Magnetic and structural phase transitions in systems with spin crossover under pressure

The effect of the exchange interaction between excited high-spin terms of transition metal ions in magnetic Mott–Hubbard insulators on the thermodynamics of the system with singlet terms of ions in the ground state near the crossover of singlet and high-spin terms with the increase in the pressure is studied with the effective Hamiltonian. It is shown that the crossover at the temperature below the critical T* < T _N is a first-order phase transition and is accompanied by a volume jump. The crossover at the temperature above T* is accompanied by a smooth change in the crystal volume.     

Magnetic phase transitions in Nd<Subscript>1−<Emphasis Type="Italic">x</Emphasis></Subscript>Ca<Emphasis Type="Italic">x</Emphasis>MnO<Subscript>3</Subscript> manganites

The magnetic properties of manganites of the Nd_1?xCa_xMnO₃ system with x≤0.15 have been studied. It is shown that, in the 0.06≤x≤0.1 interval, the results can be interpreted using a model according to which the concentrational transition from a weakly ferromagnetic (WFM) state (x=0) to a ferromagnetic (FM) state (x>0.15) proceeds via a mixture of the exchange-coupled FM and WFM phases. In the vicinity of T=9 K, samples with 0.06≤x≤0.1 exhibit a spontaneous magnetic phase transition involving reorientation of the magnetization vectors of the WFM and the exchange-coupled FM phases. In the temperature interval between 5 and 20 K, a sample with the composition Nd^0.92Ca^0.08MnO^2.98 exhibits metamagnetic behavior. Magnetic phase diagrams in the H?T and T?x coordinates are presented. The appearance of the spin-reorientation transitions is explained in terms of the magnetic analog of the Jahn-Teller effect with allowance for the fact that, according to the neutron diffraction data, the magnetic moments of neodymium ions in the FM phase are parallel to the magnetic moments of manganese ions.     

Spin-selective low temperature spectroscopy on single molecules with a triplet-triplet optical transition: Application to the NV defect center in diamond

The spin-selective photokinetics of a single matrix-isolated impurity molecule with a triplet-triplet optical transition, T ₀–T ₁, is considered and the manifestations of the photokinetics in the fluorescence excitation spectra and intensity autocorrelation functions g ⁽²⁾(τ) of the molecule undergoing narrow-band optical excitation is studied to resolve the fine structure of the transition. The rates of intersystem crossings (ISCs) T ₁→S→T ₀ to and from a nonradiating singlet state S of the molecule and the rate of population relaxation among the ground (T ₀) state sublevels can be obtained from the spectra and g ⁽²⁾(τ) using the analytical expressions obtained. New experiments on an individual NV defect center in nanocrystals of diamond, where, for the first time, the fine structure of its triplet-triplet ³ A-³ E zero-phonon optical transition (~637 nm) at 1.4 K was resolved, are interpreted. It is concluded that the rate of the ISC transition from the m _S =0 sublevel of the excited ³ E state to the singlet ¹ A state (~1 kHz) is much slower than the rates from the m _S =±1 substates, while the rates of ISC transitions to different m _S substates of the ground ³ A state are close to each other (~1 Hz). As a result, only the optical transition between m _S =0 sublevels in the ³ A-³ E manifold contributes strongly to the fluorescence. The experimentally observed double-exponential decay of the g ⁽²⁾(τ) function is explained by the two pathways available to the center for it to leave the S state: (i) the S→ T ₀(m _S )=0) transition and (ii) the S→T ⁰(m _S =±1) transitions followed by the slow spin-lattice relaxation T ₀(m _S =±1)→T ₀(m _S =0) (rate ~0.1 Hz). The work is important for studies where the NV center is used as a single photon source or for quantum information processing.     

Magnetoresistance of a highly correlated electron liquid

The behavior in a magnetic field of a highly correlated electron liquid approaching the fermion condensation quantum phase transition from the disordered phase is considered. We show that, at sufficiently high temperatures T≥T*(x), the effective mass starts to depend on T, M* ∝T^?1/2. This T^?1/2 dependence of the effective mass at elevated temperatures leads to the non-Fermi liquid behavior of the resistivity, σ(T) ∝ T and at higher temperatures σ(T) ∝ T^3/2. The application of a magnetic field B restores the common T² behavior of the resistivity. The effective mass depends on the magnetic field, M*(B) ∝ B^?2/3, being approximately independent of the temperature at T≤T*(B) ∝ B^4/3. At T≥T*(B), the T^?1/2 dependence of the effective mass is reestablished. We demonstrate that this B-T phase diagram has a strong impact on the magnetoresistance (MR) of the highly correlated electron liquid. The MR as a function of the temperature exhibits a transition from negative values of MR at T→0 to positive values at T ∝ B^4/3. Thus, at T≥T*(B), MR as a function of the temperature possesses a node at T ∝ B^4/3.     

