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1.
Phys Rev E ; 93: 042208, 2016 04.
Artigo em Inglês | MEDLINE | ID: mdl-27176294

RESUMO

External dc bias-field effects on the nonlinear dielectric relaxation and dynamic Kerr effect of a system of permanent dipoles in a uniaxial mean-field potential are studied via the rotational Brownian motion model postulated in terms of the infinite hierarchy of differential-recurrence equations for the statistical moments f_{n}(t)=〈P_{n}〉(t) (the expectation value of the Legendre polynomials P_{n}). By solving these equations, the nonlinear dielectric and Kerr-effect ac stationary responses are evaluated for arbitrary dc field strength via perturbation theory in the ac field. Simple analytic equations based on the large separation of the time scales of the fast intrawell and slow overbarrier (interwell) relaxation processes are also derived.

2.
J Chem Phys ; 134(4): 044530, 2011 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-21280771

RESUMO

Inertial effects in the rotational brownian motion in space of a rigid dipolar rotator (needle) in a uniaxial potential biased by an external field giving rise to asymmetry are treated via the infinite hierarchy of differential-recurrence relations for the statistical moments (orientational correlation functions) obtained by averaging the Euler-Langevin equation over its realizations in phase space. The solutions of this infinite hierarchy for the dipole correlation function and its characteristic times are obtained using matrix continued fractions showing that the model simultaneously predicts both slow overbarrier (or interwell) relaxation at low frequencies accompanied by intermediate frequency Debye relaxation due to fast near-degenerate motion in the wells of the potential (intrawell relaxation) as well as the high frequency resonance (Poley) absorption due to librations of the dipole moments. It is further shown that the escape rate of a brownian particle from a potential well as extended to the Kramers turnover problem via the depopulation factor yields a close approximation to the longest (overbarrier) relaxation time of the system. For zero and small values of the bias field parameter h, both the dipole moment correlation time and the longest relaxation time have Arrhenius behavior (exponential increase with increasing barrier height). While at values of h in excess of a critical value however far less than that required to achieve nucleation, the Arrhenius behavior of the correlation time disappears.

3.
J Phys Condens Matter ; 22(37): 376001, 2010 Sep 22.
Artigo em Inglês | MEDLINE | ID: mdl-21403209

RESUMO

It is shown that the signal-to-noise ratio of the magnetic moment fluctuations in the magnetic stochastic resonance of a quantum uniaxial paramagnet of arbitrary spin value S subjected to a weak probing ac field H(t) = H cos Ωt and a dc bias magnetic field H(0) displays a pronounced dependence on S. The dependence arises from the quantum dynamics of spins which differs markedly from the magnetization dynamics of classical superparamagnets. In the large spin limit, S --> ∞, the quantum solutions reduce to those for a classical uniaxial superparamagnet.


Assuntos
Espectroscopia de Ressonância Magnética , Magnetismo , Teoria Quântica , Simulação por Computador , Eletrônica , Ruído/prevenção & controle
4.
J Chem Phys ; 131(8): 084101, 2009 Aug 28.
Artigo em Inglês | MEDLINE | ID: mdl-19725602

RESUMO

Quantum effects in the noninertial Brownian motion of a particle in a double well potential are treated via a semiclassical Smoluchowski equation for the time evolution of the reduced Wigner distribution function in configuration space allowing one to evaluate the position correlation function, its characteristic relaxation times, and dynamic susceptibility using matrix continued fractions and finite integral representations in the manner of the classical Smoluchowski equation treatment. Reliable approximate analytic solutions based on the exponential separation of the time scales of the fast intrawell and slow overbarrier relaxation processes are given. Moreover, the effective and the longest relaxation times of the position correlation function yield accurate predictions of both the low and high frequency relaxation behavior. The low frequency part of the dynamic susceptibility associated with the Kramers escape rate behaves as a single Lorentzian with characteristic frequency given by the quantum-mechanical reaction rate solution of the Kramers problem. As a particular example, quantum effects in the stochastic resonance are estimated.

5.
J Chem Phys ; 130(6): 064110, 2009 Feb 14.
Artigo em Inglês | MEDLINE | ID: mdl-19222270

RESUMO

The inertial rotational Brownian motion and dielectric relaxation of an assembly of noninteracting rodlike polar molecules in a uniaxial potential are studied. The infinite hierarchy of differential-recurrence relations for the equilibrium correlation functions is generated by averaging the governing inertial Langevin equation over its realizations in phase space. The solution of this hierarchy for the one-sided Fourier transforms of the relevant correlation functions is obtained using matrix continued fractions yielding the longitudinal dipole correlation function, the correlation time, and the complex polarizability, which are calculated for typical values of the model parameters. Pronounced inertial effects appear in these characteristics in the high-frequency region for low damping. The exact longitudinal correlation time is compared with the predictions of the Kramers theory of the escape rate of a Brownian particle from a potential well as extended by Mel'nikov and Meshkov [J. Chem. Phys. 85, 1018 (1986)]. In the low temperature limit, the universal Mel'nikov and Meshkov formula for the inverse of the escape rate provides a good estimate of the longitudinal correlation time for all values of the dissipation including the very low damping, very high damping, and Kramers turnover regimes. Moreover, the low-frequency part of the spectra of the longitudinal correlation function may be approximated by a single Lorentzian with a halfwidth determined by this universal escape rate formula.


