Redshifts in space caused by stimulated Raman scattering in cold intergalactic Rydberg matter with experimental verification

The quantized redshifts observed from galaxies in the local supercluster have recently been shown to be well described by stimulated Stokes Raman processes in intergalactic Rydberg matter (RM). The size of the quanta corresponds to transitions in the planar clusters forming the RM, of the order of 6 × 10^?6 cm^?1. A stimulated Stokes Raman process gives redshifts that are independent of the wavelength of the radiation, and it allows the radiation to proceed without deflection, in agreement with observation. Such redshifts must also be additive during the passage through space. Rydberg matter is common in space and explains the observed Faraday rotation in intergalactic space and the spectroscopic signatures called unidentified infrared bands (UIBs) and diffuse interstellar bands (DIBs). Rydberg matter was also recently proposed to be baryonic dark matter. Experiments now show directly that IR light is redshifted by a Stokes stimulated Raman process in cold RM. Shifts of 0.02 cm^?1 are regularly observed. It is shown by detailed calculations based on the experimental results that the redshifts due to Stokes scattering are of at least the same magnitude as observations.     

Vibrational transitions in Rydberg matter clusters from stimulated Raman and Rabi‐flopping phase delay in the infrared

Recently, rotational spectra of giant Rydberg matter (RM) clusters were studied in the radio frequency range (Mol. Phys. 105 (2007) 933–939), giving high‐precision bond distances in the nanometer range. However, the theoretical and experimental problem of vibrational motion or, rather, coupled electronic‐vibrational motion in the RM clusters is still unsolved; but it is expected that broad phonon bands will exist. Spectroscopic signatures from space make it likely that RM is a common form of matter in the Universe, and phonon bands in this spectroscopic range have not been taken into account so far. Spectroscopic results are now reported on transitions in the range 0.01–20 cm⁻¹, using primarily infrared (IR) lasers to probe the RM in a tunable open cavity with a Fabry–Perot interferometer to aid in the identification of the shifts. Stimulated Raman scattering from electronic transitions and Rabi‐flopping from electronic states in the clusters are observed. The broad stimulated Raman peaks are assigned to one and two consecutive vibrational (electronic‐vibrational) transitions. Theoretical values predicted for vibrations (phonon maxima) and electronic processes are in reasonable agreement with the experimental results. Improved calculations are needed to verify the assignments of the vibrational phonon distributions. Copyright © 2008 John Wiley & Sons, Ltd.     

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     

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.     

Precision bond lengths for Rydberg Matter clusters K19 in excitation levels n =4, 5 and 6 from rotational radio-frequency emission spectra

Several long series of up to 40 equally spaced lines are observed in the radio-frequency range 15–90?MHz that are attributed to stimulated emission from the electronically excited condensed matter called Rydberg Matter (RM). These frequencies are more than a factor of 1000 smaller than for most ordinary molecules, and if they did not agree with RM clusters they would indicate extremely large and heavy molecules that are unlikely to exist in the gas phase at room temperature. Theoretical predictions for RM clusters agree within 2% with the observed frequencies. Such clusters are planar, six-fold symmetric oblate rotors. The most prominent series with B?=?0.9292?±?0.0001?MHz (3.067?×?10^?5?cm^?1) agrees accurately with the theoretically predicted B value for the cluster K₁₉ in excitation level n?=?4, thus with a K–K bond length of 2.4074?nm. Two other prominent long series agree accurately with K₁₉ at n?=?5 and 6, with bond lengths of 3.804 and 5.518?nm, respectively. The ratio between the interatomic distance and the electron orbit radius for n?=?4 is found to be 2.8433?±?0.0003, a considerable improvement in precision over the theoretical value of 2.9.     

Interaction enhanced imaging of individual Rydberg atoms in dense gases

We propose a new all-optical method to image individual Rydberg atoms embedded within dense gases of ground state atoms. The scheme exploits interaction-induced shifts on highly polarizable excited states of probe atoms, which can be spatially resolved via an electromagnetically induced transparency resonance. Using a realistic model, we show that it is possible to image individual Rydberg atoms with enhanced sensitivity and high resolution despite photon-shot noise and atomic density fluctuations. This new imaging scheme could be extended to other impurities such as ions, and is ideally suited to equilibrium and dynamical studies of complex many-body phenomena involving strongly interacting particles. As an example we study blockade effects and correlations in the distribution of Rydberg atoms optically excited from a dense gas.     

