The magnetic relaxation processes in disordered two-dimensional ensembles of dipole-coupled magnetic nanoparticles are theoretically investigated by performing numerical simulations. The energy landscape of the system is explored by determining saddle points, adjacent local minima, energy barriers, and the associated minimum energy paths (MEPs) as functions of the structural disorder and particle density. The changes in the magnetic order of the nanostructure along the MEPs connecting adjacent minima are analyzed from a local perspective. In particular, we determine the extension of the correlated region where the directions of the particle magnetic moments vary significantly. It is shown that with increasing degree of disorder the magnetic correlation range decreases, i.e., the elementary relaxation processes become more localized. The distribution of the energy barriers, and their relation to the changes in the magnetic configurations are quantified. Finally, some implications for the long-time magnetic relaxation dynamics of nanostructures are discussed.
Recent Raman data on diamond and crystalline Si nanopowders are analyzed with the use of a microscopic theory of Raman scattering in ensembles of disordered nonpolar nanocrystals. The large width of the Raman peak in nanoparticles as compared to the corresponding peak in bulk materials and the peak inverse dependence on the particle size observed experimentally are explained within the framework of the theory. It is shown that this theory is capable to extract confidently from the Raman data four important microscopic characteristics of the nanopowder including the mean particle size, the vari…
Microscopic description of Raman spectra in nanopowders of nonpolar crystals is accomplished by developing the theory of disorder-induced broadening of optical vibrational eigenmodes. Analytical treatment of this problem is performed, and line shape and width are determined as functions of phonon quantum numbers, nanoparticle shape, size, and the strength of disorder. The results are found to be strongly dependent on either the broadened line is separated or it is overlapped with other lines of the spectrum. Three models of disorder, i.e. weak point-like impurities, weak smooth random potentia…
Recent advances in our understanding of thermal transport in nanocrystalline systems are responsible for the integration of new technologies into advanced energy systems, including thermoelectric refrigeration systems and renewable energy platforms. However, there is little understanding of heat energy transport mechanisms that govern the thermal properties of disordered nanocomposites. In this work, we explore thermal transport mechanisms in disordered packings of amorphous nanoparticles with and without a polymer filling the interstices in order to quantify the impact of thermal boundary sca…
Co2FeAl (CFA) nanoparticles (NPs) of different sizes were synthesized by chemical route. The effect of the size of NPs upon the structure and magnetization compared to its bulk counterpart was investigated. The structure and composition were determined from X-ray diffraction (XRD) and electron microscopy. XRD analysis shows that the samples are having single (A2-type) disordered phase. Magnetization measurements suggest that the samples are soft ferromagnetic in nature with very low coercivity. Enhanced magnetic properties like saturation magnetization, coercive force, retentivity, and Curie-t…
Disorder-induced broadening of optical vibrational eigenmodes in nanoparticles of nonpolar crystals is studied numerically. The methods previously used to treat phonons in defectless particles are adjusted for numerical evaluation of the disordered problem. Imperfections in the form of Gaussian and binary disorders as well as surface irregularities are investigated thoroughly in a wide range of impurity concentrations and disorder strengths. For dilute and weak point-like impurities the regimes of separated and overlapped phonon levels are obtained and the behavior of the linewidth predicted t…
We have investigated magnetic, dielectric and magnetodielectric properties of La2CoMnO6 nanoparticles prepared by sol-gel method. Magnetization measurements revealed two distinct ferromagnetic transitions at 218 K and 135 K that can be assigned to ordered and disordered magnetic phases of the La2CoMnO6 nanoparticles. Two dielectric relaxations culminating around the magnetic transitions were observed with a maximum magnetodielectric response reaching 10% and 8% at the respective relaxation peaks measured at 100 kHz under 5T magnetic field. The dc electrical resistivity followed an insulating b…
