Quantum control method for single-molecule chemical reactions based on NV centers

Abstract

Active quantum control at the molecular scale remains a central pursuit in nanochemistry and quantum biology. Here, we demonstrate coherent polarization transfer from a nitrogen-vacancy (NV) center to a radical pair (RP)—a ubiquitous intermediate in chiral-bridge-mediated electron transfer—via dressed-state resonance. While direct energy exchange between the NV center and external spins is typically suppressed by energy conservation, we show that the dressed-state framework overcomes this limitation, enabling efficient control over the RP spin dynamics. Using quantum master equation simulations that incorporate the NV hyperfine Hamiltonian and RP internal interactions, we elucidate the magnetic field effect induced by the NV center. The spatial dependence analysis reveals that effective control with a product yield change of 10% (5%) can be achieved within maximum NV-RP separation ranges of 3.0– 4.1 nm ( 3.3– 4.5 nm) across the vertical, parallel, and randomly oriented NV-RP configurations. These findings establish a pathway for manipulating chemical reactivity using solid-state defects, offering new perspectives for quantum sensing and control in complex molecular systems.