All-optical probe of magnetization dynamics in exchange biased bilayers on the picosecond timescale

All-optical control of the magnetization of polycrystalline exchange bias bilayer systems is achieved using short picosecond laser pulses. Due to the photoexcitation, the spin temperature across the interface between the ferromagnetic and antiferromagnetic layer is elevated, resulting in a collapse of the interfacial exchange coupling. Thus, within the first 10 ps, a fast reduction of both the exchange bias field and the coercive field is observed for three different exchange bias systems comprising both different ferromagnets and antiferromagnets. The fast thermal unpinning is followed by a slower heat diffusion dominated relaxation process, which strongly depends on the thermal conductivity of the used buffer layers and substrates. The fast optical unpinning can be understood in terms of an internal anisotropy pulse field capable of triggering ultrafast precessional magnetization dynamics of the ferromagnetic layer, which makes heat-assisted coherent magnetization rotation feasible.     

Ultrafast light-induced magnetization dynamics of ferromagnetic semiconductors

We develop a theory of ultrafast light-induced magnetization dynamics in ferromagnetic semiconductors. We demonstrate magnetization control during femtosecond time scales via the interplay between nonlinear circularly polarized optical excitation, hole-spin damping, polarization dephasing, and Mn-hole-spin interactions. Our results show magnetization relaxation and precession for the duration of the optical pulse governed by the nonlinear optical polarizations and populations.     

Formation of the front of longitudinal evolution of the magnetic moment of a ferromagnet under strong inhomogeneous excitation

The longitudinal evolution of the initial magnetization wave front (formed, for example, due to the ultrafast demagnetization of a part of the ferromagnetic material by a femtosecond laser pulse) toward the wave front with a minimum velocity occurs through an intermediate fast wave front. This fast wave front can significantly increase the relaxation rate of the net magnetization in finite-size samples.     

Transverse relaxation in the rotating frame induced by chemical exchange

In the presence of radiofrequency irradiation, relaxation of magnetization aligned with the effective magnetic field is characterized by the time constant T1rho. On the other hand, the time constant T2rho characterizes the relaxation of magnetization that is perpendicular to the effective field. Here, it is shown that T2rho can be measured directly with Carr-Purcell sequences composed of a train of adiabatic full-passage (AFP) pulses. During adiabatic rotation, T2rho characterizes the relaxation of the magnetization, which under adiabatic conditions remains approximately perpendicular to the time-dependent effective field. Theory is derived to describe the influence of chemical exchange on T2rho relaxation in the fast-exchange regime, with time constant defined as T2rho,ex. The derived theory predicts the rate constant R2rho,ex (= 1/T2rho,ex) to be dependent on the choice of amplitude- and frequency-modulation functions used in the AFP pulses. Measurements of R2rho,ex of the water/ethanol exchanging system confirm the predicted dependence on modulation functions. The described theoretical framework and adiabatic methods represent new tools to probe exchanging systems.     

Ultrafast hopping dynamics of 5f electrons in the Mott insulator UO₂ studied by femtosecond pump-probe spectroscopy

We describe a femtosecond pump-probe study of ultrafast hopping dynamics of 5f electrons in the Mott insulator UO? following Mott-gap excitation at temperatures of 5-300 K. Hopping-induced response of the lattice and electrons is probed by transient reflectivity at mid- and above-gap photon energies, respectively. These measurements show an instantaneous hop, subsequent picosecond lattice deformation, followed by acoustic phonon emission and microsecond relaxation. Temperature-dependent studies indicate that the slow relaxation results from Hubbard excitons formed by U3?-U?? pairs.     

Efficiency of paramagnetic relaxation enhancement in off-resonance rotating frame

Transferring from laboratory frame to off-resonance rotating frame for the (1)H spin can compensate the relaxivity loss for paramagnetic agents at the magnetic field strength higher than 3 Tesla and enhance water relaxation rate constant significantly. A comprehensive theory for calculating the relaxation rate constants in the off-resonance rotating frame is described. This theory considers the contributions from both inner shell and outer shell water. The derived relaxation rate constants and relaxation enhancement efficiency as a function of the magnetic field strength and the effective field parameters are directly correlated to the structures, dynamics and environments of paramagnetic agents. To validate the theoretical predictions, we have measured the relaxation enhancement efficiency for a series of macromolecule conjugated gadolinium chelates at 9.4 Tesla. The experimental results confirmed the theoretical predictions. The theory also predicts the relaxation enhancement for T(2)-type paramagnetic agents at high magnetic fields. Promising fields of applications include situations where T(1)- or T(2)-type paramagnetic agents are used for labeling molecular/cellular events.     

