Spectra

Strong chromospheric absorption lines such as H$α$ 6562.8 A and Ca II 8542.1 A provide vital diagnostics of plasma dynamics and thermal structure in the solar chromosphere. Multilayer spectral inversion (MLSI) offers a physically interpretable framework for modeling these lines using a finite number of radiative-transfer layers, but conventional MLSI relies on pixel-by-pixel nonlinear least-squares fitting, making it computationally expensive for large imaging spectroscopic data sets. Here, we introduce a physics-informed neural-network (PINN) framework to accelerate MLSI while preserving its analytic radiative-transfer formulation. The network predicts MLSI parameters directly from observed line profiles and passes them through a differentiable MLSI forward model to synthesize spectra. Training follows a two-stage approach: an initial stage optimized solely via spectral reconstruction loss, followed by fine-tuning that combines spectral consistency with parameter-space supervision from conventional MLSI results on a single reference image. This strategy eliminates the need for large precomputed training sets while maintaining physical interpretability. Applied to Fast Imaging Solar Spectrograph (FISS) observations from the Goode Solar Telescope (GST) targeting both quiet-Sun and active-region regions, MLSI-PINN parameter maps reproduce the primary spatial structures of direct inversions, achieving an arithmetic mean pixel-wise Pearson correlation coefficient of 0.933 across all evaluated parameters. The reconstructed spectra closely match both observed profiles and conventional MLSI fits. Post-training, MLSI-PINN processes a raster in approximately 5-15 seconds compared to 3-5 minutes for conventional MLSI, delivering an inference speedup of about 12-60 times without substantial loss in reconstruction quality, enabling efficient MLSI analysis on large chromospheric data sets.

Spectroscopic structure elucidation is central to molecular analysis, but recent Large Language Model (LLM)-based methods mostly formulate it as direct spectrum-to-SMILES generation. Although this paradigm can leverage paired spectral data, it does not explicitly model the analytical workflow used by spectroscopists, such as diagnostic peak interpretation, fragment reasoning, formula constraints, and chemical consistency checking. In this paper, we introduce S3C-LLM, a skill-guided and code-grounded agentic LLM for spectrum-to-structure elucidation. Rather than directly predicting a molecule, S3C-LLM retrieves modality-specific spectroscopy skills, executes analysis code to instantiate these skills on the input spectra, and integrates the resulting peak-level evidence and formula constraints before generating SMILES. Specifically, we contribute a self-evolving spectroscopy skill library, a thinking-augmented skill-code trajectory construction pipeline, and a two-stage training strategy that teaches Qwen3-4B through supervised fine-tuning (SFT) followed by our proposed step-level reinforcement learning (RL). Experiments on diverse benchmarks show that S3C-LLM consistently outperforms current general LLMs and spectrum-specific models across spectra, while using less than 1/10th of SpectraLLM's training corpus.

Large language models (LLMs) increasingly read long inputs in the agentic era, from whole documents and codebases to conversations across many turns. Their inference memory is then dominated by the key-value (KV) cache, the stored attention keys and values of every token the model has read and generated. Because the cache grows with context length and is re-read in full at every generated token, a longer context means more GPU memory. To reduce this cost, most existing methods compress the KV cache by lowering every stored value to the same low precision, a technique known as quantization. They can push this to nearly two bits per value, but rarely further, because quality drops sharply at this 2-bit cliff: four levels are too few for the cache's outlier-heavy values, where a few large entries consume the levels and collapse the rest into noise. A natural remedy is to spend more bits on the channels (feature dimensions) that matter and fewer on the rest, but the raw cache offers no handle: its channels are strongly correlated, so none stands out as more important. Our analysis shows that this handle appears once the cache is rotated into a coordinate system computed from its own statistics, removing these correlations. There, a small fraction of channels carries almost all the information, and spending the budget on those few is far more accurate than spreading it evenly. Guided by this analysis, we develop SPECTRA, a training-free, drop-in codec that re-encodes the cache into this coordinate system and concentrates the bit budget on the channels that carry the signal. On Llama-3.1-8B and Qwen2.5-7B over long-context benchmarks, SPECTRA is near-lossless at 4x compression, competitive at 8x where uniform quantization has collapsed, and reaches up to 12x, pushing usable compression past the 2-bit cliff so the same GPU holds longer contexts and larger batches.

Visible and near-infrared (vis-NIR) and mid-infrared (MIR) spectroscopy enable rapid, cost-effective prediction of soil properties. Yet, translating high-dimensional, highly collinear spectra into accurate soil property predictions remains challenging, particularly when employing machine learning. We systematically investigated regression models and dimensionality reduction approaches for spectroscopic modeling across 85 regression tasks from open benchmark datasets in pedometrics spanning field-scale digital soil mapping and a global soil spectral library. We compared an in-context learning tabular foundation model (TabPFN), a convolutional neural network (CNN), rule-based regression (Cubist), Random Forest, and partial least squares regression (PLSR) using full spectra as well as features derived from principal component analysis (PCA) and partial least squares (PLS) latent variables. TabPFN consistently delivered the best overall performance across scales, including large spectral library tasks with tens of thousands of soil samples. Notably, TabPFN applied directly to full spectra already surpassed all classical baselines, showing that explicit dimensionality reduction is not strictly required for strong performance. Further improvements were achieved through PLS, which proved to be an effective dimensionality reduction strategy for all models. Combining PLS latent variables with TabPFN yielded the best predictions overall. Our findings provide evidence-based guidance for spectroscopic calibration model selection across operational scales, demonstrating that the long-standing advantages of PLSR and modern tabular foundation models complement each other in chemometrics.

