A common framework to situate digital and physical traces in time.

In this article, three main approaches to situate forensic traces in time were revisited under the prism of the Sydney Declaration and adapted to be applicable to a large range of physical and digital traces. The first approach is based on time tags which are time-based characteristics produced as the result of an activity at a specific time. They can either be directly related to time (i.e., time stamps) or indirectly (i.e., time indicators). While relatively straightforward, time tags require scientific knowledge to be correctly interpreted and to account for the risks of desynchronisation, anomalies and manipulation. The second approach is based on time dynamics and aim at measuring changes that occur as a function of time, such as caesium pulsation (i.e., on which international atomic time is based) or body cooling after death (i.e., from which time since death can be inferred). However, time dynamics phenomena are generally also influenced by other case-specific factors (e.g., environmental factors), and thus more difficult to reliably implement in practice. Finally, the third approach relies on relative sequences, using information unrelated to time, such as relative positions or dynamics of traces at the scene. As each approach has its potential and limitations, a combination of traces from different (both material and digital) sources and approaches is recommended to answer time questions in practice (When? How long? In which succession?) and enhance the reliability of the dating endeavours. It is strongly recommended to consider the principles of the Sydney Declaration when implementing or developing dating methods, as they point at potential issues that are often forgotten in forensic research and practice, such as uncertainties linked to the concept of trace, scene investigation, the asymmetry of time, the importance of context and the multiplicity of purposes. Future research should focus on improving the reliability of these dating approaches by combining and systematising their usage in investigative practice, as well as in broader intelligence processes.

Signs of how the Sydney Declaration article is received in the forensic science literature.

The Sydney Declaration is an initiative led by an informal group of forensic scientists with diverse backgrounds. It offers a vision of forensic science based on the trace, as a vestige of a past event related to security or a possible law violation. An article published in Forensic Science International (FSI) introduces to this view [1]. Our investigation delves into how the forensic science literature has received this article (the SD article), nearly two years after its publication. One of the main challenges of this exploratory study was to define the appropriate scope of forensic scientific literature, within which the SD article must be located. In general, the publishing domain is quickly evolving, with many competing players, while still being structured around standard academic disciplines. The forensic literature, meanwhile, is scattered and poorly connected. This reflects the fragmentation of practice and research in forensic science, and the difficulty of situating a scientific activity in such a way as to bring out its forensic substance. Nonetheless, the SD article fills a gap. By deciphering the critical concept of trace, it highlights how pivotal forensic science is in addressing societal challenges. Scholarly literature expresses clear quantitative interest in the SD article. It has received significant qualitative citations on multiple levels and dimensions, in a highly relevant manner and in accordance with its aim of providing a forensic foundation for various debates that have been conducted separately, notably over the last fifteen years.

Technical note: Influence of the drying position and time on the persistence of gunshot residues on fabrics.

The influence of the drying position and time on the persistence of gunshot residues (GSR) on fabrics was investigated. Powder tattooing from a 40 cm shooting distance on targeted fabrics were slightly wetted using a spray and dried for 3 h or 48 h in horizontal or vertical positions. The GSR particles were visualised using IR fluorescence with a Video Spectral Comparator (VSC) and automatically counted with a software before the wetting and after the drying stages. While a significant rate of GSR particles (up to 22%) were lost, it was mainly due to the wetting procedure rather than the drying stage. No statistically significant difference was observed between the drying positions, indicating that both drying positions can be used in practice to dry slightly wet fabrics. The drying time had no influence on the loss, and the GSR distribution was not significantly influenced by either factor (i.e., time and position).

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.

An improved Chemcatcher-based method for the integrative passive sampling of 44 hydrophilic micropollutants in surface water - Part A: Calibration under four controlled hydrodynamic conditions.

