A comparison of the natural and groomed fingermark lipid composition of different donors using GC/MS.

The lipid composition of natural fingermarks was studied and compared with the composition of groomed residue. Approximately 100 specimens were collected from 6 donors over three sessions (in October, December and July) and analysed using gas chromatography / mass spectrometry (GC/MS). The measured lipid content was generally lower and more variable in natural fingermarks than in groomed fingermarks. Some significant variability was noticed. Relative standard deviations were the highest between donors (generally above 100%) but were also relatively high within donor within a session (from 21% to 80%) and between sessions (from 34% to 126%). The fingermarks from one of the donors generally contained higher relative amounts of lipids in both groomed and natural residue compared to the others. All other fingermarks led to very variable amounts and did not allow classifying the other donors as constantly "good" or "poor" donors. Squalene was the major compound in all marks, particularly in groomed specimens. A correlation between squalene, cholesterol, myristic acid, palmitoleic acid, stearyl palmitoleate and pentadecanoic acid was highlighted. Oleic and stearic were also correlated together but generally more in natural than groomed marks. The obtained results may be particularly useful to better understand the detection mechanisms for techniques targeting lipids and to develop artificial fingermark secretions to further support the development of detection techniques.

Differentiating individuals through the chemical composition of their fingermarks.

Fingermark patterns are one of the oldest means of biometric identification. During this last decade, the molecules that constitute the fingermark residue have gained interest among the forensic research community to gain additional intelligence regarding its donor profile including its gender, age, lifestyle or even its pathological state. In this work, the molecular composition of fingermarks have been studied to monitor the variability between donors and to explore its capacity to differentiate individuals using supervised multi-class classification models. Over one year, fingermarks from thirteen donors have been analysed by Matrix-Assisted Laser Desorption/Ionisation Mass Spectrometry Imaging (n = 716) and mined by different machine learning approaches. We demonstrate the potential of the fingermark chemical composition to help differentiating individuals with an accuracy between 80% and 96% depending on the period of sample collection for each donor and size of the pool of donors. It would be premature at this stage to transpose the results of this research to real cases, however the conclusions of this study can provide a better understanding of the variations of the chemical composition of the fingermark residue in between individuals over long periods and help clarifying the notion of donorship.

Chemical composition of the fingermark residue: Assessment of the intravariability over one year using MALDI-MSI.

These past years, the chemical composition of fingermarks have attracted interest of researchers to meet multiple objectives like the determination of an individual's age, gender or lifestyle or the impact of some fingermark detection processes, to cite a few. These studies have highlighted the need to investigate the consistency of the fingermark composition over time. This research explores the evolution of the secretion residue composition of thirteen donors over one year, focusing on the intravariability. The dual use of Matrix-Assisted Laser Desorption/Ionisation Mass Spectrometry Imaging (MALDI-MSI) and chemometrics provided valuable data regarding the evolution of composition over time as well as the consistency of presence of hundreds of compounds.

Development of a printed quality control test strip for the analysis and imaging of fingermark composition.

In the last decade, there have been many scientific developments regarding the use of mass spectrometry to analyse the composition of fingermarks. In this context, the development of a dedicated quality control test strip would benefit the forensic community by providing a way to assess the reproducibility of the measures as well as to perform inter-laboratory comparisons. To accomplish this goal, the use of a chemical printer offers the possibility of combining a visual template with artificial fingerprint secretions. The design of the quality control test strip as well as the preliminary assessment of its performance with fingermark detection reagents and matrix-assisted laser desorption-ionisation combined with mass spectrometry imaging (MALDI-MSI) are presented in this paper. The chosen template combines two geometric patterns intended to help assess the chemical analysis (full square) and imaging (lined square) capabilities of the instrument. The artificial secretion is composed of two distinct solutions: artificial sweat and artificial sebum. The printing reproducibility and chemical homogeneity of the quality control test strips were assessed in two ways: (1) using MALDI-MSI, the printed pattern was analysed and the m/z values compared to the reference list based on the artificial secretion composition, and (2) using two common fingermark detection techniques, the printed pattern was processed using an amino acid reagent (ninhydrin) and a lipid stain (Oil Red O). Overall, the results highlight the potential of a printed quality control test strip for the assessment of the quality of fingermark detection techniques as well as the possibility of performing quality monitoring of mass-spectrometry-based techniques over time.

Printed artificial sweat as replacement for natural fingermarks: Qualitative and quantitative approach considering an amino acid reagent.