The extraction of $β$-feeding distributions in Total Absorption $γ$-ray Spectroscopy constitutes a challenging inverse problem, particularly in nuclei with complex decay schemes involving a large number of excited states. In such cases, the measured spectrum arises from the superposition of many detector response functions, making the determination of the individual feedings intrinsically ill-posed and highly sensitive to the methodology employed. In this work, we present a systematic comparison between supervised Machine-Learning techniques and Response-Matrix methods using realistic Monte Carlo simulations of an experimental Total Absorption Spectrometer. Supervised Machine-Learning approaches construct a non-parametric estimator that infers level feedings from the measured spectrum after a training stage, whereas Response-Matrix methods determine the feeding distribution by directly minimizing the difference between measured and reconstructed spectra. Our results show that supervised Machine-Learning techniques achieve superior accuracy in the reconstruction of individual feeding intensities, whereas Response-Matrix methods provide robust and physically consistent initial solutions. These findings support a hybrid strategy in which a Response-Matrix method is first used to obtain an initial feeding estimate, which is then refined using a supervised Machine-Learning approach to achieve improved overall accuracy.

Inferring molecular structures from infrared (IR) spectra is a fundamental yet challenging problem. A key difficulty is that an IR spectrum provides limited structural information: different molecules may share similar functional groups and local vibrational patterns, leading to highly similar spectral responses. Thus, even when an observed spectrum has a unique underlying structure, reconstructing it from the spectrum remains ambiguous. Existing IR-to-molecule models usually generate a ranked set of candidate molecules, but this set is largely determined by the model's learned generation preference and may not fully capture the structures that best satisfy the observed spectral constraints. To address this limitation, we propose SpecCal, a training-free candidate calibration framework for IR-to-molecule prediction. SpecCal operates on the candidate outputs of existing base models and improves the prediction set by re-ranking current candidates while introducing additional structurally plausible alternatives guided by spectral consistency. The framework is plug-and-play and model-agnostic, requiring no parameter updates for integration with diverse base models. Experiments on multiple benchmarks show that SpecCal consistently improves top-k reconstruction at both SMILES and scaffold levels across different base models. Further analyses demonstrate that calibrating candidate sets under spectral ambiguity provides a practical way to improve molecular reconstruction from IR spectra. The code is available at: https://anonymous.4open.science/r/SpecCal-B18A.

X-ray absorption spectroscopy (XAS) is central to understanding the local electronic and atomic structure of materials, yet most published spectra remain inaccessible to data-driven analysis because they are embedded in figures and described through fragmented textual context in the literature. Here, we use multimodal (image and text) literature mining to transform this dispersed knowledge into an AI-ready experimental data resource. We developed a scalable spectroscopy data digitization pipeline that identifies XAS figures in full-text articles, digitizes spectral curves, and links each spectrum to accompanying metadata on the measured edge and material. Applying this pipeline to the battery literature produced an open dataset of 13,740 XAS spectra, spanning 66 absorbing elements and diverse battery chemistries, with expert validation confirming accurate extraction of spectral and metadata information. By converting literature-embedded spectra into structured numerical data, this dataset provides a foundation for large-scale XAS analysis, cross-laboratory comparison, high-throughput characterization, and autonomous discovery of advanced materials.

Autoencoder-based anomalous sound detection is attractive for machine condition monitoring because it can be trained using only normal recordings and yields an interpretable anomaly score from reconstruction error. Most prior work uses spectrogram autoencoders, but reconstructing detailed time--frequency patterns is sensitive to noise and transients, and models can reconstruct some anomalous inputs well, weakening normal--anomaly separation. We propose MemNMF, a constrained reconstruction method that operates on the Linear Predictive Coding spectrum, a compact estimate of the spectral envelope. MemNMF initializes a memory module from an NMF dictionary learned on normal LPC spectra and reconstructs each input as an attention-weighted combination of prototypical normal spectral patterns. Experiments on MIMII and DCASE 2020 Task 2 across multiple machine types and operating conditions show that LPC-spectrum inputs improve a standard autoencoder baseline and that MemNMF yields further gains, with especially strong robustness under noisy, non-stationary settings.

Modern power systems increasingly require probabilistic forecasts amid interacting uncertainties from renewable intermittency, flexible demand, market volatility, and weather-dependent generation. However, existing methods often treat multi-scale decomposition, exogenous-variable alignment, and probabilistic output as separate steps, obscuring how predictable structures and uncertainty-bearing fluctuations jointly shape the forecast distribution. This paper proposes a state-space exogenous-context and temporal-frequency resolution architecture for general probabilistic energy forecasting. Its central premise is that trend-periodic components primarily determine the baseline trajectory, whereas high-frequency residuals and external perturbations govern the spread and asymmetry of forecast uncertainty. Accordingly, the architecture adaptively separates deterministic and residual streams, aligns exogenous context with both, refines the deterministic backbone through multi-resolution spectral-temporal state-space modeling, and estimates ordered quantile boundaries from their complementary representations. Experiments on load, price, solar, and wind forecasting achieve the best continuous ranked probability score in 14 of 18 settings, reducing average CRPS by 5.74% and upper-tail quantile risk by 7.27% over the strongest baselines. These results support deterministic-stochastic separation as an effective design principle for general probabilistic energy forecasting.

