Robust Wavelength Selection for Partial Least Squares Sugar Content Estimation Using Combinatorial Bayesian Optimization
Authors: Mitsunobu Kanebako, Ami S. Koshikawa, Masaru Hitomi, Takuro Tanaka, Mahito Chiba, Maiko Mori, Masayuki Ohzeki
Organizations: Graduate School of Information Sciences, Tohoku University, Miyagi 980-8564, Japan · DIC Corporation, Tokyo 103-8233, Japan · Department of Physics, Institute of Science Tokyo, Tokyo 152-8551, Japan · Research and Education Institute for Semiconductors and Informatics, Kumamoto University, Kumamoto 860-0862, Japan · Sigma-i Co., Ltd., Tokyo 108-0075, Japan
Abstract
Wavelength selection is one of the important preprocessing methods in near-infrared spectroscopy to improve prediction accuracy and interpretability of spectral data. We formulate wavelength-region selection for sugar content estimation as a binary black-box optimization problem and propose a method based on Bayesian optimization. The proposed method constructs a sparse quadratic surrogate model and sequentially extracts interested wavelength regions by Thompson sampling. Minimizing an acquisition function is performed as a quadratic unconstrained binary optimization problem by simulated or quantum annealing. Experiments show that the proposed method improves the prediction accuracy of partial least squares regression and yields more consistent wavelength regions than genetic-algorithm-based selection and simulated annealing. Under one-bit local perturbations, the selected wavelength regions show minimal fluctuations in root mean square errors between observed and predicted values of a validation set. This local stability suggests that our method converges to a smoother error landscape and avoids isolated overfitted solutions. These results indicate that combinatorial Bayesian optimization is a useful framework for robust feature selection in spectroscopic prediction tasks.
Laser-induced breakdown spectroscopy (LIBS) quantitative analysis faces critical challenges in wavelength selection due to high-dimensional spectral data and the fundamental trade-off between prediction accuracy and feature efficiency. This paper presents a novel Multi-Adapter PPO framework that transforms wavelength selection into a reinforcement learning problem, leveraging cross-attention mechanisms and multiple specialized adapters to capture complex spectral relationships. Our approach outperforms traditional Particle Swarm Optimization (PSO) by an average of 28.4% in comprehensive score and 45.2% in prediction accuracy across steel and coal datasets. The proposed method demonstrates superior performance in balancing prediction accuracy with feature efficiency, achieving state-of-the-art results in LIBS quantitative analysis while maintaining interpretability and computational efficiency. We released our code and dataset here: https://github.com/Hflying/MAPPO
Preprocessing screening is often the most expensive part of a near-infrared spectroscopy calibration workflow. It works because smoothing, derivatives, detrending and related filters change the spectral directions seen by partial least squares (PLS) or Ridge regression, but a full external search repeatedly refits nearly the same linear model. This paper studies the case where that search can be collapsed into one calibration step. For a strict linear preprocessing operator A acting on row spectra as XA^T, the transformed PLS cross-covariance satisfies (XA^T)^T Y = A X^T Y, and Ridge regression depends on the operator-induced kernel X A^T A X^T. These identities let a finite operator bank be screened inside the model while retaining original-wavelength coefficients, and the same identity extends to cheaply evaluated linear operator chains. Sample-adaptive or fitted corrections such as SNV, MSC, EMSC and ASLS are not strict linear; we prove the boundary and keep them as fold-local branches. The cohort has 61 regression and 17 classification rows, with a strict paired regression denominator of N=32 for the eight paper variants. There, AOM-PLS reaches median RMSEP ratios of 0.991/0.990 (simple) and 0.985/1.002 (best) against PLS-default/PLS-HPO, and AOM-Ridge reaches 0.974/0.984 (simple) and 0.918/0.966 (best) against Ridge-default/Ridge-HPO. The operator-adaptive classifier AOM-PLS-DA improves balanced accuracy by a median 0.159 on N=13 datasets (12/13 wins). The practical result is the runtime gap: PLS-HPO takes a median 710.81 s per run, whereas AOM-PLS takes 1.18-1.63 s -- 436 to 602 times less PLS fitting time. Linear operator-adaptive calibration thus gives prediction quality comparable to exhaustive preprocessing screening, with orders-of-magnitude less fitting time for PLS.
A central challenge in statistical modeling is identifying the subset of features that belong in the true regression model. The classical best subset selection problem, recently made tractable via mixed-integer optimization (MIO), finds the globally optimal sparse solution. It does not, however, make use of any information beyond the observed data. In many applied settings, domain experts can meaningfully rank or score the relevance of candidate predictors, yet no existing framework integrates such probabilistic expert assessments directly into the best-subsets objective. This paper presents Expert-Implied Bayesian Best Subsets (EBBS), a method that incorporates domain-expert probability estimates of feature relevance into the MIO best-subsets problem through a maximum a posteriori (MAP) framework. Expert views from multiple respondents are aggregated into a single prior probability per feature using the Poisson binomial distribution for marginal probability estimates, the pairwise win rate for pairwise comparisons, or the normalized mean rank for ordinal rankings. This probability enters the objective function as a log-odds penalty term that smoothly encourages or discourages the selection of each feature consistent with the expert consensus. This paper provides analytic derivations of the MAP formulation and characterizes its theoretical properties. The proposed model reduces to Best Subsets when experts all have no views. Empirical results on synthetic and real datasets are forthcoming.