Conventional Solid-state Technique Research Articles

Characterization and Solid-State UV-Vis Investigations of Photoelectrocatalytically Active La5Cl7[TeO3]4, a Mixed Anion Compound with Alternating 2D Layers of Oxygen and Chlorine.

An oxide chloride, La5Cl7[TeO3]4, was synthesized using the conventional high-temperature solid-state synthesis technique in an inert atmosphere. This compound possesses a novel crystal structure that can be described with the triclinic space group P1̅ (No. 2) and unit cell parameters: a = 7.2634(3) Å, b = 8.1241(3) Å, c = 9.1993(3) Å, α = 79.373(1)°, β = 83.599(1)°, and γ = 82.511(1)°. The preference of Te(IV) to coordinate to oxygen and direct its lone pair toward the lower charged chlorine results in 2D layers of both oxygen and chlorine, alternating along the crystallographic b-direction. Homoleptic coordination, solely to oxygen, and heteroleptic coordination to oxygen and chlorine are observed for lanthanum, forming layers connected through edge-sharing polyhedra. In the crystal structure, two distinct tellurium positions are observed, with three close Te-O distances, emphasizing an active lone pair. The compound has been investigated by solid-state UV-vis measurements, and a band gap of 3.44 eV has been determined by DFT calculations. Detailed photoelectrochemical measurements clearly indicate that the title compound is photoelectrocatalytically active, showing an n-type behavior. Raman spectroscopy confirms that complex tellurite ions are present in the crystal structure; several observed bands can be assigned to Te-O stretching, reflecting the relatively low crystallographic symmetry of the title compound.

Highly saturated red-emitting novel europium doped yttrium calcium borate (Eu3+: Y2CaB10O19) phosphor materials for eco-friendly solid-state lighting applications

Optical parameters like low correlated color temperature (CCT), color rendering index (CRI), color purity, thermal stability and etc. are crucial parameters for the practical applications of white light emitting diode applications. High color purity around 100 % red emitting novel europium doped yttrium calcium borate (Eu3+: Y2CaB10O19) phosphors were harvested by conventional solid-state synthesis technique. The novel host material possesses monoclinic crystal structure with no observable shift in the diffraction lines with varying dopant concentrations. FTIR studies revealed the presence of BO3 and BO4 networks in the host lattice responsible for structural rigidity and good thermal stability. The phosphor materials synthesized xEu3+: Y2CaB10O19 (x = 0.01, 0.03, 0.05, 0.07 and 0.09), are sensitive to both 250 nm (UV) and 393 nm (Near UV/blue LED) for excitation that can produce deep orange (594 nm) emission along with red emission (612 nm). The optimum Eu3+ ion concentration was fixed at 5 mol% of dopant ions to prevent the concentration quenching. As prepared optimal phosphor material possesses high color purity around 100 %, CCT of 1214 K defines its applicability in WLED applications. The synthesized phosphor materials pertain excellent switching response, thermal stability and the fabricated P-i-G possesses desired photometric parameters for its practical applications.

Aerosol Deposition of CuFeO2 Photocathode Coatings for Hydrogen Production

AbstractPhotoelectrochemical (PEC) water splitting is a viable route for green hydrogen generation. In PEC cells, the electrodes are coated with suitable semiconductor materials, which absorb the sunlight, generating charge carriers that are used to split water molecules into H2 and O2. CuFeO2 is one promising photocathode material for water splitting. However, its performance is limited by electron/hole pairs recombination within the film and at the film/substrate interface. Aerosol deposition (AD) can be employed to minimize charge recombination by spraying dense, thin films and by establishing a good back-contact interface. In this study, CuFeO2 powders were synthesized through a conventional solid-state technique and sprayed by AD under varied parameter sets. The effect of particle size distributions, carrier gas, gas pressure and substrate temperature was investigated. The best spraying parameter set was then tuned to obtain thin coatings (< 1 µm). Single-particle deformation and coatings microstructure were investigated by scanning electron microscopy. Optical properties of CuFeO2 films were analyzed by UV–Vis spectroscopy, while photoelectrochemical performances were estimated through amperometry tests under simulated sunlight. The results of this research show that CuFeO2 photocathodes can be successfully manufactured by AD. Their performance can be optimized by adjusting coating thickness and by annealing in air.

