Magnetocaloric Effect in a Frustrated Gd-Garnet with No Long-Range Magnetic Order

Chogondahalli Muniraju, Naveen Kumar; Baral, Raju; Tian, Yefan; Li, Rui; Poudel, Narayan; Gofryk, Krzysztof; Barišić, Neven; Kiefer, Boris; Ross, Joseph H.; Nair, Harikrishnan S.

doi:10.1021/acs.inorgchem.0c02074

Magnetocaloric Effect in a Frustrated Gd-Garnet with No Long-Range Magnetic Order

Journal Article · Tue Oct 06 00:00:00 EDT 2020 · Inorganic Chemistry

DOI:https://doi.org/10.1021/acs.inorgchem.0c02074· OSTI ID:1687369

Chogondahalli Muniraju, Naveen Kumar ^[1]; Baral, Raju ^[2]; Tian, Yefan ^[3]; Li, Rui ^[3]; ^[4]; ^[4]; Barišić, Neven ^[5]; Kiefer, Boris ^[6]; ^[3]; Nair, Harikrishnan S. ^[2]

Technische Univ. Wien (Austria)
Univ. of Texas at El Paso, TX (United States)
Texas A & M Univ., College Station, TX (United States)
Idaho National Lab. (INL), Idaho Falls, ID (United States)
Univ. of Zagreb (Croatia)
New Mexico State Univ., Las Cruces, NM (United States)

In this work, the hyperkagome lattice of Gd spins in a garnet compound, Gd₃CrGa₄O₁₂, is studied using bulk measurements and density functional computations, and the observation of large magnetocaloric effect corresponding to an entropy change, ΔS_m = 45 Jkg^-1K^-1 (≈ 45 J mol^-1K^-1) at 2 K, 8 T is reported. Though the compound defies long-range magnetic order down to 0.4 K, a broad feature below 10 K is observed in the specific heat with two low temperature anomalies at T* ≈ 0.7 K and T_S ≈ 2.45 K. The anomaly at T* is reminiscent of one in Gd₃Ga₅O₁₂, where it is related to the development of a complex magnetic phase, whereas the T_S-peak is accounted for by a multilevel Schottky-like model. The spin-lattice relaxation times studied by nuclear magnetic resonance experiments show that the relaxation is dominated by the magnetic fluctuations in Cr which has a longer relaxation time compared to that of the garnet, Lu₃CrGa₄O₁₂ containing a nonmagnetic rare earth. Our first-principles density functional theory calculations agree well with the experimental results and support short-range magnetic order in the Gd-sublattice and antiferromagnetism in the Cr-sublattice. The importance of spin fluctuations and short-range order in the rare earth and transition metal lattices in garnets resulting in large magnetocaloric effect is brought out through this work.

View Accepted Manuscript (DOE)

Research Organization:: Idaho National Laboratory (INL), Idaho Falls, ID (United States)

Sponsoring Organization:: Croatian Science Foundation; European Regional Development Fund; Extreme Science and Engineering Discovery Environment (XSEDE); Robert A. Welch Foundation; Swiss National Science Foundation (SNSF); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC)

Grant/Contract Number:: AC07-05ID14517

OSTI ID:: 1687369

Alternate ID(s):: OSTI ID: 1759037

Report Number(s):: INL/JOU--19-56395-Rev000

Journal Information:: Inorganic Chemistry, Journal Name: Inorganic Chemistry Journal Issue: 20 Vol. 59; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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