Multidimensional helical dichroism from a chiral molecular nanoassembly

Detecting the chirality of molecules is of great importance in optics, biomedicine, and materials science. In chiroptical spectroscopy, it's crucial to achieve strong chiroptical signals with a minimal number of chiral molecules. The molecular chiroptical signals, however, are typically weak for chiral molecular sensing in conventional circular dichroism using photonic spin angular momentum, even in the presence of a large number of chiral molecules (micromoles to millimoles). Here, by involving chiral light-matter interaction with photonic orbital angular momentum, we demonstrate strong chiroptical responses that reflect the molecular chirality in a single chiral nanoassembly. We experimentally present the helical dichroism spectra of chiral nanoassemblies synthesized from L/D-cystines, consistent with electromagnetic simulations. The asymmetry factors in the fundamental wavelength and photoluminescence emission reach values of 0.53 and 1.18, respectively, exceeding those observed in the circular dichroism mechanism. To improve the dimensions of helical dichroism spectroscopy, we analyze helical dichroism in wavelength domain, polarization domain, and momentum space. Our findings not only expand the methods for trace chiral molecular sensing but also provide insights into chiral light-matter interactions.