The kinetics of order-disorder transition of FePt nanoparticles during high temperature annealing is theoretically investigated. A model is developed to address the influence of large surface to volume ratio of nanoparticles on both the thermodynamic and kinetic aspect of the ordering process; specifically, the nucleation and growth of L10 ordered domain within disordered nanoparticles. The size- and shape-dependence of transition kinetics are quantitatively addressed by a revised Johnson-Mehl-Avrami equation that included corrections for deviations caused by the domination of surface nucleati…
We present a study on the magnetic behavior of dextran-coated magnetite nanoparticles (DM NPs) with sizes between 3 and 19 nm, synthesized by hydrothermal-assisted co-precipitation method. The decrease of saturation magnetization ($M_s$) with decreasing particle size has been modeled by assuming the existence of a spin-disordered layer at the particle surface, which is magnetically dead. Based on this core-shell model and taking into account the weight contribution of the non-magnetic coating layer (dextran) to the whole magnetization, the dead layer thickness ($t$) and saturation magnetizatio…
Exchange bias effects linked to surface spin freezing (SSF) are commonly found in iron oxide nanoparticles, while signatures of SSF in low-field temperature-dependent magnetization curves have been much less frequently reported. Here, we present magnetic properties of dense assemblies of similar-sized (~ 8 nm diameter) particles synthesized by a magnetite (sample S1) and a maghemite (sample S2) method, and the influence of long-term (4-year) sample aging under ambient conditions on these properties. The size of the exchange bias field of the different sample (fresh or aged) states is found to …
We present a systematic study of core-shell Au/Fe_3O_4 nanoparticles produced by thermal decomposition under mild conditions. The morphology and crystal structure of the nanoparticles revealed the presence of Au core of <d> = (6.9\pm 1.0) nm surrounded by Fe_3O_4 shell with a thickness of ~3.5 nm, epitaxially grown onto the Au core surface. The Au/Fe_3O_4 core-shell structure was demonstrated by high angle annular dark field scanning transmission electron microscopy analysis. The magnetite shell grown on top of the Au nanoparticle displayed a thermal blocking state at temperatures below T_B = …
Anatase TiO$_2$ is among the most studied materials for light-energy conversion applications, but the nature of its fundamental charge excitations is still unknown. Yet it is crucial to establish whether light absorption creates uncorrelated electron-hole pairs or bound excitons and, in the latter case, to determine their character. Here, by combining steady-state angle-resolved photoemission spectroscopy and spectroscopic ellipsometry with state-of-the-art ab initio calculations, we demonstrate that the direct optical gap of single crystals is dominated by a strongly bound exciton rising over…
While classical percolation is well understood, percolation effects in randomly packed or jammed structures are much less explored. Here we investigate both experimentally and theoretically the electrical percolation in a binary composite system of disordered spherocylinders, to identify the relation between structural (percolation) and functional properties of nanocomposites. Experimentally, we determine the percolation threshold $p_c$ and the conductivity critical exponent $t$ for composites of conducting (CrO$_2$) and insulating (Cr$_2$O$_3$) rodlike nanoparticles that are nominally geometr…
We study the low temperature magnetic properties of nanoparticles of pure transition metal carbide, viz., Co2C, with an average particle diameter of $40 \pm 10$ nm. These Co2C nanoparticles are ferromagnetic (FM) up to room temperature with blocking temperatures above room temperature. The coercive field shows abrupt deviation from the Kneller law below 50 K. In this low temperature regime the magnetization hysteresis loop shows shifts due to exchange bias (EB) effect, with an exchange field of ~ 250 Oe. Analysis of training of the EB effect and ac and dc magnetic measurements suggest that EB …
Using microemulsion methods, CoO-Pt core-shell nanoparticles (NPs), with diameters of nominally 4 nm, were synthesized and characterized by high-resolution transmission electron microscopy (HRTEM) and a suite of x-ray spectroscopies, including diffraction (XRD), absorption (XAS), absorption near-edge structure (XANES), and extended absorption fine structure (EXAFS), which confirmed the existence of CoO cores and pure Pt surface layers. Using a commercial magnetometer, the ac and dc magnetic properties were investigated over a range of temperature (2 K $\leq$ T $\leq$ 300 K), magnetic field ($\…
We report on spectroscopy study of elementary magnetic excitations in an Ising-like antiferromagnetic chain compound SrCo$_2$V$_2$O$_8$ as a function of temperature and applied transverse magnetic field up to 25 T. An optical as well as an acoustic branch of confined spinons, the elementary excitations at zero field, are identified in the antiferromagnetic phase below the Néel temperature of 5 K and described by a one-dimensional Schrödinger equation. The confinement can be suppressed by an applied transverse field and a quantum disordered phase is induced at 7 T. In this disordered paramagnet…