Solid state synthesis of lead-free Sm-doped Na0.5Bi4.5Ti4O15 ceramics for enhanced dielectric and electrical properties

Here we report the synthesis of Sm-doped Na0.5Bi4.5Ti4O15 (Na0.5Sm0.5Bi4Ti4O15) lead-free ceramics via a conventional solid-state technique. Investigations of Na0.5Bi4.5Ti4O15 (NBT) and Na0.5Sm0.5Bi4.5Ti4O15 (NSBT) ceramics were demonstrated in detail to understand the composition-based structure-property of Aurivillius compounds and related functional material. Dielectric properties for frequency and temperature in a wide range were analyzed. The conduction activation energy values of NSBT ceramics are obtained to be 1.40 eV, whereas, the NBT ceramics get the value to be 1.31 eV. At higher temperatures, the conduction activation energy value of NSBT ceramics is 1.32 eV for both frequencies of 100 Hz and 1 kHz, whereas, for NBT compounds, the calculated value is 1.27 eV for both frequencies. The simulation performed on the impedance data for capacitive and resistance elements shows well-fitting curves which indicates a single relaxation behavior in the material. Similarly, the AC-conductivity data were analyzed which gives different conduction processes and relaxation activation energies in the NSBT ceramics.

Enhanced dielectric, magnetic and magnetoelectric properties in 0.5BaFe12O19 - xBaTiO3 - (0.5-x)CoFe2O4 composites

(0.5)BaFe12O19 - xBaTiO3 - (0.5-x)CoFe2O4; (x = 0.1, 0.2, 0.3 & 0.4) composite system was developed through conventional solid-state technique. XRD with Rietveld refinement confirmed pure tri-phasic composites with no impurity. The microstructure of samples has inhomogeneous grain packing with average size of grains ∼0.5 μm and typically decreased with BaTiO3 increment. The dielectric constant showed low-frequency dispersion and increased with BaTiO3 increment, hence maximum at 400 °C for composite x = 0.4 (∼2.8 × 103 at 1 kHz). Composites are ferrimagnetic in nature along with presence of firm exchange coupling among BaFe12O19/CoFe2O4 ferrite phases. The samples are multiferroic owing to typically high magnetoelectric coupling coefficient which increased with BaTiO3 increment, thus composite x = 0.4 attains highest value of 4.56 mV/cm.Oe on application of ac magnetic field (Hac = 45 Oe). The results indicate that the composites are suitable for magnetic field sensors and memory storage devices.

The modifications in structural, optical, and electro-magnetic phase transition of Vanadium-doped La-based manganite ceramics La0.7Pb0.3Mn1−yVyO3 (y = 0 – 0.1)

The present paper is centred around the investigation of the structural, electrical, and magnetic properties displayed by the novel perovskite polycrystalline La0.7Pb0.3Mn1−yVyO3 (y = 0 – 0.1) prepared via the conventional solid-state technique. The structural properties of the samples were assessed through the utilisation of X-ray diffraction (XRD) analysis. Subsequently, the obtained diffraction data underwent refinement employing Rietveld refinement techniques in order to determine the structural parameters of the samples a, b, c, V and Mn–O bond length and angle. The study of X-ray diffraction (XRD) peaks reveals that all the samples exhibited crystallization in a single phase, devoid of any impurities. All of the samples exist in rhombohedral orientation with a space group of R-3c. The tolerance factor of the samples was calculated in order to assess the severity of lattice distortion, decrease from 0.872 (y = 0) to 0.831 (y = 0.1). The microstructural characteristics of the samples were analysed using a field-emission scanning electron microscope (FESEM). The morphology results reveal that a rise in the amount of V leads stimulates the grain growth in the sample, as evidenced by the increase in grain size from 2.17 µm (y = 0) to 3.71 µm (y = 0.1). The Fourier transform infrared (FTIR) analysis revealed an absorption range of 500 – 600 cm-1, which is indicative of the Mn–O bond deformation vibration. This observation suggests the presence of a MnO6 bond in the sample. The Tauc plots derived from the UV-Vis spectroscopy data reveal a notable increase in the optical bandgap (Eopt) as the concentration of V increases. Specifically, the Eopt values rise from 1.71 eV (y = 0) to 2.30 eV (y = 0.1), falling within the range typically observed for semiconductor materials. A distinct metal-insulator transition was observed in all of the samples, exhibiting a range of TMI values ranging from 250 K to 292 K. The scattering model was employed to determine the itinerant eg behaviour in the low temperature region, whilst the SPH model was used to explore the conduction behaviour in the high temperature region. The magnetic characteristic of the samples was investigated using the Alternating Current Susceptibility (ACS) and Vibrating Sample Magnetometer (VSM) techniques, which confirms the existence of a shift in phase from ferromagnetic (FM) to paramagnetic (PM). The TC value exhibits a declining trend from 298.8 K (y = 0) to 274.8 K (y = 0.1).

