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1.
Anal Chem ; 94(2): 637-649, 2022 01 18.
Artigo em Inglês | MEDLINE | ID: mdl-34931810

RESUMO

Synchronously detecting multiple Raman spectral signatures in two-dimensional/three-dimensional (2D/3D) hyperspectral Raman analysis is a daunting challenge. The underlying reasons notwithstanding the enormous volume of the data and also the complexities involved in the end-to-end Raman analytics pipeline: baseline removal, cosmic noise elimination, and extraction of trusted spectral signatures and abundance maps. Elimination of cosmic noise is the bottleneck in the entire Raman analytics pipeline. Unless this issue is addressed, the realization of autonomous Raman analytics is impractical. Here, we present a learner-predictor strategy-based "automated hyperspectral Raman analysis framework" to rapidly fingerprint the molecular variations in the hyperspectral 2D/3D Raman dataset. We introduce the spectrum angle mapper (SAM) technique to eradicate the cosmic noise from the hyperspectral Raman dataset. The learner-predictor strategy eludes the necessity of human inference, and analytics can be done in autonomous mode. The learner owns the ability to learn; it automatically eliminates the baseline and cosmic noise from the Raman dataset, extracts the predominant spectral signatures, and renders the respective abundance maps. In a nutshell, the learner precisely learned the spectral features space during the hyperspectral Raman analysis. Afterward, the learned spectral features space was translated into a neural network (LNN) model. In the predictor, machine-learned intelligence (LNN) is utilized to predict the alternate batch specimen's abundance maps in real time. The qualitative/quantitative evaluation of abundance maps implicitly lays the foundation for monitoring the offline/inline industrial qualitative/quantitative quality control (QA/QC) process. The present strategy is best suited for 2D/3D/four-dimensional (4D) hyperspectral Raman spectroscopic techniques. The proposed ML framework is intuitive because it obviates human intelligence, sophisticated computational hardware, and solely a personal computer is enough for the end-to-end pipeline.


Assuntos
Ciência de Dados , Aprendizado de Máquina , Inteligência Artificial , Humanos , Redes Neurais de Computação , Análise Espectral Raman
2.
Sci Rep ; 10(1): 12333, 2020 07 23.
Artigo em Inglês | MEDLINE | ID: mdl-32704038

RESUMO

Herein, we present the rapid synthesis of mono-dispersed carbon quantum dots (C-QDs) via a single-step microwave plasma-enhanced decomposition (MPED) process. Highly-crystalline C-QDs were synthesized in a matter of 5 min using the fenugreek seeds as a sustainable carbon source. It is the first report, to the best of our knowledge, where C-QDs were synthesized using MPED via natural carbon precursor. Synthesis of C-QDs requires no external temperature other than hydrogen (H2) plasma. Plasma containing the high-energy electrons and activated hydrogen ions predominantly provide the required energy directly into the reaction volume, thus maximizing the atom economy. C-QDs shows excellent Photoluminescence (PL) activity along with the dual-mode of excitation-dependent PL emission (blue and redshift). We investigate the reason behind the dual-mode of excitation-dependent PL. To prove the efficacy of the MPED process, C-QDs were also derived from fenugreek seeds using the traditional synthesis process, highlighting their respective size-distribution, crystallinity, quantum yield, and PL. Notably, C-QDs synthesis via MPED was 97.2% faster than the traditional thermal decomposition process. To the best of our knowledge, the present methodology to synthesize C-QDs via natural source employing MPED is three times faster and far more energy-efficient than reported so far. Additionally, the application of C-QDs to produce the florescent lysozyme protein crystals "hybrid bio-nano crystals" is also discussed. Such a guest-host strategy can be exploited to develop diverse and complex "bio-nano systems". The florescent lysozyme protein crystals could provide a platform for the development of novel next-generation polychrome luminescent crystals.

3.
Sci Rep ; 9(1): 14004, 2019 09 30.
Artigo em Inglês | MEDLINE | ID: mdl-31570739

RESUMO

Herein, we present the synthesis of mono-dispersed C-QDs via single-step thermal decomposition process using the fennel seeds (Foeniculum vulgare). As synthesized C-QDs have excellent colloidal, photo-stability, environmental stability (pH) and do not require any additional surface passivation step to improve the fluorescence. The C-QDs show excellent PL activity and excitation-independent emission. Synthesis of excitation-independent C-QDs, to the best of our knowledge, using natural carbon source via pyrolysis process has never been achieved before. The effect of reaction time and temperature on pyrolysis provides insight into the synthesis of C-QDs. We used Machine-learning techniques (ML) such as PCA, MCR-ALS, and NMF-ARD-SO in order to provide a plausible explanation for the origin of the PL mechanism of as-synthesized C-QDs. ML techniques are capable of handling and analyzing the large PL data-set, and institutively recommend the best excitation wavelength for PL analysis. Mono-disperse C-QDs are highly desirable and have a range of potential applications in bio-sensing, cellular imaging, LED, solar cell, supercapacitor, printing, and sensors.

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