Thousand-Fold Enhancement of Photothermal Signals in Near-Critical CO 2 .

Photothermal (PT) microscopy has shown strong promise in imaging single absorbing nano-objects in soft matter and biological systems. PT imaging at ambient conditions usually requires a high laser power for a sensitive detection, which prevents application to light-sensitive nanoparticles. In a previous study of single gold nanoparticles, we showed that the photothermal signal can be enhanced more than 1000-fold in near-critical xenon compared to that in glycerol, a typical medium for PT detection. In this report, we show that carbon dioxide (CO 2 ), a much cheaper gas than xenon, can enhance PT signals in a similar way. We confine near-critical CO 2 in a thin capillary which easily withstands the high near-critical pressure (around 74 bar) and facilitates sample preparation. We also demonstrate enhancement of the magnetic circular dichroism signal of single magnetite nanoparticle clusters in supercritical CO 2 . We have performed COMSOL simulations to support and explain our experimental findings.