Assuntos
Rotação , Temperatura , Fatores de Tempo
6.
Phys Rev E Stat Nonlin Soft Matter Phys ; 80(5 Pt 1): 051106, 2009 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-20364946

RESUMO

Quantum effects in the noninertial Brownian motion of a particle in a one-dimensional ratchet potential are treated in the high temperature and weak bath-particle coupling limit by solving a quantum Smoluchowski equation for the time evolution of the Wigner function in configuration space. In particular, an analytical expression for the stationary average drift velocity for constant driving forces is presented including quantum corrections to any order in Planck's constant. The corresponding frequency response is determined using continued fractions in both the linear approximation holding for small ac driving amplitude and in the nonlinear regime for arbitrary driving amplitude exhibiting pronounced ac induced frequency dependence of the dc component of the average drift velocity. Moreover, Shapiro steps are apparent in the dc characteristics for strong ac driving just as in the dc current-voltage characteristics of a point Josephson junction.


Assuntos
Transferência de Energia , Modelos Químicos , Modelos Estatísticos , Teoria Quântica , Simulação por Computador , Difusão
7.
Phys Rev E Stat Nonlin Soft Matter Phys ; 80(6 Pt 1): 061102, 2009 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-20365113

RESUMO

The normal phase diffusion problem in magnetic resonance imaging (MRI) is treated by means of the Langevin equation for the phase variable using only the properties of the characteristic function of Gaussian random variables. The calculation may be simply extended to anomalous diffusion using a fractional generalization of the Langevin equation proposed by Lutz [E. Lutz, Phys. Rev. E 64, 051106 (2001)] pertaining to the fractional Brownian motion of a free particle coupled to a fractal heat bath. The results compare favorably with diffusion-weighted experiments acquired in human neuronal tissue using a 3 T MRI scanner.


Assuntos
Algoritmos , Imagem de Difusão por Ressonância Magnética/métodos , Interpretação de Imagem Assistida por Computador/métodos , Modelos Biológicos , Simulação por Computador
8.
J Chem Phys ; 129(14): 144505, 2008 Oct 14.
Artigo em Inglês | MEDLINE | ID: mdl-19045156

RESUMO

A method of calculation of nonlinear transient responses of an assembly of noninteracting polar linear molecules due to sudden changes in a strong external dc electric field is presented. The infinite hierarchy of differential-recurrence relations for the decay functions describing the relaxation of the system is derived by averaging the underlying inertial Langevin equation. The solution of this hierarchy is obtained in terms of matrix continued fractions. The integral relaxation time and the spectrum of the electric polarization for various nonlinear transient responses (step-on, step-off, and rapidly rotating field) are calculated for typical values of the model parameters. The nonlinear transient responses exhibit pronounced nonlinear effects due to the strong dc field. Analytical equations for the quantities of interest are presented in the overdamped limit. Furthermore, the linear response relaxation function and linear dynamic susceptibility are obtained as a particular case of a general nonlinear theory.

9.
Phys Rev E Stat Nonlin Soft Matter Phys ; 78(3 Pt 1): 031114, 2008 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-18851000

RESUMO

Quantum corrections to the noninertial Brownian motion of a particle in a one-dimensional tilted cosine periodic potential are treated in the high-temperature and weak bath-particle coupling limit by solving a quantum Smoluchowski equation for the time evolution of the distribution function in configuration space. The theoretical predictions from two different forms of the quantum Smoluchowski equation already proposed-viz., J. Ankerhold [Phys. Rev. Lett. 87, 086802 (2001)] and W. T. Coffey [J. Phys. A 40, F91 (2007)]-are compared in detail in a particular application to the dynamics of a point Josephson junction. Various characteristics (stationary distribution, current-voltage characteristics, mean first passage time, linear ac response) are evaluated via continued fractions and finite integral representations in the manner customarily used for the classical Smoluchowski equation. The deviations from the classical behavior, discernible in the dc current-voltage characteristics as enhanced current for a given voltage and in the resonant peak in the impedance curve as an enhancement of the Q factor, are, respectively, a manifestation of relatively high-temperature nondissipative tunneling (reducing the barrier height) and dissipative tunneling (reducing the damping of the Josephson oscillations) near the top of a barrier.

