Guanyu
Chen
ab,
Jing
Chen
ab,
Dongming
Qu
ab,
Guang
Yang
*ab and
Huihui
Sun
*a
aCollege of Instrumentation and Electrical Engineering, Jilin University, Changchun 130061, P. R. China. E-mail: yangguang_jlu@163.com
bJilin Provincial Key Laboratory of Trace Analysis Technology and Instruments, Changchun, 130061, P. R. China
First published on 30th November 2024
NdFeB magnetic materials are widely used in daily life, such as in permanent magnet motors, loudspeakers and computer disks. The NdFeB magnetic material has excellent magnetic properties, and its magnetic properties are also the key to judge the production quality of NdFeB. Therefore, the precise quantification of the magnetic properties of NdFeB magnetic materials is crucial. Laser induced breakdown spectroscopy (LIBS) is a technique to obtain the spectrum of chemical elements by excitation of plasma on the surface of a sample with a high energy laser. In this paper, a precise classification and magnetic quantification method for NdFeB magnetic materials based on laser-induced breakdown spectroscopy is designed, which is different from the traditional direct magnetic property detection method and uses element detection to quantitatively analyze the magnetic properties indirectly. A laser-induced breakdown spectroscopy system was used to collect the characteristic spectrum of NdFeB magnetic materials, and the sliding window minimum removal base method was independently designed to further optimize the detection accuracy. A classification model and quantitative analysis method model were further established and optimized. The random forest method was used to preliminarily classify NdFeB magnetic materials, and the GA-ELM method was used to conduct quantitative analysis of magnetic properties. Quantitative magnetic properties include Br, Hcj, Hcb and (BH)max. The error analysis of the final quantitative analysis is as follows: RMSE of Br reaches 0.0001526, RMSE of Hcj reaches 0.0001937, RMSE of Hcb reaches 0.00197, and RMSE of (BH)max reaches 0.00785. It is verified that the magnetic quantification method for NdFeB magnetic materials based on laser-induced breakdown spectroscopy can effectively conduct accurate quantitative analysis of the magnetic properties of NdFeB magnetic materials and provide a fast, convenient, accurate and economical detection method for the quality control of magnetic materials workshops.
According to the quality monitoring requirements of coarse embryos, we urgently need a method that can identify the quality of the coarse embryo quickly and accurately. Traditional crude embryo detection methods, such as using a vibrating sample magnetometer or superconducting quantum magnetometer, use the detection of its magnetic properties to detect its production quality. This detection requires the NdFeB crude embryo in a cylindrical sample with a fixed thickness and a fixed diameter, if the shape varies, additional topography processing is needed. In addition, the demagnetization measurement process of magnetic materials will make the material brittle, easily damaging the material. Generally, by using the same batch of samples to test on behalf of this batch of overall evaluation, it is impossible to detect the magnetic properties of each magnetic material.8–11
In response to this issue, this article uses laser-induced breakdown spectroscopy (LIBS) technology, which has advantages such as no need for complex sample pretreatment, simultaneous analysis of multiple elements, low sample loss, and fast detection speed. It can be applied to the quality monitoring and detection requirements of neodymium iron boron rough embryos. LIBS technology uses a high-energy pulsed laser to focus on the surface of a sample, excite it, and generate a high brightness and high heat plasma. The elemental content of the sample is inferred from the spectral information of the plasma. We found that the magnetic properties of neodymium iron boron magnets are highly correlated with their elemental ratios,12–14 while laser-induced breakdown spectra are highly correlated with the elemental ratios of the sample. We utilized the powerful predictive ability of artificial intelligence machine learning methods to establish a correlation between the magnetic properties of neodymium iron boron magnets and laser-induced breakdown spectra. Quality monitoring of neodymium iron boron rough blanks is performed to achieve precise quantification of magnetic properties for all magnetic materials.15,16
In this paper, according to the uneven surface of the NdFeB coarse embryo material, a long focal optical path is designed to ensure the stability of the laser-induced breakdown spectrum when the defocusing range is ±5 mm. A self-designed minimum sliding window preprocessing method was used to remove background noise. An appropriate stoichiometric method was selected for the preliminary classification of magnetic materials, and the method was optimized to improve the classification accuracy. Finally, according to the types of magnetic materials, an appropriate stoichiometric method was selected to accurately analyze the four magnetic parameters.17,18
Brand | Br | Hcj | Hcb | (BH)max |
---|---|---|---|---|
N35 | 11.7–12.2 | 12 | 10.9 | 33–36 |
N38 | 12.2–12.5 | 12 | 11.3 | 36–39 |
N40 | 12.5–12.8 | 12 | 11.6 | 38–41 |
N35M | 11.7–12.2 | 14 | 10.9 | 33–36 |
N35H | 11.7–12.2 | 17 | 10.9 | 33–36 |
Four magnetic properties are listed in the table, namely remanence (Br), intrinsic coercivity (Hcj), magnetic inductance coercivity (Hcb) and maximum magnetic energy product ((BH)max). It can be seen that their 4 parameters are different, and the 4 magnetic parameters of the sample of the same grade are also different, and it is necessary to conduct accurate quantitative analysis of magnetic parameters after sample grade classification.
