On entropy production

We investigate the case of a dynamical system when irreversible time evolution is generated by a nonHermitian superoperator on the states of the system. We introduce a generalized scalar product which can be used to construct a monotonically changing functional of the state, a generalized entropy. This will depend on the level of system dynamics described by the evolution equation. In this paper we consider the special case when the irreversibility derives from imbedding the system of interest into a thermal reservoir. The ensuing time evolution is shown to be compatible both with equilibrium thermodynamics and the entropy production near the final steady state. In particular, Prigogine’s principle of minimum entropy production is discussed. Also the limit of zero temperature is considered. We present comments on earlier treatments.     

On the assumption of initial factorization in the master equation for weakly coupled systems I: General framework

We analyze the dynamics of a quantum mechanical system in interaction with a reservoir when the initial state is not factorized. In the weak-coupling (van Hove) limit, the dynamics can be properly described in terms of a master equation, but a consistent application of Nakajima-Zwanzig’s projection method requires that the reference (not necessarily equilibrium) state of the reservoir be endowed with the mixing property.     

Ab initio theory of complex electronic ground state of superconductors: I. Nonadiabatic modification of the Born-Oppenheimer approximation

The ARPES of high-T_c cuprates and theoretical results of low-Fermi energy band structure fluctuation for different groups of superconductors indicate that electron coupling to pertinent phonon modes drive system from adiabatic into anti-adiabatic state (ω>E_F). At these circumstances, not only Migdal-Eliashberg approximation is not valid, but basic adiabatic Born-Oppenheimer approximation (BOA) does not hold. At these circumstances, electronic structure has to be studied as explicitly dependent on instantaneous nuclear coordinates Q as well as on instantaneous nuclear momenta P.In the present paper—part I, it has been shown that Q, P-dependent modification of the BOA for ground electronic state can be derived by sequence of canonical transformations of the basis functions. The effect of nuclear coordinates and momenta on electronic structure is presented in the form of corrections to zero-, one- and two-particle terms of clamped nuclear Hamiltonian. In the anti-adiabatic state, correction to electronic ground state energy (zero-particle term correction) is negative and system can be stabilized in the anti-adiabatic state at distorted geometry with respect to adiabatic equilibrium structure and gap in one-particle spectrum of quasi-continuum states at Fermi level can be opened. Stabilization effect is solely the consequence of nuclear dynamics (P) that is crucial in anti-adiabatic state. It has been shown that nuclear dynamics also increases electron correlation until system at nuclear motion remains in a bound state. Corresponding corrections to electronic wave function are also specified.On the other hand, when system remains at vibration motion of nuclei in adiabatic state, the influence of nuclear dynamics (P-dependence) is negligible. In this case, all basic effects are covered through nuclear coordinates (Q-dependence) within the adiabatic BOA and standard results of solid-state (or molecular) physics are recovered.     

Low temperature specific heat of bi-layered manganites La2−2xSr1+2xMn2O7 (x=0.3 and 0.5)

The specific heat (C) of bi-layered manganites La_2−2xSr_1+2xMn₂O₇ (x=0.3 and 0.5) is investigated for the ground state of low temperature excitations. A T^3/2 dependent term in the low temperature specific heat (LTSH) is identified at zero magnetic field and suppressed by magnetic fields for x=0.3 sample, which is consistent with a ferromagnetic metallic ground state. For x=0.5 sample, a T² term is observed and is consistent with a two-dimensional (2D) antiferromagnetic insulator. However, it is almost independent of magnetic field within the range of measured temperature (0.6-10 K) and magnetic field (6 T).     

Atom-field entanglement in two-atom Jaynes-Cummings model with nondegenerate two-photon transitions

An exact solution of the problem of two two-level atoms with nondegenerate two-photon transitions and nondegenerate Raman transitions interacting with two-mode radiation field is presented. Asymptotic solutions for system state vectors are obtained in the approximation of large initial coherent fields. The atom-field entanglement is investigated on the basis of the reduced atomic entropy dynamics. The possibility of the system being initially in a pure disentangled state to revive into this state during the evolution process for both models is shown. Conditions and times of disentanglement are derived.     

