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Enhancing Magneto-Optical Activity via Coordination Distortion in Chiral Er4M8 Clusters
Jia-Nan Chen1, Jiaye Chen2, Ming-Qiang Qi1
1State Key Laboratory of Physical Chemistry of Solid Surfaces and Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
None:
Chiral lanthanide molecular materials exhibiting robust magneto-optical (MO) responses are attractive for applications in optical sensing, optical readout, and magnetic-field-controlled circular-polarization optics. However, achieving strong MO responses remains challenging due to the formally parity-forbidden nature and weak oscillator strengths of f-f transitions. Herein, we present three pairs of chiral R/S-Er4M8 clusters (M = Co2+ for Er4Co8; Cu2+ for Er4Cu8; Zn2+ for Er4Zn8) that display pronounced circular dichroism (CD) and magnetic circular dichroism (MCD) signals spanning the UV-vis-NIR spectral region. Despite possessing nearly identical cluster frameworks, these clusters display markedly distinct MO behaviors. Interestingly, the gMCD of Er4Zn8 exceeds those of Er4Co8 and Er4Cu8. Notably, Er4Zn8 exhibits a record-value of 0.044 T-1 for the 4I15/2 → 4I13/2 transition (1400-1600 nm), exceeding its Co and Cu analogues by factors of 5.6 and 2.6, respectively. Structural analyses indicate that this enhancement correlates with pronounced local coordination asymmetry at the Er3+ sites, which promotes odd-parity crystal-field mixing and electric-dipole borrowing within the 4f manifold, thereby strengthening the Zeeman-driven MCD response. These findings suggest site-specific structural distortion as a powerful design principle for enhancing and amplifying f-f transition-driven magneto-optical responses.
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