Central Laser Facility, Research Complex at Harwell, STFC Rutherford Appleton Laboratory, UK Research and Innovation, Harwell Campus, Didcot OX11 0QX, United Kingdom.
School of Physics and Astronomy, University of Exeter, Exeter EX4 4QL, United Kingdom.
Anal Chem. 2021 May 4;93(17):6755-6762. doi: 10.1021/acs.analchem.1c00490. Epub 2021 Apr 22.
Spatially offset Raman spectroscopy (SORS) is a technique for interrogating the subsurface composition of turbid samples noninvasively. This study generically addresses a fundamental question relevant to a wide range of SORS studies, which is how deep SORS probes for any specific spatial offset when analyzing a turbid sample or, in turn, what magnitude of spatial offset one should select to probe a specific depth. This issue is addressed by using Monte Carlo simulations, under the assumption of negligible absorption, which establishes that the key parameter governing the extent of the probed zone for a point-like illumination and point-like collection SORS geometry is the reduced scattering coefficient of the medium. This can either be deduced from literature data or directly estimated from a SORS measurement by evaluating the Raman intensity profile from multiple spatial offsets. Once this is known, the extent of the probed zone can be determined for any specific SORS spatial offset using the Monte Carlo simulation results presented here. The proposed method was tested using experimental data on stratified samples by analyzing the signal detected from a thin layer that was moved through a stack of layers using both non-absorbing and absorbing samples. The proposed simple methodology provides important additional information on SORS measurements with direct relevance to a wide range of SORS applications including biomedical, pharmaceutical, security, forensics, and cultural heritage.
空间位移拉曼光谱(SORS)是一种非侵入式探测浑浊样品亚表面成分的技术。本研究一般性地解决了与广泛的 SORS 研究相关的一个基本问题,即当分析浑浊样品时,SORS 探针对于任何特定的空间偏移能探测多深,或者,为了探测特定的深度,应该选择多大的空间偏移。在假设吸收可以忽略不计的情况下,利用蒙特卡罗模拟解决了这个问题,该模拟确定了对于点状照明和点状收集 SORS 几何形状,控制探测区域范围的关键参数是介质的散射系数。这可以从文献数据中推断出来,也可以通过从多个空间偏移评估拉曼强度分布直接从 SORS 测量中估计。一旦知道了这个值,就可以使用这里给出的蒙特卡罗模拟结果来确定任何特定的 SORS 空间偏移的探测区域范围。通过分析使用非吸收和吸收样品在通过层叠的一系列层移动时从薄层检测到的信号,对分层样品的实验数据进行了测试。所提出的简单方法为 SORS 测量提供了重要的附加信息,与包括生物医学、制药、安全、法医和文化遗产等广泛的 SORS 应用具有直接相关性。