Individual Micron-Sized Aerosol Qualitative Analysis-Combined Raman Spectroscopy and Laser-Induced Breakdown Spectroscopy by Optical Trapping in Air.

The attribution of single particle sources of atmospheric aerosols is an essential problem in the study of air pollution. However, it is still difficult to qualitatively analyze the source of a single aerosol particle using noncontact in situ techniques. Hence, we proposed using optical trapping to combine gated Raman spectroscopy with laser-induced breakdown spectroscopy (LIBS) in a single levitated micron aerosol. The findings of the spectroscopic imaging indicated that the particle plasma formed by a single particle ablation with a pulsed laser within 7 ns deviates from the trapped particle location. The LIBS acquisition field of view was expanded using the 19-bundle fiber, which also reduces the fluctuation of a single particle signal. In addition, gated Raman was utilized to suppress the fluorescence and increase the Raman signal-to-noise ratio. Based on this, Raman can measure hard-to-ionize substances with LIBS, such as sulfates. The LIBS radical can overcome the restriction that Raman cannot detect ionic chemicals like fluoride and chloride in halogens. To test the capability of directly identifying distinctive feature compounds utilizing spectra, we detected anions using Raman spectroscopy and cations using LIBS. Four typical mineral aerosols are subjected to precise qualitative evaluations (marble, gypsum, baking soda, and activated carbon adsorbed potassium bicarbonate). To further validate the application potential for substances with indistinctive feature discrimination, we employed machine learning algorithms to conduct a qualitative analysis of the coal aerosol from ten different origin regions. Three data fusion methodologies (early fusion, intermediate fusion, and late fusion) for Raman and LIBS are implemented, respectively. The accuracy of the late fusion model prediction using StackingClassifier is higher than that of the LIBS data (66.7%) and Raman data (86.1%) models, with an average accuracy of 90.6%. This research has the potential to provide online single aerosol analysis as well as technical assistance for aerosol monitoring and early warning.

[1]  J. Keskinen,et al.  Elemental analysis of single ambient aerosol particles using laser-induced breakdown spectroscopy , 2022, Scientific Reports.

[2]  Yun‐Hong Zhang,et al.  Direct Measurement of pH Evolution in Aerosol Microdroplets Undergoing Ammonium Depletion: A Surface-Enhanced Raman Spectroscopy Approach. , 2022, Environmental science & technology.

[3]  N. Bordel,et al.  A critical evaluation of the chlorine quantification method based on molecular emission detection in LIBS , 2022, Spectrochimica Acta Part B: Atomic Spectroscopy.

[4]  Xiaocheng Huang,et al.  Yield-Adjusted Operation for Convolution Filter Denoising. , 2021, Analytical chemistry.

[5]  Héctor C. Goicoechea,et al.  Data Handling in Data Fusion: Methodologies and Applications , 2021 .

[6]  F. J. Fortes,et al.  Optical Trapping as a Morphologically Selective Tool for In Situ LIBS Elemental Characterization of Single Nanoparticles Generated by Laser Ablation of Bulk Targets in Air. , 2021, Analytical chemistry.

[7]  Tianlong Zhang,et al.  Novel Method Based on Hollow Laser Trapping-LIBS-Machine Learning for Simultaneous Quantitative Analysis of Multiple Metal Elements in a Single Microsized Particle in Air. , 2021, Analytical chemistry.

[8]  Yun Wang,et al.  Mechanism of signal uncertainty generation for laser-induced breakdown spectroscopy , 2020, Frontiers of Physics.

[9]  W. Krolikowski,et al.  Optical beaming of electrical discharges , 2020, Nature Communications.

[10]  R. Sullivan,et al.  Aerosol Optical Tweezers Elucidate the Chemistry, Acidity, Phase Separations, and Morphology of Atmospheric Microdroplets. , 2020, Accounts of chemical research.

[11]  Fiona Tummon,et al.  Real-time sensing of bioaerosols: Review and current perspectives , 2020, Aerosol Science and Technology.

[12]  Jidong Lu,et al.  Coal Discrimination Analysis using Tandem Laser-Induced Breakdown Spectroscopy and Laser Ablation Inductively Coupled Plasma Time of Flight Mass Spectrometry. , 2020, Analytical chemistry.

[13]  A. Järvinen,et al.  Toward elemental analysis of ambient single particles using electrodynamic balance and laser-induced breakdown spectroscopy , 2020 .

[14]  Yuzhu Liu,et al.  The in situ detection of smoking in public area by laser-induced breakdown spectroscopy. , 2020, Chemosphere.

[15]  V. K. Unnikrishnan,et al.  Echelle LIBS-Raman system: A versatile tool for mineralogical and archaeological applications. , 2020, Talanta.

[16]  R. Sullivan,et al.  In situ pH measurements of individual levitated microdroplets using aerosol optical tweezers. , 2019, Analytical chemistry.

[17]  J. Bai,et al.  Investigation on Thermally-Induced Nonlinearity of Organic Solvents and Real-Time Visualization of the Nucleophilic Addition Reaction Using Spatial Cross-phase Modulation. , 2019, The journal of physical chemistry letters.

[18]  U. Pöschl,et al.  Size-resolved Single-particle Fluorescence Spectrometer (S2FS) for Real-time Analysis of Bioaerosols: Laboratory Evaluation and Atmospheric Measurements. , 2019, Environmental science & technology.

[19]  J. Kostamovaara,et al.  Time‐gated Raman and laser‐induced breakdown spectroscopy in mapping of eudialyte and catapleiite , 2019, Journal of Raman Spectroscopy.

