Highly sensitive sulphide mapping in live cells by kinetic spectral analysis of single Au-Ag core-shell nanoparticles

Hydrogen sulphide (H2S) is a gaseous signalling agent that has important regulatory roles in many biological systems but remains difficult to measure in living biological specimens. Here we introduce a new method for highly sensitive sulphide mapping in live cells via single-particle plasmonic spectral imaging that uses Au-Ag core-shell nanoparticles as probes. This strategy is based on Ag2S formation-induced spectral shifts of the nanoprobes, which is not only highly selective towards sulphide but also shows a linear logarithmic dependence on sulphide concentrations from 0.01 nM to 10 μM. A theoretical model was established that successfully explained the experimental observations, suggesting that the local sulphide concentration as well as its oscillations can be determined indirectly from kinetic measurements of the spectral shifts of the nanoprobes. We demonstrated for the first time the real-time mapping of local variations of sulphide levels in live cells with nM sensitivity.