Evidence of equal Jahn-Teller coupling to Eg and T2g modes in KMgF3:Fe2+ from far infrared studies

From a study of the dependence of the far infrared (f.i.r.) spectra of KMgF₃:Fe²⁺ on impurity concentration and temperature, we identify them as due to magnetic dipole transition between the J = 1 and J = 2 states of Fe²⁺ and a resonant mode. The novelty of the work lies in demonstrating that in KMgF₃:Fe²⁺ the electronic orbital triplet is equally coupled to the E_g and T_2g modes of vibration and consequently vibronic interactions maintain the J-degeneracies.     

Observation of Zeeman degeneracy effects in collisional intense field resonance fluorescence

We report observation of the scattered spectrum from a Zeeman degenerate atom at high laser intensities. For a J = 0 to J = 1 transition in the presence of collisions we observe an asymmetric triplet in the polarization parallel to the incident laser and an asymmetric doublet in the polarization perpendicular to the incident laser.     

Interaction potentials of Hg* + He at moderate interatomic separations and the radiative decay of the Hg(63 P 2) metastable state in collisions with He atoms

By using the modified method of the Fermi pseudopotential and the effective Hamiltonian method, a multiconfiguration calculation of the potential curves is performed for the Hg(6^{1, 3} P _J ) + He and Hg(7^{1, 3} S _J ) + He interactions in the region of interatomic separations R≥5a ₀. In this calculation, the interactions of different excited configurations and the spin-orbit coupling of singlet and triplet states were taken into account. The Hg⁺ + He ion-atom interaction potential was obtained by the nonempirical configuration interaction method MRD-CI with the use of the relativistic effective core potential (RECP) for the Hg atom. Based on the calculated potential curves and the transition dipole moments, the process of radiative decay of the Hg(6³ P ₂) metastable state in collisions with He atoms is considered and the temperature dependence of the rate constant is calculated.     

Dynamic phenomena in layer superconducting cuprate and organic metals

Dynamic electron spin resonance (ESR) and extended x-ray absorption edge fine structure (XAFS) measurements suggest that layered organic metals and cuprate superconductors behave similarly. The response to microwave radiation in a modulated external magnetic field indicates that: (i) triplet state, T * ESR is observed below T_c for both; (ii) the condensation of free spin doublet D to T* occurs above the transition temperature to superconductivity T_c (10 ± 1 K for the organic metal (BEDT-TTF)₃Ta₂F₁₁ and 92 to 12 K for YBa₂Cu₃O_7-δ and its rare earth derivatives); (iii) antiferomagnetic (AF) resonance is detected above T_c for the organic metal. Here the exchange field between the aligned AF domains: J_AF(150 K) = 130.7 mT (153 mK) is greater than the exchange term J(150 K) ≈ 15 mT (20 mK) between free spins (S = 1/2) leading to T* states; the lifetime of AF domains τ_AF decreases below 150 K and resonance is not detected below 44 K (i.e. τ_AF < 10^-10 s) allowing a superconducting transition to appear below 10 K; (iv) the relaxation time τ₁ for the half field, triplet state ESR absorption increases fourfold near 10 K for the organic metal and, (v) the onset of superconductivity is detected in all superconductors by the appearance of an energy loss at exactly H=0 and, magnetization oscillations observed versus H below T_c when the samples are cooled in a non-zero field H. The spin-lattice relaxation time for the organic metal triplet state, half field ESR near 10 K is interpreted using the Gorter phenomenological relation τ₁ = C_H /α_H, C_H and α_H are respectively the heat capacity and the thermal contact coefficient to the lattice by the spin system, at constant field H . Complementary changes in x-ray edge widths near T_c are correlated to electron-phonon interactions.     