Phenomenology of current-induced dynamics in antiferromagnets

We derive a phenomenological theory of current-induced staggered magnetization dynamics in antiferromagnets. The theory captures the reactive and dissipative current-induced torques and the conventional effects of magnetic fields and damping. A Walker ansatz describes the dc current-induced domain-wall motion when there is no dissipation. If magnetic damping and dissipative torques are included, the Walker ansatz remains robust when the domain wall moves slowly. As in ferromagnets, the domain-wall velocity is proportional to the ratio between the dissipative torque and the magnetization damping. In addition, a current-driven antiferromagnetic domain wall acquires a net magnetic moment.     

The study of ultrafast magnetization dynamics induced by femtosecond laser pulses in GdFeCo amorphous film

The time-resolved magneto-optical Kerr spectroscopy technique is used to study the ultrafast magnetization dynamics induced by femtosecond laser pulses in GdFeCo amorphous film. We study concretely the influence of the different pump fluence and the different external magnetic field on magnetization dynamics of ultrafast demagnetization, magnetization reversal and magnetization recovery. The pump fluence dependence magnetization dynamics shows that the degree of demagnetization, the degree of magnetization reversal and the time of magnetization recovery increase with pump fluence, which can be interpreted by the “three-temperature” model. The external magnetic field dependence magnetization dynamics shows that the rate of magnetization reversal increases with the external field, which accord with the magnetization reversal mechanism based on the reversed magnetic domain nucleation and domain-wall motion.     

Dynamics of paramagnetic agents by off-resonance rotating frame technique

Off-resonance rotating frame technique offers a novel tool to explore the dynamics of paramagnetic agents at high magnetic fields (B0 > 3T). Based on the effect of paramagnetic relaxation enhancement in the off-resonance rotating frame, a new method is described here for determining the dynamics of paramagnetic ion chelates from the residual z-magnetizations of water protons. In this method, the dynamics of the chelates are identified by the difference magnetization profiles, which are the subtraction of the residual z-magnetization as a function of frequency offset obtained at two sets of RF amplitude omega(1) and pulse duration tau. The choices of omega(1) and tau are guided by a 2-D magnetization map that is created numerically by plotting the residual z-magnetization as a function of effective field angle theta and off-resonance pulse duration tau. From the region of magnetization map that is the most sensitive to the alteration of the paramagnetic relaxation enhancement efficiency R(1rho)/R1, the ratio of the off-resonance rotating frame relaxation rate constant R(1rho) verse the laboratory frame relaxation rate constant R(1), three types of difference magnetization profiles can be generated. The magnetization map and the difference magnetization profiles are correlated with the rotational correlation time tauR of Gd-DTPA through numerical simulations, and further validated by the experimental data for a series of macromolecule conjugated Gd-DTPA in aqueous solutions. Effects of hydration water number q, diffusion coefficient D, magnetic field strength B0 and multiple rotational correlation times are explored with the simulations of the magnetization map. This method not only provides a simple and reliable approach to determine the dynamics of paramagnetic labeling of molecular/cellular events at high magnetic fields, but also a new strategy for spectral editing in NMR/MRI based on the dynamics of paramagnetic labeling in vivo.     

低温生长砷化镓的超快光抽运-太赫兹探测光谱

本文采用光抽运-太赫兹探测技术系统研究了低温生长砷化镓(LT-GaAs)中光生载流子的超快动力学过程.光激发LT-GaAs薄层电导率峰值随抽运光强增加而增加,最后达到饱和,其饱和功率为54μJ/cm~2.当载流子浓度增大时,电子间的库仑相互作用将部分屏蔽缺陷对电子的俘获概率,从而导致LT-GaAs的快速载流子俘获时间随抽运光强增加而变长.光激发薄层电导率的色散关系可以用Cole-Cole Drude模型很好地拟合,结果表明LT-GaAs内部载流子的散射时间随抽运光强增加和延迟时间(产生光和抽运光)变长而增加,主要来源于电子-电子散射以及电子-杂质缺陷散射共同贡献,其中电子-杂质缺陷散射的强度与光激发薄层载流子浓度密切相关,并可由散射时间分布函数α来描述.通过对光激发载流子动力学、光激发薄层电导率以及迁移率变化的研究,我们提出适当增加缺陷浓度,可以进一步降低载流子迁移率和寿命,为研制和设计优良的THz发射器提供了实验依据.     

