Abstract
This thesis investigates the possibility of using ambient ionisation and surface mass spectrometry for the detection and quantification of drugs of abuse in latent fingerprints. The use of fingerprints for drug testing in lieu of blood, oral fluid or urine reduces the biological hazard associated with these types of samples. The sample collection procedure is non-invasive, can be monitored to prevent cheating (submitting samples from a drug free individual) and the identity of the donor is embedded in the fingerprint ridge detail. In this thesis, three techniques – desorption electrospray ionisation (DESI), liquid extraction surface analysis (LESA) and paper spray mass spectrometry, were evaluated for their ability to provide a rapid drug test from a fingerprint. Paper spray-mass spectrometry was chosen for further development due to the ease of set-up, rapid nature of the analysis and potential to provide quantitative results. The final optimised method included full scan mass spectrometry measurements (quantitative) followed by tandem mass spectrometry (MS/MS) scans (qualitative) for the detection of cocaine, benzoylecgonine (BZE) and ecgonine methyl ester (EME). Limits of detection (LOD) were calculated to be 1 ng/mL, 2 ng/mL and 31 ng/mL for cocaine, BZE and EME, respectively. Using the optimised method of analysis, 159 individual fingerprint samples (collected from individuals seeking treatment for substance abuse) were analysed with a 99% true positive rate through the detection of either cocaine, BZE or EME. The detection of these substances was corroborated by a positive oral fluid result from samples collected from the same individuals. Analysis of fingerprint samples collected from the non-drug users (n=80) indicated <2.5% false positive rate. The significance of detecting the parent drug or metabolite in fingerprint samples was determined through the analysis of samples after contact with seized cocaine from Forensic Science Ireland. Cocaine, BZE and EME were found in fingerprints produced by contact, showing that the presence of a cocaine metabolite in a fingerprint is not enough to show that a suspect has taken a drug. Furthermore, secondary transfer scenarios showed that cocaine could be transferred through handshakes. None of the hand cleaning methods employed in this research were sufficient to remove all traces of cocaine from contact residues. iii Finally, the possibility of visualising the fingerprint ridge detail prior to analysis was tested and the presence of the analytes was qualitatively confirmed in fingerprint samples after application of silver nitrate. This is an important step that allows for sample traceability, whilst still providing high throughput analysis and sensitivity.