Formation Of Short-range Order Research Articles

Alkalinity-controlled zeolite nucleation and growth: ultrafast synthesis of total-morphology zeolite L mesocrystals and adsorption evaluation

Owing to the intrinsic complexity of crystallization and the heterogeneity of precursors, the specific stages and corresponding behaviors of an actual crystallization system remain ambiguous, which makes the univariate-controlled crystallization-kinetics-regulated synthesis and design of zeolite morphology and porosity an unrealized blueprint. In this study, a facile and univariate modulation (i.e., OH-/SiO2) strategy was developed to regulate zeolite crystallization kinetics, and zeolite L mesocrystals were synthesized rapidly (within 1-2 h) with almost all LTL morphologies (from cylindrical or disc-like shapes to nanoclusters or nanocrystals) in the simplest SiO2-Al2O3-K2O-H2O system. Using time-resolved analysis of the change in the solid-liquid Si/Al nutrient and crystallinity evolution, the intertwined and complex crystallization processes of zeolite L were clearly distinguished into four distinct stages: induction, nucleation, growth, and ripening. Under alkalinity-controlled conditions, the reactivity, Si/Al distribution, and state of aluminosilicates were critical to the formation of short-range order in the amorphous matrix, which greatly influenced the nucleation frequency and assembly state. Subsequently, these nucleation differences evoked correspondingly different kinetic growth behaviors. A putative alkalinity-controlled nonclassical crystallization mechanism was uncovered, and its validity was evaluated by analyzing morphology evolution, NH4F etching, and the effects of modifiers. Furthermore, adsorption tests demonstrated the high adsorption capacity of a series of zeolite L for guest molecules with various sizes and properties (e.g., gaseous aromatic hydrocarbon, aqueous dye, and protein).

Coupled structural-thermodynamic modelling of the molten salt system NaCl-UCl3

Molten chloride salts are ionic liquids in which the anions and cations exhibit network formation. An attractive salt system for use in molten salt reactors is NaCl-UCl3, an ionic liquid with complex non-ideal thermodynamic behaviour due to the formation of short-range order. The relationship between local structure and thermodynamic properties is investigated in this work, in which molecular dynamics simulations using the Polarizable Ion Model (PIM) and thermodynamic modelling by means of the CALPHAD method are combined. The system is simulated for a wide range of temperatures and compositions and various properties are derived derived from molecular dynamics data: density/molar volume, thermal expansion, heat capacity and excess properties including excess molar volume, mixing enthalpy and excess heat capacity. Generally, there is good agreement with previously published experimental data. An in depth analysis of the local structure of the liquid is performed for multiple temperatures. This analysis demonstrates the transition from a molecular liquid consisting of primarily Na+, Cl−, UCl63-/UCl74- at low UCl3 content to a polymeric liquid at high UCl3 content, manifesting itself in the formation of species like U2Cl126-, U3Cl178-, U4Cl2210- etc. Exceeding 40% UCl3, the liquid consists of a three-dimensional network of corner or edge-sharing uranium polyhedra. The output of the MD simulations and experimental data are incorporated into a coupled structural-thermodynamic model for the NaCl-UCl3 system based on the quasi-chemical formalism in the quadruplet approximation, that provides a physical description of the melt and reproduces (in addition to the thermodynamic data) the chemical speciation of uranium polymeric species predicted from the simulations.

Reaction Kinetics Regulated Formation of Short-Range Order in an Amorphous Matrix during Zeolite Crystallization.

The crystallization of zeolites, a disorder-to-order transformation of aluminosilicates, has not been thoroughly understood because the nucleation events in the amorphous matrix are difficult to recognize from the diverse structural changes, especially for the dense hydrogel systems. Therefore, relationships between the synthesis conditions, the generated amorphous species, and the crystallization behavior of zeolites remain unclear. Herein, by comparatively investigating the structural evolution of the aluminosilicate matrix in a dense hydrogel system when different Si reactants (fumed silica and silicate solution) are employed, we demonstrate that the reactivity of the reactants and the kinetics of the condensation reaction is critical to the formation of short-range order in an amorphous matrix, which greatly influences the nucleation frequency of zeolites. It was revealed that an amorphous solid containing plentiful Al-rich four-membered rings and Si-rich six-membered rings could be produced when fumed silica gradually reacted with sodium aluminate solution at 80 °C. It is considered that the interaction between these rings promotes the construction of the essential building units of zeolite X (FAU). In contrast, a complex aluminosilicate matrix was formed immediately when sodium silicate solution was mixed with sodium aluminate solution due to the intense condensation reaction. Furthermore, this complex matrix became more stable when the reactant mixture was hydrothermally treated at 80 °C, which significantly impedes the crystallization process. Aging the reactant mixture at ambient temperature before heating, instead, facilitated the formation of short-range order in the amorphous matrix, which increases the nucleation frequency of zeolites.

