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     

Rabi oscillations between ground and Rydberg states with dipole-dipole atomic interactions

We demonstrate Rabi oscillations of small numbers of 87Rb atoms between ground and Rydberg states with n< or =43. Coherent population oscillations are observed for single atoms, while the presence of two or more atoms decoheres the oscillations. We show that these observations are consistent with van der Waals interactions of Rydberg atoms.     

Quantum corrections to the energy density of a homogeneous Bose gas

Quantum corrections to the properties of a homogeneous interacting Bose gas at zero temperature can be calculated as a low-density expansion in powers of , where is the number density and a is the S-wave scattering length. We calculate the ground state energy density to second order in . The coefficient of the correction has a logarithmic term that was calculated in 1959. We present the first calculation of the constant under the logarithm. The constant depends not only on a, but also on an extra parameter that describes the low energy scattering of the bosons. In the case of alkali atoms, we argue that the second order quantum correction is dominated by the logarithmic term, where the argument of the logarithm is ,and is the length scale set by the van der Waals potential. Received 2 February 1999     

Fluid and plastic flow dynamics of the critical state for a strongly pinned 2D superconductor

The frequency of the Raman active A_1g radial breathing mode has been widely used as a tool to estimate the distribution of diameters of single wall carbon nanotubes (SWNT). However, the relation between frequency and diameter is not straightforward and results are model-dependent. Because most of the experiments are performed on bundles and not on isolated tubes, the model should especially take into account the van der Waals intertube interactions. Here, we use a pair-potential approach to account for such interactions and we derive a nonlinear relation between the SWNT diameter and the frequency of the A_1g radial breathing modes. We demonstrate a good agreement between calculations and the diameters derived from diffraction experiments on the same samples. Received 22 December 1999 and Received in final form 17 July 2000     

Two-dimensional Rydberg gases and the quantum hard-squares model

We study a two-dimensional lattice gas of atoms that are photoexcited to Rydberg states in which they interact via the van?der?Waals interaction. We explore the regime of dominant nearest-neighbor interaction where this system is intimately connected with a quantum version of Baxter's hard-squares model. We show that the strongly correlated ground state of the Rydberg gas can be analytically described by a projected entangled pair state that constitutes the ground state of the quantum hard-squares model. This correspondence allows us to identify a phase boundary where the Rydberg gas undergoes a transition from a disordered (liquid) phase to an ordered (solid) phase.     

Formation of small water cluster anions by attachment of very slow electrons at high resolution

Using a high resolution laser photoelectron attachment method, we have studied the formation of (H ₂ O) _q ^- (q = 2, 6, 7, 11, 15) cluster ions in collisions of slow free electrons (E = 1-80 meV) and Rydberg electrons (n = 12-300) with water clusters. Resonances at zero energy have been observed, the shapes of which are strongly dependent on cluster size. The results are discussed in terms of the formation of metastable negative ions. Received 8 March 1999     

Long-range molecular resonances in a cold Rydberg gas

We present evidence for molecular resonances in a cold dense gas of rubidium Rydberg atoms. Single UV photon excitation from the 5s ground state to np Rydberg states (n=50-90) reveals resonances at energies corresponding to excited atom pairs (n-1)d+ns. We attribute these normally forbidden transitions to avoided crossings between the long-range molecular potentials of two Rydberg atoms. These strong van der Waals interactions result in avoided crossings at extremely long range, e.g., approximately 58 000 times the Bohr radius (a(0)) for n=70.     

Hydrogenic Rydberg states of molecular van der Waals complexes: resolved Rydberg spectroscopy of DABCO-N2

The complementary threshold ionization techniques of MATI and ZEKE spectroscopy have been used to reveal well-resolved, long-lived (>10 micros) hydrogenic Rydberg series (50< or =n< or =98) in a van der Waals complex formed between a polyatomic molecule and a diatomic molecule for the first time. The series are observed within 50 cm(-1) of the adiabatic ionization threshold as well as two core-excited thresholds corresponding to excitation of up to two quanta in the van der Waals vibrational mode.     

