Abstract
We investigated the magnetic and optical properties of ${(2,3\text{-dmpyH})}_{2}{\text{CuBr}}_{4}$, an unusual antiferromagnetic quantum spin ladder with strong rail interactions that can be saturated in a 30 T field. This transition drives a field-induced color change, a dramatic example of charge-spin coupling in a molecular material. Spin-density calculations reveal that electronic structure is sensitive to the magnetic state because magnetic orbital character depends on the spin arrangement between adjacent ${\text{CuBr}}_{4}^{2\ensuremath{-}}$ chromophores. This finding suggests that molecular architecture and the magnetic arrangement between molecular units might be used to control magnetochromism.
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