Kinetically Inhibited Order in a Diamond-Lattice Antiferromagnet

Abstract

Frustrated magnetic systems exhibit highly degenerate ground states and strong fluctuations, often leading to new physics. An intriguing example of current interest is the antiferromagnet on a diamond lattice, realized physically in A-site spinel materials. This is a prototypical system in three dimensions where frustration arises from competing interactions rather than purely geometric constraints, and theory suggests the possibility of unusual magnetic order at low temperature. Here we present a comprehensive single-crystal neutron scattering study of CoAl2O4, a highly frustrated A-site spinel. We observe strong diffuse scattering that peaks at wavevectors associated with Neel ordering. Below the temperature T*=6.5 K, there is a dramatic change in the elastic scattering lineshape accompanied by the emergence of well-defined spin-wave excitations. T* had previously been associated with the onset of glassy behavior. Our new results suggest instead that T* signifies a first-order phase transition, but with true long-range order inhibited by the kinetic freezing of domain walls. This scenario might be expected to occur widely in frustrated systems containing first-order phase transitions and is a natural explanation for existing reports of anomalous glassy behavior in other materials.

40 pages, 9 figures, Introduction and discussion altered and expanded. Additional section and figure added to Supplementary Information

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• CaMn${}_2$Sb${}_2$: Spin waves on a frustrated antiferromagnetic honeycomb lattice
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• Spin glass behavior in frustrated quantum spin system CuAl2O4 with a possible orbital liquid state
• Structural transition and orbital glass physics in near itinerant CoV2O4
• Frustrated Heisenberg $J_1-J_2$ model within the stretched diamond lattice of LiYbO2
• Antiferromagnetic and Orbital Ordering on a Diamond Lattice Near Quantum Criticality
• Approaching the Ground State of Frustrated A-site Spinels: A Combined Magnetization and Polarized Neutron Scattering Study
• Experimental Evidence for the Spiral Spin Liquid in LiYbO${}_2$
• Continuous spin excitations in the three-dimensional frustrated magnet K2Ni2(SO4)3
• Revisiting the ground state of CoAl${}_2$O${}_4$: comparison to the conventional antiferromagnet MnAl${}_2$O${}_4$
• Quasi-local critical nature of cooperative paramagnetic fluctuations in CaRuO${}_3$ metal
• Cluster glass transition and relaxation in random spinel CoGa2O4
• Nonconventional magnetic order in frustrated diamond lattice antiferromagnet CoAl2O4 studied by neutron diffraction and classical Monte-Carlo simulation
• Spin Freezing in the Spin Liquid Compound FeAl2O4
• Magnetism on the stretched diamond lattice in lanthanide orthotantalates
• Evolution of Magnetic and Orbital Properties in the Magnetically-Diluted A-Site Spinel Cu${}_{1-x}$Zn${}_x$Rh${}_2$O${}_4$
• A molecular diamond lattice antiferromagnet as a Dirac semimetal candidate
• Realising square and diamond lattice $S=1/2$ Heisenberg antiferromagnet models in the $\alpha$ and $\beta$ phases of the coordination framework, KTi(C${}_2$O${}_4$)${}_2\cdot$\textit{x}H${}_2$O
• Magnetic order and exchange couplings in the frustrated diamond lattice antiferromagnet MnSc${}_2$Se${}_4$
• Multistage ordering and critical singularities in Co1-xZnxAl2O4 (0 < x < 1):Dilution and pressure effects in a magnetically frustrated system
• Line-Graph Approach to Spiral Spin Liquids
• Disorder effects in spiral spin liquids: Long-range spin textures, Friedel-like oscillations, and spiral spin glasses
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• Magnetic ordering in the $J_{\mathrm{eff}}$ = 0 Nickelate NiRh${}_2$O${}_4$ prepared via a solid-state metathesis
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• Frustrated $J_1-J_2$ Diamond Lattice Antiferromagnet Co${}_2$Ti${}_3$O${}_8$ with a Vacancy-ordered Spinel Structure Synthesized via a Topochemical Reaction
• Codimension-Two Spiral Spin-Liquid in the Effective Honeycomb-Lattice Compound Cs${}_3$Fe${}_2$Cl${}_9$