Predictive modeling (calibration or training) with various data formats, such as near-infrared (NIR) spectra and quantitative structure−activity relationship (QSAR) data, provides essential information if a proper model is selected. Similarly, with a general model selection approach, spectral model maintenance (updating) from original modeling conditions to new conditions can be performed for dynamic modeling. Fundamental modeling (partial least-squares (PLS) and others) and maintenance processes (domain adaptation or transfer learning and others) require selection of tuning parameter(s) values to isolate models that can accurately predict new samples or molecules, e.g., number of PLS latent variables to predict analyte concentration. Regardless of the modeling task, model selection is complex and without a reliable protocol. Tuning parameter selection typically depends on only one model quality measure assessing model bias using prediction accuracy. Developed in this paper is a generic model selection process using concepts from consensus modeling and QSAR activity landscapes. It is a consensus filtering approach that prioritizes model diversity (MD) while conserving prediction similarity (PS) fused with a common bias-variance trade-off measure. A significant feature of MDPS is that a cross-validation scheme is not needed because models are selected relative to predicting new samples or molecules, i.e., model selection uses unlabeled samples (without reference values) for active predictions. The versatility and reliability of MDPS model selection is shown using four NIR data sets and a QSAR data set. The study also substantiates the Rashomon effect where there is not one best model tuning parameter value that provides accurate predictions.

Updating a calibration model formed in original (primary) sample and spectral measurement conditions to predict analyte values in novel (secondary) conditions is an essential activity in analytical chemistry in order to avoid a complete recalibration. Established model updating methods require sample analyte reference values for a small set of secondary domain samples (labeled data) to be used in updating processes. Because obtaining reference values is time consuming and is the costly part of any calibration, methods are needed that do not require labeled secondary samples, thereby allowing on demand model updating. This paper compares model updating methods with and without labeled secondary samples. A hybrid model updating approach is also developed and evaluated. Unfortunately, a major impediment to adapting a model without secondary analyte reference values has been model selection. Because multiple tuning parameters are commonly involved in model updating methods, thousands of models are formed, making model selection complex. A recently developed framework is evaluated for automatic model selection of several two to three tuning parameter-based model updating methods without secondary analyte reference values (labels). The model selection method is based on model diversity and prediction similarity (MDPS) of the unlabeled samples to be predicted. The new secondary samples to be predicted can be used to form the updated models and again to select the final predicting models. Because models are formed and selected on demand to directly predict target samples, complicated cross-validation processes are not needed. Four near-infrared data sets covering 40 model updating situations are evaluated showing that MDPS can select reliable updated models outperforming or rivaling prediction errors from total recalibrations with secondary reference values.

No abstract

No abstract

No abstract