[20]  F. J. Fortes,et al.  Subfemtogram Simultaneous Elemental Detection in Multicomponent Nanomatrices Using Laser-Induced Plasma Emission Spectroscopy within Atmospheric Pressure Optical Traps. , 2019, Analytical chemistry.

[21]  Y. Duan,et al.  Novel combined instrumentation for laser-induced breakdown spectroscopy and Raman spectroscopy for the in situ atomic and molecular analysis of minerals , 2019, Instrumentation Science & Technology.

[22]  G. Galbács,et al.  Qualitative discrimination of coal aerosols by using the statistical evaluation of laser-induced breakdown spectroscopy data , 2019, Spectrochimica Acta Part B: Atomic Spectroscopy.

[23]  Tianlong Zhang,et al.  Determination of coal properties using laser-induced breakdown spectroscopy combined with kernel extreme learning machine and variable selection , 2018 .

[24]  P. Cheng,et al.  Laser ablation single particle aerosol mass spectrometry for the direct analysis of raw coal samples , 2018 .

[25]  Yong-Le Pan,et al.  Optical trapping and manipulation of single particles in air: Principles, technical details, and applications , 2018, Journal of Quantitative Spectroscopy and Radiative Transfer.

[26]  V. K. Unnikrishnan,et al.  A hyphenated echelle LIBS-Raman system for multi-purpose applications. , 2018, The Review of scientific instruments.

[27]  J. Bai,et al.  Particle trapping and manipulation using hollow beam with tunable size generated by thermal nonlinear optical effect , 2018 .

[28]  J. Heikkonen,et al.  Time-Gated Raman Spectroscopy for Quantitative Determination of Solid-State Forms of Fluorescent Pharmaceuticals , 2018, Analytical chemistry.

[29]  F. J. Fortes,et al.  Spectral Identification in the Attogram Regime through Laser-Induced Emission of Single Optically Trapped Nanoparticles in Air. , 2017, Angewandte Chemie.

[30]  H. W. Chen,et al.  Diffraction-free, Self-reconstructing Bessel beam generation using thermal nonlinear optical effect , 2017, 2018 Conference on Lasers and Electro-Optics (CLEO).

[31]  R. Sullivan,et al.  Emulsified and Liquid-Liquid Phase-Separated States of α-Pinene Secondary Organic Aerosol Determined Using Aerosol Optical Tweezers. , 2017, Environmental Science and Technology.

[32]  Yong-Le Pan,et al.  Detection and characterization of chemical aerosol using laser-trapping single-particle Raman spectroscopy. , 2017, Applied optics.

[33]  J. Hermann,et al.  Laser-induced plasma emission: from atomic to molecular spectra , 2017 .

[34]  F. J. Fortes,et al.  Atomization efficiency and photon yield in laser-induced breakdown spectroscopy analysis of single nanoparticles in an optical trap , 2017 .

[35]  J. Axson,et al.  Atmospheric Aerosol Chemistry: Spectroscopic and Microscopic Advances. , 2017, Analytical chemistry.

[36]  Chuji Wang,et al.  Optical configurations for photophoretic trap of single particles in air. , 2016, The Review of scientific instruments.

[37]  N. Bordel,et al.  Quantification of fluorine traces in solid samples using CaF molecular emission bands in atmospheric air Laser-Induced Breakdown Spectroscopy , 2016 .

[38]  Ruth Signorell,et al.  Ultraviolet broadband light scattering for optically-trapped submicron-sized aerosol particles. , 2016, Physical chemistry chemical physics : PCCP.

[39]  Yong-Le Pan,et al.  Optical trap for both transparent and absorbing particles in air using a single shaped laser beam. , 2015, Optics letters.

[40]  Yong-Le Pan,et al.  Photophoretic trapping-Raman spectroscopy for single pollens and fungal spores trapped in air , 2015 .

[41]  Weidou Ni,et al.  Application of a Spectrum Standardization Method for Carbon Analysis in Coal Using Laser-Induced Breakdown Spectroscopy (LIBS) , 2014, Applied spectroscopy.

[42]  Pavel Yaroshchyk,et al.  Automatic correction of continuum background in Laser-induced Breakdown Spectroscopy using a model-free algorithm , 2014 .

[43]  Olivier Forni,et al.  Elemental analysis of halogens using molecular emission by laser-induced breakdown spectroscopy in air , 2014 .

[44]  V. Motto-Ros,et al.  Dual-wavelength differential spectroscopic imaging for diagnostics of laser-induced plasma , 2012 .

[45]  J. Almirall,et al.  Quantitative analysis of liquids from aerosols and microdrops using laser induced breakdown spectroscopy. , 2012, Analytical chemistry.

[46]  S. Groh,et al.  100% efficient sub-nanoliter sample introduction in laser-induced breakdown spectroscopy and inductively coupled plasma spectrometry: implications for ultralow sample volumes. , 2010, Analytical chemistry.

[47]  Yong-Le Pan,et al.  Particle-fluorescence spectrometer for real-time single-particle measurements of atmospheric organic carbon and biological aerosol. , 2009, Environmental science & technology.

[48]  D. Hahn,et al.  Plasma-particle interactions in a laser-induced plasma: implications for laser-induced breakdown spectroscopy. , 2006, Analytical chemistry.

[49]  D. Hahn,et al.  Calibration effects for laser-induced breakdown spectroscopy of gaseous sample streams: analyte response of gas-phase species versus solid-phase species. , 2005, Analytical chemistry.

[50]  R. Russo,et al.  Laser ablation molecular isotopic spectrometry (LAMIS): current state of the art , 2016 .