Mapping the magnetic state as a function of antisite disorder in 
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 double perovskite thin films

Majumder, Supriyo; Tripathi, Malvika; Raghunathan, Rajamani; Rajput, Parasmani; Jha, S. N.; Souza, Danilo Oliveira de; Olivi, Luca; Chowdhury, Sourav; Choudhary, R. J.; Phase, D. M.

doi:10.1103/physrevb.105.024408

Cited by 15 publications

(30 citation statements)

References 66 publications

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“…Deconvolution analysis of spectroscopic results as discussed in Ref. [19], confirm that in both S HO and S I samples, Ni and Mn transition metals have mixed valence nature with fractional concentrations: 55±1% Ni 2+ , 45±1% Ni 3+ and 54±2% Mn 4+ , 46±2% Mn 3+ . In early reports on bulk La 2 NiMnO 6 (LNMO) system, contradicting explanations were found whether the charge state of transition metal ions are Ni 3+ , Mn 3+ [13,30]; or Ni 2+ , Mn 4+ [14,31].…”

Section: Resultssupporting

confidence: 54%

“…The growth conditions during the fabrication of SNMO thin films, as discussed in Ref. [19], are exploited as the tuning knobs to effectively tailor the Ni/Mn cation arrangements in the system. Real time in situ reflection high energy electron diffraction and high resolution X-ray diffraction rocking ω scans suggest similar growth mode, similar surface morphology, and similar dislocation defect densities in different SNMO films irrespective of having different growth conditions.…”

Section: Resultsmentioning

confidence: 99%

“…The degree of ASD concentration and their distribution morphology are probed at both microscopic and macroscopic level implementing extended X-ray absorption fine structure, bulk magnetometry and random alloy structure simulations. The details about aforementioned structural characterizations are discussed elsewhere [19]. In present work, to explore the role of varying ASD on magnetic and electronic states of SNMO system, two samples are selected as the representing platform, (i) more ordered Mn 4+ species at T=300 K, with varying metal -ligand hybridization strength.…”

Section: Resultsmentioning

confidence: 99%

“…Following the recipe reported in Ref. [19], epitaxial SNMO thin films (thickness ∼140±5 nm) were deposited on (001) oriented SrTiO 3 single crystal substrates by pulsed laser deposition using a KrF excimer laser system (Lambda Physik, wavelength λ=248 nm, pulse width 20 ns). For magnetization measurements MPMS 7-Tesla SQUID-VSM (Quantum Design Inc., USA) system was used.…”

Section: Experimental Methodologymentioning

confidence: 99%

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Robust electronic and tunable magnetic states in Sm$ _{2} $NiMnO$ _{6} $ ferromagnetic insulator

Majumder,

Tripathi,

Píš

et al. 2022

Preprint

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Ferromagnetic insulators (FM-Is) are the materials of interest for new generation quantum electronic applications. Here, we have investigated the physical observables depicting FM-I ground states in epitaxial Sm 2 NiMnO 6 (SNMO) double perovskite thin films fabricated under different conditions to realize different level of Ni/Mn anti-site disorders (ASDs). The presence of ASDs immensely influence the characteristic magnetic and anisotropy behaviors in SNMO system by introducing short scale antiferromagnetic interactions in predominant long range FM ordered host matrix. Charge disproportion between cation sites in form of N i 2+ + M n 4+ −→ N i 3+ + M n 3+ , causes mixed valency in both Ni and Mn species, which is found insensitive to ASD concentrations. Temperature dependent photo emission, photo absorption measurements duly combined with cluster model configuration interaction simulations, suggest that the eigenstates of Ni and Mn cations can be satisfactorily described as a linear combination of the unscreened d n and screened d n+1 L (L: O 2p hole) states. The electronic structure across the Fermi level (E F ) exhibits closely spaced Ni 3d, Mn 3d and O 2p states. From occupied and unoccupied bands, estimated values of the Coulomb repulsion energy (U ) and ligand to metal charge transfer energy (∆), indicate charge transfer insulating nature, where remarkable modification in Ni/Mn 3d -O 2p hybridization takes place across the FM transition temperature. Existence of ASD broadens the Ni, Mn 3d spectral features, whereas spectral positions are found to be unaltered. Hereby, present work demonstrates SNMO thin film as a FM-I system, where FM state can be tuned by manipulating ASD in the crystal structure, while I state remains intact.

