Publication date: 15th December 2025
Colloidal lead halide perovskite nanocrystals (NCs) are generally regarded as diamagnetic; however, emerging evidence suggests that quantum confinement and lattice distortion can induce unexpected magnetic responses. In this work, we present the first systematic investigation of size-dependent excitonic Zeeman splitting in colloidally synthesized CsPbX₃ (X = Cl, Br) nanocrystals. Using variable-field and temperature-dependent magnetic circular dichroism (MCD) spectroscopy, we reveal a pronounced Curie-type (1/T) temperature dependence and unusually large negative excitonic g-factors (g_eff ≈ −20) in strongly confined CsPbBr₃ NCs. The magnitude of the Zeeman splitting decreases monotonically with increasing NC size, directly correlating magnetic response with confinement-induced lattice strain. Comparative analysis shows that CsPbBr₃ exhibits a significantly stronger magnetic response than CsPbCl₃, which is attributed to its orthorhombic crystal structure and enhanced Pb–Br bond asymmetry. These structural distortions promote the formation of local paramagnetic centers associated with Pb oxidation-state fluctuations (Pb²⁺ → Pb¹⁺/Pb³⁺). In contrast, CsPbCl₃ NCs, which adopt a more symmetric cubic structure, remain relatively strain-free and display a much weaker Zeeman response despite a higher halide vacancy density. These results establish structural strain—rather than vacancy concentration alone, as a key parameter governing emergent magnetism in perovskite nanocrystals, providing new design principles for magnetically tunable quantum and spin-optoelectronic materials.
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