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Official websites use. Share sensitive information only on official, secure websites. Synthetic cannabinoids SCs make up a class of novel psychoactive substances NPS , used predominantly in prisons and homeless communities in the U. SCs can have severe side effects, including psychosis, stroke, and seizures, with numerous reported deaths associated with their use. The chemical diversity of SCs presents the major challenge to their detection since approaches relying on specific molecular recognition become outdated almost immediately. Ideally one would have a generic approach to detecting SCs in portable settings. The problem of SC detection is more challenging still because the majority of SCs enter the prison estate adsorbed onto physical matrices such as paper, fabric, or herb materials. That is, regardless of the detection modality used, the necessary extraction step reduces the effectiveness and ability to rapidly screen materials on-site. Herein, we demonstrate a truly instant generic test for SCs, tested against real-world drug seizures. The test is based on two advances. First, we identify a spectrally silent region in the emission spectrum of most physical matrices. Second, the finding that background signals including from autofluorescence can be accurately predicted is based on tracking the fraction of absorbed light from the irradiation source. Finally, we demonstrate that the intrinsic fluorescence of a large range of physical substrates can be leveraged to track the presence of other drugs of interest, including the most recent iterations of benzodiazepines and opioids. We demonstrate the implementation of our presumptive test in a portable, pocket-sized device that will find immediate utility in prisons and law enforcement agencies around the world. The major body of evidence suggests that these are cannabinoid receptor agonists, hence the common acronym synthetic cannabinoid receptor agonists SCRAs , but there is mounting evidence for interaction with other receptors and enzymes. SCs are the dominant NPS and one of the most used drugs within the prison estate. SC-soaked personal mail is a well-established mechanism of entry of SCs into prisons and can be effectively ameliorated through screening of personal mail and photocopying. Typically, lab-based identification is achieved through hyphenated techniques such as gas chromatography mass spectrometry GC-MS or liquid chromatography mass spectrometry LC-MS. For example, devices that utilize ion mobility spectrometry IMS , Raman spectroscopy, and near-infrared IR NIR spectroscopy are commercially available and have been successfully implemented in many prisons and drug checking sites globally. We have previously demonstrated that SCs can be accurately detected using fluorescence spectral fingerprints FSFs —enumerated excitation emission matrices. An example is shown in Figure 1 A. Such detection would be beneficial for point-of-care analysis to assess patients who are nonresponsive but are suspected of SC use. C1 — C4 correspond to the spectral windows captured by each of the band-pass filters in the device described below. Excitation for the spectra was at nm. However, more recent variants show a similar emission profile, i. The notable exception are OXIZIDs, a recent generation of SCs with an oxoindole core, 21 , 22 where the emission band is red-shifted, and we discuss this below. Potentially, generic discrimination of SCs might not require a full FSF but instead observation of the major emission band using a single excitation wavelength. We hypothesize that with a sufficiently intense irradiation source, SC fluorescence might be observable deconvolved from the autofluorescence of the physical substrate onto which it is adsorbed, without requiring a full FSF to be collected. Herein, we detail the confirmation of this hypothesis and its implementation into an ultraportable, hand-held device, allowing instant detection of SCs on a broad range of materials. We further illustrate the potential of this approach to detect other drugs of abuse. Figure 1 B shows an example of spectra acquired via excitation using a nm light-emitting diode LED for a seized paper sample in the presence and absence of an SC. These data are collected via direct irradiation of the sample no extraction of the sample required , with spectral acquisition via a fiber optic attached to a spectrometer. The reflected light retains the spectral characteristics of the incident source, including the center wavelength and bandwidth. The magnitude of detected light in this spectral region will vary according to the intensity of the source, the absorption of the incident light by the sample matrix including the analyte , and specular reflection. This spectral region is an absolute minimum of the acquired spectrum when it is irradiated at UV—C wavelengths. To note, we do not anticipate that this region is spectrally silent at all excitation wavelengths. The total emission in this region will be determined by the background signal primarily arising from the irradiation source; C1 , the quantum yield of the SC, its concentration, and quenching by the matrix material including via fluorescence resonance transfer FRET to endogenous molecules see below. At higher concentrations, we find that the signal saturates as one anticipates from the classical inner filter effect. At least for the range of samples we have studied, we find that a large emission band in the C3—C4 region is correlated with optically bright materials, e. That is, any material treated with such agents is likely to display a similar emission profile. Materials that are not treated with such agents may display diffuse emission bands that can be attributed to endogenous fluorophores or scattering. In