A single nanoparticle (NP) mass spectrometry method was used to measure sublimation rates as a function of nanoparticle temperature (TNP) for a number of individual graphite and graphene NPs. Initially, the NP sublimation rates were ~400 times faster than that for bulk graphite, and there were large NP-to-NP variations. Over time, the rate slowed substantially, though remaining well above the bulk rate. The initial activation energies (Eas) were correspondingly low and doubled as a few monolayer's worth of material were sublimed from the surfaces. The high initial rates and low Eas are attributed to large numbers of edge and other low coordination sites on the NP surfaces, and the changes are attributed to atomic-scale "smoothing" of the surface by preferential sublimation of the less stable sites. The emissivity of the NPs also changed after heating, most frequently increasing. The emissivity and sublimation rates were anti-correlated, leading to the conclusion that high densities of low-coordination sites on the NP surfaces enhances sublimation but suppresses emissivity
Results are presented for thermal emission from individual trapped carbon nanoparticles (NPs) in the temperature range from ~1000 to ~2100 K. We explore the effects on the magnitude and wavelength dependence of the emissivity, ϵ(λ), of the NP size and charge, and of the type of carbon material, including graphite, graphene, diamond, carbon black, and carbon dots. In addition, it is found that heating the NPs, particularly to temperatures above ~1900 K, results in significant changes in the emission properties, attributed to changes in the distribution of surface and defect sites caused by annealing and sublimation.
Gas phase spectral measurements for CdSe/ZnS core/shell nanocrystal quantum dots (QDs) before and after heating with both infrared (CO2) and visible lasers are reported. As-trapped QDs are spectrally similar to the same QDs in solution; however their photoluminescence (PL) intensities are very low, at least partly due to low absorption cross sections. After heating, the PL intensities brighten by factors ranging from ∼4 to 1800 depending on the QD size and pump laser wavelength. The emission spectra no longer resemble solution spectra and are similar, regardless of the QD diameter. Emission extends from the pump laser wavelength into the near-IR, with strong emission features above the band gap energy, between 645 and 775 nm, and in the near-infrared. Emission spectra from brightened QD ensembles, single QD aggregates, and single QD monomers are similar, showing that even single QDs support PL from a wide variety of states. The heating and cooling processes for QDs in this environment are analyzed, providing limits on the magnitudes of the absorption cross sections before and after thermal brightening. A model, based on absorption bleaching by extra electrons in the conduction band, appears to account for the changes in absorption and emission behavior induced by charging and heating.
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