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Titel |
Evolution of the complex refractive index in the UV spectral region in ageing secondary organic aerosol |
VerfasserIn |
J. M. Flores, D. F. Zhao, L. Segev, P. Schlag, A. Kiendler-Scharr, H. Fuchs, Å. K. Watne, N. Bluvshtein, Th. F. Mentel, M. Hallquist, Y. Rudich |
Medientyp |
Artikel
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Sprache |
Englisch
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ISSN |
1680-7316
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Digitales Dokument |
URL |
Erschienen |
In: Atmospheric Chemistry and Physics ; 14, no. 11 ; Nr. 14, no. 11 (2014-06-11), S.5793-5806 |
Datensatznummer |
250118787
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Publikation (Nr.) |
copernicus.org/acp-14-5793-2014.pdf |
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Zusammenfassung |
The chemical and physical properties of secondary organic aerosol (SOA)
formed by the photochemical degradation of biogenic and anthropogenic
volatile organic compounds (VOC) are as yet still poorly constrained. The evolution
of the complex refractive index (RI) of SOA, formed from purely biogenic VOC
and mixtures of biogenic and anthropogenic VOC, was studied over a diurnal
cycle in the SAPHIR photochemical outdoor chamber in Jülich, Germany.
The correlation of RI with SOA chemical and physical properties such as
oxidation level and volatility was examined. The RI was retrieved by a newly
developed broadband cavity-enhanced spectrometer for aerosol optical
extinction measurements in the UV spectral region (360 to 420 nm). Chemical
composition and volatility of the particles were monitored by a high-resolution time-of-flight aerosol mass spectrometer, and a volatility tandem
differential mobility analyzer. SOA was formed by ozonolysis of either (i) a
mixture of biogenic VOC (α-pinene and limonene), (ii) biogenic VOC
mixture with subsequent addition of an anthropogenic VOC
(p-xylene-d10), or (iii) a mixture of biogenic and anthropogenic VOC.
The SOA aged by ozone/OH reactions up to 29.5 h was found to be
non-absorbing in all cases. The SOA with p-xylene-d10 showed an
increase of the scattering component of the RI correlated with an increase
of the O / C ratio and with an increase in the SOA density. There was a
greater increase in the scattering component of the RI when the SOA was
produced from the mixture of biogenic VOCs and anthropogenic VOC than from
the sequential addition of the VOCs after approximately the same ageing time.
The increase of the scattering component was inversely correlated with the
SOA volatility. Two RI retrievals determined for the pure biogenic SOA
showed a constant RI for up to 5 h of ageing. Mass spectral characterization
shows the three types of the SOA formed in this study have a significant
amount of semivolatile components. The influence of anthropogenic VOCs on
the oxygenated organic aerosol as well as the atmospheric implications are
discussed. |
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