Direct detection of blood in fingermarks by MALDI MS profiling and Imaging

The determination of the presence of blood in fingermarks constitutes important intelligence in a criminal investigation as it helps to reconstruct the events that have taken place at a scene of crime. Various methodologies have been reported and are currently employed for the detection of the presence of blood including optical, spectroscopic and chemical development approaches. However, most methods only give an indication that blood may be present and, therefore, these methods are described as presumptive tests.Here we show the use of Matrix-Assisted Laser Desorption Ionisation Mass Spectrometry Profiling and Imaging (MALDI MSP and MALDI MSI) for the determination of the presence of blood in fingermarks by specifically detecting the molecules of haem and haemoglobin through their mass-to-charge ratios. Furthermore, preliminary experiments are shown which demonstrate that this technology is compatible with other methods currently employed for enhancing fingermarks in blood (or contaminated by blood). The application of the developed protocols to a crime scene blood trace, demonstrates the feasibility of using this technology in routine casework. These findings open up a new line of research for the development of robust MALDI MSP and MALDI MSI protocols for the detection and chemical imaging of bloodied marks.     

Application of 3D Imaging Technology to Latent Fingermark Aging Studies

In most latent fingermark aging studies, two‐dimensional (2D) features are obtained from photo images, scans, or inked impressions. However, some relevant information is possibly being missed because fingermarks are three‐dimensional (3D) objects that age in all three dimensions. A feature that has not been carefully examined is how the height of ridges changes over time. In this report, a 3D imaging technology—called optical profilometry—is introduced as a tool for the visual examination of the aging process. Optical profilometry is a nondestructive technology that allows the visualization and data acquisition of unprocessed latent fingermarks. Detailed ridge images and spatiotemporal data were successively obtained on the x‐, y‐ and z‐axis, delivering 3D topographical information. OP was able to detect the loss of ridge heights over time. The feasibility of employing this technology to collect data on the aging process of ridges has been proven.     

Fixing Transient Iodine on Developed Latent Fingermarks

In the present study, a simple and novel fume–mist technique is described which can be used efficiently to fix the latent fingermarks developed using iodine. It is well known that the residues left over in the fingermarks interact with iodine to give transient brown impressions which disappear in a short time. Also, iodine forms colored complexes with various organic solvents. Based on iodine–fingermark interaction and iodine–solvent complex formation, latent fingermarks were developed on paper surface using iodine fumes which were subsequently fixed by spraying polar and nonpolar solvents. The fingermarks developed with this technique were not only clear but also permanent in nature. The interaction of fingermark residue, iodine, and solvent forming a ternary structure is believed to be a possible reason for the stability of iodine‐developed fingermarks. Ease of method, availability of chemicals, and minimum training make the method adaptable in routine development of forensic fingermarks present on paper surface.     

The detection and enhancement of latent fingermarks using infrared chemical imaging

The use of a new technique, Fourier transform infrared (FTIR) chemical imaging, has been demonstrated for the enhancement of latent fingermarks on a number of surfaces. Images of untreated fingermarks on glass backgrounds with excellent ridge detail were acquired using infrared chemical imaging. High quality fingermarks on glass backgrounds were also developed using ethyl cyanoacrylate (super glue) fuming and subsequent infrared chemical imaging. This new method allows the collection of images from backgrounds that traditionally pose problems for current fingermark detection methods. The background may, for example, be highly colored, have a complex pattern, or possess other pattern or image characteristics that make it difficult to separate fingermark ridges using traditional optical or luminescent visualization. One background that has proven to be a challenging surface for the development of latent fingermarks is the Australian polymer banknote. To demonstrate the power and applicability of infrared chemical imaging, fingermarks fumed with ethyl cyanoacrylate were successfully imaged from Australian polymer banknotes.     

