Terahertz-nanoscale visualization of the microscopic spin-charge architecture of colossal magnetoresistive switching

Abstract

Resolving sub-10 nm spin switching and the associated terahertz (THz) electrodynamics during the colossal magnetoresistance (CMR) transition is a definitive frontier in reaching the fundamental spatial, temporal, and energy-dissipation limits of spin-based microelectronics and quantum logic architectures. Yet, the requirement of simultaneous control of high magnetic field, cryogenic environment, and nanometer-scale resolution has remained an elusive benchmark for terahertz nanoscopy, leaving the obscured nano-scale high-frequency dynamics of these transitions largely unexplored. Here, we overcome these limitations by utilizing a custom-built cryogenic magneto-THz scattering-type scanning near-field optical microscopy (cm-THz-sSNOM) platform to resolve the nanoscale, THz spectroscopic evolution of the magnetic field-driven CMR transition in a manganite single crystal $\text{Pr}_{2/3}\text{Ca}_{1/3}\text{MnO}_{3}$. Our measurements provide a real-space visualization of the local THz conductivity, capturing the moment that magnetic-field-induced spin switching triggers the phase transition from an antiferromagnetic insulator to a ferromagnetic metal. THz nano-imaging, together with an ellipsoidal near-field model, reveals a multi-scale transition initiated by 1-2 nm isolated spin-flip sites at low magnetic fields, which coalesce into $\sim$15~nm conducting regions as the threshold field is approached. These results provide an in situ, previously inaccessible THz real-space view of CMR switching, establishing a general analysis framework for mapping spin-charge-lattice-orbit-coupled dynamics at spatial scales that transcend the nominal sSNOM resolution.