10.
J Chem Phys ; 127(7): 074502, 2007 Aug 21.
Artigo em Inglês | MEDLINE | ID: mdl-17718615

RESUMO

Quantum effects in the Brownian motion of a particle in the symmetric double well potential V(x)=ax(2)2+bx(4)4 are treated using the semiclassical master equation for the time evolution of the Wigner distribution function W(x,p,t) in phase space (x,p). The equilibrium position autocorrelation function, dynamic susceptibility, and escape rate are evaluated via matrix continued fractions in the manner customarily used for the classical Fokker-Planck equation. The escape rate so yielded has a quantum correction depending strongly on the barrier height and is compared with that given analytically by the quantum mechanical reaction rate solution of the Kramers turnover problem. The matrix continued fraction solution substantially agrees with the analytic solution. Moreover, the low-frequency part of the spectrum associated with noise assisted Kramers transitions across the potential barrier may be accurately described by a single Lorentzian with characteristic frequency given by the quantum mechanical reaction rate.

11.
Phys Rev E Stat Nonlin Soft Matter Phys ; 75(3 Pt 1): 031101, 2007 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-17500662

RESUMO

The anomalous translational diffusion including inertial effects of nonlinear Brownian oscillators in a double well potential V(x)=ax{2}/2+bx{4}/4 is considered. An exact solution of the fractional Klein-Kramers (Fokker-Planck) equation is obtained allowing one to calculate via matrix continued fractions the positional autocorrelation function and dynamic susceptibility describing the position response to a small external field. The result is a generalization of the solution for the normal Brownian motion in a double well potential to fractional dynamics (giving rise to anomalous diffusion).

12.
J Chem Phys ; 126(8): 084502, 2007 Feb 28.
Artigo em Inglês | MEDLINE | ID: mdl-17343453

RESUMO

It is shown how the rotational diffusion model of polar molecules (which may be described in microscopic fashion as the diffusion limit of a discrete time random walk on the surface of the unit sphere) may be extended to anomalous nonlinear dielectric relaxation and the dynamic Kerr effect by using a fractional kinetic equation. This fractional kinetic equation (obtained via a generalization of the noninertial kinetic equation of conventional rotational diffusion to fractional kinetics to include anomalous relaxation) is solved using matrix continued fractions yielding the complex nonlinear dielectric susceptibility and the Kerr function of an assembly of rigid dipolar particles acted on by external superimposed dc E0 and ac E1(t)=E1 cos omegat electric fields of arbitrary strengths. In the weak field limit, analytic equations for nonlinear response functions are also derived.

13.
Phys Rev E Stat Nonlin Soft Matter Phys ; 76(5 Pt 1): 051104, 2007 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-18233620

RESUMO

Nonlinear longitudinal relaxation of a spin in a uniform external dc magnetic field is treated using a master equation for the quasiprobability distribution function of spin orientations in the configuration space of polar and azimuthal angles (analogous to the Wigner phase space distribution for translational motion). The solution of the corresponding classical problem of the rotational Brownian motion of a magnetic moment in an external magnetic field essentially carries over to the quantum regime yielding in closed form the dependence of the longitudinal spin relaxation on the spin size S as well as an expression for the integral relaxation time, which in linear response reduces to that previously given by D. A. Garanin [Phys. Rev. E 55, 2569 (1997)] using the density matrix approach. The nonlinear relaxation is dominated by a single exponential having as time constant the integral relaxation time. Thus a simple description in terms of a Bloch equation holds even for the nonlinear response of a giant spin.

14.
Phys Rev E Stat Nonlin Soft Matter Phys ; 74(1 Pt 1): 011105, 2006 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-16907059

RESUMO

The fractional translational diffusion of a particle in a double-well potential (excluding inertial effects) is considered. The position correlation function and its spectrum are evaluated using a fractional probability density diffusion equation (based on the diffusion limit of a fractal time random walk). Exact and approximate solutions for the dynamic susceptibility describing the position response to a small external field are obtained. The exact solution is given by matrix continued fractions while the approximate solution relies on the exponential separation of the time scales of the fast "intrawell" and low overbarrier relaxation processes associated with the bistable potential. It is shown that knowledge of the characteristic relaxation times for normal diffusion allows one to predict accurately the anomalous relaxation behavior of the system for all relevant time scales.

15.
J Chem Phys ; 123(9): 94503, 2005 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-16164349

RESUMO

The Kramers theory of the escape rate of a Brownian particle from a potential well as extended by Mel'nikov and Meshkov is used to evaluate the relaxation times and the dynamic susceptibility for the rotational Brownian motion of fixed axis rotators in an asymmetric double-well potential. An expression for the escape rate valid for all values of the dissipation including the very low damping (VLD), very high damping (VHD), and crossover regimes is derived. It is shown that this expression provides a good asymptotic estimate of the inverse of the smallest nonvanishing eigenvalue lambda(1) of the underlying Fokker-Planck operator calculated by using the matrix-continued fraction method. For low barriers, where the Mel'nikov and Meshkov approach is not applicable, analytic equations for the correlation time tau( parallel) of the longitudinal dipole correlation function in the VLD and VHD limits are derived and a simple extrapolating equation valid for all values of the damping is proposed.