Can latent fingerprint disclose the sex of the donor? A preliminary test study using GC–MS analysis of latent fingerprints

While fingerprints are a highly used means of identification, not every fingerprint left behind on a potential crime scene can be used for identification purposes. In some cases, the fingerprint may be smudged, partially preserved or overlapping with other prints hence distorting the ridge pattern and may therefore be not appropriate for identification. Further, fingermark residue yields a very low abundance of genetic material for DNA analysis. In such cases, the fingermark may be used to retrieve basic donor information such as sex. The focus of this paper was to assess the possibility of differentiating between the sexes of the donor of latent fingermarks. Analytical method was GC–MS analysis of the chemical compounds of latent fingermarks using 22 male and 22 female donors. Results showed 44 identified compounds. Two alcohols, octadecanol C₁₈ and eicosanol C₂₀, were found to show a difference that was statistically significant between male and female donors. There is also some evidence for the possibility of distinguishing sex of the fingermark donor based on the distribution of branched chain fatty acids, as free compounds or esterified in wax esters.     

Development of Latent Fingermarks on Various Surfaces Using ZnO‐SiO2 Nanopowder

Fingermarks are one of the most useful forms of evidence in identification and can provide generalized proof of identity in crime investigation. They are developed using various conventional powders. The novel nanopowder ZnO‐SiO₂ was synthesized via the conventional heating method and characterized by Fourier transform infrared spectroscopy (FTIR), scanning electron microscope (SEM), energy‐dispersive X‐ray (EDX) analysis, transmission electron microscope (TEM), and X‐ray diffraction (XRD). The mean particle size of ZnO‐SiO₂ nanopowder calculated through TEM was 32.9 nm. The development of fingermarks was carried out by powder dusting and small particle reagent (SPR) methods. Powder dusting method was used for the development of latent fingermarks on various dry, nonporous, and semi‐porous surfaces. The SPR method was also applied to wet nonporous surface. The developed latent fingermarks using ZnO‐SiO₂ nanopowder were found to have excellent quality with very clear third‐level ridges detail and had better visibility than commercially available white powder.     

ZnS和ZnS:Cu无机紫外荧光材料的制备及其在汗潜手印显现中的应用

目的制备荧光强度高、客体适用性广、显现效果优良且合成方法简单的ZnS及ZnS:Cu无机紫外荧光材料,并将其用于汗潜手印的显现。方法通过一步溶液反应共沉淀法制备ZnS无机紫外荧光材料,并在ZnS材料中加入Cu^2+得到ZnS:Cu以改善荧光性质,将其应用于普通客体(白色捺印纸、载玻片、铁架台、乳白色花纹瓷砖表面、磨砂化学实验台面、不锈钢表面)和复杂客体(拼色花纹瓷砖、农夫山泉塑料标签和杂志封面铜版纸)上汗潜手印的显现,并与传统荧光粉末显现效果进行对比。结果ZnS材料具有荧光性,并且在ZnS材料中掺杂Cu^2+后得到的ZnS:Cu材料荧光强度增强,荧光光谱范围变广,稳定性提升。显现汗潜手印时,适用客体范围更广,并且可通过调节激发光的波长呈现不同的显现效果。结论通过在无机荧光材料ZnS中掺杂Cu^2+可改善材料的荧光范围,从而得到适用于不同客体上汗潜手印显现且效果更好的ZnS:Cu无机紫外荧光材料。     

Visualization of Fingermarks Deposits on Untreated Thermal Paper Exploiting the Near Infrared Luminescence

Thermal paper is widely used as a print medium for different applications but it constitutes a tricky substrate for fingermark visualization. An earlier work (J Forensic Sci 2015; 60 :1034) reported how to visualize fingermarks on untreated thermal paper by illuminating the item with a UV-A light source. In the present paper, the potential of the near infrared (NIR) luminescence has been tested on thermal paper compared to the mentioned method. A controlled study was carried out utilizing eccrine enriched fingermarks. The promising outcomes obtained were further confirmed by performing a pseudo-operational trial. Data clearly showed that the use of the NIR filter gave better results. Finally, preliminary tests suggested a different mechanism of reaction induced by fingermarks with respect to the one behind the thermal printing. Thus, NIR luminescence represents a refinement to the suite of optical examination processes, including the potential to increase the number of marks recovered in a noncontact, nondestructive way.     

