Mechanistic insight into the fluorescence activity of forensic fingerprinting reagents.
Journal article
Hunnisett, L., Kelly, P F, Bleay, S., Plasser, F., King, R, McMurchie, B. and Goddard, P. (2021). Mechanistic insight into the fluorescence activity of forensic fingerprinting reagents. The Journal of Chemical Physics. 154 (12), p. 124313. https://doi.org/10.1063/5.0040555
| Authors | Hunnisett, L., Kelly, P F, Bleay, S., Plasser, F., King, R, McMurchie, B. and Goddard, P. |
|---|---|
| Abstract | Fingerprint detection is still the primary investigative technique for deciphering criminal inquiries and identifying individuals. The main forensic fingerprinting reagents (FFRs) currently in use can require multiple treatment steps to produce fingerprints of sufficient quality. Therefore, the development of new, more effective FFRs that require minimal chemical treatment is of great interest in forensic chemistry. In this work, prudently crafted density functional theory and time-dependent density functional theory calculations are utilized to derive mechanistic insight into the optical activity of the non-fluorescent product of ninhydrin, diketohydrindylidenediketohydrindamine (DYDA), and fluorescent product of DFO (1,8-diazafluoren-9-one). We investigate various protonation sites to gain an understanding of isomeric preference in the solid-state material. A relaxed scan of a single torsion angle rotation in the S minimized geometry of the O-protonated DYDA isomer suggests a conical intersection upon ∼10° rotation. We show that the absence of a rigid hydrogen-bonded network in the crystal structure of DYDA supports the hypothesis of torsion rotation, which leads de-excitation to occur readily. Conversely, for the fluorescent DFO product, our calculations support an avoided crossing suggestive of a non-radiative mechanism when the torsion angle is rotated by about ∼100°. This mechanistic insight concurs with experimental observations of fluorescence activity in DFO and may aid the photophysical understanding of poorly visualized fingerprints due to weak fluorescence. We show that identifying suggestive avoided crossings via the method described here can be used to initialize thoughts toward the computational design of FFRs. |
| Year | 2021 |
| Journal | The Journal of Chemical Physics |
| Journal citation | 154 (12), p. 124313 |
| Publisher | AIP |
| ISSN | 1089-7690 |
| Digital Object Identifier (DOI) | https://doi.org/10.1063/5.0040555 |
| Publication dates | |
| Online | 31 Mar 2021 |
| Publication process dates | |
| Accepted | 01 Mar 2021 |
| Deposited | 30 Apr 2021 |
| Accepted author manuscript | License File Access Level Open |
| Additional information | This article may be downloaded for personal use only. Any other use requires prior permission of the author and AIP Publishing. This article appeared in Journal of Chemical Physics and may be found at https://aip.scitation.org/doi/10.1063/5.0040555 |
Permalink -
https://openresearch.lsbu.ac.uk/item/8w8yy
Download files
122
total views179
total downloads1
views this month1
downloads this month
Export as
Related outputs
Chemistry of Fingerprint Residue
Frick, A. A., Spindler, X and Bleay, S. M. (2023). Chemistry of Fingerprint Residue. in: Encyclopedia of Forensic Sciences, Third Edition, vol. 1 Elsevier. pp. pp. 521–529
Comparison of three active 1,2-indanedione-zinc formulations for fingermark detection in the context of limited resources and supply chain risks in Seychelles
Bouzin, J .T., Horrocks, A.J., Sauzier, G., Bleay, S. and Lewis, S. (2022). Comparison of three active 1,2-indanedione-zinc formulations for fingermark detection in the context of limited resources and supply chain risks in Seychelles. Forensic Chemistry. 30, p. 100439. https://doi.org/10.1016/j.forc.2022.100439Dynamics and mechanism of the physical developer process for visualization of latent fingerprints on paper.
Coulston, J.L., Sears, V., Bleay, S. and Hillman, A. R. (2022). Dynamics and mechanism of the physical developer process for visualization of latent fingerprints on paper. Forensic Science International. 333, p. 111195. https://doi.org/10.1016/j.forsciint.2022.111195Replacing Synperonic® N in the physical developer fingermark visualisation process: Pseudo-operational trial and parameter studies.