Etude des proprietes thermodynamiques d'un groupement tetranucleaire: Application au compose Na3RuO4

The exact eigenvalues spectrum of the spin hamiltonian $\text{H}\text{= ?2}\text{∑}\text{(i, j)}\text{J}{}_{\mathrm{ij}}\text{S}\text{?}{}_{\mathrm{i}}\text{S}\text{?}{}_{\mathrm{j}}$ have been calculated for a tetranuclear cluster formed by four spins 3/2 at the vertices of a lozenge. Two isotrope exchange interactions J₁ and J₂ are able to explain the thermodynamic properties (magnetic susceptibility, entropy, specific heat). A ground state transition from singlet to triplet state occurs when the $\text{J}{}_2\text{J}{}_1$ ratio reaches the value $\text{4}\text{3}$. The magnetic susceptibility data of Na₃RuO₄ fit well with the theoretical values proposed for $\text{J}{}_1\text{K}\text{= (?19,5 K)}$ and J₂/k (?22,5 K).     

Electron correlations and instability of a two-center bipolaron

The energy of a large bipolaron is calculated for various spacings between the centers of the polarization potential wells of the two polarons with allowance made for electron correlations (i.e., the explicit dependence of the wave function of the system on the distance between the electrons) and for permutation symmetry of the two-electron wave function. The lowest singlet and triplet 2³S states of the bipolaron are considered. The singlet polaron is shown to be stable over the range of ionic-bond parameter values η≤η_m≈0.143 (η=?_∞/?₀, where ?_∞ and ?₀ are the high-frequency and static dielectric constants, respectively). There is a single energy minimum, corresponding to the single-center bipolaron configuration (similar to a helium atom). The binding energy of the bipolaron for η → 0 is J_bp=?0.136512e⁴m^*/?²? _∞ ² (e and m* are the charge and effective mass of a band electron), or 25.8% of the double polaron energy. The triplet bipolaron state (similar to an orthohelium atom) is energetically unfavorable in the system at hand. The single-center configuration of the triplet bipolaron corresponds to a sharp maximum in the distance dependence of the total energy J_bp(R); therefore, a transition of the bipolaron to the orthostate (e.g., due to exchange scattering) will lead to decay of the bound two-particle state. The exchange interaction between polarons is antiferromagnetic (AFM) in character. If the conditions for the Wigner crystallization of a polaron gas are met, the AFM exchange interaction between polarons can lead to AFM ordering in the system of polarons.     

Effect of single-ion uniaxial anisotropy on the phase diagrams of magnetic system in the presence of internal spin fluctuation

Basing on the two-spin-per-site Heisenberg model, the effect of single-ion uniaxial anisotropy on the phase diagrams of magnetic system in the presence of internal spin fluctuation has been investigated by use of the mean field theory. It was found that single-ion uniaxial anisotropy has important effect on the phase digrams. In the ferromagnetic case (J₃>0) the positive single-ion uniaxial anisotropies (D) suppress the internal spin fluctuation and raise the phase trasition temperature, and negative single-ion uniaxial anisotropies (D) increase the internal spin fluctuation and reduce the phase trasition temperature. In the antiferromagnetic case (J₃<0), there exist two critical values J_c1 and J_c2 (|J_c2|<|J_c1|) in the positive D values. In the |J₃|<|J_c2| range intra-spin exchange coupling prevails inter-spin exchange coupling, the positive D values suppress the internal spin fluctuation and raise the phase transition temperature. In the |J₃|>|J_c1| range the two sub-spins behave as a rigid spin and the positive D values make the reduction of the phase transition temperature. We also observe that the larger D values make the range of internal spin fluctuation to move towards the larger |J₃| range.     

Collisional transfer between rotational levels of OCS

Steady-state four-level microwave double-resonance experiments are described for pure OCS and OCS diluted with CH₃OH, H₂, and He. For pure OCS, interactions of higher order than first-order dipole-dipole dominate the behavior of some four-level systems, and the rates of ΔJ = 2 quadrupole-type collision-induced transitions are found to be greater than one-half of the ΔJ = 1 dipolar rates. For OCSCH₃OH mixtures, the dipolar rates are significantly enhanced with respect to the pure gas, but ΔJ = 2 transitions are still important. For the mixtures of astrophysical interest, OCSH₂ and OCSHe, all four-level systems show ΔJ = 2 collisional preferences. The ΔJ = 2 transition rates are comparable to those of ΔJ = 1 transitions, and there is evidence that ΔJ = 3 transition rates are substantial.     