practice, we find that matrices such as brown papers and untreated fabrics have exceptionally low emission in this spectral region so as to be effectively spectrally silent. Given that the C2 region is spectrally silent for essentially all paper, fabric, and herb materials we have surveyed, we hypothesized that detection of SCs would be possible by sensitively monitoring emission in this region, subtracted from the background. We tested our hypothesis using seized, suspected SC materials, obtained from the Avon and Somerset Police between and , adsorbed onto different physical matrices. The identity of SC compounds in these samples are reported in Table S1. Out of these samples, 6 samples contained no SC. TLC was used for the initial comparison and as an indication of the number of SC compounds present. Running NMR analysis in tandem with LC-MS detection was invaluable for identifying compounds with virtually indistinguishable mass spectra, e. Figure 2 shows the spectra acquired from these samples. Figure 2 D shows exemplars of these materials, although they vary significantly in presentation. Figure 2 G shows example processed spectra in which SCs were detected on the physical matrix with no processing. Figure 2 H shows the integral of the C2 region for each of the samples tested. Direct spectral acquisition of samples seized by Avon and Somerset Police, suspected to have SCs present. G Highlighted spectrally silent C2 region as in Figure 1 with examples from the panels above paper and herb spectra with and without SC. H Integral of the spectral C2 region, ranked by magnitude and annotated with the detected material in the inset. Excitation for spectra was at nm. While there are several reports of cannabis giving a measurable fluorescence signal, at least for the excitation wavelengths used here, there is no detectable signal. As we expect from the structures, our data do not show a signal arising from these molecules at least at the concentrations present nor do we expect any significant quenching effect from such molecules. The data in Figure 2 suggest that the integration of spectral data could be a means to identify SCs on complex matrices without any processing of the sample. We have therefore developed a device capable of high sensitivity detection within each of the spectral regions of interest Figure 2. The device is shown in Figure 3. The device consists of an array of photodiodes PDs with wavelength selection via a band-pass BP filter. The PDs are amplified and with detection maxima optimized for the spectral region of interest, as described in the Materials and Methods section. Data for each of C1—C4 are collected via an analog to digital converter ADC and passed to a microcontroller. The data are returned as a raw signal, essentially a voltage. The data are then numerically manipulated described below to give a visual report of the presence and absence of SCs through lights on the exterior of the device Figure 3 C. Also see Figure S2 for further views of the device, including a battery-operated version. We posit that the small amount of variance is related to internal heating from the heat sink. However, these data demonstrate that the data are consistent and reproducible with the device. Schematic of the SC detection device. Panels A, B show a three-dimensional 3D printed housing for an assembly comprising the following: Band-pass BP filters corresponding to each spectral region C1—4; Figure 1 B are paired with a powered photodiode PD optimized for that spectral region. The optical elements are protected via a sapphire window aligned with the optical path and focal length of the PDs. The assembly is protected by an exterior shell with integrated vents aligned with the heat sink of the LED. User signal reporting is via an integrated LED ring on the top of the device. Panel C shows the external case, and further views of the fully constructed device are given in Figure S2. From Figure 2 H, the magnitude of the SC signal may be varied. Potentially, one can apply an empirical threshold based on the observation of a large number of samples with known backgrounds. Ideally, one would a priori know the background signal and the expected magnitude of signal change for an SC on any given physical matrix. Figure 4 A shows the plot of the values of C1 versus C2 for a range of physical matrices including paper a range of colored paper with a range of inks, including printed, crayon, pencil, etc. From Figure 4 A, as the magnitude of C1 increases, C2 increases. These data can be fit using a linear relationship. This relationship is shown as the fitted solid red line in Figure 4 A. The presence of this relationship seems logical since as a material becomes more absorptive, the background signal arising from the irradiation will decrease and vice versa. However, the simplified trend shown in Figure 4 A gives a useful framework, as we describe below. Predictive model for quantifying the background signal arising from the abroad range of physical matrices collected on the device described in Figure 3. A Relationship between the magnitude of C1 and C2. The solid fitted red line is a simple exponential function fitted to the data. The blue dashed is the threshold based on how the C2 signal of SCs varies on matrices as shown in panel B. B How the C2 signal varies for a range of SCs on a selection of white and brown papers. The consistent trend followed in Figure 4 A provides a means to calculate the predicted background at C2 C2 pred from a collected reading of C1. That is, the red fitted line in Figure 4 A reflects C2 pred. These data demonstrate an accurate, predictive model for the background signal arising in the spectral region where SC fluorescence emission is detected. From Figure 4 A, using this C2 pred solely to assess a cutoff for the presence