The study presented in this paper aims at assessing how printed fingermarks can be used to generate realistic latent marks bearing varying quantities of materials to be detected. Considering dilution series of artificial sweat (eccrine secretion) and 1,2-indanedione/zinc as amino acid reagent, we assessed how printed marks behave in comparison to natural fingermarks provided by a set of 30 donors. The results were assessed in terms of relative intensity (contrast, luminescence) and expert grading (ridge details, overall quality). With regards to the set of 30 donors, this study brought a quantitative look to the influence of intra- and inter-variability on the relative intensity values observed when processing natural fingermarks. This provided new data to further understand the concept of "donorship". With regards to the use of printed marks, it has been illustrated how dilution series of a concentrated solution allows covering a range of cases: unnatural marks (intensity values well above those obtained with donors), rich marks (corresponding to fingermarks left by good donors), and faint marks (associated with the kind of results observed with poor donors). Such a range of detection performance offers the possibility to generate fine-tuned detection exercises of varying difficulty levels. Printed items made of artificial sweat could hence constitute a valuable alternative to natural secretions in the context of education and proficiency testing.

Automatic assessment of fingermarks quality: Exploration of the possible application in the context of detection and comparison with human examiners.

In forensic science, particularly in the context of latent fingermarks detection, forensic scientists are often faced with the need to assess the quality of the detected fingermarks to quantitatively interpret their results and express conclusions. Today this process is mainly carried out by human examiners referring to guidelines or provided quality scales. The largest the set of fingermarks (e.g., hundreds, thousands), the longest and the most labor-intensive this task becomes. Moreover, it is difficult to guarantee a fully objective process since the subjectivity of each individual is almost impossible to avoid, especially with regards to the interpretation of the quality scale levels or when facing fingermarks detected in an inhomogeneous manner. In this paper, the possibility of automatizing the quality assessment step is explored. The choice has been made to consider the use of quality assessment algorithms currently applied in an identification context. 150 natural fingermarks from ten donors were deposited on three different supports. These marks were detected using 1,2-indanedione/zinc or cyanoacrylate fumigation depending on the support. Then, their quality was assessed by five examiners, according to the UNIL scale, and by seven algorithms (i.e., Lights Out, Latent Fingerprint Image Quality 1 and 2, Latent Quality Metric, Expected Score Likelihood Ratio, NIST Fingerprint Image Quality, MINDTCT). Spearman and Pearson correlations were calculated, and the distribution of scores for each algorithm was charted (using boxplots) against the results provided by the human examiners. The most promising results were obtained with the LQM algorithm, more specifically with the fingermark clarity metric.

Providing illicit drugs results in five seconds using ultra-portable NIR technology: An opportunity for forensic laboratories to cope with the trend toward the decentralization of forensic capabilities.

The analysis of illicit drugs faces many challenges, mainly regarding the production of timely and reliable results and the production of added value from the generated data. It is essential to rethink the way this analysis is operationalised, in order to cope with the trend toward the decentralization of forensic applications. This paper describes the deployment of an ultra-portable near-infrared detector connected to a mobile application. This allows analysis and display of results to end users within 5s. The development of prediction models and their validation, as well as strategies for deployment within law enforcement organizations and forensic laboratories are discussed.

Interpol review of fingermarks and other body impressions 2016-2019.

This review paper covers the forensic-relevant literature in fingerprint and bodily impression sciences from 2016 to 2019 as a part of the 19th Interpol International Forensic Science Managers Symposium. The review papers are also available at the Interpol website at: https://www.interpol.int/content/download/14458/file/Interpol%20 Review%20 Papers%202019. pdf.

Effect of water immersion on multi- and mono-metallic VMD.

The use of vacuum metal deposition (VMD) for fingermark detection has been known for almost 40 years. The technique is applicable on a wide variety of substrates and on wetted items. Several publications compare the relative efficiency of VMD (conventionally based on a successive vaporization of gold followed by zinc) with other detection techniques, or its ability to detect marks on difficult substrates, but few are known about the application of monometallic VMDs and about the impact of immersion on the detection performances. This study aims at partially filling that gap by offering a quantitative and qualitative glance at three VMD processes (i.e., gold/zinc, silver, and sterling silver) applied to dry and wetted substrates. The impact of immersion on the detection process has been studied by using split marks (one half kept dry, the other one wetted). On immersed substrates, a modification of colour shades has been observed with monometallic VMDs (on all substrates considered) and of contrast with conventional VMD (on polyethylene). In terms of ridge details, a relatively good resistance of secretion residue towards immersion has been emphasized (in regards with VMD). This study provides original data, which will hopefully help getting a better understanding of the VMD detection mechanism.

Further investigations into the single metal deposition (SMD II) technique for the detection of latent fingermarks.