Enhanced Visualization of Latent Fingermarks on Rough Aluminum Surfaces Using Sequential Au and Zn/ZnS/ZnO Depositions

Detection and visualization of fingermarks on rough and diffuse surfaces is a relatively challenging task. We succeeded in developing latent fingermarks on scratched and rough aluminum surfaces by sequential deposition of a thin layer of gold followed by one of zinc or zinc‐based compounds on the fingermarks. The best image enhancement was achieved with sequential Au and ZnS depositions. Using this combination, we could enhance the visualization of latent fingermarks aged over 65 days in normal conditions. The optical reflectance from the fingermarks with the deposited layers of metal/dielectric is analyzed as a stratified medium. Significant contrast in the reflectance from the regions of the ridges and the valleys of the fingermark would enhance the visualization. Our results show that the Au and ZnS bi‐layer combination can have a large reflection contrast and improved fingermark visualization at wavelengths corresponding to the green light for specific thickness of ZnS.     

Fluorescence spectra and images of latent fingerprints excited with a tunable laser in the ultraviolet region

Fluorescence spectra of sebum-rich latent fingerprints were studied with a tunable laser for non-destructive fingerprint detection without chemical treatment. The tunable laser consists of a nanosecond pulsed Nd-YAG laser and an optical parametric oscillator (OPO) crystal. The fluorescence spectra and images were measured at various excitation wavelengths in the ultraviolet region by the time-resolved fluorescence method. We have previously reported that a typical fluorescence spectrum of fingerprints consists of two peaks located at c. 330 and 440 nm. In order to determine the wavelength of optimal excitation, excitation spectra were measured at wavelengths ranging from 220 to 310 nm. The fluorescence intensity of the 330 nm peak became maximal with excitation at 280 nm. The images of latent fingerprints on white papers were also measured and the clearest image was obtained with excitation at 280 nm. The influence of continuous irradiation on the fluorescence of fingerprints was measured at the optimal excitation wavelengths. The 330 nm peak was strong at first and decreased with continuous irradiation, whereas the 440 nm peak, which was weak at first, increased gradually.     

Recovery of DNA from Latent Fingerprint Tape Lifts Archived Against Matte Acetate

This study was driven by court order to examine methods to remove, extract, and STR‐type potential DNA entrapped between latent fingerprint lifting tape and matte acetate that was collected from a 1977 crime scene. Results indicate that recovery of appreciable quantities of DNA is more challenging once adhesive is attached to matte acetate cards and even more difficult when fixed following black powder enhancement. STR amplification of extracts from entrapped fingermarks collected following the dusting/lifting procedure did not produce robust profiles, and extraneous peaks not expressed by print donors were detected for some samples. A hearing was set to argue whether there was DNA remaining to be tested, and if so, whether that DNA could be exculpatory in this postconviction matter. The studies herein provided the basis for the court's decision to not require the testing.     

An efficient strategy to detect latent fingermarks on metallic surfaces

The aim of this work is to use metal sputtering for the development of latent fingermarks on metallic surfaces by taking advantage of the prints' topography. In order to promote the preferential deposition onto fingerprints' ridges the deposition parameters should be optimized. After a previous selection, copper and gold thin films were deposited by magnetron sputtering onto stainless steel substrates where fingermarks were intentionally placed. After optimizing the deposition parameters, the influence of the fingermarks' age was studied. The quality of the developed fingermarks was evaluated visually and through optical and scanning electron microscopy. The morphology of the copper and gold thin films was examined by high resolution scanning electron microscopy. The preferential magnetron sputtering deposition of copper and gold thin films, 20-30 nm thick, allows latent fingermarks to be successfully developed. The gold films are more promising, especially for detecting non-fresh fingermarks and for conserving the developed marks. It was possible to detect the contours of the ridges and localize minutiae features in a one-month aged impression developed by gold deposition. These films present discontinuous surface and columnar cross-sections, while copper thin films have a featureless morphology.     

Studies into exfoliation and coating of Egyptian blue in methanol for application to the detection of latent fingermarks

We have recently demonstrated that coated exfoliated Egyptian blue powder is effective for detecting latent fingermarks on a range of highly-patterned non-porous and semi-porous surfaces. In this extension of that work, we present our studies into an alternative approach to prepare exfoliated Egyptian blue coated with cetrimonium bromide and Tween® 20 using a simpler technique. The quality of the latent fingermarks developed with these exfoliated powders and the commercial powder were compared in a comprehensive study. Depletion series of natural fingermarks from a wide range of donors (12 males and females) deposited on non-porous (glass slides) and semi-porous (Australian banknotes) surfaces were used in this study. Enhancement in the performance of the coated exfoliated particles compared to the commercial powder was observed, particularly in the case of aged fingermarks and polymer banknotes as challenging substrates.     

