An Examination of the Sequence of Intersecting Lines using Microspectrophotometry

The potential of microspectrophotometry as a technique to determine the sequence of intersecting lines was examined. The technique was used to determine the sequence of heterogeneous line intersections produced using inkpad, stamp‐pad ink and ballpoint pens, gel pens, fountain pens, laser and ink‐jet printers. The study was carried out with an assumption that the peak characteristics of spectra from the point of intersection should correspond to the peak characteristics of pure ink which was executed later. According to spectral reflectance curves, microspectrophotometry was possible to determine whether the ink was above or below the inkpad/stamp‐pad ink seals. In blind testing, microspectrophotometry technique results were directly compared to those obtained by five experienced forensic document examiners using optical microscopy regularly employed in casework. As the results obtained from the study were positive, microspectrophotometry technique was found to be very successful in determining the sequence of heterogeneous line intersections under some conditions.     

Preliminary Study on Determining the Sequence of Intersecting Lines by Fluorescence Technique

The determination of the sequence of intersecting lines is an important part of questioned document examinations. A fluorescence technique was used to determine the sequence of heterogeneous intersecting lines produced using inkpad ink, stamp‐pad ink, ballpoint pens, gel pens, fountain pens, colorants of carbon paper, photocopiers, laser printers, and inkjet printers. A SteREO Discovery.V20 equipped with the ZEN Blue Lite software was chosen to perform the tests.As the results obtained from the study were positive under most conditions, the fluorescence technique was found to be very successful in determining the sequence of intersecting lines from ballpoint pen, gel pen, fountain pen, photocopier, laser and inkjet printers, and inkpad inks. The method was also successful in determining the sequence of intersecting lines from ballpoint pen, photocopier, laser printer, and stamp‐pad inks under most conditions. The technique was not successful in determining the order of crossing lines blending together.     

Application of Micro‐Attenuated Total Reflectance Fourier Transform Infrared Spectroscopy to Ink Examination in Signatures Written with Ballpoint Pen on Questioned Documents

Questioned documents examined in a forensic laboratory sometimes contain signatures written with ballpoint pen inks; these signatures were examined to assess the feasibility of micro‐attenuated total reflectance (ATR) Fourier transform infrared (FTIR) spectroscopy as a forensic tool. Micro‐ATR FTIR spectra for signatures written with 63 ballpoint pens available commercially in Korea were obtained and used to construct an FTIR spectral database. A library‐searching program was utilized to identify the manufacturer, blend, and model of each black ballpoint pen ink based upon their FTIR peak intensities, positions, and patterns in the spectral database. This FTIR technique was also successfully used in determining the sequence of homogeneous line intersections from the crossing lines of two ballpoint pen signatures. We have demonstrated with a set of sample documents that micro‐ATR FTIR is a viable nondestructive analytical method that can be used to identify the origin of the ballpoint pen ink used to mark signatures.     

Forensic analysis of bicomponent fibers using infrared chemical imaging

The application of infrared chemical imaging to the analysis of bicomponent fibers was evaluated. Eleven nominally bicomponent fibers were examined either side-on or in cross-section. In six of the 11 samples, infrared chemical imaging was able to spatially resolve two spectroscopically distinct regions when the fibers were examined side-on. As well as yielding characteristic infrared spectra of each component, the technique also provided images that clearly illustrated the side-by-side configuration of these components in the fiber. In one case it was possible to prepare and image a cross-section of the fiber, but in general the preparation of fiber cross-sections proved very difficult. In five of the 11 samples, the infrared spectra could be used to identify the overall chemical composition of the fibers, according to a published classification scheme, but the fiber components could not be spatially resolved. Difficulties that are inherent to conventional "single-point" infrared spectroscopy, such as interference fringing and sloping baselines, particularly when analyzing acrylic type fibers, were also encountered in the infrared chemical image analysis of bicomponent fibers. A number of infrared sampling techniques were investigated to overcome these problems, and recommendations for the best sampling technique are given. Chemical imaging results were compared with those obtained using conventional fiber microscopy techniques.     