Enhanced Mechanical Properties of Fe-Mn-Al-C Low Density Steel via Aging Treatment

This study investigated the tensile properties and deformation behavior of an aged Fe-26Mn-6Al-1C (mass%) alloy with a stacking fault energy of approximately 60 mJ·m−2. The results show that an ordered phase with a “short-range ordering” (SRO) structure formed after aging at 550°C for 10 h, further increasing the aging time to 48 h. Lamellar second-phase precipitates appeared at the austenitic grain boundaries. The aged sample at 550°C for 10 h exhibited an enhanced tensile strength (∼898 MPa) without notably sacrificing uniform elongation (∼46.3%), which was mainly attributed to the relatively high strain hardening in the entire plastic deformation due to the synergistic effects of planar slip, twinning-induced plasticity (TWIP), microband-induced plasticity (MBIP), and especially the formation of short-range ordering.

Dust-Acoustic Wave Dispersion in Thermal Dusty Plasmas at Weak and Moderate Couplings

The dispersion of dust-acoustic waves (DAWs) in weakly and moderately coupled thermal dusty plasmas is studied in the framework of the linear density-response formalism with the static local-field correction for interdust interactions. The plasma medium composition and the charge of dust particles are simultaneously determined within a recently developed chemical model (Physical Review E, vol. 101, 063203, 2020) based on minimizing the Helmholtz free energy of the system under investigation. Stemming from the generalized Poisson-Boltzmann equation, the renormalization procedure is consistently applied to derive an interdust screened potential that takes into account the finiteness of dust grains. Within the framework of the Ornstein-Zernike relationship in the hypernetted chain approximation, the static structure factor of the dust component is evaluated to manifest the appearance of local extrema on its wavenumber dependence, thereby indicating the short-range order formation in the arrangement of dust particles with respect to one another. It is shown that the DAW dispersion law is completely governed by the static structure factor and, therefore, exhibits a nonmonotonic dependence on the wavenumber as well. In the long-wavelength limit, the acoustic-like behavior of the DAW dispersion is strictly confirmed and the corresponding phase speed, reduced in units of the dust thermal velocity, is ultimately expressed via the static structure factor at zero wavenumber.

THE SHORT-RANGE ORDER AND ITS INFLUENCE ON RADIATION STABILITY OF LOW-CONCENTRATION Fe-Cr ALLOYS

The analysis of the structural phase state of Fe-Cr low concentration solid solutions and steel 1X13, associated with the formation of short-range order (SRO) of various types in them has been performed at the mesoscopic level. A comparison of the SRO and swelling of alloys under irradiation was carried out. It was shown that there is a fairly good qualitative correlation between them.

Structure of liquid Al[sbnd]Sn alloys

The short-range order of liquid AlSn alloys (0, 3, 8, 13, 20, 35, 50, 75, 100 at. % Sn) at 973 and 1273 K has been studied by X-ray diffraction and Reverse Monte Carlo simulation. The analysis of the experimental and simulation data points out the presence of atomic clusters with a local structure similar to liquid Sn even at low tin content (8 at. %). An impact of these clusters on the formation of short-range order of AlSn melts becomes dominant at 35 at. % Sn, resulting in the similarity between experimental structure factors and pair correlation functions of binary melts and liquid tin. On the other hand, the short-range order of liquid binary alloy with high Al content (97 at. %) is structurally homogeneous and based on the local atomic structure of liquid aluminium. The comparison between the short-range order of the liquid AlSn, AlGe, and AlSi alloys has been discussed.

