Absorption enhancement of BC particles in a Mediterranean city and countryside: effect of PM chemistry, aging and trend analysis

. Black carbon (BC) is recognized as the most important warming agent among atmospheric aerosol particles. The absorption efficiency of pure BC is rather well known, nevertheless the mixing of BC with other aerosol particles can enhance the BC light absorption efficiency, thus directly affecting the Earth radiative balance. The effects on climate of the BC absorption enhancement due to the mixing with these aerosols is not yet well constrained because these effects depend on the availability 5 of material for mixing with BC, thus creating regional variations. Here we present the mass absorption cross-section, MAC, and absorption enhancement of BC particles, (E abs ), at different wavelengths (from 370 nm to 880 nm for on-line measurements and at 637 nm for off-line measurements) measured at two sites in the Western Mediterranean, namely Barcelona (BCN; urban background) and Montseny (MSY; regional background). E abs values ranged between 1.24 and 1.51 at the urban station depending on the season and wavelength used as well as on the 10 pure BC MAC used as a reference. The largest contribution to E abs was due to the internal mixing of BC particles with other aerosol compounds, on average between a 91 and a 100 % at 370 and 880 nm, respectively. Additionally, 14.5 and 4.6 % of the total enhancement stations from off-line measurements enabled a decade-long trend analysis of E abs at 637 nm, that showed positive statistically 25 significant trends of E abs during the warmer months at MSY station. This s.s. positive trend at MSY mirrored the observed increase of the OC:EC ratio with time. Moreover, in BCN during the COVID-19 lockdown in spring 2020 we observed a sharp increase of E abs due to the observed sharp increase of OC to elemental carbon (EC) ratio. Our results show similar values of E abs to those found in the literature for similar background stations. 2015); al. BCN; and al. Pey et al. al. 2014a, 2016) for MSY. These supersites are part of the Quality Monitoring Network and are part of ACTRIS and GAW networks. Aerosol optical properties at BCN and MSY are measured following

[1]  M. Minguillón,et al.  Compositional changes of PM2.5 in NE Spain during 2009-2018: A trend analysis of the chemical composition and source apportionment. , 2021, The Science of the total environment.

[2]  M. Minguillón,et al.  Increase in secondary organic aerosol in an urban environment , 2021, Atmospheric Chemistry and Physics.

[3]  X. Querol,et al.  Lessons from the COVID-19 air pollution decrease in Spain: Now what? , 2021, Science of The Total Environment.

[4]  A. Stohl,et al.  Changes in black carbon emissions over Europe due to COVID-19 lockdowns , 2020, Atmospheric Chemistry and Physics.

[5]  N. Pérez,et al.  Aircraft vertical profiles during summertime regional and Saharan dust scenarios over the north-western Mediterranean basin: aerosol optical and physical properties , 2020, Atmospheric Chemistry and Physics.

[6]  A. Prévôt,et al.  The new instrument using a TC–BC (total carbon–black carbon) method for the online measurement of carbonaceous aerosols , 2020, Atmospheric Measurement Techniques.

[7]  M. G. Adam,et al.  Light Absorbing Properties of Primary and Secondary Brown Carbon in a Tropical Urban Environment. , 2020, Environmental science & technology.

[8]  M. Minguillón,et al.  Evaluation of the Semi-Continuous OCEC analyzer performance with the EUSAAR2 protocol. , 2020, The Science of the total environment.

[9]  G. Močnik,et al.  Substantial brown carbon emissions from wintertime residential wood burning over France. , 2020, The Science of the total environment.

[10]  A. Tobías,et al.  Changes in air quality during the lockdown in Barcelona (Spain) one month into the SARS-CoV-2 epidemic , 2020, Science of The Total Environment.

[11]  R. Saleh From Measurements to Models: Toward Accurate Representation of Brown Carbon in Climate Calculations , 2020, Current Pollution Reports.

[12]  P. Hopke,et al.  Source apportionment of particle number size distribution in urban background and traffic stations in four European cities. , 2019, Environment international.

[13]  Qi Zhang,et al.  Light Absorption by Ambient Black and Brown Carbon and its Dependence on Black Carbon Coating State for Two California, USA, Cities in Winter and Summer , 2019, Journal of Geophysical Research: Atmospheres.

[14]  A. Prévôt,et al.  Evidence of major secondary organic aerosol contribution to lensing effect black carbon absorption enhancement , 2018, npj Climate and Atmospheric Science.

[15]  Bi-wen Wu,et al.  The influence of photochemical aging on light absorption of atmospheric black carbon and aerosol single-scattering albedo , 2018, Atmospheric Chemistry and Physics.

[16]  C. Chan,et al.  Chemical characteristics of brown carbon in atmospheric particles at a suburban site near Guangzhou, China , 2018, Atmospheric Chemistry and Physics.

