Origin of the structural local transition in the molecular impurity ion MnO<Stack><Subscript>4</Subscript><Superscript>2−</Superscript></Stack> in the K<Subscript>3</Subscript>Na(CrO<Subscript>4</Subscript>)<Subscript>2</Subscript> ferroelastic

A new model is proposed for a local transition in a Jahn-Teller impurity center in a crystal with a ferroelastic (ferroelectric) phase transition. This model is based on direct interaction of the order parameter of the phase transition in the matrix with the Jahn-Teller impurity degrees of freedom. It is shown that, under these conditions, the order parameter field can induce lifting of degeneracy of the electronic states active in the Jahn-Teller effect, which is accompanied by a transition from the Jahn-Teller effect to the pseudo-Jahn-Teller effect with its subsequent suppression. As a result, a decrease in temperature gives rise to a structural local transition in the region of the low-symmetry ferroelastic (ferroelectric) matrix phase from the many-well local adiabatic to a single-well potential. The model proposed allows interpretation of experimental data obtained in an EPR study of the molecular impurity ion MnO ₄ ^2? in the K₃Na(CrO₄)₂ ferroelastic.     

Charged cores in ionized $\mathsf{{^{4}He}}$ clusters III: A quantum modeling for the collisional relaxation dynamics

When a pure ⁴He droplet is ionized by electron impact, the most abundant fragment detected in mass spectra after ionization is He₂ ⁺ . All the models that have been proposed thus far to explain the experimental evidence therefore involve the formation of the He₂ ⁺ molecular ion. The understanding of the interactions between this ion and the surrounding He atoms in the cluster and of their dynamical behavior during cluster break-up is an important element for the modeling of the cluster evolution after the ionization event. In previous works [1,2] we have computed and described the Potential Energy Surface (PES) of the electronic ground state for the He₃ ⁺ system that provides the required forces between He₂ ⁺ and He. After ionization He₂ ⁺ is presumably formed by association of an He ⁺ and any of the neutral atoms in the cluster via a 3-body collision process. The ensuing vibrational quenching of the hot molecular ion may release the energy necessary to evaporate the entire droplet, or most of it, and give the fragmentation patterns detected by experiments. We present here a model quantum dynamics that generates vibrational deexcitation cross-sections and the corresponding rate coefficients for the collision of He₂ ⁺ with He. A timescale of the cluster evaporation due to vibrational relaxation is estimated and the present findings are compared with earlier studies on the same system.Received: 15 June 2004, Published online: 24 August 2004PACS: 31.15.Qg Molecular dynamics and other numerical methods - 34.50.Ez Rotational and vibrational energy transfer - 36.40.Wa Charged clusters     

Structural phase transition in elpasolite-like (NH4)2KWO3F3

A new chemical compound, (NH₄)₂KWO₃F₃, was synthesized. The Rietveld-refined crystal structure was found to be cubic at room temperature and to belong to the elpasolite family (space group ). The heat capacity and unit cell parameters were studied within a broad temperature range. A second-order phase transition was found to occur at 235.4 K and to be well described in terms of phenomenological theory. Hydrostatic pressure broadens the temperature interval of stability of the cubic phase (dT₀/dp = −10.8 K GPa⁻¹). A possible model of structural ordering based on a comparison of the entropy parameters and electron density distribution in oxygen and fluorine atoms is discussed.     

Lifetime of the Cs 6P1/2 state in bcc and hcp solid 4He

We present the first experimental study of time-resolved fluorescence from laser-excited Cs(6P_1/2) atoms isolated in a solid ⁴He matrix. The results are compared to the predictions of the bubble model including the interaction of the atomic dipole with its radiation reflected at the bubble interface. Our results show that in liquid He as well as in the body-centered cubic (bcc) crystalline phase of He the lifetime of excited Cs atoms does not depend on He pressure, in agreement with our theory. When going from the bcc to the hexagonally close-packed (hcp) phase of ⁴He the lifetime is reduced by ≈10% and decreases further with increasing He pressure. We assign this effect to the formation of Cs^*He_n exciplexes, and determine the pressure dependence of the probability that the 6P_1/2 state decays via this nonradiative channel.     