Effects of annealing on hardness, yield strength and dislocation structure in single crystals of the equiatomic Cr-Mn-Fe-Co-Ni high entropy alloy

We report that in contrast to the anticipation, the macroscopic mechanical strength of single crystals of the face-centered-cubic single-phase equiatomic Cr-Mn-Fe-Co-Ni high entropy alloy is not influenced by thermal annealing during which short-range ordering is expected to develop. Experimental evidence shows that hardness at room temperature, critical resolved shear stress at room temperature and at 77 K and activation volume values of the alloys do not significantly vary with the annealing temperature in the range from 900 to 1200°C. The stacking fault energies in the specimens deformed at 77 K following annealing at 1000 and 1200°C respectively are essentially identical to each other. These results clearly indicate that the impact of the formation of chemical short-range order on the macroscopic yield strength of the equiatomic Cr-Mn-Fe-Co-Ni high entropy alloy is insignificant, even if it exists.

Effects of Annealing on Hardness, Yield Strength and Dislocation Structure in Single Crystals of the Equiatomic Cr-Mn-Fe-Co-Ni High Entropy Alloy

We report that in contrast to the anticipation, the macroscopic mechanical strength of single crystals of the face-centered-cubic (FCC) single-phase equiatomic Cr-Mn-Fe-Co-Ni high entropy alloy (HEA) is not influenced by thermal annealing during which short-range ordering (SRO) is expected to develop. Experimental evidence shows that hardness at room temperature, critical resolved shear stress at room temperature and at 77 K and activation volume values of the alloys do not significantly vary with the annealing temperature in the range from 900 to1200°C. The stacking fault energies (SFEs) in the specimens deformed at 77 K following annealing at 1000 and 1200°C respectively are essentially identical to each other. These results clearly indicate that the impact of the formation of SRO on the macroscopic yield strength of the equiatomic Cr-Mn-Fe-Co-Ni HEA is insignificant, even if it exists.

A Review on Developments in Magnesium Alloys

In order to facilitate the understanding of the current research efforts and directions, this article first introduces the anomalous/problematic features of magnesium, and presents the recent approach of stacking fault energy (SFE)-based alloying element selection to lessen or eliminate these problem. SFE computations via ab initio techniques necessitate an understanding of the free electron density distribution around atoms in a solid solution. Therefore, the assessment of the role of atoms by also considering the possibility of short range order (SRO) formation rather than a random solid solution has been revisited. Two possible types of SRO have been indicated. The relevant electronic interactions between the host Mg and the alloying element atoms are more clearly incorporated in, a generally less known model, by Miedema’s based on atomic level thermodynamics rather than in Hume-Rothery rules. This more successful approach has also been addressed here. An evaluation founded on these premises, introducing the relatively more recent magnesium alloy systems, has been given in terms of their achievements towards healing the problematic features of magnesium alloys. The spectrum of alloy systems discussed ranges from doping of magnesium to dilute alloy systems, and to some rich alloy systems that offer remarkable properties. Among the first category, an unorthodox addition, doping with oxygen, and its implications has been presented. The dilute alloy systems and their compositional design based on short range order (SRO) and SFE together with their potentials have been reviewed. Among the rich alloy compositions, the most interesting precipitate systems, i.e. the ones involving order and intermetallic formations, long period stacking order (LPSO) phases, and quasi-crystals have been discussed. Among all the alloying elements, one that deserves particular attention, with its implications such as being economical, offering environmentally friendly magnesium metallurgy, as well as remedial effects on the shortcomings of engineering properties, calcium and a closely related issue of CaO addition, have been scrutinized. This article also makes an attempt to point out the future directions throughout the text, whenever possible.

Fatigue Damage Mechanism of AL6XN Austenitic Stainless Steel at High Temperatures

By the combination of transmission electron microscope, neutron diffraction and small-angle neutron scattering methods, mechanical fatigue behavior of AL6XN austenitic stainless steel was investigated in the temperature range of 400–600 °C. At 400 °C, in addition to the occurrence of dynamic strain aging, the formation of short-range order was evidenced from the forbidden electron diffraction spot of 1/3 {422} in face-centered cubic (fcc) structure viewed down [111] zone axis, which facilitate the planar slip mode of dislocation and result in the work hardening during the fatigue deformation. The fatigue damage is mainly dominated by the accumulation of planar slip band and the interaction among various slip systems. With increasing temperature, precipitates of chi phase, Laves phase and sigma phase were formed during the fatigue tests at 500 and 600 °C. An increase in precipitation content at 600 °C has also been confirmed by both scanning electron microscope and small-angle neutron scattering analysis. The dislocation pileup originating from the uncoordinated deformation between precipitate and austenitic matrix is an important fatigue damage leading to crack. The continuous cycle softening behavior was also observed on the fatigue curve at 600 °C, which is considered to be caused by dynamic recovery.