Anomalies in the magnetic and magnetoelastic properties of Sm<Subscript>1−<Emphasis Type="Italic">x</Emphasis></Subscript>Sr<Subscript>x</Subscript>MnO<Subscript>3</Subscript> single crystals (<Emphasis Type="Italic">x</Emphasis> ∼ 0.5) at phase transitions

By studying the magnetic and magnetoelastic properties, it is established that, as the temperature is lowered, Sm_1?xSr_xMnO₃ single crystals (x=0.5, 0.55) undergo spontaneous phase transitions from the paramagnetic to a local charge-ordered state at T_co=220 K and to an A-type antiferromagnetic state at T_N=175 K. It is shown that strong magnetic fields (H_cr ～ 200 kOe) break up the antiferromagnetic order and charge ordering and drive a phase transition to a conducting ferromagnetic state. H-T phase diagrams are constructed for single crystals with x=0.5 and 0.55.     

Field Confinement Energy at a Nonlinear Interface between Nonlinear Defocusing Media

The dependences of the resistance of the layered quasi-one-dimensional semiconductor TiS₃ on the direction and magnitude of the magnetic field B have been measured. The anisotropy and angular dependences of the magnetoresistance indicate the two-dimensional character of the conductivity at T < 100 K. Below T₀ ≈ 50 K, the magnetoresistance for the directions of the field in the plane of the layers (ab plane) increases sharply, whereas the transverse magnetoresistance (B ∥ c) becomes negative. The results confirm the possibility of an electron phase transition to a collective state at T₀. The negative magnetoresistance (at B ∥ c) below T₀ is explained by the magnetic-field-induced suppression of two-dimensional weak localization. The positive magnetoresistance (at B ∥ ab) is explained by the effect of the magnetic field on the spectrum of electronic states.     

Josephson vortex lattice melting in Bi-2212 probed by commensurate oscillations of Josephson flux-flow

We studied the commensurate semifluxon oscillations of Josephson flux-flow in Bi-2212 stacked structures near T_c as a probe of melting of a Josephson vortex lattice. We found that oscillations exist above 0.5 T. The amplitude of the oscillations is found to decrease gradually with the temperature and to turn to zero without any jump at T = T₀ (3.5 K below the resistive transition temperature T_c), thus, indicating a phase transition of the second order. This characteristic temperature T₀ is identified as the Berezinskii-Kosterlitz-Thouless (BKT) transition temperature, T_BKT, in the elementary superconducting layers of Bi-2212 at zero magnetic field. On the basis of these facts, we infer that melting of a triangular Josephson vortex lattice occurs via the BKT phase with formation of characteristic flux loops containing pancake vortices and antivortices. The B-T phase diagram of the BKT phase found from our experiment is consistent with theoretical predictions.     

Effect of a magnetic field on the thermal and kinetic properties of the Sm<Subscript>0.55</Subscript>Sr<Subscript>0.45</Subscript>MnO<Subscript>3.02</Subscript> manganite

The temperature and magnetic-field dependences of the heat capacity, thermal conductivity, thermopower, and electrical resistivity of the Sm_0.55Sr_0.45MnO_3.02 ceramic material are studied in the temperature range 77–300 K and in magnetic fields up to 26 kOe. It is revealed that the quantities under investigation exhibit anomalous behavior due to a magnetic phase transition at the Curie temperature T_C. An increase in the magnetic field strength H leads to an increase in the Curie temperature T_C and a jump in the heat capacity ΔC_p at T_C. The temperature dependences of the measured quantities are characterized by hystereses that are considerably suppressed in a magnetic field of 26 kOe and depend neither on the thermocycling range nor on the rate of change in the temperature. The thermal conductivity K at temperatures above T_C shows unusual behavior for crystalline solids (dK/dT>0) and, upon the transition to a ferromagnetic state, drastically increases as a result of a decrease in the phonon scattering by Jahn-Teller distortions. It is demonstrated that the hystereses of the studied properties of the Sm_0.55Sr_0.45MnO_3.02 manganite are caused by a jumpwise change in the critical temperature due to variations in the lattice parameters upon the magnetic phase transition.     