Effect of a dc magnetic field on the magnetization relaxation of uniaxial single-domain ferromagnetic particles driven by a strong ac magnetic field

The nonlinear ac stationary response of the magnetization of noninteracting uniaxial single-domain ferromagnetic particles acted on by superimposed dc and ac magnetic fields applied along the anisotropy axis is evaluated from the Fokker-Planck equation, expressed as an infinite hierarchy of recurrence equations for Fourier components of the relaxation functions governing longitudinal relaxation of the magnetization. The exact solution of this hierarchy comprises a matrix continued fraction, allowing one to evaluate the ac nonlinear response and reversal time of the magnetization. For weak ac fields, the results agree with perturbation theory. It is shown that the dc bias field changes substantially the magnetization dynamics leading to new nonlinear effects. In particular, it is demonstrated that for a nonzero bias field as the magnitude of the ac field increases the reversal time first increases and having attained its maximum at some critical value of the ac field, decreases exponentially.     

X-ray detected ferromagnetic resonance in thin films

We discuss the physical content of X-ray Detected Magnetic Resonance (XDMR), i.e. a novel spectroscopy which uses XMCD to probe the resonant precession of the local magnetization in a strong microwave pump field. We focus on the simplest case of a steady-state precession of elemental moments in the non-linear regime of angular foldover. Like XMCD, XDMR is element and edge selective and could become a unique tool to investigate how precessional dynamics can locally affect the spin and orbital magnetization of p- or d-projected DOS. This should be possible only in the limit where there is no overdamping due to ultrafast orbit-lattice relaxation.     

Spin-flip processes and ultrafast magnetization dynamics in Co: Unifying the microscopic and macroscopic view of femtosecond magnetism

The femtosecond magnetization dynamics of a thin cobalt film excited with ultrashort laser pulses has been studied using two complementary pump-probe techniques, namely, spin-, energy-, and time-resolved photoemission and the time-resolved magneto-optical Kerr effect. Combining the two methods, it is possible to identify the microscopic electron spin-flip mechanisms responsible for the ultrafast macroscopic magnetization dynamics of the cobalt film. In particular, we show that electron-magnon excitation does not affect the overall magnetization even though it is an efficient spin-flip channel on the sub-200 fs time scale. Instead, we find experimental evidence for the relevance of Elliott-Yafet-type spin-flip processes for the ultrafast demagnetization taking place on a time scale of 300 fs.     

自旋极化度对GaAs量子阱中吸收饱和效应与载流子复合动力学的影响研究

本文研究了(001) GaAs量子阱薄膜中重空穴激子近共振抽运-探测的载流子自旋弛豫动力学, 发现载流子的自旋极化对传统的线偏振光吸收饱和效应和载流子复合动力学都有影响. 进一步的抽运流依赖的自旋弛豫和复合动力学研究表明, 自旋极化对线偏振光的吸收饱和效应的影响随抽运流降低而变弱. 在低激发流时, 自旋极化对线偏振吸收饱和效应的影响才可忽略. 然而, 又显现出自旋极化对复合动力学的影响. 分析表明复合动力学的自旋极化依赖性起源于重空穴激子形成浓度的自旋极化依赖性. 复合动力学的自旋极化依赖性表明自旋弛豫时间计算中所涉及的复合时间应该使用自旋极化载流子的复合时间. 基于二维质量作用定律的激子浓度计算表明, 库仑屏蔽效应对激子形成的影响在较低激发载流子浓度下可以忽略.     

Conservative and dissipative fiber Bragg solitons (a review)

We present a comparative review of two classes of optical solitons—conservative and dissipative solitons—propagating in single-mode optical fibers in which refractive-index gratings are induced such that their period is comparable with the radiation wavelength. Fibers that have the Kerr nonlinearity and negligibly small losses and that do not gain radiation (conservative system) are described by traditional equations of the approximation of slowly varying amplitudes, and effects caused by the nonlinearity of the medium, such as nonlinear switching, optical bistability, and formation of conservative Bragg solitons are considered. It is shown that the passage beyond the scope of the approximation of slowly varying amplitudes makes it possible to describe new important effects, including localization of soliton centers near maxima of the refractive-index grating. Bright and dark conservative solitons are demonstrated, which are formed when the Kerr nonlinearity is replaced by the nonlinearity of two-level atomic systems. The properties of conservative solitons in resonance semiconductor Bragg structures with quantum wells are considered. Results of experimental studies of nonlinear effects in fibers with Bragg gratings are presented. For an active single-mode fiber with a Bragg refractive-index grating and nonlinear gain and absorption, dissipative solitons are described using the approximation of slowly varying amplitudes and inertialess nonlinearity. It is shown that the dissipative factors qualitatively change the properties of solitons compared to the conservative case. Using the Maxwell-Bloch equations, it is demonstrated that the ratio between the gain and absorption relaxation times significantly affects the stability of localized structures. The interaction of dissipative optical Bragg solitons is described. It is shown that, beyond the scope of the approximation of slowly varying amplitudes, the average velocity of propagating dissipative Bragg solitons acquires only discrete values, and formation of pairs of solitons with two values of the phase difference becomes possible. For a birefringent fiber, dissipative vector optical Bragg solitons are demonstrated.     