Strong textured ferroelectric ceramics CaBi2Nb2O9 with superior piezoelectric response via conventional solid-state technique

Strong textured ferroelectric ceramics CaBi2Nb2O9 with superior piezoelectric response via conventional solid-state technique

Host-sensitized colour-tunable emission and Judd-ofelt analysis for Dy3+-doped ZnGa2O4 phosphor through exciton-mediated energy transfer

Single-phase Dy3+-doped zinc gallate (ZnGa2O4) phosphors were synthesized using a conventional solid-state fabrication technique. The structural properties of the host phosphor were determined through X-ray powder diffraction (XRPD) and Rietveld refinement, revealing a cubic spinal structure with a space group of Fd3m. The reflectance properties of the host and doped samples were measured using UV–Vis spectroscopy. The obtained data were used to estimate the bandgap of all the synthesized samples, ranging from 4.18 to 3.69 eV, confirming the formation of a wide bandgap semiconductor. Morphological, compositional, and surface mapping analyses were conducted using a field emission scanning electron microscope, energy dispersive electron spectroscopy, and time-of-flight secondary ion mass spectroscopy. X-ray photoelectron spectroscopy was employed to confirm the oxidation state of the constituent elements and for an in-depth study of the crystal structure. Photoluminescence excitation and emission spectra were recorded to analyze the luminescent properties of the synthesized phosphors. It was confirmed that when using an excitation wavelength of 247 nm, all samples exhibited broad host emission with decreasing intensity. In contrast, Dy3+ emission displayed an increasing trend, confirming host sensitization in this phosphor. To analyze the radiative properties of the activator ion, theoretical analysis using the Judd-Ofelt theory was carried out. The results revealed an overlapping of orbitals between the O2− ion and Dy3+, indicating its higher-order covalent nature and the increased symmetric nature of the activator ion in the present host. This characteristic allowed for the generation of near-white light emissions. A concentration of 7 mol% of Dy3+ was observed to match well with achromatic white (0.32, 0.33) on the color chromaticity diagram. The luminous properties of this material suggest that it is a desirable candidate for use in LEDs and AC electroluminescent systems.

Non-invasive thermal sensing and improved recoverable energy storage density of Bi0.5Na0.5TiO3: Er3+ doped multifunctional ferroelectric ceramic

In this work, Er3+ substituted bismuth sodium titanate ceramics with the chemical composition Bi0.5-xErxNa0.5TiO3 (x = 0.00, 0.01, 0.02, 0.03, 0.04, and 0.05) were synthesized using conventional solid state technique. The influence of Er3+ ions on structural, optical, ferroelectric, and temperature sensing properties have been investigated. The prepared ceramic powders were initially heated at a calcination temperature 850 °C to form single phase Bi0.5-xErxNa0.5TiO3 and finally sintered at temperature 1050 °C. Formation of pure phase compositions with rhombohedral crystal structure is confirmed through X-ray diffraction studies. The typical FTIR bands near 540, 860, 910 cm−1 confirmed the presence of Ti–O stretching of octahedral groups in the perovskite structure. The decent squared shaped saturated P-E hysteresis are obtained under an electric field of 60 ≤ E ≤ 70 kV/cm, and the loops become slimmer at higher Er3+ concentrations (x = 0.04). The efficiency of energy storage density increases with Er3+ doping and an improved recoverable energy storage (Wr = 2.73 J/cm3) and a higher efficiency (η = 70.77%) are obtained for Er content, x = 0.04. The photoluminescence spectra were recorded at two excitation wavelengths (488 nm and 980 nm). Two distinct green emission bands (529 nm and 550 nm) and one weak red emission band (670 nm) were observed at both excitation wavelengths. Increasing Er3+ content beyond (x > 0.03) leads to significant quenching of light emission due to cross relaxation process and non-radiative relaxations. The pump power dependency revealed that two photons were involved in the light upconversion process. The time-resolved fluorescence spectroscopy confirmed the decrease in lifetime with increasing Er3+ concentration. The absolute and relative sensitivity of the prepared ceramic at Er3+ concentration (x = 0.03) were found to be 0.47% K−1 at 523 K and 1.1% K−1 at 303 K, respectively. These optical and electrical properties open the possibility of realizing multifunctionality in the field of energy storage and opto-electronic applications.