Preparation of Artificial Blood from the Extract of Legume Root Nodules,and the Creation of Artificial Latent Fingermarks in Blood Using Artificial Blood,

Distribution of homogeneous fingermarks in blood is essential for conducting proficiency tests in forensic science. Hence, the artificial blood was prepared using the root nodule extract of Glycine max plants. The reactivity of the artificial blood with widely used human blood detection reagents was tested. Artificial latent fingermarks in blood were printed using an inkjet cartridge case filled with artificial blood solution. The artificial latent fingermarks in blood were developed with amino acid‐sensitive reagents and could obtain development as prominent as the image of the master fingermark saved on the computer. Therefore, it has been confirmed that the extract of legume root nodules can be used as artificial blood, and the artificial blood can be used for the preparation of artificial latent fingermarks or footmarks in blood.     

Exposing latent fingermarks on problematic metal surfaces using time of flight secondary ion mass spectroscopy

Fingermarks are a key form of physical evidence for identifying persons of interest and linking them to the scene of a crime. Visualising latent (hidden) fingermarks can be difficult and the correct choice of techniques is essential to develop and preserve any fingermarks or other (e.g. DNA) evidence that might be present. Metal surfaces (stainless steel in particular) have proven to be challenging substrates from which to reliably obtain fingermarks. This is a great cause for concern among police forces around the globe as many of the firearms, knives and other metal weapons used in violent crime are potentially valuable sources of fingermark evidence. In this study, a highly sensitive and non-destructive surface science technique called time of flight secondary ion mass spectroscopy (ToF-SIMS) was used to image fingermarks on metal surfaces. This technique was compared to a conventional superglue based fuming technique that was accompanied by a series of contrast enhancing dyes (basic yellow 40 (BY40), crystal violet (CV) and sudan black (SB)) on three different metal surfaces. The conventional techniques showed little to no evidence of fingermarks being present on the metal surfaces after a few days. However, ToF-SIMS revealed fingermarks on the same and similar substrates with an exceptional level of detail. The ToF-SIMS images demonstrated clear ridge definition as well as detail about sweat pore position and shape. All structures were found to persist for over 26?days after deposition when the samples were stored under ambient conditions.     

Preliminary efficiency evaluation of development methods applied to aged sebaceous latent fingermarks

Latent fingermarks are important trace evidence found in crime scenes mainly used for identification purposes. Once deposited, the composition of samples changes over time influencing the efficacy of latent fingermark development methods. In this sense, the aims of this work were to characterize the fatty acid (FA) profile of sebaceous latent fingermarks by GC–FID and to preliminarily evaluate the development efficiency of enhancement methods (powder dusting, iodine fuming and silver nitrate method) in a 30-day period of aging under controlled parameters of temperature, photoperiod and humidity. Results showed that myristic (7.51 ± 0.76% − 13.39 ± 1.26%), palmitic (35.91 ± 1.07% − 40.81 ± 2.52%), stearic (6.67 ± 0.36% − 9.13 ± 0.36%) and oleic (18.08 ± 0.25% − 20.93 ± 0.26%) acid varied significantly (p < 0.05) over the 30-day period of analysis. Regarding development efficiency, fluorescent orange powder and the silver nitrate method also increased their efficacy to develop latent fingermarks over time while the iodine fuming method decreased its efficiency. Silver black powder had constant efficacy in the tested period. Changes in the constitution of sebaceous marks possibly influenced the development efficiency of enhancement techniques. This knowledge is important to better understand the kinetic of aging and its influence on the development method.     

