We have investigated magnetic correlations in various CMR manganites on macroscopic, mesoscopic and microscopic length scales by carrying out DC magnetization, neutron depolarization, and neutron diffraction measurements. We present here the effect of substituting Mn with Fe and La with Dy in the ferromagnetic La_0.7−xCa_xMnO₃ (x ∼ 0.3–0.33) compounds. Neutron diffraction has been used in order to characterize the long-range magnetic order and its gradual suppression by the substitution. Neutron depolarization study has been carried out in order to bridge the gap in our understanding regarding the nature of magnetic correlation obtained from the macroscopic and microscopic measurements. In particular, our study on La_0.67Ca_0.33Mn_0.9Fe_0.1O₃ has established the fact that a true double exchange mediated spin-glass is insulating. In another study of La-site ionic size effect and its disorder in (La_1−xDy_x)_0.7Ca_0.3MnO₃, we have investigated the evolution of the length scale of magnetic ordering with a possible microscopic explanation and the results have been compared with that for the light rare earth substituted compounds.

We have studied the magnetic structure of Fe[Fe(CN)₆]·4H₂O, prepared by precipitation method, using neutron diffraction technique. Temperature dependent DC magnetization study down to 4.2 K shows that the compound undergoes from a high temperature disordered (paramagnetic) to an ordered magnetic phase transition at 22.6 K. Rietveld analysis of neutron diffraction pattern at 60 K (in its paramagnetic phase) revealed a face centred cubic structure with space group Fm3m. The structure contains three-dimensional network of straight Fe³⁺-C≡N-Fe³⁺ chains along the edges of the unit cell cube. Fe³⁺ ions occupy 4a (0, 0, 0) and 4b (1/2, 1/2, 1/2) positions. Fe³⁺(0, 0, 0) is surrounded octahedrally by six nitrogen atoms and Fe³⁺ (1/2, 1/2, 1/2) is surrounded octahedrally by six carbon atoms. Magnetic Rietveld refinement of neutron diffraction data at 11 K shows a ferromagnetic coupling between the two inequivalent Fe³⁺ sites. Refinement yielded an ordered moment of 4.4(6) and 0.8(6) μ_B per Fe ion located at (0, 0, 0) and (1/2, 1/2, 1/2), respectively. Ordered moments are found to align along the face diagonal. The observed net moment from low temperature neutron diffraction study is consistent with DC magnetization results.

We have synthesized polycrystalline La_0.95Nd_0.05CrO₃ sample by doping the La-site of LaCrO₃ with Nd and its magnetic properties have been studied using DC magnetization and neutron diffraction techniques. DC magnetization study shows a paramagnetic to a weak ferromagnetic-like transition at ∼295 K followed by signatures of a spin reorientation phenomenon at 233 and 166 K and, finally a transition to an antiferromagnetic-like phase at ∼21 K. Low-temperature neutron diffraction measurements confirm a weak ferrimagnetic ordering of Cr³⁺ moments at all temperatures below 295 K.

We have studied magnetic correlations in several oxide materials that belong to colossal magnetoresistive, naturally occurring layered oxide showing low-dimensional magnetic ordering, solid oxide fuel cell interconnect materials, and magnetic nanoparticles using neutron diffraction and neutron depolarization techniques. In this paper, an overview of some of these results is given.

The brownmillerite-type layered compound Ca_2.375La_0.125Sr_0.5GaMn₂O₈ has been synthesized. The crystal and magnetic structures have been refined by the Rietveld analysis of the neutron powder diffraction patterns at 300 and 20 K. This compound crystallizes in the orthorhombic symmetry under the space group Pcm2₁ ($a = 5.447(2)$, $b = 11.359(4)$ and $c = 5.322(2)$ Å). The compound is found to be antiferromagnetic at 20 K. The ordered Mn magnetic moment, aligned along the crystallographic 𝑏-direction, is derived to be $2.53(5) \mu_{B}$ per Mn ion at 20 K.

We report the results of the DC magnetization, neutron powder diffraction and neutron depolarization studies on the spin-chain compounds Ca₃Co$_{2−x}$Fe$_{x}$O₆ ($x = 0$, 0.1, 0.2 and 0.4). Rietveld refinement of neutron powder diffraction patterns at room temperature confirms the single-phase formation for all the compounds in rhombohedral structure with space group R$\bar{3}$c. Rietveld refinement also confirms that Fe was doped at the trigonal prism site, 6a (0, 0, 1/4) of Co. The high temperature magnetic susceptibility obeys the Curie–Weiss law; the value of the paramagnetic Curie temperature ($\theta_{p}$) decreases as the concentration of iron increases and it becomes negative for $x = 0.4$. No extra Bragg peak as well as no observable enhancement in the intensity of the fundamental (nuclear) Bragg peaks has been observed in the neutron diffraction patterns down to 30 K. No depolarization of neutron beam has been observed down to 3 K confirming the absence of ferro- or ferrimagnetic-like correlation.