The single crystal growth, structure, and basic magnetic properties of ErMgGaO4 are reported. The structure consists of triangular layers of magnetic ErO6 octahedra separated by a double layer of randomly occupied non-magnetic (Ga,Mg)O5 bipyramids. The Er atoms are positionally disordered. Magnetic measurements parallel and perpendicular to the c axis of a single crystal reveal dominantly antiferromagnetic interactions, with a small degree of magnetic anisotropy. A weighted average of the directional data suggests an antiferromagnetic Curie Weiss temperature of approximately -30 K. Below 10 K …
The finite size and surface roughness effects on the magnetization of NiO nanoparticles is investigated. A large magnetic moment arises for an antiferromagnetic nanoparticle due to these effects. The magnetic moment without the surface roughness has a non-monotonic and oscillatory dependence on $R$, the size of the particles, with the amplitude of the fluctuations varying linearly with $R$. The geometry of the particle also matters a lot in the calculation of the net magnetic moment. An oblate spheroid shape particle shows an increase in net magnetic moment by increasing oblateness of the part…
Disorder among surface spins largely dominates the magnetic response of ultrafine magnetic particle systems. In this work, we examine time-dependent magnetization in high-quality, monodisperse hollow maghemite nanoparticles with a 14.8 $\pm$ 0.5 nm outer diameter and enhanced surface-to-volume ratio. The nanoparticle ensemble exhibits spin-glass-like signatures in dc magnetic aging and memory protocols and ac magnetic susceptibility. The dynamics of the system slows near 50 K, and becomes frozen on experimental time scales below 20 K. Remanence curves indicate the development of magnetic irrev…
We report a systematic study on the structural and magnetic properties of Co_{x}Fe_{3-x}O_{4} magnetic nanoparticles with sizes between $5$ to $25$ nm, prepared by thermal decomposition of Fe(acac)_{3} and Co(acac)_{2}. The large magneto-crystalline anisotropy of the synthesized particles resulted in high blocking temperatures ($42$ K \leqq $T_B$ $\leqq 345$ K for $5 \leqq$ d $\leqq 13$ nm ) and large coercive fields ($H_C \approxeq 1600$ kA/m for $T = 5$ K). The smallest particles ($<d>=5$ nm) revealed the existence of a magnetically hard, spin-disordered surface. The thermal dependence of st…
Finite-Size and surface effects in maghemite nanoparticles: Monte Carlo simulations
用蒙特卡罗模拟模拟了$γ$ O $_3$（磁赤铁矿）单颗粒模型，研究了细颗粒体系中的晶粒尺寸效应和表面效应.周期性边界条件已被用来模拟的整体性质和结果相比，一个球形粒子与自由边界的证据所发挥的作用，表面上的异常磁性显示这些系统在低温下。该模型的几个结果与实验结果定性一致。随着颗粒尺寸的减小，磁有序温度、自发磁化强度和矫顽场均降低。此外，磁滞回线变得拉长与高值的微分磁化率，类似于那些从挫折或无序系统。这些事实是形成具有比核心更高程度的磁无序的表面层的结果，对于小尺寸，核心主导颗粒的磁化过程。然而，与一些作者的假设相矛盾的是，我们的模型并没有预测表面层冻结成类似自旋玻璃的状态。结果表明，磁无序在表面简单地促进热退磁的颗粒在零场，而磁化强度增加，在中等领域，因为表面无序减少亚铁磁相关的颗粒内。磁滞回线的形状与颗粒尺寸的变化表明，反转模式的强烈影响，减少原子的协调和无序的表面。
Metallic Ni$_{1-x}$V$_x$ alloys are known to exhibit a ferromagnetic to paramagnetic disordered quantum phase transition (QPT) at the critical concentration $x_c \sim$ 0.114 in bulk. Such a QPT is accompanied by a quantum Griffiths phase (QGP), the physical observables in which follow non-universal power-law temperature dependences, in a finite temperature range on the paramagnetic side of the transition. In the present work, we explore the occurrence of QGP in nanoparticles of this alloy system. Nanoalloys with $x$ in the neighbourhood of $x_c$ and mean diameter 18-33 nm were prepared by a ch…
We develop a model based on the fractional exclusion statistics (FES) applicable to non-homogeneous interacting particle systems. Here the species represent elementary volumes in an (s+1)-dimensional space, formed by the direct product between the s-dimensional space of positions and the quasiparticle energy axis. The model is particularly suitable for systems with localized states. We prove the feasibility of our method by applying it to systems of different degrees of complexities. We first apply the formalism on simpler systems, formed of two sub-systems, and present numerical and analytica…
We report on isothermal pulsed (20 ms) field magnetization, temperature dependent AC - susceptibility, and the static low magnetic field measurements carried out on 10 nm sized Pr0.5Ca0.5MnO3 nanoparticles (PCMO10). The saturation field for the magnetization of PCMO10 (~ 250 kOe) is found to be reduced in comparison with that of bulk PCMO (~300 kOe). With increasing temperature, the critical magnetic field required to 'melt' the residual charge-ordered phase decays exponentially while the field transition range broadens, which is indicative of a Martensite-like transition. The AC - susceptibil…
