When Convolutional Neural Networks Meet Laser-Induced Breakdown Spectroscopy: End-to-End Quantitative Analysis Modeling of ChemCam Spectral Data for Major Elements Based on Ensemble Convolutional Neural Networks
Abstract
:1. Introduction
- Firstly, our model architecture is specially tailored for spectra analysis. Most deep learning models used currently in spectrum analysis employ ANN architectures imported from natural language processing or computer vision, and the details of the model architectures are often random.
- Secondly, unlike most of the data-driven deep learning models, we integrate prior domain knowledge of wavelength interval selection and screening into deep learning to improve the interpretation and robustness of learning systems.
- Lastly, compared with the traditional single modeling method, we provide a further extension by designing an ensemble method that can explicitly exploit the complementary knowledge from various submodels.
2. Materials and Methods
2.1. Basic Principles and Datasets of LIBS
2.2. CNN Modeling and Training Process
2.3. Optimization of the CNN Analysis Model
2.4. Quantitative Prediction Models for Comparison
2.5. Evaluation of the Prediction Model
3. Results
3.1. Comparison of the ECNN Model and the Traditional Chemometric Modeling Method
3.2. Influence of CNN Parameter Values on the Predictive Ability of the Model
3.3. Visualization of Features Extracted by the CNN Network
4. Discussion
4.1. Model Design
4.1.1. Number of Network Layers
4.1.2. Effects of Convolution Kernel Parameters
4.2. Understanding the Models
4.3. Future Development Trends
- Consider the measurement uncertainty that affects the results of the models: In several remote LIBS measurements, such as ChemCam, issues that limit the accuracy and precision of the elemental composition of targets are not necessarily related to the post processing of the data, but in some cases with the experimental conditions [54,55]. The proposed method should be tried out for more than just the chemical matrix effect, such as with different sample states, variable laser-target distances, etc.
- Implement data augmentation algorithms: As demonstrated in the part of the results section, a large enough training set size is crucial to the CNN model. However, as can be seen from Table 1, after the size of the calibration dataset was expanded, the range of the three elements was also greatly expanded. The most intuitive tendency may be the diversification of the samples in LIBS detection. The fine distinction between the sample quantity and the sample material diversity should be noted. In actual situations, the dataset is usually unbalanced and limited. Thus, the number of samples available for calibration modeling may be limited. In fact, this problem should be fundamentally solved by increasing the number of training samples for each material, that is, data augmentation. The augmentation simulates slightly different spectral acquisition scenarios (e.g., instrumental offset, background lighting, etc.) so that they created multiple (slightly different) copies of the original spectrum for the same target value. The training sample dataset can be remarkably expanded so the models can become robust to unseen variations. Actually, the problem of small dataset learning occurs in various practical applications [56,57,58], which confirms that the model which was established based on the original small dataset may not be inapplicable when predicting future samples, since they are also valid data. Thus, in our future work, we will try to fill the information gaps by systematically generating virtual samples.
- Design of lightweight models: Hardware deployment for lightweight models is also an important future research direction for Mars rovers. The CNN spectral analysis method is combined with portable hardware [36,59,60] to promote the practical application of portable spectrometers in various fields. Two-dimensional CNNs have unique advantages in image feature extraction, but 1D CNNs are better matches in terms of dimensionality. In addition, 1D CNN models have more compact structures and lower hardware requirements, making real-time, efficient, and low-cost complete configurations possible. Therefore, the authors would like to emphasize that the simpler the model, the easier it is to utilize and interpret in practical situations [61,62]. For example, to deploy a computational model in a realistic Mars environment, it is much more desirable to have a lighter, simpler model that can run on modest microprocessors than a highly complex architecture that demands more computation cost.
5. Conclusions
Author Contributions
Funding
Data Availability Statement
Acknowledgments
Conflicts of Interest
Appendix A. Hyperparameter Selection
- Effect of CKW on the Generalizability of the Prediction Model
- 2.