Environmental perturbations on foreign atoms and molecules in solid argon,krypton and xenon

Perturbations which are responsible for the shifts of electronic and vibrational spectra of species trapped in a solid are considered in terms of the intermolecular potential which describes interactions between these species and neighbouring atoms. It is shown that in certain instances London's theory can give an adequate approximation to the dispersion energy between an electronically excited species and a rare gas atom. The experimental shifts in the electronic absorption spectra of Hg, NH and C₂ at lattice sites in rare gas crystals at 4·2°k are explained quantitatively on the basis of a Lennard-Jones (6-12) or (6-8-12) potential between the trapped species and the rare gas atoms. The theory does not adequately explain the shifts in those cases where strong angular dependent forces differing appreciably in the two electronic states are present, data on trapped NH₂ free radicals being presented as a case in point. The interaction of sodium atoms with argon at 4·2°k is very complex, the data being consistent with multiple trapping sites for the atoms, a large repulsive interaction between the excited state of sodium and the rare gas, and apparent removal of the three-fold orbital degeneracy in the excited state by the environmental perturbation. The three-fold orbital degeneracy in the ³P₁ state of mercury was found also to be removed. The blue shift of 1281 cm^-1 for the ³P₁ ← ¹S₀ transition of mercury in solid argon at 4·2°k corresponds almost exactly with the position of one of the two prominent features in the spectrum of mercury in argon gas at comparable densities and illustrates the similarity of structure in the two physical states. The interesting perturbations on the vibrational states of NH and C₂ suggest a close similarity to the effect which causes environmental variations of coupling constants for hyperfine interactions in trapped hydrogen atoms.     

The binding of alkali atoms to the surfaces of liquid helium and hydrogen

Alkali atoms have been shown previously to have only unstable binding states inside liquid⁴He. We calculate the equilibrium configurations and binding energies of single alkali atoms near the liquid-vapor interface of⁴He and³He. A simple interface model is used to predict the surface deformation due to the presence of the atoms. A more realistic density functional model yields somewhat higher energies in the case of⁴He. For all alkali atoms, we find the surface binding energies to be around 10 to 20 K. A similar analysis with atom-H₂ interactions finds that alkali atoms tend to submerge into liquid H₂, with the exception of Li.     

Coherence and recombination in two-dimensional atomic hydrogen on the surface of superfluid <Superscript>4</Superscript>He

Experimental results on the achievement of high degrees of quantum degeneration in two-dimensional atomic hydrogen (2D H↓) by the magnetic-compression method are analyzed by taking into account current data on the binding energy E _a = 1.14(1) K of hydrogen atoms with the ⁴He surface and the constant K _ab of the two-particle exchange recombination of adsorbed H atoms. The behavior of pair and three-particle correlation functions, as well as the transverse delocalization of the wavefunction of adsorbed atoms due to their interaction with each other, is taken into account self-consistently. A new mechanism of cooling of the compression region by means of the flow of H atoms on the helium surface with the subsequent evaporation and emission from a magnetic trap is proposed. This mechanism prevails at high densities, whereas the heat transfer at low densities occurs owing mainly to the interaction of ripplons with the phonons of the helium film. Existing data corroborate the achievement of the phase density σλ² ? 10, which is certainly higher than the density necessary for both the arrangement of local coherence in 2D H↓ and its transition to the superfluid state. The results agree with the representations on quasi-condensation; however, direct evidence of this phenomenon is not revealed. The probability of three-particle dipole recombination that is corrected for the quantum correlation and delocalization is equal to 7(2) × 10^?26 cm⁴ s^?1 (T = 0.15, …, 0.21 K, B = 6.6 T, and σλ² = 1, …, 9). The results are compared with other theoretical and experimental data.     

Spin physics in solid helium: Experimental results and applications

We have observed optical pumping signals from Cs atoms trapped in solid⁴He. While the longitudinal electronic spin relaxation timeT ₁ is found to be in the range of 1–2 s, the transverse relaxation timeT ₂, as inferred from magnetic resonance linewidths has a lower bound of 150 s, and is determined by magnetic field inhomogeneities. We present a quantitative discussion of how paramagnetic species trapped in solid He might be used in a highly sensitive search for permanent atomic electric dipole moments.     

Basic connection between superconductivity and superfluidity

A basic and inherently simple connection is shown to exist between superconductivity and superfluidity. It is shown that the author's previously derived general equation, which agrees well with the superconducting transition temperatures for the heavy-electron superconductors, metallic superconductors, oxide superconductors, metallic hydrogen, and neutron stars, also works well for the superfluid transition temperature of 2.6 mK for liquid³He. Reasonable estimates are made from 10^–3 to 10⁹ K — a range of 12 orders of magnitude. The same paradigm applies to the superfluid transition temperature of liquid⁴He, but results in a slightly different equation. The superfluid transition temperature for dilute solutions of³He in superfluid⁴He is estimated to be l–10K. This paradigm works well in detail for metallic, cuprate, and organic superconductors.     

