Emergent Random Spin Singlets in Disordered Spin-1/2 perovskite BaCu${}_{1/3}$Ta${}_{2/3}$O${}_3$

Abstract

We investigate the disordered perovskite BaCu${}_{1/3}$Ta${}_{2/3}$O${}_3$, where Cu (spin-1/2) and Ta randomly occupy a pseudo-cubic lattice. Synchrotron X-ray diffraction and X-ray absorption spectroscopy establish the local nature of the disorder, revealing the presence of structurally constrained magnetic exchange paths. No magnetic ordering or spin freezing is observed down to 0.1 K. The low-temperature magnetic and thermodynamic behavior is captured by a broad but non-singular distribution $P(J)$ of exchange couplings $J$. These results open the possibility of realizing a disordered quantum ground state where the exchange randomness is broad yet intrinsically bounded, departing from the conventional infinite-randomness fixed point driven random-singlet phase.