- Effect of NCK on the Generalizability of the Prediction Model
- 3.
- Effect of Stride Step on the Generalizability of the Prediction Model
- 4.
- Effect of Mini-Batch Size on the Generalizability of the Prediction Model
- 5.
- Paradigm for the Overall Design of CNN Parameters
- (1)
- The CKW should not be too small. If the CKW is too small, the convolution kernel extracts the characteristics in some subintervals that are not near the characteristic spectral line, and the model constructed based on these features usually has poor generalization performance. When the CKW is moderate, each feature captured by the convolution kernel contains spectral information near the characteristic spectral line, and the model constructed from these features usually has good generalization performance.
- (2)
- The NCK should not be too large. When the CKW is small, the number of features captured by a single convolution kernel is relatively large. In this case, if the NCK is continuously increased, the total number of features captured by all the convolution kernels will double, and the number of features will vastly exceed the number of samples, causing overfitting and a gradual decrease in the model’s predictive performance. In contrast, when the CKW is large, the model’s predictive performance increases, and after the NCK reaches a threshold value, further increasing the NCK slightly reduces the model’s predictive performance. Therefore, a higher NCK value is not necessarily better. When the CKW value is appropriate, the NCK should not exceed 60.
- (3)
- The stride step should be smaller than the CKW. When the stride step is small, more characteristics can be captured, which helps enhance the model’s prediction ability.
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Element | Set | No. of Samples | Concentration, wt% | |
---|---|---|---|---|
Range | Mean ± STD 1 | |||
Original calibration dataset | ||||
Si | Calibration | 200 | 8.70–75.41 | 49.46 ± 14.84 |
Prediction | 40 | 30.90–75.41 | 54.20 ± 13.35 | |
Al | Calibration | 200 | 0.17–23.71 | 11.56 ± 5.95 |
Prediction | 40 | 0.17–23.71 | 10.93 ± 5.11 | |
K | Calibration | 200 | 0.03–5.60 | 1.33 ± 1.37 |
Prediction | 40 | 0.05–5.43 | 1.56 ± 1.63 | |
Expanded calibration dataset | ||||
Si | Calibration | 1435 | 0.21–84.90 | 55.99 ± 14.38 |
Prediction | 287 | 0.21–84.63 | 56.35 ± 13.65 | |
Al | Calibration | 1435 | 0.01–38.79 | 15.48 ± 5.84 |
Prediction | 287 | 0.01–38.79 | 16.43 ± 5.91 | |
K | Calibration | 1435 | 0.002–12.05 | 2.51 ± 1.89 |
Prediction | 287 | 0.002–12.05 | 2.22 ± 1.89 |
Element | Model | Calibration | Prediction | ||
---|---|---|---|---|---|