Label | Br | Hcj | Hcb | (BH)max |
---|---|---|---|---|
1 | 12.803 | 10.882 | 11.359 | 38.047 |
2 | 12.841 | 10.842 | 11.314 | 38.384 |
3 | 12.815 | 10.799 | 11.245 | 38.246 |
4 | 12.822 | 10.535 | 11.386 | 38.263 |
5 | 12.878 | 10.761 | 11.317 | 38.424 |
6 | 12.813 | 10.965 | 11.436 | 38.171 |
7 | 12.784 | 10.528 | 11.121 | 38.878 |
8 | 12.621 | 10.757 | 11.307 | 37.135 |
9 | 12.615 | 10.711 | 11.254 | 37.251 |
10 | 12.862 | 10.492 | 11.204 | 37.605 |
11 | 12.842 | 10.926 | 11.401 | 38.233 |
12 | 12.72 | 10.706 | 11.196 | 37.51 |
13 | 12.807 | 10.762 | 11.296 | 38.053 |
14 | 12.804 | 10.62 | 11.026 | 38.171 |
15 | 13.052 | 10.641 | 11.128 | 39.531 |
16 | 12.831 | 10.993 | 11.444 | 38.151 |
17 | 12.802 | 10.618 | 11.324 | 37.997 |
18 | 12.936 | 10.904 | 11.345 | 38.318 |
19 | 12.813 | 10.908 | 11.335 | 38.058 |
20 | 12.73 | 10.781 | 11.386 | 37.216 |
For accurate quantitative analysis of magnetic properties, we divided the 20 samples into two parts: a training set and test set. In order to ensure the quality of the analysis model, samples with the largest 2 values, the smallest 2 values and the middle 2 values of the 4 kinds of magnetic property parameters were selected as the training set data, as shown in Table 3.
Br | Hcj | Hcb | (BH)max | ||||
---|---|---|---|---|---|---|---|
12.615 | 9 | 10.492 | 10 | 11.026 | 14 | 37.135 | 8 |
12.621 | 8 | 10.528 | 7 | 11.121 | 7 | 37.216 | 20 |
12.72 | 12 | 10.535 | 4 | 11.128 | 15 | 37.251 | 9 |
12.73 | 20 | 10.618 | 17 | 11.196 | 12 | 37.51 | 12 |
12.784 | 7 | 10.641 | 14 | 11.204 | 10 | 37.605 | 10 |
12.802 | 17 | 10.62 | 15 | 11.245 | 3 | 37.878 | 7 |
12.803 | 1 | 10.706 | 12 | 11.254 | 9 | 37.997 | 17 |
12.804 | 14 | 10.711 | 9 | 11.296 | 13 | 38.047 | 1 |
12.807 | 13 | 10.757 | 8 | 11.307 | 8 | 38.053 | 13 |
12.813 | 6 | 10.761 | 5 | 11.314 | 2 | 38.058 | 19 |
12.813 | 19 | 10.762 | 13 | 11.317 | 5 | 38.151 | 16 |
12.815 | 3 | 10.781 | 20 | 11.324 | 17 | 38.171 | 6 |
12.822 | 4 | 10.799 | 3 | 11.335 | 19 | 38.171 | 14 |
12.831 | 16 | 10.842 | 2 | 11.345 | 18 | 38.233 | 11 |
12.836 | 18 | 10.882 | 1 | 11.359 | 1 | 38.246 | 3 |
12.841 | 2 | 10.904 | 18 | 11.386 | 4 | 38.263 | 4 |
12.842 | 11 | 10.908 | 19 | 11.386 | 20 | 38.318 | 18 |
12.862 | 10 | 10.926 | 11 | 11.410 | 11 | 38.384 | 2 |
12.878 | 5 | 10.965 | 6 | 11.436 | 6 | 38.424 | 5 |
13.052 | 15 | 10.993 | 16 | 11.444 | 16 | 39.531 | 15 |
Finally, samples 2, 5, 6, 7, 8, 9, 10, 13, 14, 15, 16, 19 and 20 were selected as training set data and samples 1, 3, 4, 11, 12, 17 and 18 were selected as test set data.
