Monitoring Chemical Reactions with Terahertz Rotational Spectroscopy

Published

Journal Article

© 2018 American Chemical Society. Rotational spectroscopy is introduced as a new in situ method for monitoring gas-phase reactants and products during chemical reactions. Exploiting its unambiguous molecular recognition specificity and extraordinary detection sensitivity, rotational spectroscopy at terahertz frequencies was used to monitor the decomposition of carbonyl sulfide (OCS) over an aluminum nanocrystal (AlNC) plasmonic photocatalyst. The intrinsic surface oxide on AlNCs is discovered to have a large number of strongly basic sites that are effective for mediating OCS decomposition. Spectroscopic monitoring revealed two different photothermal decomposition pathways for OCS, depending on the absence or presence of H2O. The strength of rotational spectroscopy is witnessed through its ability to detect and distinguish isotopologues of the same mass from an unlabeled OCS precursor at concentrations of <1 nanomolar or partial pressures of <10 μTorr. These attributes recommend rotational spectroscopy as a compelling alternative for monitoring gas-phase chemical reactants and products in real time.

Full Text

Cited Authors

  • Swearer, DF; Gottheim, S; Simmons, JG; Phillips, DJ; Kale, MJ; McClain, MJ; Christopher, P; Halas, NJ; Everitt, HO

Published Date

  • August 15, 2018

Published In

Volume / Issue

  • 5 / 8

Start / End Page

  • 3097 - 3106

Electronic International Standard Serial Number (EISSN)

  • 2330-4022

Digital Object Identifier (DOI)

  • 10.1021/acsphotonics.8b00342

Citation Source

  • Scopus