Rc2 | RMSECV | Rp2 | RMSEP | ||
Original calibration dataset | |||||
Si | PLS | 0.9787 | 2.1614 | 0.9554 | 2.9609 |
ELM | 0.8376 ± 0.0487 | 5.9013 ± 0.8821 | 0.7601 ± 0.0360 | 6.9684 ± 0.5136 | |
CNN | 0.9789 ± 0.0071 | 2.2148 ± 0.3184 | 0.9724 ± 0.0173 | 2.2099 ± 0.6013 | |
ECNN1 | 0.9899 ± 0.0034 | 1.5561 ± 0.2847 | 0.9848 ± 0.0031 | 1.6728 ± 0.1759 | |
C-QuEST | 0.9695 | 2.5846 | 0.9287 | 3.7354 | |
Al | PLS | 0.9837 | 0.7579 | 0.9540 | 1.1499 |
ELM | 0.8795 ± 0.0228 | 2.0529 ± 0.1909 | 0.7614 ± 0.0384 | 2.5271 ± 0.2042 | |
CNN | 0.9869 ± 0.0059 | 0.6983 ± 0.1235 | 0.9768 ± 0.0126 | 0.8326 ± 0.1841 | |
ECNN1 | 0.9927 ± 0.0020 | 0.5799 ± 0.0431 | 0.9868 ± 0.0015 | 0.6785 ± 0.0898 | |
C-QuEST | 0.9577 | 1.2220 | 0.8862 | 1.8028 | |
K | PLS | 0.9768 | 0.2079 | 0.9636 | 0.3280 |
ELM | 0.8272 ± 0.0329 | 0.5651 ± 0.0555 | 0.7895 ± 0.0400 | 0.7746 ± 0.0906 | |
CNN | 0.9813 ± 0.0079 | 0.2134 ± 0.0411 | 0.9632 ± 0.0536 | 0.3345 ± 0.1275 | |
ECNN1 | 0.9885 ± 0.0039 | 0.1907 ± 0.0447 | 0.9834 ± 0.0028 | 0.2545 ± 0.0374 | |
C-QuEST | 0.9605 | 0.2714 | 0.8714 | 0.6057 | |
Expanded calibration dataset | |||||
Si | PLS | 0.8888 | 4.6200 | 0.8839 | 4.8997 |
ELM | 0.8861 ± 0.0743 | 4.6073 ± 1.4011 | 0.8751 ± 0.0831 | 4.7240 ± 1.3965 | |
CNN | 0.9163 ± 0.0851 | 3.8111 ± 1.6685 | 0.9053 ± 0.0942 | 3.8803 ± 1.6132 | |
ECNN1 | 0.9345 ± 0.0608 | 3.4640 ± 1.2408 | 0.9270 ± 0.0669 | 3.4894 ± 1.1912 | |
ECNN2 | 0.9616 ± 0.0022 | 2.8140 ± 0.0825 | 0.9524 ± 0.0012 | 2.9782 ± 0.0398 | |
Al | PLS | 0.8578 | 2.2083 | 0.8572 | 2.2395 |
ELM | 0.8638 ± 0.0651 | 2.1042 ± 0.4747 | 0.8596 ± 0.0713 | 2.1729 ± 0.5160 | |
CNN | 0.8787 ± 0.0843 | 1.9536 ± 0.5737 | 0.8661 ± 0.1264 | 2.0313 ± 0.7457 | |
ECNN1 | 0.9095 ± 0.0458 | 1.7129 ± 0.3973 | 0.9065 ± 0.0507 | 1.7604 ± 0.4131 | |
ECNN2 | 0.9498 ± 0.0036 | 1.3087 ± 0.0483 | 0.9436 ± 0.0013 | 1.4042 ± 0.0167 | |
K | PLS | 0.8608 | 0.7065 | 0.8614 | 0.7069 |
ELM | 0.8446 ± 0.0722 | 0.7277 ± 0.1660 | 0.8301 ± 0.0671 | 0.7669 ± 0.1480 | |
CNN | 0.9034 ± 0.0816 | 0.5453 ± 0.2214 | 0.8924 ± 0.0934 | 0.5713 ± 0.2371 | |
ECNN1 | 0.9348 ± 0.0578 | 0.4490 ± 0.1788 | 0.9271 ± 0.0671 | 0.4706 ± 0.1934 | |
ECNN2 | 0.9687 ± 0.0011 | 0.3349 ± 0.0062 | 0.9645 ± 0.0020 | 0.3550 ± 0.0103 |
Element | CCCT Name | Actuals | ECNN2 | CNN | ELM | PLS | ||||
---|---|---|---|---|---|---|---|---|---|---|
Predicted | RER | Predicted | RER | Predicted | RER | Predicted | RER | |||
Si | Norite | 47.88 | 47.19 | 1.42% | 46.69 | 2.45% | 46.61 | 2.63% | 46.24 | 3.40% |
Picrite | 43.59 | 44.08 | 1.14% | 42.05 | 3.50% | 41.28 | 5.27% | 40.34 | 7.42% | |
Shergottite | 48.42 | 48.30 | 0.23% | 46.63 | 3.69% | 45.70 | 5.60% | 45.17 | 6.55% | |
