000263854 001__ 263854
000263854 005__ 20190622141210.0
000263854 022__ $$a1867-1381
000263854 022__ $$a1867-8548
000263854 0247_ $$a10.5194/amt-12-525-2019$$2doi
000263854 02470 $$2isi$$a000456989000002
000263854 037__ $$aARTICLE
000263854 245__ $$aAtmospheric particulate matter characterization by Fourier transform infrared spectroscopy: a review of statistical calibration strategies for carbonaceous aerosol quantification in US measurement networks
000263854 260__ $$c2019-01-28
000263854 269__ $$a2019-01-28
000263854 336__ $$aReviews
000263854 520__ $$aAtmospheric particulate matter (PM) is a complex mixture of many different substances and requires a suite of instruments for chemical characterization. Fourier transform infrared (FT-IR) spectroscopy is a technique that can provide quantification of multiple species provided that accurate calibration models can be constructed to interpret the acquired spectra. In this capacity, FT-IR spectroscopy has enjoyed a long history in monitoring gas-phase constituents in the atmosphere and in stack emissions. However, application to PM poses a different set of challenges as the condensed-phase spectrum has broad, overlapping absorption peaks and contributions of scattering to the mid-infrared spectrum. Past approaches have used laboratory standards to build calibration models for prediction of inorganic substances or organic functional groups and predict their concentration in atmospheric PM mixtures by extrapolation. In this work, we review recent studies pursuing an alternate strategy, which is to build statistical calibration models for mid-IR spectra of PM using collocated ambient measurements. Focusing on calibrations with organic carbon (OC) and elemental carbon (EC) reported from thermal-optical reflectance (TOR), this synthesis serves to consolidate our knowledge for extending FT-IR spectroscopy to provide TOR-equivalent OC and EC measurements to new PM samples when TOR measurements are not available. We summarize methods for model specification, calibration sample selection, and model evaluation for these substances at several sites in two US national monitoring networks: seven sites in the Interagency Monitoring of Protected Visual Environments (IMPROVE) network for the year 2011 and 10 sites in the Chemical Speciation Network (CSN) for the year 2013. We then describe application of the model in an operational context for the IMPROVE network for samples collected in 2013 at six of the same sites as in 2011 and 11 additional sites. In addition to extending the evaluation to samples from a different year and different sites, we describe strategies for error anticipation due to precision and biases from the calibration model to assess model applicability for new spectra a priori. We conclude with a discussion regarding past work and future strategies for recalibration. In addition to targeting numerical accuracy, we encourage model interpretation to facilitate understanding of the underlying structural composition related to operationally defined quantities of TOR OC and EC from the vibrational modes in mid-IR deemed most informative for calibration. The paper is structured such that the life cycle of a statistical calibration model for FT-IR spectroscopy can be envisioned for any substance with IR-active vibrational modes, and more generally for instruments requiring ambient calibrations.
000263854 536__ $$aFNS$$c200021_143298
000263854 536__ $$aFNS$$c200021_169506
000263854 536__ $$aOther foundations$$cEPRI MA10003745
000263854 542__ $$fCC BY
000263854 650__ $$aMeteorology & Atmospheric Sciences
000263854 650__ $$aMeteorology & Atmospheric Sciences
000263854 6531_ $$apartial least-squares
000263854 6531_ $$asecondary organic aerosol
000263854 6531_ $$aopen-path ftir
000263854 6531_ $$apositive matrix factorization
000263854 6531_ $$areflectance tor measurements
000263854 6531_ $$afunctional-group composition
000263854 6531_ $$avariable selection methods
000263854 6531_ $$ainitio molecular-dynamics
000263854 6531_ $$amass-spectrometry
000263854 6531_ $$amultivariate calibration
000263854 700__ $$g221094$$aTakahama, Satoshi$$0246202
000263854 700__ $$aDillner, Ann M.
000263854 700__ $$aWeakley, Andrew T.
000263854 700__ $$g253843$$aReggente, Matteo$$0248730
000263854 700__ $$g223780$$aBurki, Charlotte$$0253785
000263854 700__ $$aLbadaoui-Darvas, Maria
000263854 700__ $$aDebus, Bruno
000263854 700__ $$aKuzmiakova, Adele
000263854 700__ $$aWexler, Anthony S.
000263854 773__ $$q525-567$$k1$$j12$$tAtmospheric Measurement Techniques
000263854 8564_ $$uhttps://infoscience.epfl.ch/record/263854/files/Atmospheric%20particulate%20matter%20characterization%20by%20Fourier%20transform%20infrared%20spectroscopy%3A%20a%20review%20of%20statistical%20calibration%20strategies%20for%20carbonaceous%20aerosol%20quantification%20in%20US%20measurement%20networks.pdf$$zFinal$$s6544739
000263854 8560_ $$fbeatrice.marselli@epfl.ch
000263854 909C0 $$pAPRL$$xU12574$$zCharbonnier, Valérie$$0252418$$mmarie.sudki@epfl.ch
000263854 909CO $$preview$$pENAC$$ooai:infoscience.epfl.ch:263854$$particle
000263854 961__ $$aalain.borel@epfl.ch
000263854 973__ $$rREVIEWED$$sPUBLISHED$$aEPFL
000263854 980__ $$aARTICLE
000263854 981__ $$aoverwrite