Role of ZnMn2O4 phase in formation of varistor characteristics in ZnO:Mn ceramics

The samples ZnO:Mn were prepared using the conventional solid-state technique. To dope them with manganese, we used water solutions of MnSO4 and MnCl2. The properties inherent to both types of the obtained ceramics have been compared. It was found that the former demonstrated nonlinear current-voltage characteristics, whereas those of the latter were, in fact, linear. The analysis of EPR, diffuse reflectance and Raman spectra obtained for prepared ceramics allowed concluding that, in the samples doped with MnSO4, formation of Mn-related phase, namely, ZnMn2O4 spinel occurred at ZnO grain boundaries under sintering. It has been ascertained that a thin layer of this substance separates adjacent ZnO grains, which provides appearance of the back-to-back Schottky barriers at grain boundaries and “varistor behavior” of current-voltage characteristics.

Structural and photoluminescent properties of Gd3+ doped barium aluminate phosphor

Gd3+-doped barium aluminate was synthesized using a conventional solid-state technique and annealed at 1200 °C. The X-ray powder diffraction results confirmed the formation of a hexagonal structure with the space group of P6322 for the studied phosphors. The average crystallite size of 75 nm was calculated using Scherrer's equation based on the X-ray line broadening of all the major diffraction peaks. The shape, distribution, and level of agglomeration of the synthesized samples were confirmed using a field emission scanning electron microscope and energy-dispersive X-ray spectroscopy. The distribution of various ions in the host and doped sample was confirmed using time-of-flight secondary ion mass spectroscopy equipped with a Bi+ ion gun. UV–Visible spectroscopy was employed to record the reflectance of the studied samples, and bandgaps were calculated using the Kubelka-Munk function. The bandgaps were found to be in the range of 3.96–4.75 eV, confirming the formation of a room-temperature wide bandgap semiconductor. Photoluminescence spectroscopy was used to record the excitation and emission spectra of all the samples, which displayed an intense peak at 314 nm attributed to the 6P7/2 → 8S7/2 transition. Moreover, all samples displayed an additional peak in the emission spectrum at a wavelength of 627 nm, which was subsequently confirmed to be generated by second-order diffraction. The decay time for all the Gd3+ doped samples was calculated for λex of 274 nm and λem of 314 nm and was observed to be a few microseconds. The strong emission peak in the wavelength range of Ultraviolet-B has the potential to be utilized for phototherapy to treat skin problems that respond to photons in the range of 312–315 nm.

Low-temperature sintering vanadium-substituted ZnNb2O6 microwave dielectric ceramics for LTCC applications

The ZnNb2-xVx/2O6-1.25x (0.1 ≤ x ≤ 0.6) dielectric ceramics were synthesized through conventional solid-state technique and sintered at 925 °C–975 °C for 6 h. The specimens with the substitution of V5+ for Nb5+ could be sintered at a lower temperature than pure ZnNb2O6 ceramic, densifying the microstructure more densely and improving the quality factor. Density analysis proves that the dielectric constant is related to the relative density. In addition, the [NbO6] octahedral distortion, the bond valence and the average bond energy of the Nb–O bond also change, leading to a nonlinear variation for the temperature coefficient of the resonance frequency from x = 0.1 to 0.6. The ZnNb2-xVx/2O6-1.25x (x = 0.2) ceramics sintered at 950 °C exhibited the superior characteristic while taking into account the applications of low temperature co-fired ceramics technology. Not only did it possesses outstanding dielectric performances of εr = 22.25, Q×f = 51,701 GHz, and τf = −67.02 ppm/°C, but also has excellent chemical compatibility with the widely used Ag electrode.

Optical properties of Zn0.75Mg0.25O:Mn ceramics

Mn-doped ZnO, MgO and Zn0.75Mg0.25O samples ([Mn] = 0.1 at.%) were produced by conventional solid-state technique and investigated by means of XRD, EPR, absorption, photocurrent, photo- and cathodoluminescence methods. It was shown that Zn0.75Mg0.25O solid solution with hexagonal structure has the bandgap of Eg ∼3.65 eV. The quenching of host defect-related luminescence in ZnO:Mn and in hexagonal Zn0.75Mg0.25O:Mn was observed, while the Mn-related emission being absent. The energy level of MnZn2+ center in hexagonal Zn0.75Mg0.25O:Mn was found to be at 2.16 eV below conduction band (c-band) bottom and all excited states of MnZn2+ ions, including the lowest one, reside in c-band, as it takes place in ZnO:Mn. It is concluded that the necessary condition to obtain Mn-related light emission in Mn-doped alloys is to make deeper the lowest excited level of MnZn2+ ions. One of the solutions is to produce Zn1-xMgxO:Mn solid solution with the bandgap energy larger than 4.0 eV using nonequilibrium fabrication approaches.

