities α₂ (in ) are determined to be 7.45(20) × 10⁴ for the 7D_3/2 state and 1.183(35) × 10⁶ for the 9D_3/2 state; the electric field calibration is based on measurements of the 10D_3/2 state, for which α₂ is well established. The α₂ value for the 7D_3/2 state differs by ca. 15% from the existing experimentally measured value.     

Enhanced four-wave mixing in mercury isotopes, prepared by stark-chirped rapid adiabatic passage

We demonstrate significant enhancement of four-wave mixing in coherently driven mercury isotopes to generate vacuum-ultraviolet radiation at 125 nm. The enhancement is accomplished by preparation of the mercury atoms in a state of maximum coherence, i.e. maximum nonlinear-optical polarization, driven by Stark-chirped rapid adiabatic passage (SCRAP). In this technique, a pump laser at 313 nm excites the two-photon transition between the ground state 6s²¹S₀ and the target state 7s ¹S₀ in mercury. A strong, off-resonant radiation field at 1064 nm generates dynamic Stark shifts. These Stark shifts serve to induce a rapid adiabatic passage process on the two-photon transition. During the process a coherent superposition of the two states is established, which enhances the nonlinear-optical polarization in the medium to the maximum possible value. The maximum coherence permits efficient four-wave mixing of a pump laser and an additional probe laser at 626 nm. The efficiency is further enhanced, as the SCRAP process allows to stimulate the complete set of different mercury isotopes to participate in the frequency conversion process. This enlarges the effective atomic density of the medium. Thus, we observe the generation of vacuum-ultraviolet radiation at 125 nm enhanced by more than one order of magnitude with respect to conventional frequency conversion. Parallel to the frequency conversion process, we monitored the evolution of the population in the medium by laser-induced fluorescence. These data demonstrate efficient coherent population transfer by SCRAP.     

Spectroscopic characterization of the potential energy functions of Ne2 Rydberg states in the vicinity of the Ne(S0) + Ne(4p′) dissociation limits

The gerade autoionizing Rydberg states of Ne₂ have been studied in the range 162 000-172 000 cm⁻¹ by 1 + 1′ resonant two-photon excitation from the Ne₂ X ground state via different vibrational levels of the Ne₂ C state. A rotationally resolved part of the spectrum allowed the determination of the potential energy functions of two states of 1_g and characters in the vicinity of the Ne(2p⁶¹S₀) + Ne (2p⁵4p′) dissociation limit. The presence of maxima in these potential energy functions is interpreted as originating from a repulsive interaction between the Rydberg electron and the neutral atom.     

Multi-step laser excitation of the highly excited states of zinc

We report experimental data on the highly excited states of zinc in the energy range 74,625-75,740 cm⁻¹ using two-step laser excitation scheme in conjunction with a thermionic diode ion detector. The 4s4p ³P₁ inter-combination level at 32501.399 cm⁻¹ was populated using a frequency doubled dye laser. The 4s5s ³S₁ level at 53672.28 cm⁻¹ gets populated from the ASE (amplified spontaneous emission) of the second step dye laser. The Rydberg series 4snp ³P₂ (12 ? n ? 60), 4snp ¹P₁ (16 ? n ? 30) and parity forbidden transitions 4sns ³S₁ (19 ? n ? 44) have been observed. A two parameter fit to excitation energies of the observed series yields the binding energy of the 4s5s ³S₁ level as 22097.03 ± 0.03 cm⁻¹ and consequently, the first ionization potential of zinc is determined as 75769.31 ± 0.05 cm⁻¹, that is in excellent agreement with the earlier work.     

A three-step laser stabilization scheme for excitation to Rydberg levels in <Superscript>85</Superscript>Rb

We demonstrate a three-step laser stabilization scheme for excitation to nP and nF Rydberg states in ⁸⁵Rb, with all three lasers stabilized using active feedback to independent Rb vapor cells. The setup allows stabilization to the Rydberg states 36P_3/2–70P_3/2 and 33F_7/2–90F_7/2, with the only limiting factor being the available third step laser power. We study the scheme by monitoring the three laser frequencies simultaneously against a self-referenced optical frequency comb. The third step laser, locked to the Rydberg transition, displays an Allan deviation of 30 kHz over 1 second and <80 kHz over 1 hour. The scheme is very robust and affordable, and it would be ideal for carrying out a range of quantum information experiments.     

Measurements of photoionization cross sections from the 4p, 5d and 7s excited states of potassium

New measurements of the photoionization cross sections from the 4p ²P_1/2,3/2, 5d ²D_5/2,3/2 and 7s ²S_1/2 excited states of potassium are presented. The cross sections have been measured by two-step excitation and ionization using a Nd:YAG laser in conjunction with a thermionic diode ion detector. By applying the saturation technique, the absolute values of the cross sections from the 4p ²P_3/2 and 4p ²P_1/2 states at 355 nm are determined as 7.2±1.1 and 5.6±0.8 Mb, respectively. The photoionization cross section from the 5d ²D_5/2,3/2 excited state has been measured using two excitation paths, two-step excitation and two-photon excitation from the ground state. The measured values of the cross sections from the 5d ²D_5/2 state by two-photon excitation from the ground state is 28.9±4.3 Mb, whereas in the two-step excitation, the cross section from the 5d ²D_3/2 state via the 4p ²P_1/2 state and from the 5d ²D_5/2,3/2 states via the 4p ²P_3/2 state are determined as 25.1±3.8 and 30.2±4.5 Mb, respectively. Besides, we have measured the photoionization cross sections from the 7s ²S_1/2 excited state using the two-photon excitation from the ground state as 0.61±0.09 Mb.     

