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Biologically important molecules span a size range from very largebiomacromolecules, such as proteins to small metabolite molecules.Consequently, spectroscopic techniques which can detect and characterize thestructure of inherently chiral biomolecules over this range of scale at thefemtomole level are necessary to develop novel biosensing and diagnostictechnologies. Nanophotonic platforms uniquely enable chirally sensitivestructural characterisation of biomacromolecules at this ultrasensitive level.However, they are less successful at achieving the same level of sensitivityfor small chiral molecules, with less than nanomole typical. This poorerperformance can be attributed to the optical response of the platform beingsensitive to a much larger volume of the near field than is occupied by thesmall molecule. Here we show that by combining chiral plasmonic metasurfaceswith Raman reporters, which can detect changes in electromagnetic environmentat molecular dimensions, chiral discrimination can be achieved for attomolequantities of a small molecule, the amino acid cysteine. The signal-to-noise,and hence ultimate sensitivity, of the measurement can be further improved bycombining the metasurfaces with gold achiral nanoparticles. This indirectenantiomeric detection is 9 orders of magnitude more sensitive than strategiesrelying on monitoring the Raman response of target chiral molecules directly.Given the generic nature of the phenomenon,this study provides a framework fordeveloping novel technologies for detecting a broad spectrum of smallbiomolecules, which would be useful tools in the field of metabolomics.

Attomole enantiomeric discrimination of small molecules using an achiral SERS reporter and chiral plasmonics