In situ measurement of the surface stress evolution during magnetron sputter-deposition of Ag thin film

We measured the evolution of in situ surface stress of Ag thin film during the magnetron sputter deposition. The measurement of force per width of Ag thin film showed that both the surface state and surface stress of Ag layer can be controlled through the variation of the deposition conditions such as the deposition temperature and rate. At room temperature, the force per width curve of Ag film deposited to 1 Å/s showed a typical curve consisting of three stages of surface stress. A brief presence of initial compressive stage and broad tensile maximum resulting in a compressive state had a tendency to disappear with increasing the deposition temperature. Meanwhile, a development of final compressive stage was more at higher temperature. Similar effect was observed but less obvious on increasing the deposition rate.     

Magnetic phase transitions in TbAuIn compound

Magnetic properties of frustrated antiferromagnet TbAuIn are investigated by AC susceptibility, resistivity as well as specific heat measurements. In temperature dependence of the susceptibility two anomalies are visible, one at 33 K and another at 48 K. According to neutron diffraction studies the Néel temperature is 35 K. The second anomaly in the AC susceptibility seems to be attributed to antiferromagnetic cluster-glass state of Tb magnetic moments. The resistivity measurements confirm that TbAuIn exhibits long-range magnetic order below 35 K, moreover they reveal an anomalous behaviour above that temperature. However in the temperature dependence of the specific heat only one anomaly at 30 K is visible. The low temperature behaviour of susceptibility, resistivity and specific heat of the investigated antiferromagnetic material can be described, with a good accuracy, within the spin-wave theory with linear dispersion relation.     

The influence of substrate temperature variation on tungsten oxide thin film growth in an HFCVD system

Tungsten oxide (WO₃) thin films were deposited by a modified hot filament chemical vapor deposition (HFCVD) technique using Si (1 0 0) substrates. The substrate temperature was varied from room temperature to 430 °C at an interval of 100 °C. The influence of the substrate temperature on the structural and optical properties of the WO₃ films was studied. X-ray diffraction and Raman spectra show that as substrate temperature increases the film tends to crystallize from the amorphous state and the surface roughness decreases sharply after 230 °C as confirmed from AFM image analysis. Also from the X-ray analysis it is evident that the substrate orientation plays a key role in growth. There is a sharp peak for samples on Si substrate due to texturing. The film thickness also decreases as substrate temperature increases. UV-vis spectra show that as substrate temperature increases the film property changes from metallic to insulating behavior due to changing stoichiometry, which was confirmed by XPS analysis.     

Optical absorption and emission properties of Gd in silica host

We present a study of the optical properties of Gd-doped sol-gel silica glasses densified at different temperatures (from 450 up to 1050 °C) by means of optical absorption (OA) and radio luminescence (RL). The effect of a post-densification rapid thermal treatment (RTT) at approximately 1800 °C is also considered. Room temperature OA and RL measurements have revealed a slight low-energy shift of Gd³⁺ absorption/emission lines by densification temperature increasing accompanied by a parallel increase of Gd³⁺ RL intensities, especially strong after RTT. These effects are interpreted on the basis of structural modifications of the silica matrix and of the removal of non-radiative channels competing with Gd³⁺ emission. Moreover, RL spectra of fully densified samples display high-energy shoulders on the ⁶P_7/2-⁸S Gd³⁺ emission possibly related to crystal field splitting of the ⁶P_7/2 state. This interpretation is supported by the temperature dependence of RL spectra, investigated in the 10-320 K temperature interval: an increase of the intensity of high-energy components vs. temperature has been observed, which can be interpreted as due to thermally assisted excitation of electrons belonging to the lower ⁶P_7/2 state to higher crystal field states and their subsequent radiative recombination.     

Optical switching by controlling the double-dark resonances in a N-tripod five-level atom

We have investigated the optical switching in a five-level atom in a novel configuration of electromagnetically induced transparency. This N-tripod type level scheme combines the attractive features of cross-phase modulation appearing in N-type atoms with the ability to slow light pulses associated with tripod atoms. The addition of a new driving field to the usual tripod configuration allows to control the double-dark resonances which appear in the four-level tripod system and thus enables to manipulate the probe absorption and dispersion properties. We have studied the temporal dynamics of two pulses, a probe pulse and a switch propagating pulse through the sample. In the presence of the switching field, a deep in the absorption at resonance due to one-photon electromagnetically induced transparency appears and the atomic system is transparent to the probe field, which propagates at a very small group velocity. By tuning the fields, one of the usual double-dark resonances appearing in tripod system can be controlled (Stark-shifted) and the medium, which is transparent in the absence of the control field, will become highly absorptive. The linear and cross-phase modulation susceptibilities have been calculated and we predict the possibility to realize two-photon switching and giant cross-phase modulation. Finally we address the question about the generation of an entangled coherent state and we show that the giant cross-phase modulation provided by this N-tripod atomic system can be used for realizing polarization quantum phase gates.     