Classification of black powder toners on the basis of integrated analytical information provided by Fourier transform infrared spectrometry and X-ray fluorescence spectrometry

Differentiating between black powder toners used in laser printers and copiers can be challenging for forensic examiners. One hundred and sixty-two samples from 82 different types of cartridges produced by 21 manufacturers that are currently available on the Polish market were studied using Fourier transform infrared spectrometry (FT-IR) and energy-dispersive X-ray fluorescence spectrometry (XRF). The spectra obtained by these two methods were classified into 14 groups and 28 groups using FT-IR and XRF, respectively. These classifications served as a basis for the development of an analytical scheme for differentiating black powder toners. This scheme can be used with any two methods that supply different information about an examined sample. The research will show that if two samples are similar in polymer composition (e.g., FT-IR spectra), additional quantitative elemental composition from XRF analyses may provide more discrimination. It was possible to differentiate 82.5% pairs of examined samples using only FT-IR, 90.8% pairs of examined samples using only XRF, and 95.8% pairs of examined samples using these two methods. Obtained spectra and all the available information could be used to create/build a database. The results obtained confirm the multiplicity and compatibility of toners. Additionally, it was stated that not all the samples were original (OEM).     

Examination of heterogeneous crossing sequences between toner and rollerball pen strokes by digital microscopy and 3-D laser profilometry

The determination of line crossing sequences between rollerball pens and laser printers presents difficulties that may not be overcome using traditional techniques. This research aimed to study the potential of digital microscopy and 3-D laser profilometry to determine line crossing sequences between a toner and an aqueous ink line. Different paper types, rollerball pens, and writing pressure were tested. Correct opinions of the sequence were given for all case scenarios, using both techniques. When the toner was printed before the ink, a light reflection was observed in all crossing specimens, while this was never observed in the other sequence types. The 3-D laser profilometry, more time-consuming, presented the main advantage of providing quantitative results. The findings confirm the potential of the 3-D laser profilometry and demonstrate the efficiency of digital microscopy as a new technique for determining the sequence of line crossings involving rollerball pen ink and toner.     

Determination of the Sequence of Intersecting Lines Between Toners and Seals by Laser Fluorescence Microscope

Fluorescence microscope is considered to be one of the most effective ways to examine the sequence of intersecting seal and toner lines of questioned documents. In reality, however, the toner (mainly divided into compact and noncompact toners) and seal of a questioned document have such a complex morphology and sequence of crossing lines that current methods cannot meet the requirement of practical document identification. In view of the challenges of document examination, a laser fluorescence microscope and method are developed in this study. The developed microscope provides additional functionality to traditional fluorescence microscopes of transmitted light modality, laser excitation, selectable excitation wavelength, and selectable fluorescence filters. The results obtained from the method of comparisons between transmitted light and fluorescence modalities were positive under most conditions, particularly for noncompact toner examination for which a 100% accuracy rate and 90% detection rate were achieved in blind testing.     

An evaluation of matching unknown writing inks with the United States International Ink Library

Utilizing a database of standards for forensic casework is a valuable resource. Undoubtedly, as more standards (and corresponding information about the specimens) are collected, there is a greater certainty of identification when a questioned and a known item cannot be distinguished after a series of analyses. The United States Secret Service and the Internal Revenue Service National Forensic Laboratory jointly maintain the largest known forensic collection of writing inks in the world, which is comprised of over 8500 ink standards collected worldwide, dating back to the 1920s. This study was conducted to evaluate the reliability of matching arbitrarily purchased pens with known inks from a database. One hundred pens were randomly obtained from a variety of sources and their respective ink compositions were compared with standards. Eighty-five of the inks were determined to be suitable for comparison utilizing optical examinations and thin-layer chromatography. Three of the inks did not match any of the specimens on record; one of these inks was similar to an ink from an identical brand of pen that was in the database, but had a modified formulation.     

Determination of the sequence of intersecting lines using Focused Ion Beam/Scanning Electron Microscope

The aim of this study was to verify that the combination of focused ion beam (FIB) and scanning electron microscope/energy‐dispersive X‐ray (SEM/EDX) could be applied to determine the sequence of line crossings. The samples were transferred into FIB/SEM for FIB milling and an imaging operation. EDX was able to explore the chemical components and the corresponding elemental distribution in the intersection. The technique was successful in determining the sequence of heterogeneous line intersections produced using gel pens and red sealing ink with highest success rate (100% correctness). These observations show that the FIB/SEM was the appropriate instrument for an overall examination of document.     

The discrimination potential of ultraviolet-visible spectrophotometry, thin layer chromatography, and Fourier transform infrared spectroscopy for the forensic analysis of black and blue ballpoint inks

The knowledge of the discriminating power of analytical techniques used for the differentiation of writing inks can be useful when interpreting results. Ultraviolet-visible (UV-VIS) spectrophotometry, thin layer chromatography (TLC), and diffuse reflectance Fourier transform infrared spectroscopy (FT-IR) were used to examine a population of 21 black and 12 blue ballpoint writing inks. Based on corroborative results of these methods, the discrimination power for UV-VIS, TLC, and FT-IR was determined to be 100% and 98% for the black and blue inks, respectively. Generally, TLC and UV-VIS can be used to differentiate the colorant components (i.e., dyes and some pigments) found in inks. As FT-IR can be utilized to identify some of the noncolorant components, it was determined to be an excellent complementary technique that can be implemented into an analytical scheme for ink analysis.     