High-frequency electric modulus, impedance and conductance studies of gadolinium/niobium substituted barium titanate-lithium ferrite solids

Using conventional solid-state techniques, BaTiO3- Li0.5Fe2.5O4composites doped with Gd/Nb are prepared. Investigations are made on the electric and micro-structural characteristics of composites at high frequencies. The tetragonal structure without phase change is confirmed by the composites BTO, BTOLF, BGN-1, and BGN-2. Using FESEM micrographs, the grain size of the composite samples BTO, BTOLF, BGN-1, and BGN-2 was determined. The Impedance (Z′), Complex Impedance (Z′′), and Mod of Impedance (|Z |) of all composites exhibit dispersion among the samples in the frequency range between 1 MHz and 1 GHz. The capacitance (C′) of BGN-2 falls between BTOLF and BGN-1 as a result of the effect of grain size.Due to the Gd/Nb doping in BTOLF, the true part of the composite's conductance (YS′) peak migrated towards lower and higher frequencies. All composites experience a rise in frequency beyond 1 GHz and a sharp peak in both the real component of the electric modulus (M') and the imaginary part of the electric modulus (M'').

Synthesis and Characterization of Oxide Chloride Sr2VO3Cl, a Layered S = 1 Compound.

The mixed-anion compound with composition Sr2VO3Cl has been synthesized for the first time, using the conventional high-temperature solid-state synthesis technique in a closed silica ampule under inert conditions. This compound belongs to the known Sr2 TmO3Cl (Tm = Sc, Mn, Fe, Co, Ni) family, but with Tm = V. All homologues within this family can be described with the tetragonal space group P4/nmm (No. 129); from a Rietveld refinement of powder X-ray diffraction data on the Tm = V homologue, the unit cell parameters were determined to a = 3.95974(8) and c = 14.0660(4) Å, and the atomic parameters in the crystal structure could be estimated. The synthesized powder is black, implying that the compound is a semiconductor. The magnetic investigations suggest that Sr2VO3Cl is a paramagnet at high temperatures, exhibiting a μeff = 2.0 μB V-1 and antiferromagnetic (AFM) interactions between the magnetic vanadium spins (θCW = -50 K), in line with the V-O-V advantageous super-exchange paths in the V-O layers. Specific heat capacity studies indicate two small anomalies around 5 and 35 K, which however are not associated with long-range magnetic ordering. 35Cl ss-NMR investigations suggest a slow spin freezing below 4.2 K resulting in a glassy-like spin ground state.

DFT-guided flux synthesis of a family of layered titanates crystallizing in the lepidocrocite structure type

K0.72Fe0.72Ti1.28O4, a layered mixed-metal oxide belonging to the lepidocrocite structure type, was grown out of a molten KCl-KF mixture at 800 °C. The compound crystallizes in orthorhombic space group Cmcm and exhibits two-dimensional layers, composed of mixed Fe/Ti octahedra, separated by K ions that occupy the interlayer layer space and maintain charge balance. The targeted flux synthesis of the Ni, Cu, and Zn analogs was carried out after density functional theory (DFT) calculations predicted their formation to be energetically favorable, yielding K0.77Ni0.38Ti1.62O4, K0.77Cu0.38Ti1.62O4, and K0.73Zn0.36Ti1.64O4. All four compositions can be prepared via conventional solid-state technique by mixing and heating stoichiometric amounts of KNO3, appropriate transition metal oxide precursors, and TiO2.