When monitoring water quality with hydrophilic integrative passive sampling devices, it is crucial to use accurate sampling rates (RS) that account for exposure conditions such as hydrodynamics. This study aims at calibrating Chemcatcher-like passive samplers - styrene-divinylbenzene reverse phase sulfonate (SDB-RPS) extraction disk covered by a polyethersulfone (PES) membrane - at four water flow velocities (5 to 40 cm s-1) in a channel system. First, the four hydrodynamic conditions were characterized by measuring the mass transfer coefficients of the water boundary layer (kw) at the surface of the samplers using the alabaster dissolution method. Then, fifty-six samplers were deployed in the channels and exposed for 7 different intervals varying from 1 to 21 days. Thus, RS were determined at four different kw for 44 hydrophilic compounds, ranging from 0.015 to 0.115 L day-1. Relationships were established between kw and RS using models for mixed rate control by the membrane and the water boundary layer. The estimated parameters of those relationships are suitable for the determination of accurate RS when kw is measured in situ, for example by co-deploying silicone disks spiked with performance and reference compounds (PRC) as implemented in Part B.

An improved Chemcatcher-based method for the integrative passive sampling of 44 hydrophilic micropollutants in surface water - Part B: Field implementation and comparison with automated active sampling.

Integrative passive sampling is particularly useful in the monitoring of hydrophilic contaminants in surface water, but the impact of hydrodynamics on contaminant uptake still needs to be better considered. In part A (Glanzmann et al., 2023), Chemcatcher-like hydrophilic samplers (i.e., SDB-RPS extraction disks covered by PES microporous membranes) were calibrated to determine the sampling rates RS of 44 hydrophilic contaminants (pesticides, pharmaceuticals, industrial products) taking into account the hydrodynamic conditions. In this study, Chemcatcher-like passive sampling devices that allowed co-deploying hydrophilic samplers and performance reference compounds (PRC)-spiked silicone disks were tested in a Swiss river with intermediate water velocities (5-50 cm s-1, 23 cm s-1 on average) during 11 consecutive 14-day periods. The PRC dissipation from silicone disks - combined with the calibration data from part A - allowed to determine in-situ RS that took into account hydrodynamic conditions. The obtained aqueous time-weighted average (TWA) concentrations were found to be robust with good concordance between duplicates (mean quotient of 1.16 between the duplicates). For most measurements (76 %), TWA concentrations showed no major difference (20 cm s-1). RS from the literature (RS,LIT) - obtained at water velocities between 8 and 37 cm s-1 - were also shown to provide comparable TWA concentrations in the studied hydrodynamic conditions (average water velocity of 24 cm s-1). The estimated errors due to the use of RS,MAX or RS,LIT rather than in-situ RS are given as a function of the water velocity to determine in which conditions the developed method is required (or not) in monitoring programs.

Towards more relevance in forensic science research and development.

Many different issues have been identified in forensic science for more than 10 years. While quality management has often been suggested as a path forward, research is generally considered as an essential part of the solution. Through an overview of current forensic science research, this paper aims at evaluating if and how research answer the challenges forensic science is currently facing. While forensic related publications have massively increased over the years, approximately half of the publications were published in non-forensic sources, indicating that forensic science research tends to be led by other disciplines. Over the years, forensic science research has remained largely oriented towards methodological and technological development rather than relevance to the forensic science discipline and practice. Practical implementation of the techniques is rarely discussed from a forensic perspective, and thus research rarely move from the "proof-of-concept" stage to its utilisation in case investigation. The digital transformation also generated a massive increase of data, making it challenging to find the relevant pieces of information in the mass of "forensic" publications available on-line. Thus, we propose to refocus forensic science research on forensic fundamental and practical questions to strengthen the discipline and its impact on crime investigation and security issues. Our propositions represent an incentive to further discuss forensic science research and knowledge transmission through the definition of a common culture within the community, focusing on common fundamental knowledge such as a better understanding of the concept of trace and its case-based information content.

Should inorganic or organic gunshot residues be analysed first?

