Zhou Jiayuan, Huang Weihua, Sattar Harse, Hu Qiangwei, Liu Hongde, Wang Guangda, Zhang Deng, Guo Lianbo
Wuhan National Laboratory for Optoelectronics (WNLO), Huazhong University of Science and Technology, Wuhan, Hubei, 430074, China.
School of Integrated Circuits, Huazhong University of Science and Technology (HUST), Wuhan, Hubei, 430074, China.
Talanta. 2026 Jan 1;296:128453. doi: 10.1016/j.talanta.2025.128453. Epub 2025 Jun 12.
Laser-induced breakdown spectroscopy (LIBS) models are extensively utilized for rapid elemental measurements in various scientific and industrial applications. However, elemental differences in different matrices can cause huge deviations in the captured spectra, constituting a major bottleneck for the wide application of LIBS technique. Therefore, we proposed an innovative fusion method named acoustic-optical spectra fusion laser induced breakdown spectroscopy (AOSF-LIBS) to compensate the spectral deviations due to LIBS matrix effects. Based on the standard spectral intensity calculation model, five main factors affected by the spectral difference of the matrix were analyzed, and the deviation between the ideal spectrum and the actual spectrum was calculated. Subsequently, the acoustic signals were transformed from the time domain (LIPA) to the time-frequency domain (acoustic spectrogram) to fully characterize the time-frequency evolution of the rapidly varying pressure wave generated by the plasma. Extract energy and area information from the acoustic spectrogram to characterize the total number density and plasma acquisition direction length. Fusing them with the plasma temperature, electron number density, and elemental interference calculated from the LIBS spectra, a spectral deviation mapping model was established to compensate the spectral deviation caused by matrix effect. To verify the wide adaptability of AOSF-LIBS, the spectral deviations of four matrices, including aluminum, iron, titanium, and nickel matrices, is corrected. After being compensated by AOSF-LIBS, the R were all improved to more than 0.98, and the root mean square error (RMSE), mean absolute percentage error (MAPE), and relative standard deviation (RSD) of the training set decreased dramatically by 11.42 %, 42.33 % and 3.22 % on average, and those of the test set decreased by 11.40 %, 41.13 and 2.84 % on average. And the ablation study was conducted to verify the contribution of the acoustic signal in the deviation compensation model. The experimental results show that AOSF-LIBS can effectively compensate the spectral deviations of different matrices and realize high-precision elemental quantitative measurement. Therefore, AOSF-LIBS is expected to further promote the application of LIBS for elemental quantification.
激光诱导击穿光谱（LIBS）模型在各种科学和工业应用中被广泛用于快速元素测量。然而，不同基体中的元素差异会导致所采集光谱出现巨大偏差，这构成了LIBS技术广泛应用的主要瓶颈。因此，我们提出了一种名为声光光谱融合激光诱导击穿光谱（AOSF-LIBS）的创新融合方法，以补偿由于LIBS基体效应引起的光谱偏差。基于标准光谱强度计算模型，分析了受基体光谱差异影响的五个主要因素，并计算了理想光谱与实际光谱之间的偏差。随后，将声学信号从时域（LIPA）转换到时频域（声谱图），以充分表征由等离子体产生的快速变化压力波的时频演化。从声谱图中提取能量和面积信息，以表征总数密度和等离子体采集方向长度。将它们与从LIBS光谱计算得到的等离子体温度、电子数密度和元素干扰进行融合，建立了光谱偏差映射模型，以补偿由基体效应引起的光谱偏差。为了验证AOSF-LIBS的广泛适应性，对包括铝、铁、钛和镍基体在内的四种基体的光谱偏差进行了校正。经AOSF-LIBS补偿后，相关系数R均提高到0.98以上，训练集的均方根误差（RMSE）、平均绝对百分比误差（MAPE）和相对标准偏差（RSD）平均显著降低了11.42%、42.33%和3.22%，测试集的分别平均降低了11.40%、41.13%和2.84%。并且进行了烧蚀研究，以验证声学信号在偏差补偿模型中的贡献。实验结果表明，AOSF-LIBS能够有效补偿不同基体的光谱偏差，实现高精度元素定量测量。因此，AOSF-LIBS有望进一步推动LIBS在元素定量分析中的应用。
