Unraveling Dynamic Disorder in Metal Halide Perovskite Quantum Dots: Atomistic Insights Into Structure–Carrier Coupling From Ab Initio and Nonadiabatic Simulations

ABSTRACT Metal–halide perovskite quantum dots (PQDs) have emerged as highly dynamic nanoscale semiconductors whose optoelectronic properties are governed by a complex interplay of lattice fluctuations, electronic excitation processes, and surface‐mediated interactions. This review provides a comprehensive atomistic perspective on the structural and carrier dynamics of PQDs, integrating insights from ab initio molecular dynamics (AIMD) and nonadiabatic molecular dynamics (NAMD) simulations. We highlight the intrinsic lattice softness, anharmonicity, and surface‐driven structural disorder that define a continuously evolving energy landscape. These features strongly influence defect formation, ionic migration, and size‐dependent phase stability, establishing PQDs as dynamically fluctuating quantum systems rather than static crystals. In parallel, ultrafast photoexcitation processes reveal tightly coupled exciton formation, hot carrier relaxation, and recombination dynamics, all modulated by quantum confinement and electron–phonon interactions. Molecular dynamics studies further elucidate the critical roles of surface chemistry, ligand motion, compositional tuning, and environmental embedding in shaping optoelectronic behavior. Finally, we discuss current limitations of atomistic and nonadiabatic frameworks and emphasize the need for multiscale, environment‐inclusive, and data‐driven approaches to achieve predictive modeling. Overall, this work establishes a unified dynamic framework linking structure and carrier physics in PQDs, providing guiding principles for rational design of next‐generation optoelectronic nanomaterials.

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