Display omitted •Optically-trapped, chemically-purposed, micron-sized, single-particle reactor (SPR) in air.•Heterogeneous reaction of solid-state Hg(II) halides on the surface SPR.•A new platform for the study of surface and heterogeneous chemistry of aerosol particles in air. We created a micron-sized, single-particle reactor (SPR) freely levitated in air using optical trapping of a single particulate-bound mercury particle formed by mixing HgCl2, HgBr2, or HgBrCl (HgX2, X = Cl, Br) with single-walled carbon nanotubes. Position- and time-resolved, single-particle Raman spectra show clear evidence of reactions of solid-state HgX2 in the presence of excessive O3 under the illumination of 532-nm light. We propose a reaction mechanism: Hg(II)X2 (solid) + O → Hg(I)X + XO, XO + O → O2 + X on the surface of the SPR. This exploratory study demonstrates that the SPR is a new tool for the study the surface and heterogeneous chemistry of mercury at atmospherically relevant surfaces, e.g., aerosols.