In this paper, a long focal coaxial optical path is designed, and the acquisition depth of field is increased by using a long focal lens to compensate for the spectral information acquisition distortion of samples in a small range of defocus. Since the optical path is a long focal coaxial receiving optical path, the overall optical path is the same as the camera imaging system, and the defocus degree is the same as the camera depth of field. We use the camera depth of field calculation method to calculate the overall optical path defocusing acceptance, and the camera optical path is shown in Fig. 1.
The depth of field is calculated as follows:
Next, the function of the telephoto coaxial receiving optical path is verified by means of spectrum acquisition. First, a telephoto coaxial optical path system is built.
The telephoto coaxial receiving optical path is constructed with a high-precision cage system, which can simultaneously ensure the stability of the experiment and the convenience of the optical path adjustment. A laser focusing mirror with a focal length of 100 mm, a fiber focusing mirror with a focal length of 50 mm and a short-wave dichroic mirror with a cut-off wavelength of 805 nm were selected to complete the functions of laser focusing, excitation sample and plasma spectrum coaxial acquisition.
In order to reduce the error caused by the uneven surface of the sample itself, we selected an aluminum alloy sample with a smooth and dense surface for laser-induced breakdown spectrum acquisition. 10 points were selected for each defocusing distance, and each point was collected 3 times for an average to represent the spectrum of this point, and the spectral intensity fluctuation of the characteristic wavelength of the sample was verified within the range of the focal length of the system ±3 mm (Fig. 2).
From the figure, we can see that within the defocusing range of ±3 mm, the fluctuation of characteristic peak intensity at different defocusing distances is small, even smaller than the spectral intensity fluctuation at different points of the same defocusing distance. It can be verified that the long focal coaxial receiving optical path designed by us can eliminate the spectral intensity fluctuation caused by the defocusing caused by the uneven surface of the sample.
In order to avoid the interference of bremsstrahlung radiation generated in the early stage of plasma generation during data collection, due to the fact that the attenuation rate of bremsstrahlung radiation is much higher than that of spectral signals, we adopt a delay measurement method. We delay until the bremsstrahlung radiation is completely attenuated before collecting the signal, which can obtain a signal with a high signal-to-noise ratio.
The final collected spectrum is shown in Fig. 4. From the spectrum, it can be seen that the elements contained in the neodymium iron boron sample have been excited, and corresponding characteristic curves can be found in the spectrum, such as Nd: 383.89 nm, Fe: 373.48 nm, and B: 345.13 nm.
From the spectrogram, it can be seen that there are still some issues such as baseline drift and background noise in the graph. It is necessary to select an appropriate analysis method and perform spectral preprocessing to further improve the final analysis accuracy.
From the comparison of the classification results, it can be seen that RF classification accuracy is higher than those of the other three algorithms and the classification error data are more concentrated, making it easier to improve classification accuracy through algorithm optimization. Therefore, we choose the RF algorithm for the next optimization analysis.
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Fig. 6 Pre-processing optimization results for sliding window lengths of 5, 10, 20 and 50 data points. |
As shown in Table 4, we validated the classification results using the RF algorithm. When the sliding window lengths are 5 data points, 10 data points, 20 data points, and 50 data points, the classification accuracies are 0.920, 0.955, 0.970, and 0.945, respectively. Compared to the classification accuracy of 0.910 without preprocessing, there is a certain improvement in both. Finally, we chose a sliding window length of 20 data points for the next step of chemometric analysis.
Sliding window size | Classification accuracy |
---|---|
5 data | 0.920 |
10 data | 0.955 |
20 data | 0.970 |
50 data | 0.945 |
Next, the SWM method was compared with common baseline correction methods, BEADS method and AIRPLS method. The classification accuracy pairs are shown in Table 5. As can be seen from the data in the table, the classification accuracy of BEADS is the highest at 0.975 and the classification accuracy of SWM and AIRPLS is 0.97. There is little difference between the three classifications.