16.
Phys Rev E Stat Nonlin Soft Matter Phys ; 72(1 Pt 1): 011103, 2005 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-16089933

RESUMO

The longitudinal and transverse components of the complex dielectric susceptibility tensor of an assembly of dipolar molecules rotating in an asymmetric double-well potential are evaluated using a fractional rotational diffusion equation (based on the diffusion limit of a fractal time random walk) for the distribution function of orientations of the molecules on the surface of the unit sphere. The calculation is the fractional analog of the Debye theory of orientational relaxation in the presence of external and mean field potentials (excluding inertial effects). Exact and approximate (based on the exponential separation for normal diffusion of the time scales of the intrawell and overbarrier relaxation processes associated with the bistable potential) solutions for the dielectric dispersion and absorption spectra are obtained. It is shown that a knowledge of the characteristic relaxation times for normal rotational diffusion is sufficient to predict accurately the anomalous dielectric relaxation behavior of the system for all time scales of interest. The model explains the anomalous (Cole-Cole-like) relaxation of complex dipolar systems, where the anomalous exponent differs from unity (corresponding to the normal dielectric relaxation), i.e., the relaxation process is characterized by a broad distribution of relaxation times (e.g., in glass-forming liquids).

17.
Phys Rev E Stat Nonlin Soft Matter Phys ; 70(4 Pt 1): 041103, 2004 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-15600393

RESUMO

It is shown how the Debye rotational diffusion model of dielectric relaxation of polar molecules (which may be described in microscopic fashion as the diffusion limit of a discrete time random walk on the surface of the unit sphere) may be extended to yield the empirical Havriliak-Negami (HN) equation of anomalous dielectric relaxation from a microscopic model based on a kinetic equation just as in the Debye model. This kinetic equation is obtained by means of a generalization of the noninertial Fokker-Planck equation of conventional Brownian motion (generally known as the Smoluchowski equation) to fractional kinetics governed by the HN relaxation mechanism. For the simple case of noninteracting dipoles it may be solved by Fourier transform techniques to yield the Green function and the complex dielectric susceptibility corresponding to the HN anomalous relaxation mechanism.

18.
J Chem Phys ; 120(19): 9199-211, 2004 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-15267857

RESUMO

The extension of the Kramers theory of the escape rate of a Brownian particle from a potential well to the entire range of damping proposed by Mel'nikov and Meshkov [J. Chem, Phys. 85, 1018 (1986)] is applied to the rotational Brownian motion of fixed axis rotators in a double well cosine potential. The procedure yields an expression for the Kramers escape rate valid for all values of the dissipation including the very low damping (VLD), very high damping (VHD), and crossover regimes. This equation provides a good asymptotic estimate of the correlation time tau per pendicular of the longitudinal dipole moment correlation function calculated by solving the underlying Langevin equation using the matrix-continued fraction method. Moreover, for low barriers, where the Mel'nikov and Meshkov approach is not applicable, analytic equations for tau in the VLD and VHD limits are derived and a simple extrapolating equation that is valid for all values of the damping is proposed.

19.
Phys Rev E Stat Nonlin Soft Matter Phys ; 69(3 Pt 1): 031114, 2004 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-15089272

RESUMO

The linear dielectric response of an assembly of noninteracting symmetrical top molecules (each of which is free to rotate in space) is evaluated in the context of fractional dynamics. The infinite hierarchy of differential-recurrence relations for the relaxation functions appropriate to the dielectric response is derived by using the underlying inertial fractional Klein-Kramers equation. On solving this hierarchy in terms of matrix continued fractions (as in the normal rotational diffusion), the complex dynamic susceptibility is obtained and is calculated for typical values of the model parameters. For the limiting case of spherical top molecules, the solution is obtained in terms of an ordinary continued fraction. It is shown that the model can reproduce nonexponential anomalous dielectric relaxation behavior at low frequencies (omegatau

20.
Phys Rev E Stat Nonlin Soft Matter Phys ; 69(2 Pt 1): 021105, 2004 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-14995425

RESUMO

Exact and approximate solutions of the fractional diffusion equation for an assembly of fixed-axis dipoles are derived for anomalous noninertial rotational diffusion in a double-well potential. It is shown that knowledge of three time constants characterizing the normal diffusion, viz., the integral relaxation time, the effective relaxation time, and the inverse of the smallest eigenvalue of the Fokker-Planck operator, is sufficient to accurately predict the anomalous relaxation behavior for all time scales of interest.

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