High resolution measurements of hyperfine structure and isotope shifts in 9 spectral lines of Nd I

Nine transitions in Nd I, originating from various levels belonging to the 4f ⁴6s ² ground state configuration, have been studied with high resolution using an actively stabilized C.W. ring dye laser in a crossed laser-atomic-beam set-up. Accurate values for the isotope shifts in all transitions as well as for the hyperfine structure constants of 7 excited states have been obtained.     

CASPT2 and CCSD(T) calculations of dipole moments and polarizabilities of acetone in excited states

The acetone molecule is investigated in its ground state and valence ^1,3n-π*, ^1,3π-π*, and ^1,3σ-π* excited states and Rydberg ^1,3n-3s, ^1,3π-3?, ^1,3n-3p_y and ^1,3π-3p_y states using the CASSCF, CASPT2, and CCSD(T) methods. Equilibrium geometries of excited states are obtained and their changes with respect to the ground state are discussed. For most excited states the C_2v symmetry of the ground state is lowered to the C_s symmetry. A series of valence vertical and adiabatic excitation energies is presented along with excitation energies for Rydberg states. The main body of the paper contains Finite-Field Perturbation Theory (FFPT) calculations of electric properties of the vertically as well as geometry relaxed excited states. Dipole moments of valence excited states decrease significantly upon excitation, being about one half of the ground state dipole moment. Polarizabilities usually change upon excitation much less (increase by about 30%) but hyperpolarizabilities are enhanced up to one or two orders of magnitude. The orientation of the dipole moment is reversed in some vertically excited Rydberg states. Properties of the ground and excited states are discussed considering alterations of the electronic structure and shifts in the geometry.     

铯原子里德伯态精细结构测量

里德伯态光谱是测量里德伯态能级结构和中性原子间相互作用的常用技术手段,特别是高精度的里德伯光谱,可以测量室温原子气室中由偶极相互作用等导致的原子能级频移.在实验中利用反向的852 nm激光和509 nm激光实现了室温原子气室中铯原子6S_(1/2)—6P_(3/2)—57S(D)跃迁的级联双光子激发,实现了里德伯态原子的制备.基于阶梯型电磁诱导透明获得了铯原子里德伯态的高分辨光谱.实验中,基于速度选择的射频边带调制技术,对光谱信号进行了频率标定,测量了铯原子里德伯态57D_(3/2)和57D_(5/2)的精细分裂,分裂间隔为(354.7±2.5)MHz,与理论计算结果基本一致.速度选择的射频调制光谱可以实现里德伯态原子的能级分裂测量,其测量精度对于单光子跃迁的绝对激光频率不敏感;实验中影响57D_(3/2)和57D_(5/2)精细分裂间隔测量精度的主要因素是功率加宽导致的电磁感应透明信号的展宽和509 nm激光频率扫描的非线性.     

The thermionic double-diode,an efficient detector in excited state laser spectroscopy

We are describing the thermionic double-diode which is a suitable instrument for excited state laser spectroscopy. In comparison to the optogalvanic technique the signal-to-noise ratio was found to be 10²?10³ times better, investigating transitions between excited Sr or Ba states. Combined with its high detection sensitivity the thermionic double-diode presents the possibility of investigating transitions between high angular momentum states. It is demonstrated by studying transitions between Rydberg levels and doubly-excited autoionizing states in Ba. Further advantages are (i) the small strength of the dc electric field and the low electron density in the laser excitation region of the double-diode commending itself for studies of Doppler-free transitions to highly excited states and (ii) the very stable working conditions allowing to vary the pressure and current conditions in the diode in a much wider range than in a discharge.     

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.     

Isotope shifts and hyperfine structure in the transitions of gadolinium

High-resolution resonance ionization mass spectrometry has been used to measure isotope shifts and hyperfine structure in all (J = 2-6) and the transitions of gadolinium (Gd I). Gadolinium atoms in an atomic beam were excited with a tunable single-frequency laser in the wavelength range of 422-429 nm. Resonant excitation was followed by photoionization with the 363.8 nm line of an argon ion laser and resulting ions were mass separated and detected with a quadrupole mass spectrometer. Isotope shifts for all stable gadolinium isotopes in these transitions have been measured for the first time. Additionally, the hyperfine structure constants of the upper states have been derived for the isotopes ^{155, 157} Gd and are compared with previous work. Using prior experimental values for the mean nuclear charge radii, derived from the combination of muonic atoms and electron scattering data, field shift and specific mass shift coefficients for the investigated transitions have been determined and nuclear charge parameters for the minor isotopes ^{152, 154} Gd have been calculated. Received 18 November 1999     