Pretreatment method | Classification accuracy |
---|---|
SWM | 0.970 |
BEADS | 0.975 |
AIRPLS | 0.970 |
The running time of the three methods is compared as shown in Table 6. SWM run time is 4.487 s, BEADS run time is 57.534 s, and AIRPLS run time is 12.053 s.
Pretreatment method | Running time (s) |
---|---|
SWM | 4.487 |
BEADS | 57.534 |
AIRPLS | 12.053 |
Finally, the SWM method is selected after comprehensive consideration.
As shown in Fig. 7, M is the number of data samples, and the final optimal parameters selected are n_tree = 50 and m_try = M/8, with a classification accuracy of 1. The classification results are shown in Fig. 8. Next, we will optimize the main parameters of the algorithm.
In the process of random forest regression modeling, two important parameters are involved: the number of randomly selected attributes (m_try) and the number of decision trees (n_tree). Optimizing the ntree value can improve the stability of the RF calibration model, and optimizing the mtry value can effectively improve the prediction accuracy of the calibration model. At the same time, these two parameters are closely related to the efficiency of the model. It is necessary to adjust the m_try while minimizing the size of the n_tree, as the computer's runtime increases geometrically with the increase of the n_tree. As shown in Fig. 7, M is the number of data samples, and the final optimal parameters selected are n_tree = 50 and m_try = M/8, with a classification accuracy of 1.
First, it is necessary to select a chemometric method suitable for neodymium iron boron samples. We still chose partial least squares (PLS), random forest (RF), and extreme learning machine (ELM).23–28 Using these three algorithms for quantitative analysis of the five neodymium iron boron samples, the RMSE results were used as the basis for evaluating the quality of the quantitative results. The RMSE results obtained using the three algorithms that have not been further optimized are shown in Table 5.29,30
From the results, it can be seen that PLS has much lower quantitative analysis ability than RF and ELM. Overall, ELM has better quantitative analysis ability than RF. Therefore, we choose the ELM algorithm for further optimization analysis (Table 7).
Magnetic parameter | PLS_RMSE | RF_RMSE | ELM_RMSE |
---|---|---|---|
Br | 0.9693 | 0.1846 | 0.1098 |
Hcj | 0.8094 | 0.1834 | 0.1180 |
Hcb | 0.7667 | 0.1725 | 0.1846 |
(BH)max | 2.7756 | 0.5389 | 0.5076 |
Magnetic parameter | ELM_RMSE | GA-ELM_RMSE |
---|---|---|
Br | 0.1098 | 0.0001526 |
Hcj | 0.1180 | 0.0001937 |
Hcb | 0.1846 | 0.00197 |
(BH)max | 0.5076 | 0.00785 |
It can be seen that the quantitative analysis errors of the four magnetic property parameters decrease with the increase of genetic generations and eventually tend to remain unchanged. Br reaches its optimal value at genetic generation 39, Hcb reaches its optimal value at genetic generation 63, Hcj reaches its optimal value at genetic generation 70, and (BH)max reaches its optimal value at genetic generation 48. Finally, we chose genetic generation 70. The full hyperparameters of GA are a population size of 20, a crossover probability of 0.7, a mutation probability of 0.01, an ‘elite selection’ selection strategy, and genetic algebra 70.
The final quantitative analysis results are shown in Fig. 9 and Table 6. The RMSE of Br reached 0.0001526, the RMSE of Hcj reached 0.0001937, the RMSE of Hcb reached 0.00197, and the RMSE of (BH)max reached 0.00785. The magnetic quantification method of neodymium iron boron magnetic materials based on laser-induced breakdown spectroscopy has been validated to effectively perform accurate magnetic property quantification analysis of neodymium iron boron magnetic materials, providing a fast, convenient, accurate, and economical detection method for quality monitoring in magnetic material workshops.
Through quantitative method selection and optimization of ELM algorithm weights and biases using the genetic algorithm, the final quantitative accuracy of the RMSE of Br reached 0.0001526, the RMSE of Hcj reached 0.0001937, the RMSE of Hcb reached 0.00197, and the RMSE of (BH)max reached 0.00785. The magnetic quantification method of neodymium iron boron magnetic materials based on laser-induced breakdown spectroscopy has been validated to effectively perform accurate magnetic property quantification analysis of neodymium iron boron magnetic materials, providing a fast, convenient, accurate, and economical detection method for quality monitoring in magnetic material workshops.
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