Machine Learning Assisted LIBS Classification of Burnt and Unburnt Paper Samples: A Forensic Perspective

IF 6.1 1区 化学 Q1 CHEMISTRY, ANALYTICAL Talanta Pub Date : 2025-04-02 DOI:10.1016/j.talanta.2025.128073
Muhammad Nadeem , Muhammad Faheem , Maryam Manzoor , Amna Gulzar , Muhammad Bilal , Yasir Jamil
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Abstract

A crucial part of investigating into a possible arson case is analyzing the chemical makeup of the fire's effects. In order to identify the chemical makeup of burnt materials that are frequently found in homes and businesses, the current study attempts to explore the potential of LIBS in forensic applications including burning of as well as forgery in paper-based documents. Various kinds of paper were chosen as a model sample to investigate the potential of Laser induced breakdown spectroscopy (LIBS) in forensics. First of all, LIBS spectra were recorded for unburnt samples by using Nd: YAG laser operated at 532nm, by optimizing the specific energy and delay between the laser pulse and shutter of the spectrometer, their elemental compositions were evaluated. The plasma parameters such as, plasma temperature, and electron number density were studied comprehensively to validate the local thermodynamic equilibrium condition. The three different kinds of ignition sources namely disposable lighter, candle, and gas stove were used to burn the sample to check the variation in elemental composition after the burning process for forensic applications as these sources are often present in homes and workplaces. The LIBS results suggest that all the samples have almost the same elemental composition even after using various kinds of ignition sources. Therefore, machine learning was applied to LIBS data by recording 100 datasets for each sample when ignited with different sources. PCA discriminates the samples slightly, but supervised machine learning algorithms LDA, QDA, and Linear SVM showed superior i.e., 100 % classification accuracies for various datasets that suggest the machine learning-assisted LIBS is a promising tool for forensic applications.

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烧毁和未烧毁纸张样本的机器学习辅助 LIBS 分类:法医学视角
调查可能的纵火案的一个关键部分是分析火灾影响的化学成分。为了确定在家庭和企业中经常发现的燃烧材料的化学成分,目前的研究试图探索LIBS在法医应用中的潜力,包括焚烧和伪造纸质文件。以不同种类的纸张为模型样本,探讨激光诱导击穿光谱(LIBS)在法医鉴定中的应用潜力。首先,利用532nm波长的Nd: YAG激光记录了未燃烧样品的LIBS光谱,通过优化激光脉冲与光谱仪快门之间的比能量和延迟,对其元素组成进行了评估。对等离子体温度、电子数密度等参数进行了综合研究,验证了局部热力学平衡条件。三种不同的点火源即一次性打火机,蜡烛和煤气炉被用来燃烧样品,以检查法医应用中燃烧过程后元素组成的变化,因为这些来源经常存在于家庭和工作场所。LIBS结果表明,即使使用不同的点火源,所有样品的元素组成也几乎相同。因此,我们将机器学习应用于LIBS数据,记录每个样本在不同来源点燃时的100个数据集。PCA对样本略有区别,但监督机器学习算法LDA、QDA和线性支持向量机(Linear SVM)对各种数据集的分类准确率为100%,这表明机器学习辅助LIBS是一种很有前途的法医应用工具。
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来源期刊
Talanta
Talanta 化学-分析化学
CiteScore
12.30
自引率
4.90%
发文量
861
审稿时长
29 days
期刊介绍: Talanta provides a forum for the publication of original research papers, short communications, and critical reviews in all branches of pure and applied analytical chemistry. Papers are evaluated based on established guidelines, including the fundamental nature of the study, scientific novelty, substantial improvement or advantage over existing technology or methods, and demonstrated analytical applicability. Original research papers on fundamental studies, and on novel sensor and instrumentation developments, are encouraged. Novel or improved applications in areas such as clinical and biological chemistry, environmental analysis, geochemistry, materials science and engineering, and analytical platforms for omics development are welcome. Analytical performance of methods should be determined, including interference and matrix effects, and methods should be validated by comparison with a standard method, or analysis of a certified reference material. Simple spiking recoveries may not be sufficient. The developed method should especially comprise information on selectivity, sensitivity, detection limits, accuracy, and reliability. However, applying official validation or robustness studies to a routine method or technique does not necessarily constitute novelty. Proper statistical treatment of the data should be provided. Relevant literature should be cited, including related publications by the authors, and authors should discuss how their proposed methodology compares with previously reported methods.
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