Entanglement-Enhanced Nanoscale Single-Spin Sensing

Detecting individual spins--including stable and metastable states--represents a fundamental challenge in quantum sensing with broad applications across condensed matter physics, quantum chemistry, and single-molecule magnetic resonance imaging. While nitrogen-vacancy (NV) centers in diamond have emerged as powerful nanoscale sensors, their performance for single-spin detection remains constrained by substantial environmental noise and restricted sensing volume. Here, we propose and demonstrate an entanglement-enhanced sensing protocol that overcomes these limitations through the strategic use of entangled NV pairs. Our approach achieves a 3.4-fold enhancement in sensitivity and a 1.6-fold reduction in spatial resolution relative to single NV centers under ambient conditions. The protocol employs carefully engineered entangled states that amplify target spin signals through quantum interference while suppressing environmental noise. Crucially, we extend these capabilities to resolve metastable single-spin dynamics, directly observing stochastic transitions between different spin states by identifying state-dependent coupling strengths. This dual functionality enables simultaneous detection of static and dynamic spin species for studying complex quantum systems. The achieved performance establishes entanglement-enhanced sensing as a viable pathway toward atomic-scale characterization of quantum materials and interface.