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1.
Analyst ; 146(12): 4010-4021, 2021 Jun 14.
Article in English | MEDLINE | ID: mdl-34019607

ABSTRACT

Here we show a new and significant application area for mass spectrometry imaging. The potential for fingerprints to reveal drug use has been widely reported, with potential applications in forensics and workplace drug testing. However, one unsolved issue is the inability to distinguish between drug administration and contamination by contact. Previous work using bulk mass spectrometry analysis has shown that this distinction can only be definitively made if the hands are washed prior to sample collection. Here, we illustrate how three mass spectrometry imaging approaches, desorption electrospray ionisation (DESI), matrix assisted laser desorption ionisation (MALDI) and time of flight secondary ion mass spectrometry (ToF-SIMS) can be used to visualise fingerprints at different pixel sizes, ranging from the whole fingerprint down to the pore structure. We show how each of these magnification scales can be used to distinguish between cocaine use and contact. We also demonstrate the first application of water cluster SIMS to a fingerprint sample, which was the sole method tested here that was capable of detecting excreted drug metabolites in fingerprints, while providing spatial resolution sufficient to resolve individual pore structure. We show that after administration of cocaine, lipids and salts in the fingerprint ridges spatially correlate with the cocaine metabolite, benzoylecgonine. In contrast after contact, we have observed that cocaine and its metabolite show a poor spatial correlation with the flow of the ridges.


Subject(s)
Cocaine , Lipids , Spectrometry, Mass, Matrix-Assisted Laser Desorption-Ionization , Spectrometry, Mass, Secondary Ion , Substance Abuse Detection
2.
Nanoscale ; 6(16): 9632-9, 2014 Aug 21.
Article in English | MEDLINE | ID: mdl-24990707

ABSTRACT

Electrical connectivity in networks of nanoscale junctions must be better understood if nanowire devices are to be scaled up from single wires to functional material systems. We show that the natural connectivity behaviour found in random nanowire networks presents a new paradigm for creating multi-functional, programmable materials. In devices made from networks of Ni/NiO core-shell nanowires at different length scales, we discover the emergence of distinct behavioural regimes when networks are electrically stressed. We show that a small network, with few nanowire-nanowire junctions, acts as a unipolar resistive switch, demonstrating very high ON/OFF current ratios (>10(5)). However, large networks of nanowires distribute an applied bias across a large number of junctions, and thus respond not by switching but instead by evolving connectivity. We demonstrate that these emergent properties lead to fault-tolerant materials whose resistance may be tuned, and which are capable of adaptively reconfiguring under stress. By combining these two behavioural regimes, we demonstrate that the same nanowire network may be programmed to act both as a metallic interconnect, and a resistive switch device with high ON/OFF ratio. These results enable the fabrication of programmable, multi-functional materials from random nanowire networks.

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