Temperature-Selected Defect-Moiré Coupling Controls Nonradiative Charge Recombination in Twisted MoS2.

Moiré superlattices in twisted transition-metal dichalcogenides provide a versatile platform for engineering charge carrier dynamics, yet interactions between intrinsic defects and dynamically reconstructed moiré potentials under experimentally relevant conditions remain poorly understood. Here, we develop a machine-learning-accelerated nonadiabatic molecular dynamics (ML-NAMD) framework combining a DeePMD-based ML force field, an E(3)-equivariant Hamiltonian neural network, and NAMD, enabling nanosecond-scale structural sampling and electronically resolved carrier recombination dynamics in thousand-atom pristine and sulfur-vacancy-containing 3.48° twisted bilayer MoS2 supercells. We show that the sulfur vacancy is not a static recombination center; instead, its local moiré environment is thermally selected through coupling to dynamic lattice reconstruction. At 300 K, the vacancy-adjacent region evolves toward an RMoMo-like environment, an R-type Mo-on-Mo stacking with vertically aligned Mo atoms across the layers, whereas at 50 K it favors reconstructed commensurate domains or nearby domain wall configurations. This temperature-selected local stacking governs defect-moiré coupling and, consequently, carrier recombination. Sulfur vacancies induce femtosecond electron capture into defect trap states, but subsequent nonradiative recombination is strongly stacking dependent. In reconstructed regions, a deep-trap-mediated pathway accelerates recombination, whereas in the RMoMo region it is strongly suppressed, producing a 6.7-fold longer carrier lifetime. These findings establish a microscopic mechanism of temperature-selected defect-moiré coupling, in which local lattice reconstruction determines whether defect and moiré potentials cooperate to activate, or compete to suppress, trap-mediated nonradiative recombination. This mechanism suggests practical strategies for reducing nonradiative losses and improving the performance of moiré optoelectronic devices by controlling local reconstruction, temperature, twist angle, and defect passivation.