Low-energy singlet sector in the spin-1/2 <Emphasis Type="Italic">J</Emphasis><Subscript>1</Subscript>–<Emphasis Type="Italic">J</Emphasis><Subscript>2</Subscript> Heisenberg model on a square lattice

Based on a special variant of the plaquette expansion, an operator is constructed whose eigenvalues give the low-energy singlet spectrum of a spin-\(\frac{1}{2}\) Heisenberg antiferromagnet on a square lattice with nearest-heighbor and frustrating next-nearest-neighbor exchange couplings J ₁ and J ₂. It is well known that a nonmagnetic phase arises in this model for 0.4 ? J ₂/J ₁ ? 0.6, sandwiched by two Néel ordered phases. In agreement with previous results, we observe a first-order quantum phase transition (QPT) at J ₂ ≈ 0.64 J ₁ from the non-magnetic phase to the Néel one. A large gap (? 0.4J ₁) is found in the singlet spectrum for J ₂ < 0.64J ₁, which excludes a gapless spin-liquid state for 0.4 ? J ₂/J ₁ ? 0.6 and the deconfined quantum criticality scenario for the QPT to another Néel phase. We observe a first-order QPT at J ₂ ≈ 0.55J ₁, presumably between two nonmagnetic phases.     

Temperature dependence of pressure broadening of NH3 perturbed by H2 and N2

The temperature dependence of pressure broadening of 134 rovibrational transitions of several branches in the ν₄ and 2ν₂ bands of ammonia perturbed by H₂ and N₂ has been measured using a high-resolution Fourier transform spectrometer. The temperature range covered during the experiments was between 235 and 296 K. The pressure-broadening linewidths were obtained using the method of multipressure fitting to the measured shapes of the lines. These broadenings were also calculated using a semiclassical model leading to a reasonable agreement with the observations and reproduces well the strong systematic experimental J and K quantum number dependencies. The retrieved values of the linewidths, along with those previously determined from the spectra at room temperature, were used to derive the temperature dependence of both H₂ and N₂ broadening of NH₃ lines. The broadening coefficients were shown to fit closely the well-known exponential law. For both experimental and theoretical results, the temperature exponent n has been obtained. Careful inspection of the experimental values shows that, contrary to the linewidths, the coefficient n is nearly K independent within each J multiplet. Also for a given J it does not seem to exhibit any noticeable variation with the type of rotational transition. On the other hand, the calculated n values exhibit a strong J and K systematic dependencies. n increases with K for a given J, decreases with J for a given K and are independent of the type of rotational transition.     

Rectification of the dipole force in a monochromatic field created by elliptically polarized waves

The rectification of the force of induced light pressure in laser fields formed by elliptically polarized running waves in zero magnetic field is considered. Explicit analytic expressions for the induced and spontaneous forces of light pressure exerted on a stationary atom are obtained for two classes of closed optical transitions: J _g=J→J _e=J+1 and J _g=J→J _e=J (J is half-integral), where J _g and J _e are the total angular momenta of the ground and excited energy levels. It is shown that the ellipticity of waves is the necessary condition for the emergence of the rectification of the induced force in a monochromatic field. The optimal parameters of the field and the maximum rectification coefficient are calculated for a number of optical transitions. The dependence of the rectified force on the velocity is investigated analytically and numerically for the simplest 1/2→1/2 transition.     

Phase diagram of the Ising antiferromagnet with nearest-neighbor and next-nearest-neighbor interactions on a square lattice

The phase diagram of the Ising model in the presence of nearest-neighbor (J₁) and next-nearest-neighbor (J₂) interactions on a square lattice is studied within the framework of the differential operator technique. The Hamiltonian is solved by effective-field theory in finite cluster (we have chosen N=4 spins). We have proposed a functional for the free energy (similar to Landau expansion) to obtain the phase diagram in the (T,α) space (α=J₂/J₁), where the transition line from the superantiferromagnetic (SAF) to the paramagnetic (P) phase is of first-order in the range 1/2<α<0.95 in contrast to previous study of CVM (Cluster Variational Method) that predict first-order transition for α=1.0. Our results for α=1.0 are in accordance with MC (Monte Carlo) simulations, that predict a second-order transition.     