Gunshot residues (GSR) collected during the investigation of firearm-related incidents can provide useful information for the reconstruction of the events. Two main types of GSR traces can be targeted by forensic scientists, the inorganic (IGSR) and the organic GSR (OGSR). Up to now, forensic laboratories have mainly focused on the detection of inorganic particles on the hands and clothes of a person of interest using carbon stubs analysed by scanning electron microscopy coupled with energy dispersive X-ray spectrometry (SEM/EDS). Several approaches have been proposed to also analyse the organic compounds since they might bring additional information for the investigation. However, implementing such approaches might disrupt the detection of IGSR (and vice versa depending on the applied sequence of analysis). In this work, two sequences were compared for the combined detection of both types of residues. One carbon stub was used for collection, and the analysis was performed either by targeting the IGSR or the OGSR first. The aim was to evaluate which one allows maximum recovery of both types of GSR while minimising losses that might occur at different stages of the analysis process. SEM/EDS was used for the detection of IGSR particles while an ultra-high performance liquid chromatography tandem mass spectrometry (UHPLC-MS/MS) was used for the analysis of OGSR compounds. Extracting OGSR first required the implementation of an extraction protocol that did not interfere with the IGSR particles present on the stub. Both sequences allowed good recovery of the inorganic particles since no significant difference was observed in the detected concentrations. However, OGSR concentrations were lower after IGSR analysis than before for two compounds (ethyl and methylcentralite). Thus, it is advised to extract rapidly the OGSR before or after IGSR analysis to avoid losses during the storage and analysis processes. The data also indicated that there was a low correlation between IGSR and OGSR highlighting the potential of a combined detection and analysis of both types of GSR.

An efficient method to detect series of fraudulent identity documents based on digitised forensic data.

Document fraud is a transnational form of crime, and its serial character has already been highlighted. To combat this phenomenon, the Interstate Database of Fraudulent Identity Documents (BIDIF) has been created and implemented in Switzerland. It supports the comparison of documents and the detection of series, i.e., documents that share a common source. To efficiently use such a system, forensic document examiners would benefit from a harmonised and proven profiling method. Thus, the aim of this study is to develop a method for comparing documents and establishing series. The method is meant to improve the detection capabilities of forensic document examiners operating BIDIF or engaged in the profiling of fraudulent documents. First, a method based on the visual characteristics of digitised images of fraudulent identity documents has been developed. Subsequently, the method was qualitatively and quantitatively evaluated using four tests. The first test verified the ability of the method to detect pre-existing series. The second test checked the capability of the method to detect links amongst isolated documents. Finally, two further tests were carried out to compare the method impact on the successful detection of series. These tests were carried out by professional forensic document examiners and Master students in forensic science, respectively. This allowed a comparison of the method influence on series detection. The method allowed a significant increase in the number of series and links detected, while also decreasing the occurrence of false negatives and false positives. Furthermore, links were more rapidly detected.

The potential of digital technologies in problem-based forensic learning activities.

Forensic practice is the concluding practical course of the forensic science bachelor program at the School of Criminal Justice of the University of Lausanne. Learning activities are constructed around five main objectives for the resolution of simulated forensic case problems: 1) select relevant traces and items to be collected at the scene and perceive their potential value in the reconstruction process, 2) apply appropriate detection techniques in sequence to obtain clues of good quality, 3) process traces using Analysis, Comparison, Evaluation and Verification (ACE-V) methodology, 4) produce and summarise information in oral and written forms to help an investigation, and 5) work collaboratively to benefit from the diversity of group members. Simulating and supervising realistic activities is a complex task that became more and more challenging with a continuously increasing number of students over the years (from ca. 30 in 2016 to more than 60 in 2021). Thus, an educational innovation project was launched and aimed at implementing digital technologies to support the teaching staff. A computer-based crime scene simulation tool (allowing students to visualize 360° crime scenes and relevant items) and a communication tool (to simplify and centralise the communication between the students and the teaching staff) were implemented. This article describes the implementation, added value and limitations of these digital technologies in problem-based learning activities. Prior to 2020, the practical course forensic practice was delivered entirely on-site without specific technologies, and entirely on-line in 2020 (due to the sanitary restrictions related to the COVID-19 pandemic). Finally, in 2021, on-line and on-site activities were implemented with success, combining the best of both approaches in a blended teaching mode. An overall increase in the satisfaction of students and teaching staff was observed with the implementation of these tools. Limiting presence on-site allowed students to take a step back from the activities and collected items. This promoted critical thinking, and together with an increase in structured (on-line and on-site) interactions allowed for a positive, continuous learning experience. While the evaluations of these novel technologies were very positive, students still expressed their willingness to perform certain tasks on-site and a preference for face-to-face interactions.

