Electronic Action Spectroscopy on Single Nanoparticles in the Gas Phase.

Abstract

We present electronic excitation spectra of individual nanoparticles (NPs) in the gas phase obtained by messenger-mediated single nanoparticle action spectroscopy at cryogenic temperatures (cryo-SNAS). Single ∼100 nm diameter SiO2 NPs, either colorless or dye-loaded, are trapped and coated with multiple layers of N2 in a temperature-controllable modified quadrupole ion-trap at 100 K. The NP's mass is monitored quasi-continuously and nondestructively by light scattering. Absorption of electromagnetic radiation from a tunable (400-800 nm), quasi-continuous, supercontinuum laser leads to heating of the NP and subsequent evaporation of N2 molecules. The average change in NP mass as a function of the irradiation wavelength then yields the cryo-SNAS spectrum without further correction. The obtained spectra are similar to direct absorption spectra of the corresponding NP suspensions but reveal narrower bands due to the lower NP temperature. These experiments demonstrate that cryo-SNAS allows the determination of photoabsorption spectra of single, free NPs independently of scattering processes.