Cartledge, E.M., Guo, Z.Y., Bleay, S.M., Sears, V.G. and Hussey, L.J. (2021). Replacing Synperonic® N in the physical developer fingermark visualisation process: Pseudo-operational trial and parameter studies. Forensic Science International. 326, p. 110916. https://doi.org/S0379-0738(21)00236-XThe effect of corrosive substances on fingermark recovery: a pilot study
Bleay, S. and Masterson, A. (2021). The effect of corrosive substances on fingermark recovery: a pilot study. Science & Justice. 61 (5). https://doi.org/10.1016/j.scijus.2021.07.004New light on old fingermarks: The detection of historic latent fingermarks on old paper documents using 1,2-indanedione/zinc
Bouzin, J., Merendino, J., Bleay, S., Sauzier, G. and Lewis, S. (2020). New light on old fingermarks: The detection of historic latent fingermarks on old paper documents using 1,2-indanedione/zinc. Forensic Science International: Reports. 2, p. 100145. https://doi.org/10.1016/j.fsir.2020.100145The forensic exploitation of fingermark chemistry: a review
Bleay, S., Bailey, M., Croxton, R. and Francese, S. (2020). The forensic exploitation of fingermark chemistry: a review. WIRes Forensic Science. https://doi.org/10.1002/wfs2.1403The visualisation on Pangolin scales using gelatine lifters
Smith, P A, Moorat, G, Reed, J A, Bleay, S, Amaral, M P, Chappell, B, Pamment, N and Plowman, C (2020). The visualisation on Pangolin scales using gelatine lifters. Forensic Science International. 313. https://doi.org/10.1016/j.forsciint.2020.110221Commentary for Chapter 1: Mass Spectrometry Methods for the Recovery of Forensic Intelligence from Fingermarks
Bleay, S (2020). Commentary for Chapter 1: Mass Spectrometry Methods for the Recovery of Forensic Intelligence from Fingermarks. in: Francese, S (ed.) Emerging Technologies for the Analysis of Forensic Traces Springer.Fingerprinting: the UK landscape: processes, stakeholders, and interactions
Earwaker, H C, Charlton, D and Bleay, S (2015). Fingerprinting: the UK landscape: processes, stakeholders, and interactions. Horsham, West Sussex Knowledge Transfer Network.Home Office Fingerprint Source Book
Bandey, H, Bleay, S, Bowman, V, Downham, R, Sears, V, Gibson, A, Selway, C, Ramadani, J and Ciuksza, T (2018). Home Office Fingerprint Source Book. London Home Office.Introduction: Fingerprint Development Techniques: Theory and Application
Bleay, SM, Croxton, RS and De Puit, M (2018). Introduction: Fingerprint Development Techniques: Theory and Application. in: Fingerprint Development Techniques: Theory and Application Chichester Wiley. pp. 1-500The effect of DNA recovery on the subsequent quality of latent fingermarks: a pseudo-operational trial
Fieldhouse, S., Parsons, R., Bleay, S. and Walton-Williams, L. (2019). The effect of DNA recovery on the subsequent quality of latent fingermarks: a pseudo-operational trial. Forensic Science International. 307, p. 110076. https://doi.org/10.1016/j.forsciint.2019.110076An evaluation of the effect of incorporating metal salts into 1,8 diazafluoren-9-one (DFO) formulations for fingermark enhancement
Mayse, K, Sears, VG, Nicolasora, N and Bleay, S (2019). An evaluation of the effect of incorporating metal salts into 1,8 diazafluoren-9-one (DFO) formulations for fingermark enhancement. Science and Justice. 59 (3), pp. 349-358. https://doi.org/10.1016/j.scijus.2019.01.002A comparative evaluation of the disulfur dinitride process for the visualisation of fingermarks on metal surfaces
Bleay, S, Kelly, P, King, R and Thorngate, S (2019). A comparative evaluation of the disulfur dinitride process for the visualisation of fingermarks on metal surfaces. Science and Justice. 59 (6), pp. 606-621. https://doi.org/10.1016/j.scijus.2019.06.011Assessing phosphomolybdic acid as a fingermark enhancement reagent
Davis, LWL, Bleay, SM and Kelly, PF (2018). Assessing phosphomolybdic acid as a fingermark enhancement reagent. Journal of Forensic Identification. 68 (2), pp. 257-280.Fingermark visualisation on metal surfaces: An initial investigation of the influence of surface condition on process effectiveness
Pitera, M., Sears, V.G, Bleay, S.M and Park, S. (2018). Fingermark visualisation on metal surfaces: An initial investigation of the influence of surface condition on process effectiveness. Science and Justice. 58 (5), pp. 372-383. https://doi.org/10.1016/j.scijus.2018.05.005Visualising the past – An evaluation of processes and sequences for fingermark recovery from old documents
Bleay, S, Fitzgerald, L, Sears, V and Kent, T (2018). Visualising the past – An evaluation of processes and sequences for fingermark recovery from old documents. Science and Justice. 59 (2), pp. 125-137. https://doi.org/10.1016/j.scijus.2018.10.005