Novel O‐propyl,S‐propyl,and N‐propyl substituted 1,4‐naphthoquinones and 1,4‐anthraquinones as potential fingermark development reagents for porous surfaces

Lawsone is a 2‐substituted‐1,4‐naphthoquinone derivative, which has been proposed as an alternative to the reagents currently used for fingermark detection on porous surfaces. 2‐substituted‐anthraquinones, which contain an additional conjugated benzene ring, have a similar chemical structure to that of lawsone. In this study, a new series of 2‐substituted‐1,4‐naphthoquinones and 2‐substituted‐1,4‐anthraquinones were synthesized and completely characterized by¹H NMR,¹³C NMR, IR, and HPLC‐TOF/MS analyses. All newly synthesized 2‐substituted‐1,4‐quinones were investigated for their ability to develop latent fingermarks on porous surfaces, and this ability was compared with that of lawsone. Each fingermark developed was graded using an established method; thus, quantitative data were attributed to each fingermark. It has been demonstrated that the 1,4 ‐ quinones react with amino acids present in latent fingermarks on selected paper surfaces to produce faint yellow‐orange impressions, which exhibit strong photoluminescence when illuminated with a forensic light source at 440 nm and observed through a red filter. None of the compounds caused background darkening. The results obtained were generally similar to those of lawsone, however, 8‐dibromo‐2‐(propylamino)naphthalene‐1,4‐dione and 5,8‐dibromo‐2‐(propylthio)naphthalene‐1,4‐dione yielded better results for copier paper and colored (blue) copier paper used in this analysis. To the best of our knowledge, this is the first study to examine the role of 1,4‐anthraquinone derivatives as potential fingermark development reagents. The results indicate that 1,4‐quinones have a potential to be used as reagents for enhancement of latent fingermarks.     

Forensic applications of chemical imaging: latent fingerprint detection using visible absorption and luminescence

Chemical imaging technology is a rapid examination technique that combines molecular spectroscopy and digital imaging, providing information on morphology, composition, structure, and concentration of a material. Among many other applications, chemical imaging offers an array of novel analytical testing methods, which limits sample preparation and provides high-quality imaging data essential in the detection of latent fingerprints. Luminescence chemical imaging and visible absorbance chemical imaging have been successfully applied to ninhydrin, DFO, cyanoacrylate, and luminescent dye-treated latent fingerprints, demonstrating the potential of this technology to aid forensic investigations. In addition, visible absorption chemical imaging has been applied successfully to visualize untreated latent fingerprints.     

A Small Population Study on Friction Skin Ridges: Differences in Ridge Widths Between Latent and Inked Fingerprints

Morphological changes in the width of latent fingermark ridges occur naturally over time. This could be used to examine the aging process of latents and eventually estimate time of deposition. In a crime context, it is common practice to compare a questioned (aged) fingermark with a database of known (inked) prints. Therefore, in the absence of fresh fingermarks for aging purposes, it is of interest to reveal correlations between these two categories of fingerprints with regard to the widths of their ridges. The present study explores correlations of ridge widths between flat and rolled inked prints with latent fingermarks visualized with carbon black (CB) and titanium dioxide (TiO₂)-based powders among a small population of ten donors. Results revealed consistent differences between the ridge widths of latent and inked prints as well as flat and rolled impressions. Latent fingermarks visualized with CB and TiO₂ powders showed ridges with comparable widths.     

Chemical Imaging of Human Fingermark by X-ray Photoelectron Spectroscopy (XPS)

X-ray photoelectron spectroscopy (XPS) is a widely used technique to characterize the surface chemistry of materials. It plays a crucial role in accessing qualitative and quantitative information and in detecting the presence of chemical functional groups on the surface of any material. The forensic methods available to detect and identify elements and organic/inorganic compounds are often destructive, so evidence cannot be re-analyzed. However, XPS allows rapid analysis of samples without damaging them. Recently, an increasing number of forensic researchers have begun to study certain chemical information on fingermarks. In this study, the authors aimed to present the applicability and power of XPS imaging in fingermark analysis which can also provide specific information about the fingermark chemical composition. Herein, monochromated X-ray (Al Kα) spot size was fixed at 50 μm. XPS mapping resulted in the acquisition of spectra at each pixel, in an array of 41 × 30 pixels with a step size of 50 μm. Then, a simple discussion has been made about how the scanned surface spectrum and basic snapshot spectra are used to identify different components at a fingertip of a scanned surface area (~3 mm²). Hence, a fingermark pattern contaminated with caffeine, TiO₂, and Pb/PbO deposited on the silicon wafer can be chemically mapped and visualized by XPS using principal component analysis (PCA). Thus, the present study showed the possible applicability of XPS for the identification of illicit drugs of abuse, gunshot residue, and skin care products on latent fingermark by mimicking a crime scene evidence.