Hall coefficient in heavy fermion metals

Experimental studies of the antiferromagnetic (AF) heavy fermion metal YbRh₂Si₂ in a magnetic field B indicate the presence of a jump in the Hall coefficient at a magnetic-field tuned quantum state in the zero temperature limit. This quantum state occurs at B ≥ B_c0 and induces the jump even though the change of the magnetic field at B = B_c0 is infinitesimal. We investigated this by using the model of heavy electron liquid with the fermion condensate. Within this model, the jump takes place when the magnetic field reaches the critical value B_c0 at which the ordering temperature T_N(B = B_c0) of the AF transition vanishes. We show that at B → B_c0, this second order AF phase transition becomes the first order one, making the corresponding quantum and thermal critical fluctuations vanish at the jump. At T → 0 and B = B_c0 the Grüneisen ratio as a function of the temperature T diverges. We demonstrate that both the divergence and the jump are determined by the specific low temperature behavior of the entropy \(S(T) \propto S_0 + a\sqrt T + bT\) with S₀; a and b are temperature independent constants.     

Phase transitions in hybrid SFS structures with thin superconducting layers

Calculations of critical temperature T _c of the phase transition to superconducting state of a superconductor/ ferromagnet/superconductor (SFS) hybrid structure with proximity effect is performed on the base of linearized Usadel equations. It is shown that the proximity effect between S and F metals and the exchange interaction can induce an inhomogeneous superconducting state with longitudinal to layers Δ _∝ exp(ipz) modulation of the superconductivity order parameter, which is characterized by nonzero value of the wave number p, describing the Larkin–Ovchinnikov–Fulde–Ferrell instability. Influence of this instability on transitions between 0- and π-states of the SFS structure is studied. It is shown that the 0–π transition is accompanied by a nonmonotonic dependence of both the critical temperature T _c and the effective penetration depth Λ of the magnetic field into the hybrid structure on the characteristic size of the ferromagnetic region.     

Nonperturbative phenomena in QCD at finite temperature in a magnetic field

The norperturbative QCD vacuum at finite temperature in a external magnetic field is studied. Equations that relate nonperturbative QCD condensates at finite temperature to the thermodynamic pressure at T ≠ 0 and H ≠ 0 are obtained, and low-energy theorems are derived. The free energy of the QCD vacuum in the hadronic phase at H ≠ 0 is calculated, and expressions for the quark and gluon condensates are obtained. Various limiting cases for the behavior of the condensates at low and high temperatures and in weak and strong magnetic fields are investigated. A new interesting phenomenon that consists in the freezing of the quark condensate by a magnetic field is found. The character of spontaneous chiral-symmetry breaking in finite-temperature QCD in a magnetic field is studied. For this purpose, the Gell-Mann-Oakes-Renner formula relating the pion mass M _π and the axial-vector coupling constant F _π to the quark condensate is derived at T ≠ 0 and H ≠ 0. It is shown that this formula preserves its form at finite temperature after taking into account a magnetic field—that is, no additional terms independent of T and H appear. Thus, the scheme of soft chiral-symmetry breaking remains unchanged. The quark-hadron phase transition in QCD in a magnetic field is studied. It is shown that the phase-transition temperature becomes lower than that in the case of zero magnetic field.     

Influence of the ground state of the Pr<Superscript>3+</Superscript> ion on magnetic and magnetoelectric properties of the PrFe<Subscript>3</Subscript>(BO<Subscript>3</Subscript>)<Subscript>4</Subscript> multiferroic

The magnetic, magnetoelectric, and magnetoelastic properties of a PrFe₃(BO₃)₄ single crystal and the phase transitions induced in this crystal by the magnetic field are studied both experimentally and theoretically. Unlike the previously investigated ferroborates, this material is characterized by a singlet ground state of the rare-earth ion. It is found that, below T _N = 32 K, the magnetic structure of the crystal in the absence of the magnetic field is uniaxial (l ∥ c), while, in a strong magnetic field H ∥ c (H _cr ～ 43 kOe at T = 4.2 K), a Fe³⁺ spin reorientation to the basal plane takes place. The reorientation is accompanied by anomalies in magnetization, magnetostriction, and electric polarization. The threshold field values determined in the temperature interval 2–32 K are used to plot an H-T phase diagram. The contribution of the Pr³⁺ ion ground state to the parameters under study is revealed, and the influence of the praseodymium ion on the magnetic and magnetoelectric properties of praseodymium ferroborate is analyzed.     