Development of the reaction time accelerating molecular dynamics method for simulation of chemical reaction

We present a novel and efficient method to integrate chemical reactions into molecular dynamics to simulate chemical reaction systems. We have dubbed this method RTAMD, an acronym for reaction time accelerating molecular dynamics. The methodology we propose here requires no more than the knowledge of the empirical intermolecular potentials for the species at play as well as the elementary reaction path among them. Bond formation during the simulation is performed by changing the inter-atomic potentials from those of the non-bonded species to those of the bonded ones, and a reaction is deemed to occur by the distance separating the bond forming atoms. In this way the energy barrier for a reaction is no longer considered; the estimation of the reaction rate, however, is possible by introducing the principles of the transition state theory. The simplicity of the present scheme to simulate chemical reactions enables it to be used in large-scale MD simulations involving a large number of simultaneous chemical reactions and to evaluate kinetic parameters. In this paper, the basic theory of the method is presented and application to simple equiatomic reaction system where the reaction rates were estimated was illustrated.     

Non-equilibrium dynamics for impurities in semiconductors

This paper summarizes the ‘first-principles’ calculations of the vibrational properties of impurities, which are critical to the optical identification of defects. The issue of temperature control for non-equilibrium molecular dynamics (NEMD) is discussed. Applications of NEMD include the calculations of the temperature-dependence of vibrational lifetimes and of the thermal conductivity of semiconductors as a function of their impurity content.     

A Hamilton-Jacobi formalism for thermodynamics

We show that classical thermodynamics has a formulation in terms of Hamilton-Jacobi theory, analogous to mechanics. Even though the thermodynamic variables come in conjugate pairs such as pressure/volume or temperature/entropy, the phase space is odd-dimensional. For a system with n thermodynamic degrees of freedom it is 2n+1-dimensional. The equations of state of a substance pick out an n-dimensional submanifold. A family of substances whose equations of state depend on n parameters define a hypersurface of co-dimension one. This can be described by the vanishing of a function which plays the role of a Hamiltonian. The ordinary differential equations (characteristic equations) defined by this function describe a dynamical system on the hypersurface. Its orbits can be used to reconstruct the equations of state. The ‘time’ variable associated to this dynamics is related to, but is not identical to, entropy. After developing this formalism on well-grounded systems such as the van der Waals gases and the Curie-Weiss magnets, we derive a Hamilton-Jacobi equation for black hole thermodynamics in General Relativity. The cosmological constant appears as a constant of integration in this picture.     

The microstructure investigation of GeTi thin film used for non-volatile memory

GeTi thin film has been found to have the reversible resistance switching property in our previous work. In this paper, the microstructure of this material with a given composition was investigated. The film was synthesized by magnetron sputtering and treated by the rapid temperature process. The results indicate a coexist status of amorphous and polycrystalline states in the as-deposited GeTi film, and the grains in the film are extremely fine. Furthermore, not until the film annealed at 600 °C, can the polycrystalline state be detected by X-ray diffraction. Based on the morphological analysis, the sputtered GeTi has the column growth tendency, and the column structure vanishes with the temperature increasing. The microstructure and thermal property analysis indicate that GeTi does not undergo evident phase change process during the annealing process, which makes the switching mechanism of GeTi different from that of chalcogenide memory material, the most widely used phase change memory material.     

