Computer Controlled Raman Microspectroscopy (CC-Raman)

Computer-controlled Raman microspectroscopy: A method for the rapid characterization of individual atmospheric aerosol particles

Raman microspectroscopy has a great deal of promise for identifying secondary species and their mixing with primary components, as it can provide detailed information on functional groups present, morphology, and internal structure. However, as with many other detailed spectroscopic techniques, manual analysis by Raman microspectroscopy can be slow, limiting single particle statistics and the number of samples that can be analyzed. Herein, the application of computer-controlled Raman (CC-Raman) for detailed physicochemical analysis that increases throughput and minimizes user bias is described. CC-Raman applies automated mapping to increase analysis speed allowing for up to 100 particles to be analyzed in an hour. CC- Raman is applied to both laboratory and ambient samples to demonstrate its utility for the analysis of both primary and, most importantly, secondary components (sulfate, nitrate, ammonium, and organic material). Reproducibility and precision are compared to computer controlled-scanning electron microscopy (CCSEM). The greater sample throughput shows the potential for CC-Raman to improve particle statistics and advance our understanding of aerosol particle composition and mixing state, and, thus, climate-relevant properties.

Craig, R. L.G; Bondy, A. L.G; Ault, A. P.* Computer-Controlled Raman Microspectroscopy (CC-Raman): A Method for the Rapid Characterization of Individual Atmospheric Aerosol Particles, Aerosol Science & Technology, 2017, 51(9), 1099-1112. https://doi.org/10.1080/02786826.2017.1337268

(a) Optical image of laboratory generated aerosol particles composed of L-alanine, (NH4)2SO4, and NaNO3. (b) The same image now with aerosol particles to be analyzed identified by the particle area (blue), particle perimeter (green), and the center of the particle where the Raman spectrum is collected (red). (c) DCA-clustered Raman spectra of the analyzed aerosol particles, showing individual and mixed particles including: L-alanine, L-alanine/(NH4)2SO4, (NH4)2SO4, and L-alanine/(NH4)2SO4/NaNO3. Vibrational modes are shown for NaNO3 (orange), (NH4)2SO4 (yellow), and L-alanine (green). (d) Optical image with some identified particle types with four identified clusters - L-alanine particles, L-alanine/(NH4)2SO4 mixed particles, (NH4)2SO4 particles, and L-alanine/(NH4)2SO4/NaNO3 mixed particles.