Quantum sensing of nanoscale electronic phase segregation

Abstract

Doping of transition metal oxides such as CaFe$_3$O$_5$ offers a controlled way to tune the interplay of charge, spin, and lattice degrees of freedom, yet local-probe studies remain difficult because strong correlations and dynamic charge-spin fluctuations obscure fine spectroscopic features in powder samples. Here, we employ quantum magnetometry based on nitrogen-vacancy (NV) centers in nanodiamonds impressed into an Mn-doped CaFe$_3$O$_5$ powder pellet to probe static and dynamic magnetic fields at the nanoscale across the weak ferromagnetic transition. The splitting and broadening of the optically detected magnetic resonance (ODMR) spectra exhibit an order-parameter-like increase by ~ 15 MHz upon cooling below the critical temperature, T$_{\rm c}$. Concomitantly, the spin-lattice relaxation rate, 1/T$_1$, exhibits a pronounced, divergence-like enhancement at T$_{\rm c}$, increasing by about one order of magnitude from its high-temperature value. Moreover, detailed lineshape fits of ODMR spectra together with the stretched-exponential NV magnetization recovery curves corroborate the proposed electronic phase segregation in charge-ordered and charge-averaged phases at the nanometric scales. The presented study demonstrates the viability of using nanodiamonds as a platform for nanoscale magnetic probing of strongly correlated matter, including phenomena such as electronic phase separation.