Mass Spectrometric Fingerprinting of Tank Waste Using Tunable, Ultrafast Infrared Lasers

The principal scientific thrust of this project was to demonstrate a novel method for precision matrix-assisted laser desorption-ionization (MALDI) mass spectrometry (MS) of model tank-waste materials using, using the sodium nitrate component of the tank waste both as the matrix and as an internal calibration standard. Conventional nanosecond and femtosecond single-frequency lasers and a tunable, mid-infrared free-electron laser were used in the development of the MS protocols and in measurements of the MALDI dynamics. In addition to developing a model of the processes which lead to efficient desorption and ionization of organic molecules (e.g., toluene, benzene, chelators, various organic acids, crown ethers) from sodium nitrate, we developed protocols for quantitative analysis based on the use of the sodium nitrate in tank waste as an internal standard. Comparisons of MALDI-MS using nanosecond and picosecond lasers, and of infrared and ultraviolet lasers, have been especially instructive, and demonstrate the superior potential of IR-MALDI for this purpose, as well as for a number of related analytical and thin-film applications