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Machine Learning Enhanced Laser Spectroscopy for Multi-Species Gas Detection in Complex and Harsh Environments

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.

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