Spin-polaron transport and magnetic phase diagram of iron monosilicide

The study of galvanomagnetic, magnetic, and magnetooptical characteristics of iron monosilicide in a wide range of temperatures (1.8–40 K) and magnetic fields (up to 120 kOe) has revealed the origin of the low-temperature sign reversal of the Hall coefficient in FeSi. It is shown that this effect is associated with an increase in the amplitude of the anomalous component of the Hall resistance ρ_H (the amplitude increases by more than five orders of magnitude with decreasing temperature in the range 1.8–20 K). The emergence of the anomalous contribution to ρ_H is attributed to the transition from the spin-polaron to coherent regime of electron density fluctuations in the vicinity of Fe centers and to the formation of nanosize ferromagnetic regions, i.e., ferrons (about 10 Å in diameter), in the FeSi matrix at T<T_C=15 K. An additional contribution to the Hall effect, which is observed near the temperature of sign reversal of ρ_H and is manifested as the second harmonic in the angular dependences ρ_H(?), cannot be explained in the framework of traditional phenomenological models. Analysis of magnetoresistance of FeSi in the spin-polaron and coherent spin fluctuation modes shows that the sign reversal of the ratio Δρ(H)/ρ accompanied by a transition from a positive (Δρ /ρ>0, T>T_m) to a negative (Δρ/ρ<0, T<T_m) magnetoresistance is observed in the immediate vicinity of the mictomagnetic phase boundary at T_m=7 K. The linear asymptotic form of the negative magnetoresistance Δρ/ρ ∝?H in weak magnetic fields up to 10 kOe is explained by the formation of magnetic nanoclusters from interacting ferrons in the mictomagnetic phase of FeSi at T<T_m. The results are used for constructing for the first time the low-temperature magnetic phase diagram of FeSi. The effects of exchange enhancement are estimated quantitatively and the effective parameters characterizing the electron subsystem in the paramagnetic (T>T_C), ferromagnetic (T_m<T< T_C), and mictomagnetic (T<T_m) phases are determined. Analysis of anomalies in the aggregate of transport, magnetic, and magnetooptical characteristics observed in the vicinity of H_m≈35 kOe at T<T_m leads to the conclusion that a new collinear magnetic phase with M∥H exists on the low-temperature phase diagram of iron monosilicide.     

Evolution of spin susceptibility from the Pauli to Curie-Weiss type in strongly correlated Fermi systems

The magnetic properties of strongly correlated Fermi systems are studied within the framework of the fermioncondensation model—phase transition associated with the rearrangement of the Landau quasiparticle distribution, resulting in the appearance of a plateau at T=0 exactly in the Fermi surface of the single-particle excitation spectrum. It is shown that the Curie-Weiss term ～T^?1 appears in the expression for the spin susceptibility χ_ac(T) of the system after the transition point at finite temperatures. The behavior of χ_ac(T, H) as a function of temperature and static magnetic field H in the region where the critical fermion-condensation temperature T _f is close to zero is discussed. The results are compared with the available experimental data.     

Mössbauer study of the modulated magnetic structure of FeVO<Subscript>4</Subscript>

Mössbauer spectroscopy is used to study the FeVO₄ multiferroic, which undergoes two magnetic phase transitions at T _N1 ≈ 22 K and T _N2 ≈ 15 K. The first transition (T _N1) is related to transformation from a paramagnetic state into a magnetically ordered state of a spin density wave, and the second transition (T _N2) is associated with a change in the type of the spatial magnetic structure of the vanadate. The electric field gradient tensor at ⁵⁷Fe nuclei is calculated to perform a crystal-chemical identification of the partial Mössbauer spectra corresponding to various crystallographic positions of Fe³⁺ cations. The spectra measured in the range T _N2 < T < T _N1 are analyzed on the assumption about amplitude modulation of the magnetic moments of iron atoms μ_Fe. The results of model intersection of the spectra recorded at T < T _N2 point to a high degree of anharmonicity of the helicoidal magnetic structure of the vanadate and to elliptic polarization of μ_Fe. These features are characteristic of type-II multiferroics. The temperature dependences of the hyperfine interaction parameters of ⁵⁷Fe nuclei that were obtained in this work are analyzed in terms of the Weiss molecular field model on the assumption of orbital contribution to the magnetic moments of iron cations.     

Phase transitions and magnetoelectric coupling in BiFe<Subscript>1−<Emphasis Type="Italic">x</Emphasis></Subscript>Zn<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript>O<Subscript>3</Subscript> multiferroics

Multiferroic BiFe_1?xZn _x O₃ ceramics were prepared by solution combustion method. Their structure, magnetoelectric, dielectric, magnetic, thermal characteristics were studied. The magnetic M(T) and heat capacity C _p (T) measurements demonstrate an antiferromagnetic to paramagnetic phase transition (T _N ) around 635 K. The anomaly on the temperature dependence of the dielectric constant near T _N was observed, which could be induced by the magnetoelectric coupling between electric and magnetic ordering. The magnetoelectric behavior was also confirmed by the linear relation between Δε and M², which is in the agreement of the Ginzburg-Landau theory for the second-order phase transition.     