Comparison of four commercial solid-phase micro-extraction (SPME) fibres for the headspace characterisation and profiling of gunshot exhausts in spent cartridge casings.

Headspace solid-phase micro-extraction (SPME) is a promising technique for the characterisation and profiling of gunshot exhausts in spent cartridge casings, especially for health and environmental risk assessments, as well as forensic purposes. To date, however, no comprehensive investigation has been carried out to objectively assess the kinds of compound released during a discharge that can be recovered by this approach, the selectivity of the main commercially available fibres, and their relative performances for the analysis of gunshot exhausts and the discrimination of different ammunition types. This study aimed to fill this gap. Gunshot exhausts in spent cartridge casings from four different ammunition types were analysed by GC-MS, after extraction with four different commercial fibres: 100 µm polydimethylsiloxane (PDMS), 85 µm polyacrylate (PA), 65 µm polydimethylsiloxane/divinylbenzene (DVB), and 85 µm carboxen/polydimethylsiloxane (CAR). Results showed that, overall, a total of 120 analytes could be observed across the cartridges, but the different tested fibres also displayed distinct performances, which were, to some extent, complementary for the characterisation of gunshot exhausts. DVB, in particular, recovered the most compounds simultaneously. On the other hand, the observed variability between measurements was also high, making it a poor candidate for (semi-)quantitative applications (e.g. estimation of time since discharge and/or source profiling). In this regard, PA demonstrated the highest potential for broad use and implementation in multi-purpose methods.

Determining the Mass Transfer Coefficient of the Water Boundary Layer at the Surface of Aquatic Integrative Passive Samplers.

Passive sampling devices (PSDs) offer key benefits for monitoring chemical water quality, but the uptake process of PSDs for hydrophilic compounds still needs to be better understood. Determining mass transfer coefficients of the water boundary layer (kw) during calibration experiments and in situ monitoring would contribute toward achieving this; it allows for combining calibration data obtained at different temperature and hydrodynamic conditions and facilitate the translation of laboratory-derived calibration data to field exposure. This study compared two kw measurement methods applied to extraction disk housings (Chemcatcher), namely, alabaster dissolution and dissipation of performance reference compounds (PRCs) from silicone. Alabaster- and PRC-based kw were measured at four flow velocities (5-40 cm s-1) and two temperatures (11 and 20 °C) in a channel system. Data were compared using a relationship based on Sherwood, Reynolds, and Schmidt numbers. Good agreement was observed between data obtained at both temperatures, and for the two methods. Data were well explained by a model for mass transfer to a flat plate under laminar flow. It was slightly adapted to provide a semi-empirical model accounting for the effects of housing design on hydrodynamics. The use of PRC-spiked silicone to obtain in situ integrative kw for Chemcatcher-type PSDs is also discussed.

An application example of the likelihood ratio approach to the evaluation of organic gunshot residues using a fictional scenario and recently published data.