Determining molecular structures from spectroscopic data remains fundamentally challenging because the inverse problem is intrinsically underdetermined: individual spectra are sparse, low-dimensional, and encode only partial structural evidence relative to the vast space of possible molecules. We address this challenge by formulating automated structure elucidation as a scalable hypothesis-refinement paradigm that tightly integrates spectral evidence with large-scale molecular priors. To supply structure-resolving NMR signals for multimodal learning, we construct \textbf{QM9SPIN}, a DFT-derived dataset comprising diverse 1D and 2D spectra, including J-coupling, DEPT experiments, and explicit spin--spin interactions. On this foundation, we introduce \textbf{SpectroMol}, a spectrum-to-structure model that proposes chemically valid molecular hypotheses conditioned on multimodal spectral inputs. Complementarily, we develop \textbf{MS-Mol2Mol}, a high-resolution mass-constrained molecular generator that integrates molecular formula, exact mass, and degree of unsaturation within a conditional generative prior trained on 400 million molecules, ensuring global compositional consistency and chemically realistic refinement. The integrated system achieves 93.8% top-1 accuracy on the simulated benchmark, adapts effectively from simulated to experimental spectra with limited experimental fine-tuning, and further improves experimental predictions through mass-guided refinement, establishing a scalable route toward automated, data-driven organic structure elucidation.

Robot imitation learning for manipulation should preserve demonstrated task geometry while producing dynamically admissible robot motions. Existing pipelines often learn task-dependent trajectories and impose execution limits afterward through filtering, smoothing, clipping, or time scaling, which may distort task-critical end-effector paths. We propose the Spectral Movement Primitive (SMP), a frequency-domain imitation learning framework that couples task-space skill generation with joint-space execution regulation. Demonstrations are represented by truncated finite-horizon Fourier coefficients. An empirically selected low-frequency task band captures the dominant motion geometry, while higher harmonics contribute disproportionately to derivative growth. A frame-aware context-conditioned GMM/GMR prior predicts the task-band coefficients in a canonical task frame, and the resulting Cartesian trajectory is mapped to joint space through sequential inverse kinematics. A phase-coupled regulator then limits the requested phase progression without modifying the spectral coefficients, thereby enforcing joint velocity and acceleration limits while preserving the represented path. Experiments evaluate task-band reconstruction, robustness to composite demonstration corruption, out-of-distribution cross-board generalization, joint-space dynamic admissibility, end-effector path preservation, and deployment on a Franka Panda robot. Results show compact geometric reconstruction, consistent transfer across unseen task frames, substantial reductions in dynamic violations and jerk, and preservation of the intended end-effector path during phase regulation.

Near-Infrared (NIR) spectroscopy has emerged as a promising alternative to traditional soil analysis methods, offering advantages such as speed, low cost, and non-destructive testing. This work proposes a machine learning (ML) approach to calibrate predictive models for carbon (C) and nitrogen (N) content in Oxisols and Inceptisols, utilizing NIR spectral data acquired with a portable MyNIR device. Various preprocessing methods were evaluated, with the most effective being the Savitzky-Golay (SG) filter and a robust outlier removal method based on the Nonlinear Iterative Partial Least Squares (NIPALS) algorithm coupled with a Huber loss function. Multiple validation strategies were compared, including 10-fold cross-validation, leave-one-out, and holdout via the Kennard-Stone method, followed by standardization. Stacking ensemble learning models were employed, using Partial Least Squares (PLS), Support Vector Regression (SVR), and Ridge as base models, with linear regression as the meta-model. The models were evaluated using R2, Root Mean Squared Error (RMSE), Mean Absolute Error (MAE), and Ratio of Performance Deviation (RPD) metrics. The performance gap between soil types suggests the influence of pedological characteristics. Furthermore, the models achieved an RPD > 2.0 with low overfitting, validating the potential of this approach for rapid C and N quantification. This study contributes to the optimization of sustainable agricultural practices, aligning with the demand for efficient and environmentally friendly analytical methods. The developed technique enables faster decision-making for producers and consultants based on organic matter content, fertility indicators, and nutrient availability.

Laser-induced breakdown spectroscopy (LIBS) faces challenges in high-accuracy quantitative measurement under few-shot scenarios due to spectral noise and data scarcity. Traditional preprocessing methods often fail to preserve subtle spectral features or capture nonlinear correlations. This work proposes a standardized processing pipeline integrating diffusion-based denoising, attention-based autoencoder for dimensionality reduction, group shuffling data augmentation, and ordinary least squares regression. The diffusion module employs a 3D UNet architecture to remove spectral noise while preserving essential emission features. The attention-autoencoder captures nonlinear spectral correlations, effectively reducing high-dimensional spectral data to compact latent representations. Group shuffling data augmentation enhances model robustness by creating synthetic samples through feature group permutation. Experimental results on multiple elemental concentrations demonstrate that our Diffusion-DA-AE pipeline achieves superior performance with a mean RMAE of 0.2847, representing 37.7% and 37.6% improvements over baseline autoencoder and traditional PCA-PLS regression, respectively. The framework's effectiveness validates its generalizability and establishes a new benchmark for few-shot LIBS regression.