Schottky-like anomaly in the low-temperature specific heat of single-crystal NdMnO3

The specific heat of single-crystal NdMnO₃ was investigated from 2 to 20 K under different magnetic fields up to 8 T. All the specific heat data show a Schottky-like anomaly, which becomes more indistinctive as increasing magnetic field. The experiment data were successfully fitted by taking into account factors such as crystal-field splitting, the two-level Schottky anomaly, the lattice vibration, and type-A antiferromagnetic (A-AF) spin waves. It was found that the splitting of the ground state doublet of Nd³⁺ ion increases linearly with magnetic field. The above phenomena can be interpreted in terms of the model of unchanged effective molecular field at Nd³⁺ site caused by the ferromagnetic component of A-AF structure of Mn spins. This ferromagnetic component is likely caused by the GdFeO₃-type octahedron rotation. In addition, it was also found that the magnetic field increases the spin-wave stiffness coefficient, but reduces the Debye temperature.     

On the assumption of initial factorization in the master equation for weakly coupled systems II: Solvable models

We analyze some solvable models of a quantum mechanical system in interaction with a reservoir when the initial state is not factorized. We apply Nakajima-Zwanzig’s projection method by choosing a reference state of the reservoir endowed with the mixing property. In van Hove’s limit, the dynamics is described in terms of a master equation. We observe that Markovianity becomes a valid approximation for timescales that depend both on the form factors of the interaction and on the observables of the reservoir that can be measured.     

Thermomagnetic transitions and coercivity mechanism in bulk composite Nd60Fe30Al10 alloys

The thermomagnetic behaviour (within the temperature range 553-300 K) for the bulk composite Nd₆₀Fe₃₀Al₁₀ alloy is described in terms of a transition from paramagnetic to superferromagnetic state at T=553 K, followed by a ferromagnetic ordering for T<473 K. For the superferromagnetic regime, the alloy thermomagnetic response was associated to a homogeneous distribution of magnetic clusters with mean magnetic moment and size of 1072 μ_B and 2.5 nm, respectively. For T<473 K, a pinning model of domain walls described properly the alloy coercivity dependence with temperature, from which the domain wall width and the magnetic anisotropy constant were estimated as being of ≈8 nm and ≈10⁵ J/m³, typical values of hard magnetic phases. Results are supported by microstructural and magnetic domain observations.     

Carrier injection level dependence of post-breakdown metastability in semi-insulating GaAs

Recently, a room temperature electrically induced metastability in semi-insulating (SI)-GaAs has been reported in which the normally high resistance state of SI-GaAs converts into a low resistance state when breakdown electric fields are applied to the metal/SI-GaAs/metal system. The low resistance state continues to persist when the electric field is lowered below the breakdown bias and as such may be treated as metastable state of the material. This phenomenon is believed to be closely related to the ‘lock-on’ effect utilized in high power photoconductive semiconductor switches made from SI-GaAs. The present study seeks to understand the mechanism for this electrically induced metastability by studying the influence of the injection current on the metastable phase. The data favor an interpretation of the high current state of the SI-GaAs in terms of double carrier injection and the sustaining of an internal electron-hole plasma in the material.     

Distinct critical fluctuations and molecular motions manifest in a model biomembrane

Lattice dynamics in bis-(n-C₁₆H₃₇NH₃)₂SnCl₆, where the hydrocarbon part is analogous to lipid membrane, was investigated by means of 200 MHz ¹H nuclear magnetic resonance. As a result, critical fluctuations and molecular dynamics associated with the phase transitions, an order-disorder and a conformational phase transition, were distinguished in a wide temperature range. The dynamical origin of the critical fluctuations, observed in the long-chain compounds but not in the short-chain compounds, by the laboratory frame spin-lattice relaxation measurements, is revealed and discussed in this work.     

Magnetic properties of the charge ordered Nd0.75Na0.25MnO3

Nd_0.75Na_0.25MnO₃ polycrystalline ceramic is prepared via sol-gel process and its magnetic properties and electron spin resonance (ESR) spectra have been investigated experimentally. As the compound is cooled from room temperature, a charge-ordered state first develops below 170 K. A high magnetic field melts the charge ordered state and stabilizes a ferromagnetic (FM) state below 170 K. A field induced transition, analogous to a spin flip transition, is observed between 40 and 170 K. The critical temperature for spin flip increases with increasing temperature. Below 130 K, the compound tends to be intrinsically inhomogeneous, i.e. FM clusters and paramagnetic domains coexist in this system at least, which is confirmed by ESR measurements. When the external magnetic field is zero, long range FM interaction is not developed in this system; however, a tendency of re-entrant FM transition is observed in this compound.