Experimental study on the possibility of formation of a condensate of excited states in a substance (Rydberg matter)

The results of experimental study of a condensate of cesium excited states (Rydberg matter) are presented. The possibility of condensate formation was predicted theoretically first by Prof. É.A. Manykin and coauthors from the Russian Research Center Kurchatov Institute and experimentally observed by L. Holmlid and coauthors from the Chalmers University, Sweden. In a thermionic energy converter with interelectrode medium, where, according to the data of Swedish researchers, Rydberg matter is formed, we observed similarities and distinctions between our and Swedish data on the formation of a condensate of cesium excited states.     

The Rydberg matter laser: excitation, delays and mode effects in the laser cavity medium

Temporal and temperature effects are studied in Rydberg matter (RM) formed from K atoms and N₂ molecules as the active medium in a cavity. The function of this setup as a laser was recently described. Temperature-variation studies show that the photons re-exciting the RM clusters usually have a longer wavelength than the photons emitted in the stimulated emission process in the cavity. The deficit is probably covered by background photons. Very long time constants observed after emitter temperature changes indicate that long-wavelength photon energy is accumulated in the RM clusters. Long-wavelength modes are located farther from the RM emitter. The modal structure can be TEM₀₁ or TEM₀₀, as observed clearly by the spatial structure in rapid pulsing experiments. The in-cavity chopped beam signal is delayed by approximately 50 μs. The initial growth rate of the signal during chopping is temperature dependent. Tailing is also observed by chopping, but rapid pulsing of the beam with a spinning mirror does not show any delay of the start of the lasing. The conclusion is that delays exist in the stimulated emission process. The broad intense band appearing at 11 000 nm is shown to be formed partly by light in the range 3500–5000 nm, probably by standing wave interaction at the grating surface (grating bands).     

Assignments of optically pumped CD3OH laser lines

Six FIR laser lines from CD₃OH pumped by the 10R(36) and the 10R(18) CO₂ laser lines are assigned to specific rotational energy levels in the excited C–0 stretch state. It is found that their upper laser levels are shifted by a Fermi resonance between the C–0 stretch vibration and the third and forth harmonics of the torsional mode. The Fermi resonance shifts are +0.332 cm^–1 and +2.251 cm^–1 for the upper laser levels pumped by the 10R(36) and the 10R(18) CO₂ laser lines, respectively. Calculated frequencies of the pump and the laser transitions agree with those of the pump CO₂ laser lines and the observed FIR laser lines within estimated accuracy.     

Atom counting statistics in ensembles of interacting Rydberg atoms

We show that the probability distributions for the number of Rydberg excitations in small ensembles of cold atoms, excited using short (100 ns) laser pulses, can be highly sub-Poissonian. The phenomenon occurs if the atom density and the principal quantum number of the excited Rydberg level are sufficiently high. Our observations are attributed to a blockade of the Rydberg atom excitation.     

Eu原子4f~76snlRydberg态的研究

利用三步双色共振激发技术和三步三色孤立实激发技术,系统地研究了铕原子在42250—44510 cm~(-1)能域内的光谱特性,提供了该能域内56个束缚高激发态的光谱信息.为了能确定这些态的光谱归属,进行了两方面的探索:第一,观察能否利用孤立实激发技术,把处于这些态上的铕原子进一步共振激发到自电离态,从而推断这些态属于单电子激发的束缚Rydberg态还是属于双电子激发的价态,并对Rydberg态的电子组态进行了光谱确认;第二,通过计算这些态相对于各个电离阈的量子亏损并观察它们分别收敛于哪个电离阈,以便获取其主量子数的信息.最后,设计并采用了三种不同的激发路径,分别将原子布居到同一高激发能域并探测它们在该能域的光电离光谱.通过比较这些光谱的异同并结合上述激发路径所对应的跃迁选择定则,便可惟一地确定这些高激发态的总角动量.研究发现:所探测到的高激发束缚态只有三个属于单电子激发的束缚Rydberg态,其余都是价态.本文确定了这三个Rydberg态的电子组态和原子状态.