Single metal deposition (SMD II), a recently proposed method for the development of latent fingermarks, was investigated by systematically altering aspects of the procedure to assess their effect on the level of development and contrast achieved. Gold nanoparticle size, temperature of the deposition solution bath, and orbital shaking during detection were shown to affect the levels of development and contrast obtained. Gold nanoparticles of diameter 15-21nm were found to be most effective for satisfactory visualisation of latent fingermarks, while solutions that were applied at room temperature were found to adequately balance the ratio between the contrast of the fingermark ridge detail and the level of background staining achieved. Finally, optimum levels of development and contrast were obtained through constant agitation of both solution baths at approximately 50RPM throughout the submersion time. SMD II was also tested on a large variety of substrate types and shown to be effective on a range of porous, non-porous, and semi-porous surfaces; however, the detection quality can be significantly influenced by the substrate nature. This resulted in the production of dark grey, white, or gold coloured fingermarks on different surfaces, as well as reversed detection on certain types of plastic, similarly seen through the use of vacuum metal deposition.

Functionalised silicon oxide nanoparticles for fingermark detection.

Over the past decade, the use of nanotechnology for fingermark detection has been attracting a lot of attention. A substantial number of nanoparticle types has thus been studied and applied with varying success. However, despite all efforts, few publications present clear supporting evidence of their superiority over standard and commonly used techniques. This paper focuses on a rarely studied type of nanoparticles that regroups all desired properties for effective fingermark detection: silicon oxide. These nanoparticles offer optical and surface properties that can be tuned to provide optimal detection. This study explores their potential as a new method for fingermark detection. Detection conditions, outer functionalisations and optical properties were optimised and a first evaluation of the technique is presented. Dye-doped silicon oxide nanoparticles were assessed against a one-step luminescent cyanoacrylate. Both techniques were compared on natural fingermarks from three donors collected on four different non-porous substrates. On average, the two techniques performed similarly but silicon oxide detected marks with a better homogeneity and was less affected by donor inter-variability. The technique remains to be further optimised and yet silicon oxide nanoparticles already show great promises for effective fingermark detection.

Cadmium-free quantum dots in aqueous solution: Potential for fingermark detection, synthesis and an application to the detection of fingermarks in blood on non-porous surfaces.

The use of quantum dots (QDs) in the area of fingermark detection is currently receiving a lot of attention in the forensic literature. Most of the research efforts have been devoted to cadmium telluride (CdTe) quantum dots often applied as powders to the surfaces of interests. Both the use of cadmium and the nano size of these particles raise important issues in terms of health and safety. This paper proposes to replace CdTe QDs by zinc sulphide QDs doped with copper (ZnS:Cu) to address these issues. Zinc sulphide-copper doped QDs were successfully synthesized, characterized in terms of size and optical properties and optimized to be applied for the detection of impressions left in blood, where CdTe QDs proved to be efficient. Effectiveness of detection was assessed in comparison with CdTe QDs and Acid Yellow 7 (AY7, an effective blood reagent), using two series of depletive blood fingermarks from four donors prepared on four non-porous substrates, i.e. glass, transparent polypropylene, black polyethylene and aluminium foil. The marks were cut in half and processed separately with both reagents, leading to two comparison series (ZnS:Cu vs. CdTe, and ZnS:Cu vs. AY7). ZnS:Cu proved to be better than AY7 and at least as efficient as CdTe on most substrates. Consequently, copper-doped ZnS QDs constitute a valid substitute for cadmium-based QDs to detect blood marks on non-porous substrates and offer a safer alternative for routine use.

Detection of fingermarks by colloidal gold (MMD/SMD)--beyond the pH 3 limit.

This work is part of a continuing goal to improve the multimetal deposition technique (MMD), as well as the single-metal deposition (SMD), to make them more robust, more user-friendly, and less labour-intensive. Indeed, two major limitations of the MMD/SMD were identified: (1) the synthesis of colloidal gold, which is quite labour-intensive, and (2) the sharp decrease in efficiency observed when the pH of the working solution is increased above pH 3. About the synthesis protocol, it has been simplified so that there is no more need to monitor the temperature during the synthesis. The efficiency has also been improved by adding aspartic acid, conjointly with sodium citrate, during the synthesis of colloidal gold. This extends the range of pH for which it is possible to detect fingermarks in the frame of the MMD/SMD. The operational range is now extended from 2 to 6.7, compared to 2-3 for the previous formulations. The increased robustness of the working solution may improve the ability of the technique to process substrates that tend to increase the pH of the solution after their immersion.

Use of quantum dots in aqueous solution to detect blood fingermarks on non-porous surfaces.

