PMID- 34645262 OWN - NLM STAT- MEDLINE DCOM- 20211101 LR - 20211101 IS - 1520-6882 (Electronic) IS - 0003-2700 (Print) IS - 0003-2700 (Linking) VI - 93 IP - 42 DP - 2021 Oct 26 TI - Revealing Contamination and Sequence of Overlapping Fingerprints by Unsupervised Treatment of a Hyperspectral Secondary Ion Mass Spectrometry Dataset. PG - 14099-14105 LID - 10.1021/acs.analchem.1c01981 [doi] AB - Time-of-flight secondary ion mass spectrometry (ToF-SIMS) has been successfully applied for chemical imaging of overlapping fingermarks. The resulting big dataset has been treated by means of an unsupervised machine learning approach based on uniform manifold approximation and projection. The hyperspectral matrix was composed of 49 million pixels associated with 518 peaks. However, the single-pixel spectrum results in a very poor signal intensity, mostly like a barcode. Contrary to what has been reported in the literature recently, we have not applied a crude approach based on binning but a sophisticated machine learning method capable of separating the chemical signals of the two fingerprints from each other and from the substrate in which they were impressed. Moreover, using ToF-SIMS, an extremely surface-sensitive technique, the sequence of deposition of the fingerprints has been determined. FAU - Tuccitto, Nunzio AU - Tuccitto N AUID- ORCID: 0000-0003-4129-0406 AD - Consorzio per lo Sviluppo dei Sistemi a Grande Interfase, CSGI, Viale A. Doria 6, 95125 Catania, Italy. AD - Department of Chemical Sciences, Universita degli Studi di Catania, Viale A. Doria 6, 95125 Catania, Italy. FAU - Bombace, Alessandra AU - Bombace A AD - Department of Chemical Sciences, Universita degli Studi di Catania, Viale A. Doria 6, 95125 Catania, Italy. FAU - Auditore, Alessandro AU - Auditore A AD - Department of Chemical Sciences, Universita degli Studi di Catania, Viale A. Doria 6, 95125 Catania, Italy. FAU - Valenti, Andrea AU - Valenti A AUID- ORCID: 0000-0001-8645-3331 AD - Consorzio per lo Sviluppo dei Sistemi a Grande Interfase, CSGI, Viale A. Doria 6, 95125 Catania, Italy. FAU - Torrisi, Alberto AU - Torrisi A AUID- ORCID: 0000-0002-0940-7750 AD - Department of Chemical Sciences, Universita degli Studi di Catania, Viale A. Doria 6, 95125 Catania, Italy. FAU - Capizzi, Giacomo AU - Capizzi G AD - Electrical, Electronic and Computer Engineering, Universita degli Studi di Catania, Viale A. Doria 6, 95125 Catania, Italy. FAU - Licciardello, Antonino AU - Licciardello A AUID- ORCID: 0000-0001-5146-8971 AD - Consorzio per lo Sviluppo dei Sistemi a Grande Interfase, CSGI, Viale A. Doria 6, 95125 Catania, Italy. AD - Department of Chemical Sciences, Universita degli Studi di Catania, Viale A. Doria 6, 95125 Catania, Italy. LA - eng PT - Journal Article PT - Research Support, Non-U.S. Gov't DEP - 20211013 PL - United States TA - Anal Chem JT - Analytical chemistry JID - 0370536 SB - IM MH - *Machine Learning MH - *Spectrometry, Mass, Secondary Ion PMC - PMC8552212 COIS- The authors declare no competing financial interest. EDAT- 2021/10/15 06:00 MHDA- 2021/11/03 06:00 PMCR- 2021/10/28 CRDT- 2021/10/14 05:22 PHST- 2021/10/15 06:00 [pubmed] PHST- 2021/11/03 06:00 [medline] PHST- 2021/10/14 05:22 [entrez] PHST- 2021/10/28 00:00 [pmc-release] AID - 10.1021/acs.analchem.1c01981 [doi] PST - ppublish SO - Anal Chem. 2021 Oct 26;93(42):14099-14105. doi: 10.1021/acs.analchem.1c01981. Epub 2021 Oct 13.