The analysis of gunshot residues (GSR) can provide important information with regard to the involvement of a person of interest (POI) in a firearm-related incident. Organic gunshot residues (OGSR) have been investigated in order to provide additional and complementary information to the traditional inorganic gunshot residue (IGSR) particles detected by scanning electron microscopy (SEM). Currently, many procedures and analytical methods have been developed to detect OGSR-related compounds collected from the shooter's hands. However, such studies provide no information regarding the inclusion of such results in an activity level evaluation for discharging a firearm. The aim of this article is to assess the feasibility of using the likelihood ratio (LR) approach as a tool to evaluate OGSR results for activity level propositions. The developed model focuses on the assignment of an LR for several compounds detected in OGSR. A simple worst-case simulation was investigated in order to assess the applicability of the LR approach to evaluate OGSR traces. This simulation highlighted the importance of addressing an appropriate pair of activity level propositions when evaluating the results.

Shifting forensic science focus from means to purpose: A path forward for the discipline?

Forensic science is facing a persistent crisis that is often addressed by organizational responses, with a strong focus on the improvement and standardisation of means and processes. However, organisations and processes are highly dependent on the political, economical and legal structures in which they operate. This may explain why most proposed solutions had difficulties in addressing the crisis up to now, as they could hardly be applied transversally to all forensic science models. Moreover, new tools and technologies are continuously developed by a quasi-infinite number of different scientific disciplines, thus leading to further diversity and fragmentation of forensic science. In this paper, it is proposed to shift the focus from means to purpose and consider forensic science current challenges in terms of discipline, before addressing organisations' specific issues. As a distinct discipline, forensic science can refocus research and development on shared principles and purposes, such as reconstructing, monitoring, and preventing crime and security issues. This focus change will facilitate a better understanding of the trace as the object of study of forensic science and eventually lead to a more impactful and long-lasting effect. This approach will also foster the development of a forensic science culture (instead of a primarily technological culture) unified by purpose rather than means through more relevant education and research.

A different perspective on the forensic science crisis.

Recurrent mentions of a forensic science crisis are reported in the literature. Some 15 years ago, the discussion was focused on the backlog problem. Other issues have been regularly debated since then, including the risk of error, need for independence, importance and risk of contextualisation, increasing fragmentation into separate processes and specialisations. Proposed solutions to solve one problem often led to other issues in other parts of the process. This paper attempts to address the apparent crisis using a different perspective, through a comparison with established disciplines, namely material science, medicine and historical science. The comparison with material science shows that, despite the varied organisational and legal models and the interdisciplinary nature of the field, a common element to all forensic science endeavours exists: the trace. A greater focus on the trace might thus help the development of a holistic approach in forensic science. The comparison with medicine demonstrates that, through the overall process, the main risk shifts from the risk to overlook important hypotheses or traces at the beginning of the process (e.g. problems in the detection of traces/symptoms and formulation of hypotheses) to the risk of supporting the wrong hypothesis at the end of the process (e.g. erroneous test of the hypotheses/diagnostic). Further, in medicine, symptoms are rarely evaluated in isolation, while traces are often evaluated separately. By analogy, epidemiology illustrates forensic science's critical role in preventing crime through forensic intelligence, supporting a more extensive and more collaborative application of forensic science in security issues. The comparison with historical science also indicates that a single trace (i.e. the observed effect) is rarely sufficient to reason on its cause. Retrodiction (abduction) is proposed as an alternative reasoning approach to reconstruct events from the past based on signs uncovered in the present. Finally, the impact of science in investigating crimes is presented as an evolving process. A new trace or information can bring an entirely different light on the reconstruction of past events or prevention of future issues. Thus, issues or challenges in the first stages of the process (i.e., crime scene investigation) should be addressed in priority for subsequent stages to function correctly.

Use of ion mobility-high resolution mass spectrometry in metabolomics studies to provide near MS/MS quality data in a single injection.

