Abstract. Forensic evidentiary backlogs are indicative of the growing need for costeffective, high-throughput instrumental methods. One such emerging technology that shows high promise in meeting this demand while also allowing on-site forensic investigation is portable mass spectrometric (MS) instrumentation, particularly that which enables the coupling to ambient ionization techniques. While the benefits of rapid, on-site screening of contraband can be anticipated, the inherent legal implications of field-collected data necessitates that the analytical performance of technology employed be commensurate with accepted techniques. To this end, comprehensive analytical validation studies are required before broad incorporation by forensic practitioners can be considered, and are the focus of this work. Pertinent performance characteristics such as throughput, selectivity, accuracy/precision, method robustness, and ruggedness have been investigated. Reliability in the form of false positive/negative response rates is also assessed, examining the effect of variables such as user training and experience level. To provide flexibility toward broad chemical evidence analysis, a suite of rapidly-interchangeable ion sources has been developed and characterized through the analysis of common illicit chemicals and emerging threats like substituted phenethylamines.
The complexity of field-borne sample matrices and the instrumental constraints of portable mass spectrometers (MS) often necessitate that preparative steps are added prior to ambient MS methods when operated on-site, but the corresponding decrease in throughput and experimental simplicity can make field operation impractical. To this end, we report a modified ambient MS method, filter cone spray ionization (FCSI), specifically designed for simple, yet robust, processing of bulk forensic evidence and environmental samples using a fieldable MS system. This paper-crafted source utilizes low-cost laboratory consumables to produce a conical structure that serves as a disposable, spray-based ionization source. Integrated extraction and filtration capabilities mitigate sample heterogeneity and carryover concerns and expedite sample processing, as characterized through the analysis of a variety of authentic forensic evidence types (e.g., abused pharma tablets, counterfeit/adulterated tablets, crystal-based drugs, synthetic marijuana, toxicological specimens) and contaminated soil samples. The data presented herein suggests that the FCSI-MS design could prove robust to the rigors of field-borne, bulk sample screening, overcoming the inefficiencies of other ambient MS methods for these sample classes. Novel applications of FCSI-MS are also examined, such as the coupling to trace evidence vacuum filtration media.
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