Microwave and optical spectroscopy of carotenoid triplets in light-harvesting complex LHC II of spinach by absorbance-detected magnetic resonance

Absorbance-detected magnetic resonance (ADMR) of the light-harvesting complex LHC II of spinach revealed two triplet contributions, having differentD values, but equalE value (|E|=0.00379 cm^?1). The two triplets are assigned to two of the three carotenoids present in LHC II: lutein (|D|=0.03853 cm^?1) and neoxanthin (|D|=0.04003 cm^?1). The ADMR-detected Triplet-minus-Singlet (T—S) optical difference spectrum of the carotenoid (Car) triplet transition of LHC II showed, apart from bands in the Car absorption region, a contribution in the chlorophyll (Chl) absorption region due to a change in interaction between lutein and Chla at 670 nm, and neoxanthin and Chla at 670 and 677 nm. From Linear Dichroic (LD-)ADMR-detected LD-(T—S) spectra we have determined that the tripletz-axis (which corresponds roughly to the polyenal axis) of lutein and neoxanthin makes an angle of 47° and 38° with theQ _y transition moment of their adjacent Chla molecules, for the Chls absorbing at 670 and 677 nm, respectively. TheT _z triplet magnetic transition moment of lutein is parallel to the lutein singlet and triplet absorptions, whereas theT _x axis of neoxanthin makes an angle of about 20 degrees with the optical transition moments of the carotenoid molecule. The major Chla absorption bands of the optical absorption spectrum and the ADMR-detected T—S spectrum is best explained by assuming that all Chla is present in dimers. It is proposed that a free Chl dimer absorbs at 664 and 670 nm, whereas a Chl dimer bound to a carotenoid absorbs at 670 and 677 nm.     

Phase transitions and critical properties of the frustrated Heisenberg model on a layer triangular lattice with next-to-nearest-neighbor interactions

The critical behavior of the three-dimensional antiferromagnetic Heisenberg model with nearest-neighbor (J) and next-to-nearest-neighbor (J ₁) interactions is studied by the replica Monte Carlo method. The first-order phase transition and pseudouniversal critical behavior of this model are established for a small lattice in the interval R = |J ₁/J| = 0?C0.115. A complete set of the main static magnetic and chiral critical indices is calculated in this interval using the finite-dimensional scaling theory.     

Quantum entanglement and quantum phase transitions in frustrated Majumdar-Ghosh model

By using the density matrix renormalization group technique, the quantum phase transitions in the frustrated Majumdar-Ghosh model are investigated. The behaviors of the conventional order parameter and the quantum entanglement entropy are analyzed in detail. The order parameter is found to peak at J₂∼0.58, but not at the Majumdar-Ghosh point (J₂=0.5). Although, the quantum entanglements calculated with different subsystems display dissimilarly, the extremes of their first derivatives approach to the same critical point. By finite size scaling, this quantum critical point J^C₂ converges to around 0.301 in the thermodynamic limit, which is consistent with those predicted previously by some authors (Tonegawa and Harada, 1987 [6]; Kuboki and Fukuyama, 1987 [7]; Chitra et al., 1995 [9]). Across the J^C₂, the system undergoes a quantum phase transition from a gapless spin-fluid phase to a gapped dimerized phase.     