The use of ion mobility separations (IMSs) in metabolomics approaches has started to be deeply explored in the last years. In this work, the use of liquid chromatography (LC) coupled to IMS-quadrupole time-of-flight mass spectrometry (QTOF MS) has been evaluated in a metabolomics experiments using single injection of the samples. IMS has allowed obtaining cleaner fragmentation spectra, of nearly tandem MS quality, in data-independent acquisition mode. This is much useful in this research area as a second injection, generally applied in LC-QTOF MS workflows to obtain tandem mass spectra, is not necessary, saving time and evading possible compound degradation. As a case study, the smoke produced after combustion of herbal blends used to spray synthetic cannabinoids has been selected as study matrix. The smoke components were trapped in carbon cartridges, desorbed and analyzed by LC-IMS-QTOF MS using different separation mechanisms (reversed phase and HILIC) and acquiring in both positive and negative mode to widen the chemical domain. Partial Least Squares-Discriminant Analysis highlighted several compounds, and ratio between N-Isopropyl-3-(isoquinolinyl)-2-propen-1-amine and quinoline allowed differentiating between tobacco and herbal products. These two compounds were tentatively identified using the cleaner fragmentation spectra from a single injection in the IMS-QTOF MS, with additional confidence obtained by retention time (Rt) and collisional cross section (CCS) prediction using artificial neural networks. Data from this work show that LC-IMS-QTOF is an efficient technique in untargeted metabolomics, avoiding re-injection of the samples for elucidation purposes. In addition, the prediction models for Rt and CCS resulted of help in the elucidation process of potential biomarkers.

Can forensic science learn from the COVID-19 crisis?

This paper draws parallels between the current COVID-19 crisis and the apparent forensic science crisis. It investigates if shared approaches of the problem and solutions could emerge. Some relevant aspects of the medical system as it reacted to the pandemic crisis and the situation in forensic science are presented. Further, three main stages of the COVID-19 crisis and its impact on individuals and society are proposed, highlighting similarities to the effects of forensic science. Finally, some lessons from COVID-19 for forensic science are identified and discussed. It is concluded that forensic science's best assurance to address current and future challenges, particularly in an increasingly digital environment, remains a sound scientific approach, including critical thinking and inter-disciplinary collaborations.

Time since last discharge of firearms and spent ammunition elements: state of the art and perspectives.

The estimation of the time since last discharge of firearms or spent ammunition elements (e.g., casings) may provide crucial information in the investigation of a shooting incident and, eventually, the following trial. Herein, an exhaustive review of the methods described in the literature is reported, with the aim to evaluate their potential and limitations from a forensic perspective. This work, in particular, highlighted the fact that a number of investigations have been carried out in the field during the last century (with an especially high rate in the last 30 years), but the implementation of related procedures in forensic laboratories is still rare. The situation has been discussed and a series of propositions have been forwarded, in order to overcome challenges and facilitate the implementation of dating approaches in real casework.

Changes in latent fingermark glyceride composition as a function of sample age using UPLC-IMS-QToF-MSE.

The composition of fingermark residue has been an important topic in forensic science, mainly in efforts to better understand and eventually improve the efficacy of latent fingermark detection methods. While the lipid fraction has been extensively studied, there is currently little information about how the glyceride fraction of latent fingermarks is chemically altered over time following deposition. A previously reported untargeted ultra performance liquid chromatography-ion mobility spectrometry-quadrupole time-of-flight mass spectrometry (UPLC-IMS-QToF-MSE) method was used to investigate changes over time in fingermark di- and triglycerides. Charged latent fingermark samples from 5 donors were analysed up to 28 days following deposition. Significant changes in glyceride composition occurred with increased sample age, attributed primarily to the oxidation of unsaturated triglycerides through ozonolysis. Considerably fewer unsaturated TGs were identified in samples 7 and 28 days following deposition, while mono- and diozonides of these lipids were identified as major components of aged samples. Additional compounds were identified as possible aldehyde and carboxylic acid derivatives resulting from the reaction of water with ozonolysis intermediates. While the onset of these processes occurred rapidly following deposition, continuing oxidation over time was seen via the progressive ozonolysis of diunsaturated triglycerides. These results represent a further step towards understanding the factors affecting fingermark composition, ageing and subsequent detection under operational conditions.