Mechanical properties and crystallization kinetics of Er-containing Cu–Zr–Al bulk metallic glasses with excellent glass forming ability

Investigations were carried out to explore the consequences of Er adding on the glass forming ability (GFA), mechanical properties, and crystallization kinetics of Cu50Zr43Al7 bulk metallic glass (BMG). It is found that the (Cu50Zr43Al7)100-xErx (x = 0, 2, 4, 6 at %) BMGs reflects its best GFA at x = 2 and correlate well with GFA indicator (γ and K) and thermal stability parameter (ΔTx). The Er-containing BMGs showed high compressive strength and Young module in the range of 1816–1890 Mpa and 116–120 GPa, respectively, but no plastic deformation observed in them. The crystallization kinetics lagged with 2 at % Er addition. The large atomic radius of Er and large negative mixing enthalpy of Er with the other constituent elements causes the significant atomic size mismatch and the formation of short-range order in the melt which restrict the long-range diffusion and ordering of atoms that lead to improving GFA and lagging the crystallization kinetics of (Cu50Zr43Al7)98Er2.

The concentration effect of Pd and Pt-doped Cu on short range order formation in the rapid cooling process with molecular-dynamics simulation

In this study, the formation of bonded pairs which represent amorphous and crystalline structures of Cu-Pd and Cu-Pt ordered alloy systems for different composition of copper was determined with molecular dynamic simulation method during the fast cooling process. The structural properties and phase transformation of systems at different temperatures were investigated with radial distribution functions. The structural formation of bonded pairs was obtained by using Honeycutt-Andersen (HA) method. Physical interactions among atoms were modelled using Sutton-Chen (SC) type of the Embedded Atom Method (EAM) based on many-body interactions. During the rapid cooling process, an amorphous phase conversion was observed at 300K and an increase in the number of bound pairs representing the amorphous phase was detected.

A new approach for coupled modelling of the structural and thermo-physical properties of molten salts. Case of a polymeric liquid LiF-BeF2

The (Li,Be)Fx fluoride salt is an ionic liquid with complex non-ideal thermodynamic behaviour due to the formation of short-range order. In this work, we explore the relationship between local structure, thermo-physical and thermodynamic properties in this system using a multidisciplinary approach that couples molecular dynamics simulations using the Polarizable Ion Model (PIM) and thermodynamic modelling assessment using the CALPHAD method. The density, thermal expansion, viscosity, thermal conductivity, molar and mixing enthalpies and heat capacity of the (Li,Be)Fx melt are extracted from the polarizable ionic interaction potentials and investigated across a wide range of compositions and temperatures. The agreement with the available experimental data is generally very good. The local structure is also examined in detail, in particular the transition between a molecular liquid with Li+, BeF42− and F− predominant species at low BeF2 content, and a polymeric liquid at high BeF2 content, with the formation of polymers (Be2F73−, Be3F104−, Be4F135−, etc.), and finally of a three-dimensional network of corner-sharing tetrahedrally coordinated Be2+ cations for pure BeF2. Based on the available experimental information and the output of the MD simulations, we moreover develop for the first time a coupled structural-thermodynamic model for the LiF-BeF2 system based on the quasi-chemical formalism in the quadruplet approximation, that provides a physical description of the melt and reproduces (in addition to the thermodynamic data) the chemical speciation of beryllium polymeric species predicted from the simulations.

Thermophysical properties of refractory W-50.4%Re and Mo-39.5%Re thin alloy layers deposited on silicon and silica substrates

The examined samples were W-Re and Mo-Re thin alloy layers with high content of Rhenium, applied in industry as protective coatings. The 550 nm of W-50.4%Re and 580 nm of Mo-39.5%Re alloys were deposited on crystalline silicon and amorphous silica substrates by magnetron sputtering method. For thermal characterization of investigated layers the scanning thermal microscopy (SThM) and high frequency photothermal radiometry (HF-PTR) measurements were carried out. The thermal methods were supported by the microstructural studies performed by the atomic force microscopy (AFM) and X-ray diffraction (XRD). The SThM method allowed determining the thermal conductivity (κ) of the alloy layers. From the HF-PTR the effective thermal conductivity (κeff) was determined directly. Estimation of the thermal boundary resistance (Rth) between particular alloy layer and its substrate enabled determination of the real κ of the layer with its thermal diffusivity (α) and effusivity (ε) from the HF-PTR fitting. The results showed, that W-Re and Mo-Re layers deposited on Si are characterized by higher κ, α, and ε values, and lower Rth in comparison to those deposited on SiO2. The κ values for W-Re and Mo-Re layers deposited on Si and SiO2 substrates were estimated in the range from 7 W·m−1 K−1 to 12 W·m−1 K−1, and 1.6 W·m−1 K−1 to 4 W·m−1 K−1, respectively. The correlation between the alloy layer structure, it's thermophysical properties and substrate structure was observed. The AFM and XRD measurements confirmed the short range order formation in Mo-Re layers deposited on Si.