First-order transition features of the triangular Ising model with nearest- and next-nearest-neighbor antiferromagnetic interactions

We implement a new and accurate numerical entropic scheme to investigate the first-order transition features of the triangular Ising model with nearest-neighbor (J_nn) and next-nearest-neighbor (J_nnn) antiferromagnetic interactions in ratio R=J_nn/J_nnn=1. Important aspects of the existing theories of first-order transitions are briefly reviewed, tested on this model, and compared with previous work on the Potts model. Using lattices with linear sizes L=30,40,…,100,120,140,160,200,240,360 and 480 we estimate the thermal characteristics of the present weak first-order transition. Our results improve the original estimates of Rastelli et al. and verify all the generally accepted predictions of the finite-size scaling theory of first-order transitions, including transition point shifts, thermal, and magnetic anomalies. However, two of our findings are not compatible with current phenomenological expectations. The behavior of transition points, derived from the number-of-phases parameter, is not in accordance with the theoretically conjectured exponentially small shift behavior and the well-known double Gaussian approximation does not correctly describe higher correction terms of the energy cumulants. It is argued that this discrepancy has its origin in the commonly neglected contributions from domain wall corrections.     

A Comparison of Lineshape Models in the Analysis of Modulated and Natural Rotational Line Profiles: Application to the Pressure Broadening of OCS and CO

We report on the self and pressure broadening of the J=9←8 transition of O¹²CS and O¹³CS and the J+1←J, with J=0, 1, 2, 3, rotational transitions of ¹²CO and ¹³CO. In particular, the J=9← 8 of OCS and J=1← 0 of CO have been investigated for a detailed comparison of lineshape models in the analysis of natural and modulated line profiles. Since the frequency modulation technique improves the instrumental sensitivity, allowing the study of weak transition line profiles, a thorough test of this technique applied to lineshape analysis has been carried out. Finally, the self and pressure broadening coefficients are also given. Due to the important role covered by CO in the atmospheric chemistry field, we have paid particular attention to the N₂ and O₂ broadening.     

Ro-vibrational states of triplet H3 (aΣu): The lowest 19 bands

We have performed extensive calculations of the ro-vibrational states of triplet H₃⁺, using the method of hyperspherical harmonics and our recently reported double many-body expansion potential energy surface. The rotational term values of the lowest 19 states are presented here for a total angular momentum of J?10.     

Chiral spin liquid in a two-dimensional helical XY magnet with two chiral order parameters

The critical properties of an XY helimagnet on a square lattice with two chiral order parameters are studied by Monte Carlo simulations. This model is a modification of the J ₁-J ₂-J ₃ model with J ₂ = 0. The case of different third range order interactions J ₃ are considered, J ₃ ^a ?? J ₃ ^b . A first order transition is found away from the Lifshitz points 4J ₃ ^a = J ₁ and 4 J ₃ ^b = J ₁. It is pointed out that a chiral spin liquid phase possibly exists near the Lifshitz points.     

Comparison of semiempirical and ab initio absolute probabilities of rovibronic transitions for the I 1Π g − , J 1Δ g − →C 1Π u ± system of bands of the H2 molecule

The absolute values of probabilities of the I ¹Π _g ^? , v′, J′; J ¹ Δ _g ^? , v′, J′→C ¹Π _u ^± , v″, J″ spontaneous transitions in the H₂ molecule (for the vibrational and rotational quantum numbers v′=v″=0–3, J′=1–6, and J″=J′, J′ ±1) are calculated by using ab initio and semiempirical data on the dipole moments of the 3dπ ¹Π_g, 3dδ¹Δ_g→2pπ¹Π_u electronic transitions. In both cases, the calculations are performed both in the adiabatic approximation and with an allowance for the nonadiabatic effect of electronic-rotational interaction. The coefficients of expansion of the wave functions of perturbed rovibronic states in the Born-Oppenheimer basis functions used in the calculations were obtained in the approximation of pure precession from experimental values of the terms. It was found that the values of transition probabilities based on the ab initio calculations systematically exceed the corresponding semiempirical data by a factor of 1.2–1.9 for the I ¹Π_g→C ¹Π _u ^± transition and by a factor of 1.4–1.6 for the J ¹Δ _g ^? →C ¹Π _u ^± transition. It was established that the difference between the ab initio and semiempirical values of electronic transition moments virtually has no effect on the dependence of the transition probabilities on the vibrational quantum numbers. The discrepancies between the results of adiabatic and nonadiabatic calculations are significant and reach two orders of magnitude, which is indicative of the important role of perturbations in the probabilities of the transitions considered.