Application of the stabilization method to interacting resonances

The stabilization method is applied to the case of interacting resonances in the photo-dissociation of van der Waals clusters composed by a rare gas atom bound to a dihalogen molecule. The study of an illustrative two-dimensional model consisting in a T-shaped NeI₂ molecule shows the adequacy of the method whenever the projection of the stabilization wave functions on the assumed prepared initial state is accounted for. The agreement of the fragmentation cross-sections with some previous results using the effective resolvent method and accurate close-coupling calculations is excellent. The method reveals its utility as a complementary tool since allows, through the analysis of the stabilization wave function in terms of zero-order levels, a precise characterization of the resonant states involved. Received 5 April 2002 / Received in final form 24 May 2002 Published online 19 July 2002     

Suppression of excitation and spectral broadening induced by interactions in a cold gas of Rydberg atoms

We report on the observation of ultralong range interactions in a gas of cold rubidium Rydberg atoms. The van der Waals interaction between a pair of Rydberg atoms separated as far as 100,000 Bohr radii features two important effects: spectral broadening of the resonance lines and suppression of excitation with increasing density. The density dependence of these effects is investigated in detail for the S- and P-Rydberg states with principal quantum numbers n approximately 60 and n approximately 80 excited by narrow-band continuous-wave laser light. The density-dependent suppression of excitation can be interpreted as the onset of an interaction-induced local blockade.     

Rotation/translation interplay in the recoil statistics of cluster evaporation

A new statistical model has been developed in the framework of Phase Space Theory to describe the evaporation process of non-rotating clusters. The novelty of the theoretical approach resides in its ability to easily separate the total kinetic energy released in an evaporation process into the rotational and translational contributions. This new model has been tested by comparing its predictions with the results of Molecular Dynamics (MD) simulations for the unimolecular evaporation of two types of van der Waals clusters: the aniline-(argon)_n molecular clusters and the neat argon Ar_n clusters. Received 16 March 2000     

Static van der Waals interactions in electrolytes

Using a field-theoretic formalism, we calculate the static contribution to the van der Waals interaction between two dielectric semi-infinite half-spaces in the presence of mobile salt ions. The ions can be located in the slab, in one, or in both half-spaces. We include an excess polarizability of the salt ions, i.e., each (spherical) ion has a dielectric constant which in general is different from the surrounding medium. This leads to a modification of the effective dielectric constant of the medium hosting the ions. This shift can be large for high salt concentrations and therefore influences the Hamaker constant decisively. Salt ions in the slab screen the static van der Waals interaction, as was shown by Davies and Ninham. The salt-modified van der Waals interaction also contains salt-confinement and salt-correlation effects. This is clearly demonstrated by the fact that the interaction is non-zero even in the case when the dielectric constant is homogeneous throughout the system, in which case salt correlations are solely responsible for the interaction. If the salt ions are in one or both of the two half-spaces (and no ions in the slab), the van der Waals interaction is not screened but the effective Hamaker constant approaches a universal value for large slab thickness which is different from the value in the absence of salt ions and which is independent of the salt concentration and of the effective electrolyte dielectric constant. If both half-spaces contain salt, the asymptotic value of the Hamaker constant for large separation between the half-spaces is the one obtained for the interaction between two metallic half-spaces through an arbitrary dielectric medium, which is given by A≃ - 1.20. As is explicitly demonstrated, ion enrichment or depletion at the interfaces due to image-charge effects is already included on the one-loop level and therefore does not lead to a change of the screened van der Waals interaction as given by Davies and Ninham. For positive and negative ions with different valencies or different excess polarizabilities, we obtain different adsorbed surface excesses of positive and negative ions, leading to a non-vanishing surface potential, which is computed explicitly. All of these results are obtained on the linear one-loop level. For a special case we extend the calculation of the dispersion interaction to the two-loop level. We find the corrections to the one-loop results to be quite large for high salt concentrations or multivalent ions. Received 17 February 2000     

General order imaginary time correlation functions and imaginary frequency susceptibilities

Certain periodicity properties of general order imaginary time (‘temperature’) correlation functions can be used to represent the n + 1th order van der Waals pair interactions as a multiple Fourier series whose coefficients are nth-order imaginary frequency susceptibilities of the two molecules. This representation is a generalization to higher orders of the standard expression for the second-order van der Waals pair interaction in terms of imaginary frequency polarizabilities. The fourth-order dispersion energy for spherical molecules in their ground state is obtained as a sum of multiple integrals over imaginary frequencies of certain products of dynamic linear and cubic polarizabilities of the two molecules.     

Spinodal dewetting of thin liquid films at soft interfaces

We study theoretically the behavior of nanoscopic liquid films L (thickness e) intercalated between a solid S and a rubber R (elastic modulus μ). Thickness modulations involve a healing length , which results from a competition between elastic and disjoining pressure. With van der Waals interactions, , where a is a molecular size and h₀ the rubber capillary length ( , interfacial tension). If the Hamaker constant of the intercalated liquid is negative, the film dewets by amplification of peristaltic fluctuations (“spinodal dewetting”). The typical size of the contacts is predicted to scale like for films of thicknesses . The rise time of the fastest mode, predicted to scale like , should be very sensitive to the film thickness. Received 11 February 2000 and Received in final form 22 May 2000     

Photoionization of argon, krypton and xenon clusters in the inner valence shell region

