Abstract
Matrix-assisted laser desorption/ionization (MALDI), mass spectrometry profiling (MSP), and mass spectrometry imaging (MSI) are continuously pushing the boundaries of many applications in which they can be employed. In the field of forensic science, MALDI MS has proven to be a useful technique but reports were sporadic and only in an academic context until 2009. However, in the past 6 years it has been demonstrated that MALDI MSP and MSI can be practically implemented as an analytical forensic tool in the context of fingermark/fingerprint analysis. Previously always regarded ‘simply’ as physical evidence, fingermarks are an invaluable source of chemical information that can be exploited to provide intelligence on an individual’s lifestyle and activities taking place prior to the crime. A solid proof of principle of the versatility and robustness of MALDI MSP and MSI has gained MALDI a place in the newly launched Fingermark Visualisation Manual edited by the Home Office of the United Kingdom (UK), whose guidelines are followed in the UK and are highly regarded worldwide. Protocols are currently being developed to be used operationally within primarily UK law enforcement. In this chapter, a practical overview is given for informed method development. Protocols that have been successful in answering specific research questions will also be outlined along with the most significant and interesting applications of MALDI MSP and MSI in fingermark/fingerprint analysis.
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Notes
- 1.
Fingerprints are obtained intentionally, for instance at police stations or airports, while fingermarks are a result of accidental and involuntary contact with surfaces (more details below).
- 2.
In fingerprints, ridges are the ‘lines’ generated by the raised parts of the skin on fingertips.
- 3.
In a forensic context ‘fingerprinting’ refers to the process of identifying an individual through their fingerprints. This is different from ‘fingerprinting’ used in proteomics where this term refers to the identification of a protein usually through a bottom-up approach.
- 4.
Crime Scene Investigator.
- 5.
The most used definition of latent fingermark is ‘a fingermark invisible to the naked eye.’
- 6.
Blood may be present on the surface prior to the deposition of the fingermark (mark in blood) or landing some time after the fingermark deposition (coincidental association), or coming from the fingertip of the owner of the mark (blood mark).
- 7.
MALDI is reported as a new process having high potential to be implemented in the forensic practice (Cat C) but still under development to reach the required maturity (TLR 3–4).
- 8.
In fingerprints/fingermarks, furrows, otherwise termed valleys, are the ‘voids’ in between ridges and are generated by the lower parts of the skin on fingertips.
- 9.
Ungroomed fingermarks are ‘lipid-depleted’ marks from fingers that have been washed and have subsequently not touched any body parts or contaminants (to test the sensitivity of the technology). For a more comprehensive description, see Sect. 3.1.
- 10.
Common protocols include the use of soap and plenty of water or a 50/50 solution of ethanol/water.
- 11.
Grooming fingertips by touching the face is also viable, though one needs to be aware of possible contamination deriving from make-up or moisturizers, which may cause ion suppression.
- 12.
Previously cleaned with a 50/50 solution of ethanol/water.
- 13.
Saturated, mono- and polyunsaturated.
- 14.
Fingertip smears are specimens that do not allow a linkage to the biometric data of the individual. Like fingermarks, it is possible to obtain eccrine, groomed, ungroomed, and natural smears by preparing the fingertips as previously described for fingermarks and pressing the fingertip on a surface sliding it to the side.
- 15.
This includes optimization of the instrumental settings.
- 16.
The dry–wet method employing curcumin has not been trialed on other classes of molecules.
- 17.
Protein-producing apocrine glands are rarely a source of proteins in fingermarks.
- 18.
The protocol (instrumental conditions) for the detection, the mapping, and the MS/MS of heme can be retrieved in (Bradshaw et al. 2014).
- 19.
Note that another limiting factor can be the bin size of the imaging software used (e.g., BioMap; http://www.maldi-msi.org/index.php?option=com_content&view=article&id=14&Itemid=32). Even if the data were acquired in high resolution, software often cannot cope with a narrow bin sizes, thus generating (depending on the decimal places) the same uncertainties in discriminating between two species with the same nominal mass.
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Acknowledgements
My previous students Robert Bradshaw and Leesa Ferguson (now PhDs) and my current Ph.D. student Ekta Patel are gratefully acknowledged for the very hard work put into these pioneering studies and for sharing a huge enthusiasm towards this research. The Home Office and Dr. Steve Bleay are thanked for both intellectual and financial support to this research. Mr. Neil Denison is gratefully acknowledged together with West Yorkshire Police for the huge support in developing the technology in the field. The Biomedical Research Centre at Sheffield Hallam University is heartily thanked for supporting and believing in this emerging research area.
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Francese, S. (2016). Techniques for Fingermark Analysis Using MALDI MS: A Practical Overview. In: Cramer, R. (eds) Advances in MALDI and Laser-Induced Soft Ionization Mass Spectrometry. Springer, Cham. https://doi.org/10.1007/978-3-319-04819-2_6
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DOI: https://doi.org/10.1007/978-3-319-04819-2_6
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