Mössbauer effect study of Y(Fe0.022 Co0.978)2 at temperatures between 0.15 and 4.2k

A³He-⁴He dilution refrigerator was constructed to perform Mössbauer measurements well below 4.2K. Results are reported here on the pseudobinary Laves-Phase system Y (Fe_1-x Co_x)₂ for x=0.978. We found that at low temperatures, the Fe ions undergo a disordered magnetic phase transition, with a Curie temperature of approximately 4K and a saturation field of 96K0e. The easy axis of magnetization appears to be the [111] direction. This study is an extension to very low temperatures of previous work on the system with 0X0.978.Supported by the NSF Grant No. DMR 73-07665 AO 3     

Recombination channels of molecular ions He 2 + and electrons

The dependence of the intensities of atomic lines and molecular bands emitted in the afterglow of a helium discharge on the electron temperature is used to identify the processes in which states of He and He ₂ ^* are populated. It is established that the formation of He^* atoms (n = 3, 4) in decaying helium plasma occurs principally on account of the associative recombination of vibrationally excited He ₂ ⁺ ions and electrons. Analysis of the experimental reuslts leads to the conclusion that the distribution of the molecular ions He ₂ ⁺ over vibrational states is strongly nonequilibrium.Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, No. 2, pp. 67–72, February, 1984.It remains to thank N. P. Penkin for discussions and for his interest in the work.     

Improved lasing properties of the HêN 2 + system at 391 nm and 428 nm by H2 admixture

The He/N₂ system lasing on the N ₂ ⁺ (B)N ₂ ⁺ (X, 0) transition at 391 nm and on the N ₂ ⁺ (B)N ₂ ⁺ (X, 1) transition at 428 nm was investigated by e-beam excitation. By adding H₂ the lower laser state is efficiently quenched, which leads to a drastic improvement of the laser properties. A kinetic model is proposed which accounts for the experimental results. For a laser amplifier operated at 5 bar total efficiencies of 0.6% and 0.7% are predicted for the 391 nm and the 428 nm transitions respectively.     

Crystal structure and structural transition caused by charge-transfer phase transition for iron mixed-valence complex (n-C3H7)4N[FeFe(dto)3] (dto=C2O2S2)

(n-C₃H₇)₄N[Fe^IIFe^III(dto)₃] shows a new type of first order phase transition called charge-transfer phase transition around 120 K, where the charge transfer between Fe^II and Fe^III occurs reversibly. Recently, we have succeeded in obtaining single crystals of the title complex and determined the crystal structure at room temperature. Crystal data: space group P6₃, Z=2. Moreover, we have investigated the structural transition caused by the charge-transfer phase transition by means of powder X-ray diffraction measurement. When the temperature is decreased, the a-axis, which corresponds to the hexagonal ring size in two-dimensional honeycomb network structure of [Fe^IIFe^III(dto)₃]_∞, contracts by 0.1 Å at the charge-transfer transition temperature (T_CT), while the c-axis, perpendicular to the honeycomb network layer, elongates by 0.1 Å at T_CT. Consequently, when the temperature is decreased, the unit cell volume decreases without noticeable anomaly around T_CT, which is responsible for the quite small vibrational contribution to the entropy change, compared with usual spin crossover transition. Thus, the charge-transfer phase transition around 120 K for (n-C₃H₇)₄N[Fe^IIFe^III(dto)₃] is regarded as spin entropy driven phase transition.     

The influence of oxygen vacancies on the chemical bonding in titanium oxide

A self-consistent LAPW band structure calculation for TiO_0.75 has been performed, assuming long-range order of vacancies on the oxygen sublattice. The calculation is based on a hypothetical model structure which can be described as Ti ₃ ^[4] Ti^[6]O_3o, where _o denotes an oxygen vacancy. In the model structure two types of titanium atoms occur: Ti^[4] atoms which have two vacancies as neighbours and are quadratically surrounded by four oxygen atoms, and Ti^[6] atoms which are octahedrally surrounded by six oxygen atoms. The calculated density of states (DOS) and the local partial densities of states are compared with the respective values for stoichiometric TiO containing no vacancies. A characteristic difference is the appearance of two sharp peaks in the DOS curve below the Fermi energy which are caused by the vacancies. These vacancy states exhibit a considerable amount of charge in the vacancy muffin-tin sphere and are found to be derived from Ti 3d states extending into the vacancy sphere. The introduction of vacancies also leads to a lowering of the Fermi energy indicating a stabilizing effect. The bonding situation in TiO_0.75 as compared to TiO as well as the changes in chemical bonding in the series TiC_0.75–TiN_0.75–TiO_0.75 are discussed on the basis of electron density plots. The loss of Ti^[4]–O bonds (as compared to TiO) is compensated by the formation of Ti^[4]–_o–Ti^[4] bonds across the vacancy and by an increase of the bond strength of the Ti^[4]–O bonds. On the other hand, the Ti^[4]–Ti^[4] and particularly the Ti^[4]–Ti^[6] bonds are weakened by the introduction of vacancies.Dedicated to Professor F. Kohler on the occasion of his 65^th birthday     