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Section: Resultssupporting

confidence: 54%

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Experimental Methodologymentioning

confidence: 99%

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Robust electronic and tunable magnetic states in Sm$ _{2} $NiMnO$ _{6} $ ferromagnetic insulator

Majumder,

Tripathi,

Píš

et al. 2022

Preprint

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“…Noteworthily, the characteristic electronic and magnetic behaviors of ANMO systems vary significantly among different reports available in literature [12,13]. These discrepancies can be correlated with the fact that different growth kinetics can lead to distinct cationic arrangement, which could eventually modify the physical observables [14]. As a consequence, the reliability and reproducibility related to any functional aspects of ANMO series is questionable which limits their feasibility in device applications.…”

Section: Introductionmentioning

confidence: 99%

Microscopic insights of magnetism in Sm$ _{2} $NiMnO$ _{6} $ double perovskite

Majumder,

Tripathi,

Fischer

et al. 2022

Preprint

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The functional characteristics of double perovskites with unique ferromagnetic-insulator ground state have been controversial due to the unavoidable presence of anti-site disorders (ASDs). Here, we aim to investigate the origin of magnetic ordering on local and global scales in Sm2NiMnO6 (SNMO) double perovskite system. Different calcination routes are exploited to generate different cation arrangements in SNMO and the corresponding magnetic configurations are examined using the high energy (E ∼0.3 eV) 'hot neutrons', which has helped to overcome Sm absorption as well as to record total (Bragg's+diffuse) scattering profiles with high momentum transfer (Qmax ∼24 Å−1 ). We have observed that the Ni-Mn sublattice adopts long range collinear ferromagnetic FxFz structure with commensurate k=(0, 0, 0) propagation vector, below ordering temperature T 160 K, irrespective of variable ASD concentrations. In addition, the signatures indicating the antiparallel polarization of Sm paramagnetic moments with respect to Ni-Mn network, are noticed in the vicinity of anomalous magnetic transitions at T 35 K. The real space pair distribution function calculations have provided a direct visualization of ASDs by means of broadening in Ni/Mn-Mn/Ni linkage. Employing the Reverse Monte Carlo approach on diffuse magnetic scattering profiles, we have observed the negative spin-spin correlation function which suggests the Ni-Ni antiferromagnetic exchange interactions ranging up to first nearest neighbor distance. These results confirm that the existence of ASDs in cation ordered host matrix leads to competing ferromagnetic-antiferromagnetic phases in a broad temperature range, which quantitatively governs the temperature dependent bulk magnetic observables of SNMO system.

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Study of Optical, Magnetic, and Magnetocaloric Properties of Double Perovskites Dy2NiMnO6: First Principles Approach and Monte Carlo Simulations

Bessimou,

Masrour

2024

J Inorg Organomet Polym

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Mapping the magnetic state as a function of antisite disorder in Sm2NiMnO6 double perovskite thin films

Cited by 15 publications

References 66 publications

Robust electronic and tunable magnetic states in Sm$ _{2} $NiMnO$ _{6} $ ferromagnetic insulator

Robust electronic and tunable magnetic states in Sm$ _{2} $NiMnO$ _{6} $ ferromagnetic insulator

Microscopic insights of magnetism in Sm$ _{2} $NiMnO$ _{6} $ double perovskite

Study of Optical, Magnetic, and Magnetocaloric Properties of Double Perovskites Dy2NiMnO6: First Principles Approach and Monte Carlo Simulations

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