Diary of an astronaut: examination of the remains of the late Israeli astronaut Colonel Ilan Ramon's Crew Notebook recovered after the loss of NASA's space shuttle Columbia

Two months after the fatal re-entering into the Earth's atmosphere of Columbia flight STS-107, the remains of Israeli astronaut Colonel Ilan Ramon's Crew Notebook were found strewn in a field in San Augustine County, TX. The random pile of papers was found to have survived the calamity of the Shuttle's disintegration remarkably well. Most of the papers recovered were torn and/or washed out to varying degrees but only mildly charred around the edges. The sheets of paper could be categorized into four groups: Group I: eight sides of paper written while in space in black ink and in pencil--Ramon's personal diary; the writing on these eight sides of paper survived well and is only missing where the pages were torn. Small fragments found in the field were physically matched to holes in the pages thus locating their original positions in the text. Group II: six sides of technical preparation notes written by Ramon before the mission. The writing on these pages was washed out entirely, but much of it was visualized using infrared luminescence. Group III: eight sides of personal notes prepared by Ramon before the mission written in blue ink. The writing on these pages was barely visible to the naked eye and not visualized by infrared luminescence, but was made largely legible by digital enhancement imaging. Group IV: a few sides of printed technical information. These pages were mostly intact and were not examined at length as they contained standard printed material. After completion of examinations at the Questioned Document Laboratory of the Israel Police, the diary was transferred to the Paper Conservation Department of the Israel Museum for preservation and strengthening treatments.     

An Examination of the Sequence of Intersecting Seal and Laser Printing Toner Line

Examining the sequence of intersecting seal and laser printing line is a significant method of determining the authenticity and validity of documents. In this study, five brands of stamp pad inks, three types of inkpads and seven kinds of laser printers were used to make heterogeneous line intersections. Observation method of physical characteristics, scraping technique and fluorescence method was used to determine the sequence of intersecting lines. Distinguishing features were noted between the materials produced in both sequences. As the results obtained from the study were positive, these features might provide a scientific basis for accurately determining the sequence between laser printing line and inkpad (stamp pad ink) seal.     

Investigation into the merits of infrared imaging in the investigation of tattoos postmortem

Infrared imaging has a history of use in the forensic examination of artwork and documents and is investigated here for its wider use in the detection of tattoos on the human body postmortem. Infrared photographic and reflectographic techniques were tested on 18 living individuals, displaying a total of 30 tattoos. It was observed that neither age, sex, age of the tattoo, nor, most significantly, skin color affected the ability to image the tattoos using infrared imaging techniques. Second, a piglet carcass was tattooed and the impact of the decomposition process on the visibility of the tattoos assessed. Changes were recorded for 17 days and decomposition included partial mummification and skin discoloration. Crucially, the discoloration was recorded as greatly affecting the image quality using conventional photography, but was insignificant to the infrared recording of these tattoos. It was concluded that infrared reflectography was beneficial in the investigation into tattoos postmortem.     

The use of filtered light for the evaluation of writing inks analyzed using thin layer chromatography

Thin layer chromatography (TLC) is a scientific methodology that can be used to compare and characterize ink formulations. Occasionally, when evaluating chromatographic profiles on a TLC plate with ambient light, different ink formulations, or the same inks from different batches, may appear indistinguishable. The use of filtered light can be very effective to illuminate characteristics that are not readily apparent with ambient light. There are a diverse number of components commonly found in writing inks, and it may be that some of them respond to particular wavelengths of energy that are not visible to the unaided eye (i.e., colorless). There has been very little information published that addresses the use of filtered light for evaluating TLC plates. Twenty-nine ballpoint writing ink samples were selected for TLC analysis. Further evaluation using an alternate light source, coupled with the appropriate filter, proved to be an effective means for definitive discrimination in some cases.     