Nonasymptotic critical dynamics of the asymmetric-spin model in two-loop order

The crossover behaviour in the dynamics near the Lambda transition of⁴He is analyzed on the basis of the complete renormalization-group flow equations for the asymmetric-spin model (F) in two-loop order. Our results confirm the conclusions and refine the results obtained from an earlier analysis based on the symmetric model (E) and invalidate part of a recent analysis treating model F in an unsystematic approximation. Excellent agreement is found with measurements of second-sound damping over four decades in relative temperature. Closer toT our analysis predicts a further increase of the effective amplitudeR ^eff of the thermal conductivity.Supported in part by the Fonds zur Förderung der wissenschaftlichen Forschung     

Measurement of the breakup channels in nuclear muon capture by3He and4He

The rates of the breakup reactions _B(³He) and _B(⁴He) in nuclear muon capture by³He and⁴He have been measured. The measurements were performed on the muon beam of PSI with a multi-anode high-pressure ionization chamber filled with isotopically pure³He or⁴He at 120 bar. The chamber was used as a target and detector for both the incoming muons and for the charged reaction products (tritons, deuterons and protons) of the breakup reactions _B(³He) and _B(⁴He). Our statistics, about 5 × 10⁵ of breakup events, provides a possibility to improve the precision of evaluated rates. The preliminary results: _B(³He)=720 ± 70 s^–1, _B(⁴He)=415 ± 40 s^–1 are compared to theoretical predictions and to previous experiments.     

Flow of 2D atomic hydrogen over the surface of liquid <Superscript>4</Superscript>He

Experimental evidence has been obtained for the hydrodynamic flow of a 2D gas of hydrogen atoms adsorbed on the surface of liquid helium. The observed flow manifestations are consistent with the concepts of the quantum hydrodynamics of the helium surface. This circumstance allows both investigation of the interaction of 2D hydrogen with ripplons and surface ³He quasiparticles and possible future observation of the superfluidity of the 2D Bose gas of hydrogen atoms. The experimental results on thermal compression make it possible to estimate the characteristic times of the transfer of longitudinal momentum between the subsystems of hydrogen and ³He atoms bound to the surface (τ_H3), as well as from ripplons to the substrate (τ_R). The value τ_H3 ～ 4 × 10^?8 s agrees with a value calculated using the mean-field parameter U₃₀ for the interaction of hydrogen atoms with the ground surface state of ³He. At the same time, τ_R is more than an order of magnitude shorter than the value obtained in experiments by Mantz et al. Phys. Rev. Lett. 44, 66 (1980) [Erratum: Phys. Rev. Lett. 44, 1094 (1980)]. This discrepancy can be attributed to the dependence of the ripplon momentum relaxation rate on the substrate roughness scale.     

Nonlinear renormalization-group analysis applied to the hydrodynamic light scattering spectrum of4He belowT λ

We calculate the observable critical temperature dependence of the transport coefficients entering the hydrodynamic form of the dynamic structure factor of⁴He belowT . Application of our recently introduced nonlinear renormalization-group analysis yields quantitative agreement with previous light scattering experiments in the hydrodynamic region. This resolves a long-standing problem in the critical dynamics below the superfluid transition of⁴He.Supported in part by the Fonds zur Förderung der wissenschaftlichen Forschung     

Critical behavior of short range Potts glasses

We study by means of Monte Carlo simulations and the numerical transfer matrix technique the critical behavior of the short rangep=3 state Potts glass model in dimensionsd=2,3,4 with both Gaussian and bimodal (±J) nearest neighbor interactions on hypercubic lattices employing finite size scaling ideas. Ind=2 in addition the degeneracy of the glass ground state is computed as a function of the number of Potts states forp=3, 4, 5 and compared to that of the antiferromagnetic ground state. Our data indicate a transition into a glass phase atT=0 ind=2 with an algebraic singularity, aT=0 transition ind=3 with an essential singularity of the form exp(const.T ^–2), and an algebraic singularity atT0.25 ind=4. We conclude that the lower critical dimension of the present model isd _c =3 or very close to it. Some of the critical exponents are estimated and their respective values discussed.