High-pressure magnetic properties and <Emphasis Type="Italic">P-T</Emphasis> phase diagram of iron borate

The high-pressure magnetic states of iron borate ⁵⁷FeBO₃ single-crystal and powder samples have been investigated in diamond anvil cells by nuclear forward scattering (NFS) of synchrotron radiation at different temperatures. In the low-pressure (0 < P < 46 GPa) antiferromagnetic phase, an increase of the Neél temperature from 350 to 595 K induced by pressure was found. At pressures 46–49 GPa, a transition from the antiferromagnetic to a new magnetic state with a weak magnetic moment (magnetic collapse) was discovered. It is attributed to the electronic transition in Fe³⁺ ions from the high-spin 3d⁵ (S = 5/2, ⁶A_1g) to the low-spin (S = 1/2, ²T_2g) state (spin crossover) due to the insulator-semiconductor-type transition with extensive suppression of strong d-d electron correlations. At low temperatures, NFS spectra of the high-pressure phase indicate magnetic correlations in the low-spin system with a magnetic ordering temperature of about 50 K. A tentative magnetic P-T phase diagram of FeBO₃ is proposed. An important feature of this diagram is the presence of two triple points where magnetic and paramagnetic phases of the high-spin and low-spin states coexist.     

Antiferromagnetic Resonance in GdB<Subscript>6</Subscript>

The electron spin resonance has been measured for the first time both in the paramagnetic phase of the metallic GdB₆ antiferromagnet (T_N = 15.5K) and in the antiferromagnetic state (T < T_N). In the paramagnetic phase below T* ~ 70 K, the material is found to exhibit a pronounced increase in the resonance linewidth and a shift in the g-factor, which is proportional to the linewidth Δg(T) ~ ΔH(T). Such behavior is not characteristic of antiferromagnetic metals and seems to be due to the effects related to displacements of Gd³⁺ ions from the centrosymmetric positions in the boron cage. The transition to the antiferromagnetic phase is accompanied by an abrupt change in the position of resonance (from μ₀H₀ ≈ 1.9 T to μ₀H₀ ≈ 3.9 T at ν = 60 GHz), after which a smooth evolution of the spectrum occurs, resulting eventually in the formation of the spectrum consisting of four resonance lines. The magnetic field dependence of the frequency of the resonant modes ω₀(H₀) obtained in the range of 28–69 GHz is well interpreted within the model of ESR in an antiferromagnet with the easy anisotropy axis ω/γ = (H ₀ ² +2H_AH_E)^1/2, where H_E is the exchange field and H_A is the anisotropy field. This provides an estimate for the anisotropy field, H_A ≈ 800 Oe. This value can result from the dipole?dipole interaction related to the mutual displacement of Gd³⁺ ions, which occurs at the antiferromagnetic transition.     

Superconducting Properties of Indium Nanostructured in Pores of Thin Films of SiO<Subscript>2</Subscript> Microspheres

Samples of a superconducting indium nanocomposite based on a thin-film porous dielectric matrix prepared by the Langmuir–Blodgett method are obtained for the first time, and their low-temperature electrophysical and magnetic properties are studied. Films with thickness b ≤ 5 μm were made from silicon dioxide spheres with diameter D = 200 and 250 nm; indium was introduced into the pores of the films from the melt at a pressure of P ≤ 5 kbar. Thus, a three-dimensional weakly ordered structure of indium nanogranules was created in the pores, forming a continuous current-conducting grid. Measurements of the temperature and magnetic field dependences of the resistance and magnetic moment of the samples showed an increase in the critical parameters of the superconductivity state of nanostructured indium (critical temperature T_c ≤ 3.62 K and critical magnetic field H_c at T = 0 K H_c(0) ≤ 1700 Oe) with respect to the massive material (T_c = 3.41 K, H_c(0) = 280 Oe). In the dependence of the resistance on temperature and the magnetic field, a step transition to the superconductivity state associated with the nanocomposite structure was observed. A pronounced hysteresis M(H) is observed in the dependence of the magnetic moment M of the nanocomposite on the magnetic field at T < T_c, caused by the multiply connected structure of the current-conducting indium grid. The results obtained are interpreted taking into account the dimensional dependence of the superconducting characteristics of the nanocomposite.