of SCs will lead to a large fraction of false positives. A simple route to tackling this is to arbitrarily scale C2 pred to give an acceptable false positive rate. Next, we assessed how the signal of C2 varied for a range of SCs, at similar concentrations, on a range of different matrices with increasing C1 signals. That is, a value above 1 is attributable to the SC alone. Figure 4 B shows the relationship between the average magnitude of this ratio and the measured value of C1. From Figure 4 B, there is an evident increase in the ratio of the SC signal for the same molecules as the magnitude of C1 increases on different matrices. The trend in Figure 4 B can be quantified using a simple linear function blue fitted line in Figure 4 B. That is, the greater the light absorption of the material smaller C1 , the smaller the increase in signal at C2 for the same concentration of the analyte. This indicates that detection could be more sensitive on more highly reflective materials, such as white paper, that are commonly used for drug entry routes into prisons. We can convolve this numerical relationship with the predicted background in Figure 4 A to give a threshold for detection of the analyte, shown as the dashed blue line in Figure 4 A. Signals above this threshold trigger the device alarm lights. This function then accounts for both the change in the predicted background and the anticipated increase in the magnitude of C2 at various C1 values. Our data then provide two key pieces of information. First, there is a quantifiable relationship that relates the magnitudes of C1 and C2; we can accurately predict the background signal of C2 using a simple function. Second, scaling the C2 pred values to produce a threshold for SC detection can be tailored to balance sensitivity and specificity. Combining these thus provides a numerical model for the detection of SCs on a huge range of diverse background materials and is scalable with SC concentration. We note that this curve can be scaled to remove false positives with a concomitant decrease in concentration sensitivity. Figure 3 shows the design of a device that integrates both the optical detection methodology and the numerical analysis, as described above. Using this device, we have assessed detection on a very large range of matrices including paper white, brown, blue, pink, printed, and unprinted , fabric cotton and synthetic at a range of colors and thicknesses , and herb materials as described above. We show a video of the device working with a range of seized materials in Movie S1. In an effort to assess the sensitivity and specificity of this approach and device with real-world data, we conducted a trial of a large number of paper letters, cards, etc. Clearly, the detection sensitivity of the device will be vastly less than GC-MS, and so the device will not be competitive in this sense. Therefore, to give a realistic assessment of the device, we removed samples that only showed trace amounts of SCs detected by GC-MS and envelopes that had contained positive SC materials. This resulted in samples tested with the device Table S2. This highlights how the thresholding to detection can be increased or decreased to balance false positives against sensitivity, as desired. The degree of difference this makes to sensitivity will depend on the number of borderline samples, those containing lower concentrations or lower quantum yield SCs, that are present. That the sensitivity value is so high therefore reflects a very competitive detection modality. These data therefore point to an extremely effective tool in the rapid screening of materials for the presumptive presence of SCs. Identification of a range of illegal drugs via quenching of C3 relative to C4, with data collected on the device described in Figure 3 A—C. The solid red line is the fit to a simple linear function and is to aid the eye only. C, D Absorption spectra solid lines for specific molecules E and example emission spectrum from white paper black dashed line; relative emission. The gray-colored region represents absorption arising primarily from benzene ring systems and other aromatic species. The red-colored region represents absorption features attributable to extended conjugated systems. The blue-colored region represents the bulk of emission putatively attributable to OBAs as discussed above. If our hypothesis is valid—that analytes with absorption spectra overlapping the putative OBA emission band can be detected as a change in the OBA emission spectra—notionally other molecules might be detectable in a similar way. Figure 5 B shows the resultant data. The absorption spectra for these compounds are shown in Figure 5 C, 5 D. We note that these absorption spectra are not collected on the described device but using a benchtop absorption spectrometer. Moreover, it is interesting to note that even where common absorptive compounds are added to paper e. That is, the detection setup shown in Figure 3 is capable of detecting not only SCs but also a very large range of illicit substances present on paper, without false positives arising from generic aromatic benzene-based moieties. Given that the detection is based on shifts in putative OBA emission, we anticipate that the detection will be similarly possible on fabric or other materials treated with OBAs. SCs are a critical concern in the U. Indeed, a recent study found that SCs were linked to nearly half of male non-natural deaths in prisons in England and Wales. Similarly, benzodiazepines have grown dramatically in their use in prisons, overtaking SCs as the major NPS in some cases. Detecting these drugs on complex matrices is imperative to stemming the flow into prisons and affecting the revenue stream that funds organized crime. In this study, we have shown that many materials