Nondestructive detection methods, based on vibrational spectroscopy, are vitally important in a wide range of applications including industrial chemistry, pharmacy and national defense. Recently, deep learning has been introduced into vibrational spectroscopy showing great potential. Different from images, text, etc. that offer large labeled data sets, vibrational spectroscopic data is very limited, which requires novel concepts beyond transfer and meta learning. To tackle this, we propose a task-enhanced augmentation network (TeaNet). The key component of TeaNet is a reconstruction module that inputs randomly masked spectra and outputs reconstructed samples that are similar to the original ones, but include additional variations learned from the domain. These augmented samples are used to train the classification model. The reconstruction and prediction parts are trained simultaneously, end-to-end with back-propagation. Results on both synthetic and real-world datasets verified the superiority of the proposed method. In the most difficult synthetic scenarios TeaNet outperformed CNN by 17%. We visualized and analysed the neuron responses of TeaNet and CNN, and found that TeaNet's ability to identify discriminant wavenumbers was excellent compared to CNN. Our approach is general and can be easily adapted to other domains, offering a solution to more accurate and interpretable few-shot learning.

Soil properties relevant to agricultural and environmental applications are conventionally measured using elaborate laboratory methods involving physical and chemical processing. While highly accurate, these conventional methods are costly and time-consuming. In contrast, optical spectroscopy paired with machine learning enables rapid and cost-effective predictions of multiple soil properties. However, spectroscopic modelling is often considered unreliable, as the predictive accuracy varies between soil properties and individual samples. To balance this trade-off between cost and reliability, we introduce reject-to-remeasure: an AI-based measurement framework that combines probabilistic modelling with uncertainty-guided rejection. In this framework, soil samples are first analysed using spectroscopy, after which predictions are rejected if their predictive uncertainty exceeds predefined quality constraints. Rejected samples are subsequently remeasured using conventional laboratory procedures. On a regional visible-near-infrared spectral soil library from Québec, we demonstrate that reject-to-remeasure with modern foundation models (TabPFNv2.5 and TabICLv2) can facilitate the integration of optical spectroscopy into routine laboratory workflows while meeting user-defined accuracy requirements and reducing measurement costs.

Scalable prediction of optical spectra is a critical component of high-throughput materials screening for optoelectronic applications such as solar cells. Existing surrogate models are trained on spectra computed from lower levels of theory or rely on rotation-invariant scalar features, limiting their geometric expressiveness. We explore the use of equivariant graph neural networks for optical spectra prediction, adapting GotenNet to this task and evaluating it on multiple datasets including a recently published collection of 10,533 structures with spectra computed at the level of the random phase approximation (RPA). The proposed model outperforms the current state of the art, with the largest gains in the 0-8 eV range and on predicting the static real permittivity, both of particular relevance for thin-film optics.

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

Operational disturbance monitoring in power networks requires decisions to be made from waveform windows as they arrive, rather than from completed records after the event. This study evaluates full-vector Wigner--Ville Distribution Slice (WVDS) spectra for sequential anomaly-onset detection in high-voltage grid-voltage waveforms. The approach keeps the bilinear midpoint interaction structure of the Wigner--Ville distribution and represents each 128-sample voltage window by a 128-dimensional slice spectrum, avoiding manually selected fault-frequency markers. WVDS is used with a baseline-normalized deviation (BND) score and is compared against the BND of Fast Fourier Transform (FFT-BND), raw-window autoencoders, FFT autoencoders, and WVDS autoencoders under the same thresholding and three-window persistence rule. A synthetic autoencoder--clustering teacher is used to select RTE fault records that start from an initially normal region and then transition to anomalous behavior. On the filtered test set, FFT-BND achieves the highest sensitivity, whereas WVDS-BND provides the lowest false-alarm operating point, reducing record-level pre-onset false alarms to 0.69%. The autoencoder comparison follows the same selectivity pattern: WVDS reconstruction decreases false alarms relative to FFT reconstruction but misses more examples. The results indicate that preserved WVD cross-term information can form a selective representation for online grid-waveform anomaly monitoring when false alarms are costly.

High-purity germanium gamma spectra often require time-consuming analyses from subject matter experts. Photopeaks within these spectra are carefully fitted and numerical methods are employed to assist with nuclide identification (NID) and quantification. Amending the list of nuclides identified by analysis software can be nontrivial. When many samples need to be analyzed, it is therefore challenging to make timely and correct decisions. Supervised machine-learning-based NID can serve as an expert-informed, automated tool to improve the initial set of radionuclides suggested to an analyst and more effectively drive subsequent quantification. To that end, we implemented machine learning models that map photopeaks carefully fitted by analysts to NID results for experimental spectra containing various isotopic combinations drawn from a set of 65 isotopes. The best model achieved an F1 score of 0.97, markedly surpassing the F1 score of 0.84 achieved by traditional software when compared using a nuclide library comprising the same 65 isotopes assessed by the models. Finally, we illustrated the most important input features for model predictions using Shapley Additive Explanations. These explanations revealed that the models use physically relevant photopeaks when making predictions for the isotopes in our nuclide library.

This paper evaluates a signal-processing and supervised-learning pipeline for classifying SDSS DR17 astronomical spectra into stars, galaxies, and quasars. Each spectrum is represented by its measured flux and inverse-variance information, combining spectral shape with a wavelength-dependent reliability profile. After resampling onto a common logarithmic wavelength grid, the flux and inverse-variance vectors are standardized and separately compressed using principal component analysis. The resulting components are concatenated and used to train several classifiers. The best performance was obtained with the LightGBM gradient-boosting classifier, reaching $94.6\%$ accuracy and $92.1\%$ balanced accuracy on the test set.