A new and original reagent based on the use of highly fluorescent cadmium telluride (CdTe) quantum dots (QDs) in aqueous solution is proposed to detect weak fingermarks in blood on non-porous surfaces. To assess the efficiency of this approach, comparisons were performed with one of the most efficient blood reagents on non-porous surfaces, Acid Yellow 7 (AY7). To this end, four non-porous surfaces were studied, i.e. glass, transparent polypropylene, black polyethylene, and aluminium foil. To evaluate the sensitivity of both reagents, sets of depleted fingermarks were prepared, using the same finger, initially soaked with blood, which was then successively applied on the same surface without recharging it with blood or latent secretions. The successive marks were then cut in halves and the halves treated separately with each reagent. The results showed that QDs were equally efficient to AY7 on glass, polyethylene and polypropylene surfaces, and were superior to AY7 on aluminium. The use of QDs in new, sensitive and highly efficient latent and blood mark detection techniques appears highly promising. Health and safety issues related to the use of cadmium are also discussed. It is suggested that applying QDs in aqueous solution (and not as a dry dusting powder) considerably lowers the toxicity risks.

Identification of promising antigenic components in latent fingermark residues.

An analysis of latent fingermark residues by Sodium-Dodecyl-Sulfate PolyAcrylamide Gel Electrophoresis (SDS-PAGE) followed by silver staining allowed the detection of different proteins, from which two major bands, corresponding to proteins of 56 and 64 kDa molecular weight, could be identified. Two other bands, corresponding to proteins of 52 and 48 kDa were also visualizable along with some other weaker bands of lower molecular weights. In order to identify these proteins, three antibodies directed against human proteins were tested on western blots of fingermarks residues: anti-keratin 1 and 10 (K1/10), anti-cathepsin-D (Cat.D) and anti-dermcidin (Derm.). The corresponding antigens are known to be present in the stratum corneum of desquamating stratified epithelium (K1/10, Cat.D) and/or in eccrine sweat (Cat.D, Derm.). The two major bands were identified as consistent with keratin 1 and 10. The pro-form and the active form of the cathepsin-D have also been identified from two other bands. Dermcidin could not be detected in the western blot. In addition, these antibodies have been tested on latent fingermarks left on polyvinylidene fluoride (PVDF) membrane, as well as on whitened and non-whitened paper. The detection of fingermarks was successful with all three antibodies.

Fingermark detection based on the in situ growth of luminescent nanoparticles--towards a new generation of multimetal deposition.

The in situ deposition of zinc oxide on gold nanoparticles in aqueous solution has been here successfully applied in the field of fingermark detection on various non-porous surfaces. In this article, we present the improvement of the multimetal deposition, an existing technique limited up to now to non-luminescent results, by obtaining luminescent fingermarks with very good contrast and details. This is seen as a major improvement in the field in terms of selectivity and sensitivity of detection, especially on black surfaces.

SECM imaging of MMD-enhanced latent fingermarks.

Scanning electrochemical microscopy (SECM) has been used to image latent fingermarks enhanced by adsorption of gold nanoparticles onto which silver is chemically deposited, a process known as "multi-metal-deposition" (MMD).

Single-metal deposition (SMD) as a latent fingermark enhancement technique: an alternative to multimetal deposition (MMD).

This paper proposes an alternative solution to multimetal deposition (MMD) for the development of latent fingermarks on non-porous and porous surfaces. MMD offers a good sensitivity, however it is very time-consuming and requires many reagents to be carried out. Single-metal deposition (SMD) replaces the silver enhancement of the gold colloids by a gold enhancement procedure. This reduces the number of baths by one as well as the number of reagents and their cost, utilizes reagents with a longer shelf life, and most importantly reduces the labor-intensity of the procedure. It offers quasi-identical results to MMD and thus makes a very attractive alternative.

Use of gold nanoparticles as molecular intermediates for the detection of fingermarks.

Among the numerous methods dedicated to the detection of latent fingermarks, the MultiMetal Deposition (MMD) offers, as a main advantage, the ability to be applied on a great number of porous and non-porous surfaces, e.g., paper, plastic, glass, latex, and polystyrene, even if wetted. While considered as a powerful and sensitive technique, MMD is often neglected, mainly because of operational limitations (siliconized vessels, restrictive pH domain, numerous immersion baths, ...). In this contribution, we propose a modification of the standard MMD method so that the procedure is simplified with a number of baths reduced to a minimum. To reach this goal, it was necessary to obtain a fully operable solution which could detect fingermarks in a single step. We chose to take advantage of the molecular recognition mechanisms by functionalizing the gold nanoparticles with a molecular host able to bind itself to gold while keeping the ability to trap molecules in solution. Cyclodextrins were chosen as they can be easily chemically modified to offer gold-binding abilities. Moreover, they are widely used as hosts for various molecular guests (dyes, luminescent molecules, ...). This new formulation has been tested on three different surfaces to attest the feasibility of this strategy. Successful results were obtained with detailed fingermarks offering a good contrast to allow their identification without the need to enhance the results (such as with a physical developer). If the new formulation behaves very similarly to the old one, in terms of experimental conditions, it offers the additional advantage to develop fingermarks after immersing them in only one bath. The goal is thus reached.