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Title: Magnetic frustration driven by conduction carrier blocking in Nd2Co0.85Si2.88

Journal Article · · Physical Review. B

The intermetallic compound Nd2Co0.85Si2.88 having a triangular lattice could be synthesized in single phase only with defect crystal structure. Investigation through different experimental techniques indicate the presence of two magnetic transitions in the system. As verified experimentally and theoretically, the high-temperature transition $$T_H$$ ~ 140 K is associated with the development of ferromagnetic interaction between itinerant Co moments, whereas the low-temperature transition at $$T_L$$ ~ 6.5 K is due to the coupling among Nd–4$$\textit{f}$$ and Co–3$$\textit{d}$$ moments, which is antiferromagnetic in nature. Detailed studies of temperature-dependent dc magnetic susceptibility, field dependence of isothermal magnetization, nonequilibrium dynamical behavior, viz., magnetic relaxation, aging effect, magnetic-memory effect, and temperature dependence of heat capacity, along with density functional theory (DFT) calculations, suggest that the ground state is magnetically frustrated spin glass in nature, having competing magnetic interactions of equivalent energies. DFT results further reveal that the 3$$\textit{d}$$/5$$\textit{d}$$-conduction carriers are blocked in the system and act as a barrier for the 4$$\textit{f}$$–4$$\textit{f}$$ RKKY interactions, resulting in spin frustration. Presence of vacancy defects in the crystal are also conducive to the spin frustration. This is an unique mechanism of magnetic frustration, not emphasized so far in any of the ternary $$R_2TX_3$$ ($$\textit{R}$$ = rare earth, $$\textit{T}$$ = transition elements, and $$\textit{X}$$ = Si, Ge, In) type compounds. Due to the competing character of the itinerant 3$$\textit{d}$$ and localized 4$$\textit{f}$$ moments, the compound exhibits anomalous field dependence of magnetic coercivity. Further, the system also exhibits a considerable magnetic entropy change of –Δ$$S_M$$ ~ 13.3 J/kg K with a relative cooling power (RCP) of 220 J/kg and adiabatic temperature change $$ΔT_{\text{ad}}$$ of 6 K for magnetic field change of 70 kOe.

Research Organization:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; Council of Scientific and Industrial Research (CSIR); Department of Atomic Energy (DAE) of India; USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-07CH11358
OSTI ID:
1969488
Alternate ID(s):
OSTI ID: 1963976
Report Number(s):
IS-J-11,035; TRN: US2313417
Journal Information:
Physical Review. B, Vol. 107, Issue 9; ISSN 2469-9950
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

References (74)