Integral field unit (IFU) spectroscopy provides spatially resolved spectra across galaxies, offering crucial insights into their evolution. However, its high observational cost limits current IFU datasets to $\sim 10^4$ objects. We present a multi-modal, probabilistic foundation model that predicts high-resolution spectra with calibrated uncertainties at arbitrary spatial locations within a galaxy directly from broadband images. Built on a masked autoencoder framework, our architecture injects fiber positional encodings and redshift aware wavelength encodings, enabling spatially conditioned predictions. Trained on 4.7 million images and single fiber spectroscopic observations from the Dark Energy Spectroscopic Instrument (DESI) survey, our model exploits the natural variance of fiber placements and the morphological self-similarity of galaxies to achieve IFU-like capabilities without any IFU training data. Predicted emission line flux maps match independent IFU observations from the Mapping Nearby Galaxies at APO (MaNGA) survey, with performance comparable to a supervised baseline trained directly on IFU data.

Scalable information retrieval testing needs corpora that are large enough to stress index construction, ranking latency, query routing, and evaluation tooling, yet human-judged test collections remain expensive and may be unavailable when documents are private or still under design. This paper introduces SPECTRA, a reproducible framework for generating synthetic text corpora and retrieval test collections through a separation of latent topical structure, surface text realization, metadata controls, query intent generation, and deterministic relevance oracles. The framework is intended as a diagnostic complement to Cranfield-style and TREC-style evaluation, not as a replacement for human assessment. A single-process Python prototype generated corpora up to 60,000 documents and 9.61 million tokens while preserving controllable long-tail vocabulary growth and producing graded relevance labels for 96 queries. In the local simulation study, generation remained close to linear at roughly 12K to 14K documents per second, estimated Zipf slopes stayed near 0.86 in absolute value, and increasing cross-topic distractor text reduced BM25 nDCG@10 from 1.00 at 2% distractors to 0.43 at 36% distractors. These results show that lightweight synthetic corpora can expose retrieval-system scaling and failure modes before costly collection construction begins.

Stellar spectra encode key information on the physical properties and chemical compositions of stars. Accurate stellar parameter determination is essential for addressing major questions such as galaxy and stellar evolution. Large-scale spectroscopic surveys have accumulated unprecedented spectral data. Traditional feature extraction or model-fitting approaches struggle with high-dimensional, massive datasets, limited generalization, and computational inefficiency. Recent advances in large language models demonstrate strong generalization and feature-learning in tasks like natural language processing, DNA/RNA sequence analysis, and protein/chemical parsing. Stellar spectra are continuous sequential signals, enabling the transfer of language models to stellar spectroscopy. Here, we propose a two-stage large language model framework for stellar parameter inference, achieving accurate estimation of effective temperature, surface gravity, metallicity, and abundances of ~20 chemical elements. Scaling-law analyses show systematic performance improvements with increasing data, providing a scalable framework for forthcoming large-scale surveys.

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.

Neural generative samplers for lattice field theory can be costly to train and evaluate. When they miss modes or assign them incorrect relative weights, biased observables do not reveal which collective variables are responsible. We project a trained flow-matching velocity onto vector fields built from lattice operators and Fourier modes. In two-dimensional lattice $φ^4$ theory, the projection separates changes in the overall magnetization from the lowest nonzero-momentum fluctuations and guides an explicit invertible proposal that treats them separately. Allowing the amplitude of the lowest nonzero-momentum fluctuations to depend on the magnetization improves the overlap between the proposal and target distributions, while the same two-parameter modification at higher momenta gives smaller improvements. The Metropolis--Hastings correction defines a Markov chain with the target Boltzmann distribution as its stationary law, and the normalized proposal density yields finite-volume partition-function estimates consistent with an independent HMC calculation. At the larger tested volume, the overlap between the proposal and target distributions deteriorates substantially, limiting the range over which the same parameterization remains effective.

Existing spectral benchmarks are limited in scale, modality alignment, and evaluation scope, and typically focus on either specialized models or multimodal language models (MLLMs). We introduce SpecX, a large-scale benchmark for multi-modal spectroscopy with cross-paradigm evaluation. SpecX contains 1.7M molecules with diverse spectral modalities, including NMR (1H, 13C, HSQC), IR, MS,UV,Raman and FL, and is organized into three tiers: a large-scale dataset for pretraining, an aligned multi-spectral subset for benchmarking, and a high-quality experimental subset for evaluation. SpecX supports a range of tasks such as molecular elucidation, spectrum simulation, and spectral understanding, and enables unified evaluation across both specialized spectral models and MLLMs. Experiments show that specialized models excel at signal-level modeling, while MLLMs exhibit strengths in high-level reasoning but lack precise spectral grounding. SpecX establishes a unified benchmark for spectral intelligence and highlights the need for spectrum-native foundation models.

We introduce a spectral-injection diagnostic for measuring which angular frequencies a trained equivariant force-field backbone preserves: inject a controlled angular-frequency perturbation into a molecular force field, attach a lightweight Spectral Prediction Network (SPN) to the frozen backbone, and read off which frequencies are recoverable. On aspirin, a quadratic SPN attached to an L = 2 NequIP backbone recovers the boundary signal at l = 4 but collapses at l = 5: a 11.7x cliff at the predicted drL boundary, with p dropping from 0.913 to 0.078. The same boundary-vs-above contrast persists across n = 4 independently trained backbones (raw-gain delta contrast, hierarchical cluster bootstrap) and is corroborated by a denominator-free injected-residual metric (R2_inj(4) = 0.374 versus R2_inj(5) = 0.006). A finite-degree span theorem calibrates the diagnostic: for a single marked direction, degree-d polynomials of degree-L spherical-harmonic features span exactly H less than or equal to dL with multiplicity-one saturation at the boundary (scoped to single-direction degree-bounded probes, not a function-class upper bound on multi-atom MPNNs). A synthetic C5 calibration plus capacity, activation, and cross-architecture controls rule out parameter count alone as the explanation.