Is “expanded austenite” really a solid solution? Mössbauer observation of an annealed AISI 316L nitrided sample

Expanded austenite, also known as S phase, m phase or γN phase forms during low temperature (<420 °C) nitriding of austenitic materials containing chromium. In this communication, annealing of a nitrided sample is used as a tool to understand the nature of expanded austenite. Starting from an AISI 316LN sample plasma nitrided for 4 h at 410 °C, the decomposition of expanded austenite is studied by conversion electron Mössbauer spectroscopy (CEMS) and X ray diffraction (XRD) for different annealing times at 400 °C. For the as nitrided sample, the CEMS spectra are analysed using two hyperfine field distributions (HFD). HFD A is attributed to a nitrogen enriched expanded austenite, HFD B is attributed to a bcc environment without or with very low nitrogen content. Both the local deformation of the bcc lattice and the presence of other elements as iron neighbouring atoms explain the broad range of hyperfine field in HFD B. The vanishing of HFD A, after 2 h of annealing, is explained by the formation of short-range order (SRO) between chromium and nitrogen and by the redistribution of nitrogen in excess. For the 3 h of annealing, a bcc phase is observed by XRD. We propose to describe this phase as martensite. An interplay between local internal stress and local nitrogen content is proposed to explain the unexpected formation of such a martensitic phase in a strongly gamma stabilizing environment. From the microscopic point of view expanded austenite can be considered to be constituted of at least two different environments: a gamma environment supersaturated in nitrogen and a martensitic environment without nitrogen.

Influence of minor additions on Icosahedral Short-Range Order (ISRO) and its consequences on nucleation and solidification growth kinetics in fcc alloys

The present contribution reviews the recent progress related to the influence of Icosahedral Short-Range Order (ISRO) and icosahedral Quasicrystals (i-QC) formation on the solidification of fcc alloys through minor solute element additions. From intensive crystallographic analysis of multi-twinned regions in as-cast Al-based and Au-based fcc alloys, Kurtuldu et al. have shown recently that a so-called “iQC-mediated” nucleation mechanism occurs when a few hundred ppm of Cr and Ir, respectively, are added to the melt [1] [2]. Similarly, it appears that the growth directions of dendrites in Al-Zn:Cr is also influenced by ISRO in the liquid, thus showing an attachment kinetics effect [3]. In a recent contribution, we have shown that iQC-mediated nucleation also occurs in pink gold alloys with Ir-additions, but two additional phenomena at high solidification speed [4]: (i) a spinodal-type decomposition of the liquid, leading to the formation of twinned Cu precipitates in addition to multi-twinned Au-rich grains; (ii) a change of the microstructure of the Au-rich grains, from 〈100〉 dendrites to 〈111〉 textured cells in the columnar zone.

The Role of Hydrogen in Hydrogen Embrittlement of Metals: The Case of Stainless Steel

Hydrogen embrittlement (HE) of metals has remained a mystery in materials science for more than a century. To try to clarify this mystery, tensile tests were conducted at room temperature (RT) on a 316 stainless steel (SS) in air and hydrogen of 70 MPa. With an aim to directly observe the effect of hydrogen on ordering of 316 SS during deformation, electron diffraction patterns and images were obtained from thin foils made by a focused ion beam from the fracture surfaces of the tensile specimens. To prove lattice contraction by ordering, a 40% CW 316 SS specimen was thermally aged at 400 °C to incur ordering and its lattice contraction by ordering was determined using neutron diffraction by measuring its lattice parameters before and after aging. We demonstrate that atomic ordering is promoted by hydrogen, leading to formation of short-range order and a high number of planar dislocations in the 316 SS, and causing its anisotropic lattice contraction. Hence, hydrogen embrittlement of metals is controlled by hydrogen-enhanced ordering during RT deformation in hydrogen. Hydrogen-enhanced ordering will cause the ordered metals to be more resistant to HE than the disordered ones, which is evidenced by the previous observations where furnace-cooled metals with order are more resistant to HE than water-quenched or cold worked metals with disorder. This finding strongly supports our proposal that strain-induced martensite is a disordered phase.