Magnetic properties of MnAs nanocrystals embedded in GaAs

A phenomenological model for explaining the magnetic properties of MnAs nanocrystals embedded in GaAs is proposed. It is shown that experimental data of DC magnetization as a function of temperature, obtained according to zero-field-cooled and field-cooled protocols, can be understood assuming a transition of the system from a low temperature state in which very slow dynamics is observed (frozen state) to a high-temperature state in which dynamics is fast (quasi superparamagnetic state).     

苯乙炔分子电子激发态超快动力学研究

采用飞秒时间分辨质谱技术结合飞秒时间分辨光电子影像技术研究了苯乙炔分子电子激发态超快非绝热弛豫动力学.用235 nm光作为泵浦光,将苯乙炔分子激发到第二激发态S2,用400 nm光探测激发态的演化过程.时间分辨的母体离子的变化曲线用指数和高斯函数卷积得到不同的两个组分,一个是超快衰减组分,时间常数为116 fs,一个是慢速组分,时间常数为106 ps.通过分析时间分辨的光电子影像得到光电子动能分布,结合时间分辨光电子能谱数据发现,时间常数为116 fs的快速组分反映了S2态向S1态的内转换过程.实验还表明S1态通过内转换被布局后向T1态的系间窜跃过程为重要的衰减通道.本工作为苯乙炔分子S2态非绝热弛豫动力学提供了较清晰的物理图像.     

Laser induced ultrafast demagnetization in diluted magnetic semiconductor nanostructures

We present a dynamical model that reproduces the observed time evolution of the magnetization in diluted magnetic semiconductor films after weak laser excitation. Based on a many-particle expansion of the exact p–d exchange interaction, our approach goes beyond the usual mean-field approximation. Numerical results demonstrate that the hole spin relaxation plays a crucial role for explaining the ultrafast demagnetization processes observed experimentally. The influence of the laser power on the magnetization dynamics is also investigated.     

Spin-lattice relaxation and a fast T1-map acquisition method in MRI with transient-state magnetization

The magnetization under the spin-lattice relaxation and the nuclear magnetic resonance radiofrequency (RF) pulses is calculated for a signal RF pulse train and for a sequence of multiple RF pulse-trains. It is assumed that the transverse magnetization is zero when each RF pulse is applied. The result expressions can be grouped into two terms: a decay term, which is proportional to the initial magnetization M0, and a recovery term, which has no M0 dependence but strongly depends on the spin-lattice relaxation and the equilibrium magnetization Meq. In magnetic resonance pulse sequences using magnetization in transient state, the recovery term produces artifacts and can seriously degrade the function of the preparation sequence for slice selection, contrast weighting, phase encoding, etc. This work shows that the detrimental effect can be removed by signal averaging in an eliminative fashion. A novel fast data acquisition method for constructing the spin-lattice relaxation (T1) map is introduced. The method has two features: (i) By using eliminative averaging, the curve to fit the T1 value is a decay exponential function rather than a recovery one as in conventional techniques; therefore, the measurement of Meq is not required and the result is less susceptible to the accuracy of the inversion RF pulse. (ii) The decay exponential curve is sampled by using a sequence of multiple pulse-trains. An image is reconstructed from each train and represents a sample point of the curve. Hence a single imaging sequence can yield multiple sample points needed for fitting the T1 value in contrast to conventional techniques that require repeating the imaging sequence for various delay values but obtain only one sample point from each repetition.     

A pulse EPR study of longitudinal relaxation of the stable radical in gamma-irradiated L-alanine

The longitudinal relaxation rate of the first stable alanine radical, SAR1, was studied by employing pulse EPR technique over a wide temperature interval (5-290 K). The complex nonexponential recovery of the longitudinal magnetization in this temperature interval has been described with two characteristic relaxation times, 1/T*(1a) as the faster component and 1/T*(1b) as the slower component, respectively. It was shown that 1/T*(1a) is strongly affected by the CH(3) group dynamics of the SAR1 center. The complete temperature dependence of 1/T*(1a) was described by invoking several relaxation mechanisms that involve hindered motion of the CH(3) group from classical rotational motion to coherent rotational tunneling. It was shown that all relevant relaxation mechanisms are determined by a single correlation time with the potential barrier (Delta E/k=1570 K). On the other hand the temperature dependence of 1/T*(1b) is related to the motional dynamics of the neighborly NH(3) and CH(3) groups. We found a larger average potential barrier for this motion (Delta E/k=2150 K) corresponding to smaller tunneling frequencies of the neighbor groups.