Training loss and throughput can hide distinct internal representation in language-model training. To examine these hidden mechanics, we use spectral measurements as practical and operational diagnostics. Using a controlled family of decoder-only models adapted from the modded NanoGPT codebase, we introduce an empirical protocol based on activation covariance and per-sample gradient SVD spectra. This dual-view reveals three empirical findings and one mechanistic explanation. First, batch size acts as a latent determinant of representation geometry: runs that reach equal loss settle into systematically distinct activation spectra. Second, the activation covariance tail measured early in training reliably forecasts downstream token efficiency. Third, movement of the activation spectrum head (leading modes), together with gradient spectra, characterizes underlying learning-dynamics changes, separating learning-side architectural improvements from primarily execution-side gains. These predictive and diagnostic signals persist across the 12-, 36-, and 48-layer model tiers. Finally, a mechanistic model proves the main observations and explains how activation covariance spectra correlate with task-aligned feature learning.

Laser absorption spectroscopy (LAS) is a well-established technique for non-intrusive measurement of gas species in combustion and atmospheric environments, but conventional methods struggle with multi-species mixtures under dynamic or interference-laden conditions. Overlapping spectral features, noise, and incomplete reference data limit reliability when unknown or weakly absorbing species are present. This dissertation develops diagnostics combining LAS with machine learning (ML) to address these limitations. Deep denoising autoencoders (DDAEs) are applied to shock-tube measurements during high-speed hydrocarbon pyrolysis, improving signal fidelity and detection limits for trace species. A structured unsupervised framework, HT-SIMNet, then mitigates interference from unknown species without full calibration data, using spectral augmentation and a Noise2Noise-inspired scheme to isolate species in reactive systems. Where reference spectra are unavailable, UnblindMix, an autoencoder-based blind source separation method, reconstructs concentrations and spectral signatures directly from mixture data, validated on mixtures of up to eight components. To recover weakly absorbing species masked by broader absorbers, a feature-engineering method based on first derivatives and convolutions selectively highlights minor species. Finally, VOC-certifire combines randomized smoothing with Voigt-based spectral perturbation to provide certifiable classification of volatile organic compounds under varying conditions. All techniques are experimentally validated and benchmarked. The integration of spectroscopic hardware with ML offers a path toward real-time, interference-resilient, reference-free gas detection for combustion science, environmental monitoring, and industrial safety.

While machine-learned interatomic potentials (MLIPs) accelerate phonon dispersion calculations, merely identifying dynamical instabilities in computationally predicted materials is insufficient; automated pathways to resolve them are required. We introduce VibroML, an open-source Python toolkit driven by foundational MLIPs that shifts the paradigm from stability verification to automated structural remediation. VibroML employs an energy-guided genetic algorithm that vastly outperforms traditional soft-mode following, efficiently navigating the potential energy surface to uncover diverse, dynamically stable polymorphs. As 0 K harmonic stability does not guarantee macroscopic viability, an automated molecular dynamics workflow evaluates finite-temperature structural retention. VibroML also couples with ProtoCSP, our combinatorial structure prediction engine, to stabilize frustrated crystal topologies via targeted alloying, successfully rescuing functional perovskite networks like Cs$_2$KInI$_6$ and KTaSe$_3$. Demonstrating broader applicability, we mined the Alexandria database -- where ~50% of quaternary and 99.5% of quinary elemental combinations lack any structural entries -- to identify thousands of abandoned, high-symmetry stoichiometries. Deploying ProtoCSP's "cold start" retrieval and VibroML's evolutionary search on a sample, we successfully identified dynamically stable low-symmetry candidates. Through integrated structural remediation, thermal validation, and systematic compositional exploration, VibroML enables a comprehensive deep-screening approach, yielding physically sound structural propositions that far surpass standard high-throughput workflows.

This paper introduces AutoREC, an open-source Python platform for developing, training, and evaluating reinforcement learning (RL) agents that automatically generate equivalent circuit models (ECMs) from electrochemical impedance spectroscopy (EIS) data. Although ECMs are widely used to interpret EIS measurements, their identification typically relies on manual trial-and-error, requiring domain expertise and limiting scalability, particularly in autonomous experimental pipelines such as self-driving laboratories. In AutoREC, ECM generation is formulated as a Markov decision process in which an RL agent sequentially modifies a circuit topology based on the current state, available actions, and feedback from the resulting model. The platform supports an end-to-end workflow encompassing EIS preprocessing with selectable impedance representations, agent setup and training, ECM generation for new measurements, and visualization-based evaluation and analysis of agent decision-making. AutoREC implements a configurable Double Deep Q-Network (DDQN) agent with prioritized experience replay and a dedicated dead-loop mitigation strategy for navigating the complex circuit-generation action space efficiently. To demonstrate the platform, we trained and evaluated a representative agent on synthetic EIS datasets and applied it to previously unseen experimental spectra from battery, corrosion, oxygen evolution reaction, and CO$_2$ reduction systems. These case studies illustrate the end-to-end capabilities of AutoREC while revealing challenges associated with experimental complexity and limited training-data coverage. The demonstrated agent serves as a reference implementation; AutoREC provides an extensible foundation through which users can develop and evaluate agents tailored to their specific electrochemical systems and research objectives.

