Doctor of Philosophy (PhD)
First Advisor's Name
José R. Almirall
First Advisor's Committee Title
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Third Advisor's Name
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Fourth Advisor's Name
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Fifth Advisor's Name
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Tandem, LIBS, LA-ICP-MS, Printing Inks, Data Fusion
Date of Defense
As a consequence of the widespread use of computers coupled to high-quality printers and different types of papers, forgery, counterfeiting, change of wills, anonymous letter writing and felonious use of the documents have become serious problems. Forensic analysts are always seeking methods that can provide reliable information on whether a specimen collected at the crime scene is linked to the crime or to a source of known origin. Sensitive methods that can provide more detailed characterization of natural or man-made materials or even provide information not previously available to forensic examiners.
Recent advances in rapid solid sampling of materials using laser ablation (LA) coupled to inductively coupled plasma mass spectroscopy (ICP-MS) have led to this analytical method to be regarded as the “gold standard” in the field of elemental analysis for trace level components in solids. Another, emerging, analytical technique that uses the same laser pulse to generate a plasma that can be interrogated with spectroscopy is laser induced break down spectroscopy (LIBS).
The analysis of ink and paper is also possible because of the surface removal effect of laser interactions with the samples. In the present study, printing inks were analyzed using LIBS, LA-ICP-MS and both of them in tandem mode. In the tandem setup, the light generated during the relaxation of the excited species (LIBS) was used to create a spectral signature of the elements, and the mass-to-charge ratio of the ejected particles (ICP-MS) was used to create a mass spectrum.
For a set of 319 printing ink samples, LA-ICP-MS alone provided discrimination greater than 99%. A subset of 43 printing inks, having a very similar elemental profile, was analyzed by tandem LIBS/LA-ICP-MS. The fusion of LIBS and LA-ICP-MS provided additional discrimination through the detection of elements like Ca, Si, Fe, and K by LIBS, that are difficult to detect and confirm using standalone ICP-MS because of the spectral interferences (isobaric and polyatomic) involved. The combination of these two sensors was found to minimize the individual limitations and provide a more complete and representative chemical characterization of printing inks.
Subedi, Kiran, "Elemental Analysis of Printing Inks Using Tandem Laser- Induced Breakdown Spectroscopy and Laser Ablation Inductively Coupled Plasma Mass Spectrometry" (2015). FIU Electronic Theses and Dissertations. 2263.
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