Influence of Ir Additions and Icosahedral Short Range Order (ISRO) on Nucleation and Growth Kinetics in Au-20.5Wt Pct Cu-4.5Wt PctAg Alloy

Based on detailed EBSD analyses, Kurtuldu et al. (Acta Mater. 70:240–248, 2014) have explained the grain refinement of Au-12.5 wt pctCu-12.5 wt pctAg (yellow gold) by the addition of minute amounts of Ir in terms of “icosahedral quasicrystal (iQC)-mediated nucleation”, i.e., Ir induced the formation of Icosahedral short range order (ISRO) of atoms in the liquid, leading to the formation of iQC on which the fcc-phase forms. In the present contribution, we show that: (i) this mechanism is also responsible of the grain refinement in Au-20.5 wt pctCu-4.5 wt pctAg (pink gold) with Ir addition; (ii) ISRO also influences the morphology and growth kinetics of the fcc phase: at solidification rate of a few mm/s, $$\langle 100\rangle $$ dendrites are replaced by a cellular-type morphology growing along $$\langle 111\rangle $$ when 100 wt ppm of Ir is added to the melt; (iii) iQC-mediated nucleation is accompanied by a spinodal decomposition of the liquid, which is revealed at high cooling rate by the formation of Cu-rich particles or dendrites, some of them being also twinned, in parallel to iQC-mediated grain refinement and twin formation.

Specific heat and nonlinear susceptibility in spin glasses with random fields

We study magnetic properties of spin glass (SG) systems under a random field (RF), based on the suggestion that RFs can be induced by a weak transverse field in the compound ${\mathrm{LiHo}}_{x}{\mathrm{Y}}_{1\ensuremath{-}x}{\mathrm{F}}_{4}$. We consider a cluster spin model that allows long-range disordered interactions among clusters and short-range interactions inside the clusters, besides a local RF for each spin following a Gaussian distribution with standard deviation $\mathrm{\ensuremath{\Delta}}$. We adopt the one-step replica symmetry breaking approach to get an exactly solvable single-cluster problem. We discuss the behavior of order parameters, specific heat ${C}_{m}$, nonlinear susceptibility ${\ensuremath{\chi}}_{3}$, and phase diagrams for different disorder configurations. In the absence of RF, the ${\ensuremath{\chi}}_{3}$ exhibits a divergence at ${T}_{f}$, while the ${C}_{m}$ shows a broad maximum at a temperature ${T}^{**}$ around $30%$ above ${T}_{f}$, as expected for conventional SG systems. The presence of RF changes this scenario. The ${C}_{m}$ still shows the maximum at ${T}^{**}$ that is weakly dependent on $\mathrm{\ensuremath{\Delta}}$. However, the ${T}_{f}$ is displaced to lower temperatures, enhancing considerably the ratio ${T}^{**}/{T}_{f}$. Furthermore, the divergence in ${\ensuremath{\chi}}_{3}$ is replaced by a rounded maximum at a temperature ${T}^{*}$, which becomes increasingly higher than ${T}_{f}$ as $\mathrm{\ensuremath{\Delta}}$ is enhanced. As a consequence, the paramagnetic phase is unfolded in three regions: (i) a conventional paramagnetism ($T&gt;{T}^{**}$); (ii) a region with formation of short-range order with frozen spins (${T}^{*}&lt;T&lt;{T}^{**}$); (iii) a region with slow growth of free-energy barriers slowing down the spin dynamics before the SG transition (${T}_{f}&lt;T&lt;{T}^{*}$) suggesting an intermediate Griffiths phase before the SG state. Our results reproduce qualitatively some findings of ${\mathrm{LiHo}}_{x}{\mathrm{Y}}_{1\ensuremath{-}x}{\mathrm{F}}_{4}$ as the rounded maximum of ${\ensuremath{\chi}}_{3}$ behavior triggered by RF and the deviation of the conventional relationship between the ${T}_{f}$ and ${T}^{**}$.