Coherent transition radiation (CTR) spectroscopy is a critical diagnostic for characterizing the longitudinal structure of relativistic electron bunches in laser-plasma and conventional accelerators. In practice, recovering the bunch profile from a measured CTR spectrum is an ill-posed phase-retrieval problem. Traditionally, this is addressed using Gerchberg-Saxton (GS)-type iterative algorithms. However, these implementations often rely on explicit inverse propagators, making them difficult to adapt to sophisticated experimental forward models. In this work, we introduce a flexible gradient-based framework for CTR phase retrieval. By leveraging a differentiable forward model, we propose a phase-only gradient descent (GD-Phase) approach that enforces the measured spectral amplitude as a hard constraint while optimizing the Fourier phase under physical real-space priors. Using synthetic CTR spectra spanning multi-peaked and strongly modulated profiles, we benchmark GD-Phase against traditional GS and a real-space amplitude-parametrized gradient descent (GD-Amp) algorithm. Unlike traditional methods, this formulation allows for the seamless inclusion of arbitrary differentiable experimental effects into the reconstruction loop. We demonstrate that this physics-informed approach not only reproduces the fidelity of GS methods but also establishes a robust baseline for incorporating multi-diagnostic constraints and uncertainty quantification. This enables the systematic extension to higher-dimensional, multimodal, and uncertainty-aware diagnostics, facilitating fast and scalable phase retrieval in realistic experimental settings.

Raman spectra obtained in real world applications are often a noisy combination of several spectra of various substances in a tested sample. Unmixing such spectra into individual components corresponding to each of the substances is of great value and has been a longstanding challenge in Raman spectroscopy. Existing unmixing methods are predominantly designed to invert an overdetermined mixed model and therefore require multiple mixed spectra as input. However, open domain and/or non-cooperative detection applications in Raman spectroscopy such as controlled substance detection, call for single-channel solutions which can identify individual components from thousands of candidates by analyzing only a single noisy mixed spectrum. To our knowledge, sparse regression is the only existing solution which can cope with this scenario, yet it has very low tolerance to noises and can hardly be applicable in practice. To address these limitations, we introduce a novel neural approach for single-channel Raman spectrum unmixing inspired by speech separation. It aims at solving underdetermined systems and can decompose a noisy mixed spectrum from a library of thousands of components (substances). The core of our method is a deep separation neural network (RSSNet) which takes a mixed spectrum as input and outputs spectra of pure components. We created two synthetic datasets of single-channel Raman spectra unmixing and demonstrated feasibility and superiority of RSSNet on these datasets (outperform competing methods by >4dB). Furthermore, we verified that RSSNet, trained solely on synthetic data, can successfully unmix real-world mixed spectra of mixtures of mineral powders, exhibiting strong generalization. Our approach represents a new paradigm for Raman unmixing and enables new possibilities for fast detection of Raman mixtures.

Portamento in string performance has been studied primarily as a binary presence-or-absence phenomenon, with existing research measuring frequency of occurrence and, less commonly, duration in milliseconds. This paper introduces a third quantitative descriptor; the spectrographic gradient of the portamento slide, measured in Hz/second, and demonstrates its measurement using a protocol combining Sonic Visualizer's melodic spectrogram layer, GIMP pixel analysis, and metric calibration against the spectrogram's known frequency axis. The gradient captures what duration alone cannot: the steepness of the pitch trajectory, which encodes the expressive character of the slide independently of its length. Applied to the opening measures of. Specifically because their monophonic texture permits reliable spectrographic pitch tracking. The method yields gradient values ranging from approximately 600Hz/s in late-period recordings to over 4,000Hz/s in early twentieth-century performances. The paper further documents a gain-recovery protocol that extends the analysable corpus to analogue recordings from the 1930s where portamento traces are faint in digital transfer. Applying the method to a corpus of 22 recordings spanning 1930--2012, the paper tests the hypothesis that gradient steepness correlates negatively with tempo: that slower performances produce steeper, longer slides while faster performances produce shallower slides or none at all. The results support this hypothesis, suggesting that the widely documented decline of portamento across the twentieth century is not a binary transition from presence to absence but a continuou

Computational X-ray absorption near-edge structure (XANES) is widely used to interpret local coordination environments, oxidation states, and electronic structure in chemically complex systems. In practice, routine computational XANES at scale is often constrained by workflow complexity rather than by the simulation method. We present ChemGraph-XANES, a large-language-model (LLM)-based agentic framework for XANES simulation and analysis that combines retrieval-augmented generation (RAG)-assisted parameter selection from documentation, schema-constrained tool execution, deterministic FDMNES input generation, and provenance-aware data curation. The framework supports both direct scripted execution and natural-language orchestration, with both modes routed through a deterministic backend for structure handling, absorber and edge specification, input generation, execution, spectral extraction, and post-processing. We demonstrate three proof-of-capability use cases: RAG-assisted selection and propagation of FDMNES input parameters, structure-file-based execution, and chemistry-level natural-language specification of absorber and composition requests. In a recorded trace, a simulation parameter is retrieved from the FDMNES manual by the RAG-enabled agent and propagated into a schema-validated tool call, illustrating traceable parameter selection. We further show that the same execution pathway supports both explicit local structures and chemistry-level user inputs. Because XANES calculations are independent once inputs are defined, ChemGraph-XANES is designed to support task-parallel execution and the creation of structure-linked XANES collections. ChemGraph-XANES therefore serves as a practical agentic framework for computational spectroscopy and data generation, emphasizing constrained orchestration, reproducibility, and traceable outputs.

