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Disorder can have a dominating influence on correlated and quantum materials leading to novel behaviors which have no clean limit counterparts. In magnetic systems, spin and exchange disorder can provide access to quantum criticality, frustration, and spin dynamics, but broad tunability of these responses and a deeper understanding of strong limit disorder is lacking. In this work, we demonstrate that high entropy oxides present an unexplored route to designing quantum materials in which the presence of strong local compositional disorder hosted on a positionally ordered lattice can be used to generate highly tunable emergent magnetic behavior--from macroscopically ordered states to frustration-driven dynamic spin interactions. Single crystal La(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 films are used as a structurally uniform model system hosting a magnetic sublattice with massive microstate disorder in the form of site-to-site spin and exchange type inhomogeneity. A classical Heisenberg model is found to be sufficient to describe how compositionally disordered systems can paradoxically host long-range magnetic uniformity and demonstrates that balancing the populating elements based on their discrete quantum parameters can be used to give continuous control over ordering types and critical temperatures. Theory-guided experiments show that composite exchange values derived from the complex mix of microstate interactions can be used to design the required compositional parameters for a desired response. These predicted materials are synthesized and found to possess an incipient quantum critical point when magnetic ordering types are designed to be in direct competition; this leads to highly controllable exchange bias sensitivity in the monolithic single crystal films previously accessible only in intentionally designed bilayer heterojunctions.
The possibility of investigating the dynamics of solids on timescales faster than the thermalization of the internal degrees of freedom has disclosed novel non-equilibrium phenomena that have no counterpart at equilibrium. Transition metal oxides (TM
We investigate spin correlations in the dipolar Heisenberg antiferromagnet Gd2Sn2O7 using polarised neutron-scattering measurements in the correlated paramagnetic regime. Using Monte Carlo methods, we show that our data are sensitive to weak further-
The 18.5 K superconductor PuCoGa5 has many unusual properties, including those due to damage induced by self-irradiation. The superconducting transition temperature decreases sharply with time, suggesting a radiation-induced Frenkel defect concentrat
The interplay of symmetry and quenched disorder leads to some of the most fundamentally interesting and technologically important properties of correlated materials. It also poses the most vexing of theoretical challenges. Nowhere is this more appare
We study the quantum criticality of the phase transition between the Dirac semimetal and the excitonic insulator in two dimensions. Even though the system has a semimetallic ground state, there are observable effects of excitonic pairing at finite te