Chiral SURMOFs for Vibrational Circular Dichroism: Multiscale Modeling and Experimental Insights

Chiral surface-anchored metal-organic frameworks (SURMOFs) are emerging as versatile platforms for enantioselective separation, sensing, and the manipulation of circularly polarized light. To harness their full potential, predictive modeling of their optical properties is essential, given the vast design space. Here, a multiscale computational framework is introduced that reliably captures the optical response of camphoric acid–DABCO-based pillar-layer SURMOFs incorporating either zinc or copper nodes. The approach integrates simulations from the unit-cell level to the thin-film scale. To validate the model, SURMOFs are fabricated on various substrates and characterized using infrared reflection and transmission spectroscopy, infrared scanning near-field optical microscopy, and solid-state vibrational circular dichroism (VCD) spectroscopy. Notably, the VCD spectra for the zinc-based SURMOF provide direct insight into vibrational optical activity in the solid state. The strong correlation between theoretical predictions and experimental data confirms the robustness of the model and establishes design principles for future optically active chiral MOF materials.