Comparability of Raman Spectroscopic Configurations: A Large Scale Cross-Laboratory Study
Comparability of Raman Spectroscopic Configurations: A Large Scale Cross-Laboratory Study
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DOI：
10.1021/acs.analchem.0c02696
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发表时间：
2020-12-15
影响因子：
7.4
通讯作者：
Bocklitz, Thomas
中科院分区：
文献类型：
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作者：
Guo, Shuxia;Beleites, Claudia;Bocklitz, Thomas
拉曼光谱平台的可变配置是将拉曼光谱建立为临床诊断等现实场景中有价值的物理化学方法的主要障碍之一。对于诸如诊断分类之类的现实世界应用，模型理想情况下应该可用于预测来自不同设置的数据。无论是通过使用来自许多设置的数据训练坚固模型，还是通过主复制策略（在“主”设置上开发模型并在“复制”设置上生成测试数据）来完成，只有当来自不同设置的拉曼光谱一致、可再现和可比较时，这才有可能实现。然而，拉曼光谱对测量条件非常敏感，即使测量相同的样品，拉曼光谱也会因设置而异。尽管人们越来越认识到拉曼光谱对仪器配置的依赖性是一个问题，但人们还远未完全理解拉曼光谱，需要付出巨大的努力来解决由此产生的光谱变化并对其进行校正。为了明确情况的严重性，我们提出了一项循环实验，调查来自 COST（欧洲科学技术合作）行动 Raman4clinics 的 7 个欧洲国家 15 个研究所的 35 个不同配置的拉曼光谱设备的可比性。该实验的开发方式允许各种仪器配置，从高度共焦设置到具有不同激发波长的基于光纤的系统。我们从峰移、强度变化、峰宽和噪声水平的角度说明了仪器配置引起的光谱变化。我们在本文的结尾提出了可能有助于改进实验室间研究的建议。
The variable configuration of Raman spectroscopic platforms is one of the major obstacles in establishing Raman spectroscopy as a valuable physicochemical method within real-world scenarios such as clinical diagnostics. For such real world applications like diagnostic classification, the models should ideally be usable to predict data from different setups. Whether it is done by training a rugged model with data from many setups or by a primary-replica strategy where models are developed on a 'primary' setup and the test data are generated on 'replicate' setups, this is only possible if the Raman spectra from different setups are consistent, reproducible, and comparable. However, Raman spectra can be highly sensitive to the measurement conditions, and they change from setup to setup even if the same samples are measured. Although increasingly recognized as an issue, the dependence of the Raman spectra on the instrumental configuration is far from being fully understood and great effort is needed to address the resulting spectral variations and to correct for them. To make the severity of the situation clear, we present a round robin experiment investigating the comparability of 35 Raman spectroscopic devices with different configurations in 15 institutes within seven European countries from the COST (European Cooperation in Science and Technology) action Raman4clinics. The experiment was developed in a fashion that allows various instrumental configurations ranging from highly confocal setups to fibre-optic based systems with different excitation wavelengths. We illustrate the spectral variations caused by the instrumental configurations from the perspectives of peak shifts, intensity variations, peak widths, and noise levels. We conclude this contribution with recommendations that may help to improve the inter-laboratory studies.