NO分子里德伯态O~(''''2)Ⅱ~-的双子光激发谱

通过对NO分子的里德伯态O′~2∏~-(v=0)双光子激发谱的转动分析,计算出了该能级的光谱常数;并研究了它与非里德伯态B~2∏之间的相互作用现象。     

Coherent excitation of Rydberg atoms in an ultracold gas

We demonstrate two schemes for the coherent excitation of Rydberg atoms in an ultracold gas of rubidium atoms employing the three-level ladder system 5S_1/2-5P_3/2-n?_j. In the first approach rapid adiabatic passage with pulsed laser fields yields Rydberg excitation probabilities of 90% in the center of the laser focus. In a second experiment two-photon Rydberg excitation with continuous-wave fields is applied which results in Rabi oscillations between the ground and Rydberg state. The experiments represent a prerequisite for the control of interactions in ultracold Rydberg gases and the application of ultracold Rydberg gases for quantum information processing.     

双光子激发NO分子里德伯态H~(''''2)Ⅱ~-的光谱研究

本文采用激光双光子激发的方法对NO分子的里德伯态H~(12)Ⅱ-(v=1,2)进行了研究,得到了该能级的光谱常数;观测到了H~(12)Ⅱ-与非里德伯态B~2Ⅱ之间的相互作用现象,并计算出了相应的转动能级位移;研究了H~(12)Ⅱ-能级的主要荧光跃迁通道。     

Impact broadening and shifts for 6sns 1S0 and 6snd 1D2 series of barium

Impact broadening and shifts of Ba transitions to parity forbidden Rydberg states have been measured using two-photon laser spectroscopy techniques. Broadening and shift rates for the 6sns ¹S₀ (10 < n < 19) and 6snd ¹D₂ (8 < n < 26) levels due to thermal collisional interactions with Xe, Kr and Ar as perturber gases are plotted. Perturbations due to configuration interactions are discussed.     

Thermal stability and spectroscopic properties of Er-doped lead fluorogermanate glasses

The thermal characterization and spectroscopic properties of Er³⁺-doped 0.6GeO₂-(0.4-x)PbO-xPbF₂ glasses were investigated experimentally. With the replacement of PbO by PbF₂ the thermal stability of glasses is improved and the infrared fluorescence intensity at 1530 nm is increased. The Judd-Ofelt intensity parameters, radiative transition rates, and fluorescence lifetimes of the excited ⁴I_13/2 level of Er³⁺ ions were calculated from Judd-Ofelt theory. The asymmetric ligand field around Er³⁺ ions resulted from the incorporation of PbF₂ into germanate glasses, broadens the infrared emission spectra at 1530 nm. Upconversion luminescence in the investigated glasses was observed at room temperature under the excitation of 976 nm laser diode. The glass 0.6GeO₂-0.3PbO-0.1PbF₂ exhibits the maximum upconversion emission intensity, while no frequency upconversion luminescence was observed in the 0.6GeO₂-0.4PbO glass. The quadratic dependence of the green and red emissions on excitation power indicates that two-photon absorption contributes to the visible emission under the 976-nm excitation.     

Laser spectroscopy of holmium monosulphide: Electronic, vibrational and rotational structure of the A[14.79]8.5-X8.5, A[14.79]8.5-W[0.25]7.5 and A[14.79]8.5-V[0.98]7.5 transitions

Laser induced fluorescence spectra of HoS have been obtained using a Broida oven and a ring dye laser. Dispersed fluorescence spectra showed transitions from a common upper state, A[14.79]8.5 to the v = 0 and 1 vibrational levels of three low lying states, labelled X8.5, W[0.25]7.5 and V[0.98]7.5 (the states are labelled [10⁻³T₀]Ω according to their energy and Ω assignment). High resolution excitation spectra were obtained for all six transitions and a rotational analysis yielded the following principal constants, in cm⁻¹, for the X, W and V states, respectively: T₀ = 0, 251.8713(31), 980.6969(37); B_e = 0.121903(42), 0.121729(37), 0.122561(34); ΔG_1/2 = 463.8811(46), 462.9411(45), 461.2084(127). For the A state, T₀ = 14794.6987(28) cm⁻¹ and B₀ = 0.112596(29) cm⁻¹. The three low lying states are shown to arise from the Ho²⁺[4f¹⁰(⁵I₈)6s]S²⁻ configuration in accord with Ligand Field Theory predictions. The atomic origin of each of the three low lying electronic states was determined from the observed resolved hyperfine structure.