The characterization of exoplanetary atmospheres has been transformed by the James Webb Space Telescope (JWST), whose infrared sensitivity enables transmission spectroscopy at unprecedented precision. However, stellar heterogeneities (e.g., spots and faculae) remain a dominant source of contamination that can bias atmospheric retrievals if not properly corrected. We present a methodology for reducing stellar contamination and instrument-specific noise from exoplanet transmission spectra using neural networks, in particular the so-called Denoising AutoEncoders (DAEs). Our goals are to enable fast, accurate corrections that improve the reliability of atmospheric parameter retrievals and to promote the use of unsupervised algorithms for efficient data processing. We designed and trained DAE architectures using large synthetic datasets of terrestrial (TRAPPIST-1e analogues) and sub-Neptune (K2-18b analogues) planets. Atmospheric retrieval experiments were then performed on contaminated spectra in order to compare our deep-learning approach against standard correction methods in terms of accuracy and computational cost. Our autoencoders successfully reconstruct uncontaminated spectra, preserving essential molecular features even in low-S/N regimes. In retrieval tests, the denoising autoencoder pre-processing yields atmospheric parameter estimates broadly comparable to those obtained with simultaneous stellar-contamination fitting. Notably, our method maintains a much lower computational cost, approximately one order of magnitude smaller. These results demonstrate that DAEs outperform conventional correction methods in computational efficiency while maintaining high accuracy, paving the way for their integration into future atmospheric characterization pipelines for both rocky and sub-Neptune exoplanets.

Multi-modal scene reconstruction integrating RGB and thermal infrared data is essential for robust environmental perception across diverse lighting and weather conditions. However, extending 3D Gaussian Splatting (3DGS) to multi-spectral scenarios remains challenging. Current approaches often struggle to fully leverage the complementary information of multi-modal data, typically relying on mechanisms that either tend to neglect cross-modal correlations or leverage shared representations that fail to adaptively handle the complex structural correlations and physical discrepancies between spectrums. To address these limitations, we propose ThermoSplat, a novel framework that enables deep spectral-aware reconstruction through active feature modulation and adaptive geometry decoupling. First, we introduce a Spectrum-Aware Adaptive Modulation that dynamically conditions shared latent features on thermal structural priors, effectively guiding visible texture synthesis with reliable cross-modal geometric cues. Second, to accommodate modality-specific geometric inconsistencies, we propose a Modality-Adaptive Geometric Decoupling scheme that learns independent opacity offsets and executes an independent rasterization pass for the thermal branch. Additionally, a hybrid rendering pipeline is employed to integrate explicit Spherical Harmonics with implicit neural decoding, ensuring both semantic consistency and high-frequency detail preservation. Extensive experiments on the RGBT-Scenes dataset demonstrate that ThermoSplat achieves state-of-the-art rendering quality across both visible and thermal spectrums.

Molecular structure elucidation from spectroscopic data is a long-standing challenge in Chemistry, traditionally requiring expert interpretation. We introduce NMIRacle, a two-stage generative framework that builds upon recent paradigms in AI-driven spectroscopy with minimal assumptions. In the first stage, NMIRacle learns to reconstruct molecular structures from count-aware fragment representations, capturing both fragment identities and their occurrences. In the second stage, a spectral encoder maps input spectra (IR, 1H-NMR, 13C-NMR) into a latent embedding used to condition the pre-trained generator, which is fine-tuned for direct spectra-to-molecule generation. This formulation bridges fragment-level chemical modeling with spectral evidence, yielding accurate molecular predictions. Empirical results demonstrate that NMIRacle outperforms existing baselines on molecular elucidation, while maintaining robust performance across increasing levels of molecular complexity.

Geospatial foundation models (GeoFMs), pretrained on large-scale geospatial data such as Earth observation (EO), climate, and weather data, have shown promising performance when fine-tuned on diverse downstream tasks. However, there are two challenges of adapting EO-pretrained GeoFMs to practical downstream datasets. The first challenge is how to handle spectral mismatch: pretrained patch embeddings expect a fixed set of input bands, whereas downstream sensors may provide different channels. The second challenge is how to reduce fine-tuning cost and make it efficient. While existing work has made efforts on these challenges individually, jointly improving fine-tuning performance under spectral mismatch while reducing adaptation cost remains underexplored. We propose SPECTRA, a parameter-efficient fine-tuning framework that addresses both spectral mismatch and adaptation cost. To handle spectral mismatch, SPECTRA introduces Band-Routed Embedding (BRE), which maps all available downstream bands into the band space expected by the pretrained GeoFM. By using BRE, all available bands in the downstream dataset are utilized to improve the selected-band input without changing the pretrained patch embedding interface. To reduce adaptation cost, SPECTRA further introduces a Stage-wise Transferability-aware LoRA (ST-LoRA) fine-tuning. ST-LoRA estimates stage-wise transferability before fine-tuning and assigns stage-specific LoRA ranks, concentrating trainable parameters on the stages with high transferability for the target task. Across three EO-pretrained GeoFMs and four downstream segmentation datasets, experiments show that BRE improves performance by utilizing all spectral bands, while ST-LoRA reduces trainable parameters compared with full fine-tuning and standard LoRA. Code is available at https://github.com/big-data-lab-umbc/SPECTRA.