Photoionization of rare gas clusters in the innervalence shell region has been investigated using threshold photoelectron and photoion spectrometers and synchrotron radiation. Two classes of states are found to play an important role: (A) valence states, correlated to dissociation limits involving an ion with a hole in its innervalence ns shell, (B) Rydberg states correlated to dissociation limits involving an ion with a hole in its outervalence np shell plus an excited neutral atom. In dimers, class A states are “bright”, that is, accessible by photoionization, and serve as an entrance step to form the class B “dark” states; this character fades as the size of the cluster increases. In the dimer, the “Mulliken” valence state is found to present a shallow potential well housing a few vibrational levels; it is predissociated by the class B Rydberg states. During the predissociation a remarkable energy transfer process is observed from the excited ion that loses its innershell electron to its neutral partner. Received: 10 February 1998 / Revised: 17 July 1998 / Accepted: 31 July 1998     

Laser-induced fluorescence study of the influence of N <Emphasis Type="Bold">2</Emphasis> and CH <Emphasis Type="Bold">4</Emphasis> on the <Emphasis Type="Bold">114</Emphasis>Cd intercombination line

Using a laser-induced fluorescence method a detailed analysis of profiles of the ¹¹⁴Cd 326.1 nm line perturbed by N₂ and CH₄ was performed which revealed deviations from the ordinary Voigt profile. These deviations are shown to be consistent with fits of experimental profiles to an asymmetric Voigt profile. Coefficients of the pressure broadening, shift and collision-time asymmetry are determined and compared with those calculated for van der Waals interaction potential. Received 29 November 2001 / Received in final form 12 July 2002 Published online 4 February 2003     

The dynamics of a THz Rydberg wavepacket

An optically excited Rydberg wavepacket can be generated by exciting the electron from a low-lying state to a coherent superposition of high-lying states with a short broadband optical pulse. A special kind of Rydberg wavepacket is generated in the case of a interaction of a weak THz half cycle pulse with a stationary Rydberg state, called the THz wavepacket. This THz wavepacket is a coherent superposition of the initial Rydberg state and its neighbouring states. We have investigated the time evolution of THz wavepackets by measuring the impact of two in time delayed half cycle pulses ( ≈ 200 V cm^-1) on the population of a stationary (n = 40) Rydberg state in rubidium. The first half cycle pulse creates the THz wavepacket and the second half cycle pulse probes the dynamics of the THz wavepacket. We support our experimental data by numerically solving the Schr?dinger equation and with a semi-classical picture. Whereas an optically excited wavepacket is initially localized, a THz wavepacket is initially delocalized and becomes localized after half a revival time. Received 23 August 2000 and Received in final form 27 March 2001     

Mechanical effect of van der waals interactions observed in real time in an ultracold Rydberg gas

We present time-resolved spectroscopic measurements of Rydberg-Rydberg interactions between two Rydberg atoms in an ultracold gas, revealing the pair dynamics induced by long-range van der Waals interactions between the atoms. By detuning the excitation laser, a specific pair distribution is prepared. Penning ionization on a microsecond time scale serves as a probe for the pair dynamics under the influence of the attractive long-range forces. Comparison with a Monte Carlo model not only explains all spectroscopic features but also gives quantitative information about the interaction potentials. The results imply that the interaction-induced ionization rate can be influenced by the excitation laser. Surprisingly, interaction-induced ionization is also observed for Rydberg states with purely repulsive interactions.     

Time-evolution of cascade processes of muonic atoms in hydrogen-helium mixtures

The time-dependence of the population of muonic hydrogen states in hydrogen-helium mixtures is calculated for principal quantum number n. The number of muons transferred to helium nuclei is also determined. The dependence of the population of the ground state of muonic hydrogen on time and target density and the helium concentration is also considered. The results are in agreement with recent experimental data. The comparison of the calculated yield of K lines of X-ray in pure hydrogen and deuterium with experimental data indicates the essential role of the Coulomb deexcitation process. Possible Stark mixing is also analysed. Received 17 February 1999 and Received in final form 9 June 1999     

Hydrodynamic interactions in the structural fluctuation of a ternary amphiphilic system C12E5/water/ n-octane

Dynamical fluctuations of microemulsion and lamellar structures in a ternary amphiphilic system C₁₂E ₅/water/n-octane are studied by means of neutron spin echo spectrometry. The decay rate of the time correlation of the concentration was analyzed in terms of a theory (M. Nonomura, T. Ohta, J. Chem. Phys. 110, 7516 (1999)), in which both van Hove and hydrodynamic interactions are considered. The result shows that the time correlation function is expressed mostly by a single exponential determined exclusively by hydrodynamic interactions. Received 1 December 1999 and Received in final form 12 March 2001