NAU2-LO-S | 43.78 | 43.70 | 0.17% | 45.02 | 2.85% | 47.00 | 7.37% | 48.23 | 10.17% | |
NAU2-MED-S | 37.48 | 38.54 | 2.83% | 40.31 | 7.54% | 33.42 | 10.82% | 41.71 | 11.29% | |
KGA-MED-S | 35.64 | 36.99 | 3.79% | 38.57 | 8.23% | 42.40 | 18.96% | 42.57 | 19.46% | |
Al | Norite | 14.66 | 15.01 | 2.33% | 15.57 | 6.34% | 16.22 | 10.72% | 12.50 | 14.78% |
Picrite | 12.39 | 12.86 | 3.81% | 14.02 | 13.12% | 15.32 | 23.62% | 15.52 | 25.25% | |
Shergottite | 10.83 | 11.50 | 6.16% | 12.30 | 13.77% | 12.35 | 14.07% | 12.48 | 15.27% | |
NAU2-LO-S | 7.63 | 7.69 | 0.80% | 7.83 | 2.63% | 7.06 | 7.34% | 6.85 | 10.10% | |
NAU2-MED-S | 5.72 | 5.95 | 4.12% | 6.71 | 17.36% | 7.05 | 23.33% | 7.29 | 27.54% | |
KGA-MED-S | 23.71 | 21.49 | 9.39% | 27.02 | 13.94% | 28.77 | 21.37% | 29.06 | 22.56% | |
K | Norite | 0.06 | 0.056 | 5.73% | 0.054 | 9.00% | 0.051 | 13.67% | 0.053 | 11.63% |
Picrite | 0.10 | 0.109 | 9.56% | 0.111 | 11.76% | 0.0732 | 26.80% | 0.129 | 29.66% | |
Shergottite | 0.11 | 0.114 | 4.38% | 0.103 | 6.31% | 0.143 | 29.97% | 0.100 | 9.12% | |
NAU2-LO-S | 0.40 | 0.461 | 15.48% | 0.491 | 22.77% | 0.589 | 47.41% | 0.524 | 31.17% | |
NAU2-MED-S | 0.29 | 0.312 | 7.85% | 0.169 | 41.62% | 0.141 | 51.21% | 0.143 | 50.49% | |
KGA-MED-S | 0.26 | 0.264 | 1.63% | 0.276 | 6.24% | 0.287 | 10.65% | 0.286 | 10.31% |
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Yu, Y.; Yao, M. When Convolutional Neural Networks Meet Laser-Induced Breakdown Spectroscopy: End-to-End Quantitative Analysis Modeling of ChemCam Spectral Data for Major Elements Based on Ensemble Convolutional Neural Networks. Remote Sens. 2023, 15, 3422. https://doi.org/10.3390/rs15133422
Yu Y, Yao M. When Convolutional Neural Networks Meet Laser-Induced Breakdown Spectroscopy: End-to-End Quantitative Analysis Modeling of ChemCam Spectral Data for Major Elements Based on Ensemble Convolutional Neural Networks. Remote Sensing. 2023; 15(13):3422. https://doi.org/10.3390/rs15133422
Chicago/Turabian StyleYu, Yan, and Meibao Yao. 2023. "When Convolutional Neural Networks Meet Laser-Induced Breakdown Spectroscopy: End-to-End Quantitative Analysis Modeling of ChemCam Spectral Data for Major Elements Based on Ensemble Convolutional Neural Networks" Remote Sensing 15, no. 13: 3422. https://doi.org/10.3390/rs15133422
APA StyleYu, Y., & Yao, M. (2023). When Convolutional Neural Networks Meet Laser-Induced Breakdown Spectroscopy: End-to-End Quantitative Analysis Modeling of ChemCam Spectral Data for Major Elements Based on Ensemble Convolutional Neural Networks. Remote Sensing, 15(13), 3422. https://doi.org/10.3390/rs15133422