The application of infrared chemical imaging to the detection and enhancement of latent fingerprints: method optimization and further findings

Fourier transform infrared (FTIR) chemical imaging allows the collection of fingerprint images from backgrounds that have traditionally posed problems for conventional fingerprint detection methods. In this work, the suitability of this technique for the imaging of fingerprints on a wider range of difficult surfaces (including polymer banknotes, various types of paper, and aluminum drink cans) has been tested. For each new surface, a systematic methodology was employed to optimize settings such as spectral resolution, number of scans, and pixel aggregation in order to reduce collection time and file-size without compromising spatial resolution and the quality of the final fingerprint image. The imaging of cyanoacrylate-fumed fingerprints on polymer banknotes has been improved, with shorter collection times for larger image areas. One-month-old fingerprints on polymer banknotes have been successfully fumed and imaged. It was also found that FTIR chemical imaging gives high quality images of cyanoacrylate-fumed fingerprints on aluminum drink cans, regardless of the printed background. Although visible and UV light sources do not yield fingerprint images of the same quality on difficult, nonporous backgrounds, in many cases they can be used to locate a fingerprint prior to higher quality imaging by the FTIR technique. Attempts to acquire FTIR images of fingerprints on paper-based porous surfaces that had been treated with established reagents such as ninhydrin were all unsuccessful due to the swamping effect of the cellulose constituents of the paper.     

In situ Study on the Diffusion Kinetics of Seal Ink by Microinfrared Spectroscopy

In document examination, it is of great importance to determine the composition of seal ink with different imprint times, and spectroscopic methods are widely used today. In this research, the diffusion of seal inks from three different brands on the same type of paper is monitored in situ by microinfrared spectroscopy and microinfrared imaging technology. The area of the absorption peak at 1743 cm^?1 gradually decreases with increasing diffusion time. The diffusion kinetics of seal ink on paper are also studied by analyzing the infrared spectra of seal inks at the same measuring point with different diffusion times. The research provides a basic study in understanding the diffusion behavior of seal ink on paper over short time spans.     

The detection of multiply charged dyes using matrix-assisted laser desorption/ionization mass spectrometry for the forensic examination of pen ink dyes directly from paper

Abstract:  Laser desorption mass spectrometry (LDMS) is emerging as a technique for questioned document examination. Its use is limited to detecting ink dyes that are neutral or singly charged. Several inks contain dyes that are multiply charged and LDMS cannot be employed for their identification. We have successfully detected >20 polyionic dyes that can be used in the manufacture of inks using matrix-assisted laser desorption/ionization (MALDI) MS, directly from paper, with the matrix, 2-(4-hydroxyphenylazo)benzoic acid (HABA), and the additive, diammonium hydrogen citrate (DAHC). For example, Acid Violet 49, a charged dye containing one positively-charged site and two negatively charged sulfonate groups, cannot be detected by LDMS, but forms intact, singly charged ions in the MALDI MS experiment. The method described is also useful for identifying multiply charged dye mixtures that are used in modern pen inks.     

Forensic applications of infrared imaging for the detection and recording of latent evidence

We report on a simple method to record infrared (IR) reflected images in a forensic science context. Light sources using ultraviolet light have been used previously in the detection of latent prints, but the use of infrared light has been subjected to less investigation. IR light sources were used to search for latent evidence and the images were captured by either video or using a digital camera with a CCD array sensitive to IR wavelength. Bloodstains invisible to the eye, inks, tire prints, gunshot residue, and charred document on dark background are selected as typical matters that may be identified during a forensic investigation. All the evidence types could be detected and identified using a range of photographic techniques. In this study, a one in eight times dilution of blood could be detected on 10 different samples of black cloth. When using 81 black writing inks, the observation rates were 95%, 88% and 42% for permanent markers, fountain pens and ball-point pens, respectively, on the three kinds of dark cloth. The black particles of gunshot residue scattering around the entrance hole under IR light were still observed at a distance of 60 cm from three different shooting ranges. A requirement of IR reflectivity is that there is a contrast between the latent evidence and the background. In the absence of this contrast no latent image will be detected, which is similar to all light sources. The use of a video camera allows the recording of images either at a scene or in the laboratory. This report highlights and demonstrates the robustness of IR to detect and record the presence of latent evidence.     

Exploitation of the Ultraviolet Properties and Machine Cut Edges of Paper to Associate and Sequence Sheets in a Ream

Previously unreported line patterns visible under ultraviolet light were observed on a proportion of plain white A4 printer/copier paper from different manufacturers. These Ultraviolet Line Patterns (UVLPs) usually appear as stripes down the vertical length of the paper. Typically, the UVLPs were found to “repeat” through the ream in a predictable way, while also changing. It is postulated that the repeating nature of the UVLPs is a result of the way that paper is manufactured. This leads to the ability to sequence the sheets compared to their original source paper. Even in the absence of UVLPs, it is possible to use our observation of the manufacturing process to anticipate the order of several sheets of paper and conclusively associate them, in some cases, by physically fitting their machine cut edges and crossing paper fibers. Such a novel approach to examining questioned documents would be highly useful in forensic casework.