Low Temperature Magnetic Transition of BiFeO3 Ceramics Sintered by Electric Field-Assisted Methods: Flash and Spark Plasma Sintering

Low temperature magnetic properties of BiFeO3 powders sintered by flash and spark plasma sintering were studied. An anomaly observed in the magnetic measurements at 250 K proves the clear existence of a phase transition. This transformation, which becomes less well-defined as the grain sizes are reduced to nanometer scale, was described with regard to a magneto-elastic coupling. Furthermore, the samples exhibited enhanced ferromagnetic properties as compared with those of a pellet prepared by the conventional solid-state technique, with both a higher coercivity field and remnant magnetization, reaching a maximum value of 1.17 kOe and 8.5 10-3 emu/g, respectively, for the specimen sintered by flash sintering, which possesses the smallest grains. The specimens also show more significant exchange bias, from 22 to 177 Oe for the specimen prepared by the solid-state method and flash sintering technique, respectively. The observed increase in this parameter is explained in terms of a stronger exchange interaction between ferromagnetic and antiferromagnetic grains in the case of the pellet sintered by flash sintering.

Hardening Effect in Lead-Free KNN-Based Piezoelectric Ceramics with CuO Doping.

As the most promising lead-free piezoelectric ceramics to replace lead zirconate titanate (PZT) ceramics, potassium sodium niobate (KNN) ceramics have been widely studied for their application prospects in various electronic devices. Increasing Qm while maintaining a high piezoelectric activity is quite important for piezoelectric ceramics applied in ultrasonic devices. A KNN-based ceramic with high d33 and Qm is prepared by a conventional solid-state technique to construct polycrystalline phase boundaries and induce defect dipoles. The best overall performance can reach d33 = 260 pC/N, Qm = 210, and TC = 293 °C. The temperature dependence of the relevant parameters is tested, where Qm increases but d33 decreases with the rise of temperature accompanied by escaping ferroelectric boundary, which shows that the polarization rotation plays an important role in the two parameters. The hardening effect of KNN-based ceramics with CuO doping is further studied by first-principles calculations, demonstrating that the Cu doping strongly disturbs the ferroelectric order, but the formation of defect dipoles could stabilize the ferroelectric order. It is illustrated that defect dipoles always find their ground state at the site near the domain walls and the oriented defect dipoles hinder the polarization rotation severely, confirming the role of the defect dipoles in KNN-based materials.

Improved energy storage density and efficiency in BaTiO3-BiFeO3- based relaxor-ferroelectric ceramics

It remains a huge challenge to enhance the energy-storage density (ESD) and efficiency (ESE) of Pb-free dielectrics for ES applications. However, most of the developed lead-free dielectrics do not have these properties due to some factors. In this study, 0.33BaTiO3-(0.67-x)BiFeO3-xBi(Mg2/3Ta1/3)O3 bulk relaxor-ferroelectric ceramic materials were established using a conventional solid-state technique, where a typical B-site composite perovskite-structured Bi(Mg2/3Ta1/3)O3 was used as an additive. The breakdown strength, relaxation behavior and ES performance of BaTiO3-BiFeO3 ceramics were improved after adding Bi(Mg2/3Ta1/3)O3 because of the generation of polar nanoregions (PNRs). The composite ceramics, with x = 0.10, demonstrated an excellent ESE (η) of 80.2 % and a high recoverable ESD (Wrec) of 3.0 J/cm3 at 240 kV/cm. In addition, the composite ceramics had high stability and good thermal stability in the frequency and temperature ranges of 0.5–100 Hz and 25–130 °C. These properties suggest that novel Bi(Mg2/3Ta1/3)O3-doped 0.33BaTiO3-0.67BiFeO3 ceramic is attractive for ES applications.

Atomic site preference, electronic structures, and magnetic properties of γ-brass type pseudo-binary Mn2Zn11–Ni2Zn11 at high Mn-contents

Samples loaded as MnxNi2Zn11−x (x = 0.1–5) were synthesized using conventional high-temperature solid-state techniques and characterized using X-ray diffraction, neutron powder diffraction, and energy dispersive X-ray spectroscopy. A Hume-Rothery-type mechanism was applied, following the rigid band model, to rationalize the electronic stability of these phases. This shows that at low Mn substitution for Zn, there is a structural preference for Mn atoms to be farthest apart within the same cluster, but that with increasing Mn concentration, there is a favorability in maximizing shortest Mn–Mn contacts between adjacent clusters of the γ-brass-type structure. The properties involving temperature-dependent zero-field-cooled (ZFC) and field-cooled (FC) magnetization, susceptibility, M(H) hysteresis curves, thermoremanent magnetization, and memory effect were studied for Mn1.5Ni2Zn9.5. A spin glass state has been observed below the transition temperature of ∼58.5 K, which originates predominately from the disordered substitution of Mn for Zn atoms in the inner tetrahedral and octahedral shells of the structure.