Dynamic measurements in a Heisenberg spin glass: CuMn journal May 1994
The Magnetocaloric Effect and its Applications reference-book January 2016
Multiple magnetic transitions and anomalous magnetism in Tb2CuGe3 journal March 2001
Memory effects and magnetic relaxation in single-crystallineLa0.9Sr0.1CoO3 journal July 2014
Structures and physical properties of R 2 TX 3 compounds journal May 2013
Geometrical frustration journal February 2006
Magnetic properties and magnetocaloric effect in the R2PdSi3 (R=Gd, Dy and Er) compounds journal March 2015
Magnetocaloric properties of cluster glass compound Pr2Ni0.95Si2.95 journal August 2019
Observation of enhanced magnetic transition temperature in Nd 2 PdGe 3 and superconductivity in Y 2 PdGe 3 journal April 2001
Anomalous magnetoresistance in centrosymmetric skyrmion-lattice magnet Gd 2 PdSi 3 journal August 2020
Low-field induced large magnetocaloric effect in Tm 2 Ni 0.93 Si 2.93 : influence of short-range magnetic correlation journal November 2017
High-field depinned phase and planar Hall effect in the skyrmion host Gd 2 PdSi 3 journal June 2020
Sequential Cobalt Magnetization Collapse in ErCo2: Beyond the Limits of Itinerant Electron Metamagnetism journal March 2015
Low-temperature properties of classical geometrically frustrated antiferromagnets journal November 1998
Recent advances in magnetic structure determination by neutron powder diffraction journal October 1993
From ultrasoft pseudopotentials to the projector augmented-wave method journal January 1999
Origin of the Glassy Magnetic Behavior of the Phase Segregated State of the Perovskites journal October 2004
Memory Effects in an Interacting Magnetic Nanoparticle System journal October 2003
Nonequilibrium dynamics of spin glasses journal July 1988
Fractal dynamics of spin glasses journal November 1985
Large magnetic cooling power involving frustrated antiferromagnetic spin-glass state in R 2 NiSi 3 ( R = Gd , Er ) journal September 2016
Creation and Annihilation of Skyrmions in the Frustrated Magnets with Competing Exchange Interactions journal November 2017
Disordered magnetism and spin glasses journal May 1996
Antiferromagnetism in EuCu 2 As 2 and EuCu 1.82 Sb 2 single crystals journal May 2015
Magnetic entropy change and magnetocaloric effect of DyNiSi3, Dy2Ni3Si5, DyNiSi2 and HoNiSi0.33Ga67 antiferromagnets journal April 2019
Spin-Flop Transition and Magnetocaloric Effect through Disconnected Magnetic Blocks in CoIII/CoIV Oxybromides journal May 2010
Resistivity and magnetoresistance properties of R2NiSi3 (R = Gd, Dy, Ho, Er, Tm) compounds journal October 2020
Giant magnetocaloric effect in antiferromagnetic ErRu2Si2 compound journal October 2007
Is Hund's Second Rule Responsible for the Orbital Magnetism in Solids? journal June 1998
Role of random magnetic anisotropy on the valence, magnetocaloric and resistivity properties in a hexagonal Sm 2 Ni 0.87 Si 2.87 compound journal April 2018
Symmetry properties of intra-atomic spin and angular momentum densities: application to journal August 1997
Magnetic structure of triangular lattice compound Tb2Ni0.90Si2.94 journal October 2021
Enhanced magnetocaloric effect in frustrated magnets journal March 2003
Studies on magnetocaloric effect of Tb2Ni0.90Si2.94 compound journal March 2020
Equilibrium behavior of the spin-glass ordered phase journal July 1988
Topological Nernst Effect of the Two-Dimensional Skyrmion Lattice journal August 2020
Formation Mechanism of the Helical Q Structure in Gd-Based Skyrmion Materials journal September 2020
Superconducting behavior of the solid solution, Y2Pd1−xPtxGe3 journal November 2007
Magnetic frustration induced large magnetocaloric effect in the absence of long range magnetic order journal August 2017
Complex magnetic properties associated with competing local and itinerant magnetism in $${\text {Pr}}_2 {\text {Co}}_{0.86} {\text {Si}}_{2.88}$$ journal June 2021
Geometrically frustrated magnetic materials journal January 2001
Aging and memory effects in superparamagnets and superspin glasses journal March 2005
Antiferromagnetic order and spin glass behavior in Dy2CuIn3 journal November 2011
Giant magnetocaloric effect in magnetically frustrated EuHo2O4 and EuDy2O4 compounds journal September 2012
Scaling theory of Ising spin glasses journal June 1984
Frustration-driven magnetic fluctuations as the origin of the low-temperature skyrmion phase in Co7Zn7Mn6 journal April 2021
Unusual bidirectional frequency dependence of dynamical susceptibility in hexagonal intermetallic Pr2Ni0.95Si2.95 journal October 2018
Magnetism in Condensed Matter journal January 2003
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal October 1996
Skyrmion lattice with a giant topological Hall effect in a frustrated triangular-lattice magnet journal August 2019
Commentary: The Materials Project: A materials genome approach to accelerating materials innovation journal July 2013
Quantum Skyrmions in Frustrated Ferromagnets journal December 2019
Formation enthalpies by mixing GGA and GGA + U calculations journal July 2011
Magnetic properties and magnetocaloric effect of NdMn2−xCuxSi2 compounds journal May 2014
A high-throughput infrastructure for density functional theory calculations journal June 2011
Magnetic properties and magnetocaloric effect in intermetallic compounds NdMn2−xCoxSi2 journal May 2012
Introduction to Frustrated Magnetism book January 2011
Correspondence between neutron depolarization and higher order magnetic susceptibility to investigate ferromagnetic clusters in phase separated systems journal November 2013
Memory and Chaos Effects in Spin Glasses journal October 1998
Spin glasses: Experimental facts, theoretical concepts, and open questions journal October 1986
Magnetic and magnetocaloric properties of ball milled Nd5Ge3 journal April 2012
Band structure evolution during the ultrafast ferromagnetic-paramagnetic phase transition in cobalt journal March 2017
Slow relaxation in ferromagnetic nanoparticles: Indication of spin-glass behavior journal January 2003
Oxidation energies of transition metal oxides within the GGA + U framework journal May 2006
A framework for quantifying uncertainty in DFT energy corrections journal July 2021
Exact low-temperature behavior of a kagomé antiferromagnet at high fields journal September 2004
Calculating free energies of point defects from ab initio journal June 2018
Anomalous magnetoresistance and magnetocaloric properties of NdRu 2 Ge 2 journal February 2013
Spatially limited antiferromagnetic order in a cluster glass compound Tb2Ni0.90Si2.94 journal May 2019
Calculation of the magnetic anisotropy with projected-augmented-wave methodology and the case study of disordered Fe 1 x Co x alloys journal June 2016
Magnetic phase inhomogeneity in frustrated intermetallic compound Sm2Ni0.87Si2.87 journal April 2018
Spin-glass-like state in GdCu: Role of phase separation and magnetic frustration journal April 2011
Magnetism and magnetocaloric effect in the RE2CuSi3 (RE = Dy and Ho) compounds journal April 2017
Effects of antiferro-ferromagnetic phase coexistence and spin fluctuations on the magnetic and related properties of NdCuSi journal June 2015