paper, fabric, herb give a consistent emission spectrum when excited with a ultraviolet UV source nm. The spectra include an optically silent region in which SCs emit. In addition, the magnitude of the background in this region can be predicted with a high degree of accuracy based on the intensity of the reflected excitation light alone. This enables assignment of a background signal based on the absorption of the irradiation light, giving the ability to fine-tune the detection of SCs depending on the desired specificity or false positive rate required. Finally, emission arising from putative OBA fluorescence is remarkably consistent, and variation of this spectral feature can be used to detect the presence of low-quantum-yield SCs, such as OXIZIDs, and other more complex cross-conjugated compounds, including benzodiazepines. We demonstrate that these advances can be implemented in a low-cost hand-held device with essentially instant detection. We note the future potential for enhanced chemometric approaches with the same hardware solution including the potential for machine learning to discriminate complex signals. The device will find immediate utility in relevant operational settings that include prisons but also for border security and within community programs to decrease the flow of SCs. Moreover, our finding that the detection modality can also be used to detect other NPS suggests a scalable application across different settings where different illegal drugs are present. The filtrate was collected, and the pellet was discarded. TLC spots were compared against the other samples for potential matches. The methanol was removed under reduced pressure, and the sample was redispersed in the chosen NMR solvent. Coupling constants, J, are reported in Hz. The MS was calibrated using reference calibrant introduced from the independent ESI reference sprayer. The MS was operated in all-ion mode with 3 collision energy scan segments at 0, 20, and 40 eV. The column was operated at a flow rate of 0. The VWD was set to detect at and nm wavelengths at a frequency of 2. The results were also searched against an NPS database containing compound entries with a forward score of 25, a reverse score of 70, and mass tolerances within 5 ppm of the reference library matches. Fluorescence emission spectra were collected using an Edinburgh Instruments FS5 spectrophotometer. Typically, excitation and emission slit widths were set at 1. In all cases, a quartz cell was used to collect spectral data. The device design is described in the main text Figures 3 and S2. Movie showing the ultraportable device detection of synthetic cannabinoids on variety of physical matrices Movie S1 MP4. The manuscript was written through contributions of all authors. All authors have given approval to the final version of the manuscript. This section collects any data citations, data availability statements, or supplementary materials included in this article. As a library, NLM provides access to scientific literature. Anal Chem. Find articles by Gyles E Cozier. Find articles by Rachael C Andrews. Find articles by Anca Frinculescu. Find articles by Ranjeet Kumar. Find articles by Benedict May. Find articles by Tom Tooth. Find articles by Peter Collins. Find articles by Andrew Costello. Find articles by Tom S F Haines. Find articles by Tom P Freeman. Find articles by Ian S Blagbrough. Find articles by Jennifer Scott. Find articles by Trevor Shine. Find articles by Oliver B Sutcliffe. Find articles by Stephen M Husbands. Find articles by Jonathan Leach. Find articles by Richard W Bowman. Find articles by Christopher R Pudney. Published by American Chemical Society. Open in a new tab. Similar articles. Add to Collections. Create a new collection. Add to an existing collection. 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Opiate addiction affects young adults whose life expectancy is reduced as a consequence of their habit. In the midst of the AIDS epidemic, the present study objective was to analyse recent overall and cause-specific mortality trends among opiate addicts in Catalonia Spain. Mortality was assessed retrospectively in an opiate addict cohort assembled from admissions to hospital emergency wards and drug treatment centres during the period — The cohort included 15 opiate addicts 12 men and women aged 15—44 years. Overall and cause-specific mortality trends were analysed using age as the time scale and Cox regression with staggered entry determined by the age at entry in the study. Mortality rates increased throughout the entire period from In a model including age, gender, source of entry and length of drug use, risk increased significantly in men and for longer length of use, but not with age and for source of entry into the study cohort. The causes of death associated with high mortality rates were AIDS and the causes directly related to addiction. A threefold increase in mortality rates was observed during the period, mainly accounted for by AIDS and direct addiction-related causes. Length of opiate use was an important determinant of mortality. Access to content on Oxford Academic is often provided through institutional subscriptions and purchases. If you are a member of an institution with an active account, you may be able to access content in one of the following ways:. Typically, access is provided across an institutional network to a range of IP addresses. This authentication occurs automatically, and it is not possible to sign out of an IP authenticated account. Choose this option to get remote access when outside your institution. Enter your library card number to sign in. If you cannot sign in, please contact your librarian. Many societies offer single sign-on between the society website and Oxford Academic. 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