[17]  R. Saleh,et al.  The Brown–Black Continuum of Light-Absorbing Combustion Aerosols , 2018, Environmental Science & Technology Letters.

[18]  T. Cheng,et al.  Light Absorption Enhancement of Black Carbon Aerosol Constrained by Particle Morphology. , 2018, Environmental science & technology.

[19]  N. Pérez,et al.  Impact of aerosol particle sources on optical properties in urban, regional and remote areas in the north-western Mediterranean , 2018 .

[20]  P. Forster,et al.  Climate Impacts From a Removal of Anthropogenic Aerosol Emissions , 2018, Geophysical research letters.

[21]  Jianmin Chen,et al.  Light absorption enhancement of black carbon from urban haze in Northern China winter. , 2017, Environmental pollution.

[22]  C. Reche,et al.  Trends analysis of PM source contributions and chemical tracers in NE Spain during 2004–2014: A multi-exponential approach , 2016 .

[23]  Jianmin Chen,et al.  Radiative absorption enhancement from coatings on black carbon aerosols. , 2016, The Science of the total environment.

[24]  R. Harrison,et al.  A European aerosol phenomenology-5 : Climatology of black carbon optical properties at 9 regional background sites across Europe , 2016 .

[25]  U. Dayan,et al.  Atmospheric pollution over the eastern Mediterranean during summer – a review , 2016 .

[26]  Edward Charles Fortner,et al.  Enhanced light absorption by mixed source black and brown carbon particles in UK winter , 2015, Nature Communications.

[27]  M. Minguillón,et al.  Chemical characterization of submicron regional background aerosols in the western Mediterranean using an Aerosol Chemical Speciation Monitor , 2015 .

[28]  L. Morawska,et al.  Traffic and nucleation events as main sources of ultrafine particles in high-insolation developed world cities , 2015 .

[29]  Y. Rudich,et al.  Optical properties of secondary organic aerosols and their changes by chemical processes. , 2015, Chemical reviews.

[30]  A. Laskin,et al.  Chemistry of atmospheric brown carbon. , 2015, Chemical reviews.

[31]  Griša Močnik,et al.  The "dual-spot" Aethalometer: an improved measurement of aerosol black carbon with real-time loading compensation , 2014 .

[32]  X. Querol,et al.  Climatology of aerosol optical properties and black carbon mass absorption cross section at a remote high-altitude site in the western Mediterranean Basin , 2014 .

[33]  J. Peñuelas,et al.  Effects of sources and meteorology on particulate matter in the Western Mediterranean Basin: An overview of the DAURE campaign , 2014 .

[34]  R. Harrison,et al.  Simplifying aerosol size distributions modes simultaneously detected at four monitoring sites during SAPUSS , 2014 .

[35]  Darrel Baumgardner,et al.  Characterizing elemental, equivalent black, and refractory black carbon aerosol particles: a review of techniques, their limitations and uncertainties , 2013, Analytical and Bioanalytical Chemistry.

[36]  B. DeAngelo,et al.  Bounding the role of black carbon in the climate system: A scientific assessment , 2013 .

[37]  J. Peñuelas,et al.  Volatile organic compounds in the western Mediterranean basin: urban and rural winter measurements during the DAURE campaign , 2012 .

[38]  T. Petäjä,et al.  Radiative Absorption Enhancements Due to the Mixing State of Atmospheric Black Carbon , 2012, Science.

[39]  A. Middlebrook,et al.  Brown carbon and internal mixing in biomass burning particles , 2012, Proceedings of the National Academy of Sciences.

[40]  X. Querol,et al.  Variability of aerosol optical properties in the Western Mediterranean Basin , 2011 .

[41]  R. Harrison,et al.  New considerations for PM, Black Carbon and particle number concentration for air quality monitoring across different European cities , 2011 .

[42]  D. Lack,et al.  Impact of brown and clear carbon on light absorption enhancement, single scatter albedo and absorption wavelength dependence of black carbon , 2010 .

[43]  J. Pichon,et al.  Characterization and intercomparison of aerosol absorption photometers: result of two intercomparison workshops , 2010 .

[44]  N. Pérez,et al.  Geochemistry of regional background aerosols in the Western Mediterranean , 2009 .

[45]  Mar Viana,et al.  Toward a standardised thermal-optical protocol for measuring atmospheric organic and elemental carbon: the EUSAAR protocol , 2009 .

[46]  G. Kallos,et al.  African dust contributions to mean ambient PM10 mass-levels across the Mediterranean Basin , 2009 .

[47]  G. Evans,et al.  Mass Absorption Cross-Section of Ambient Black Carbon Aerosol in Relation to Chemical Age , 2009 .

[48]  N. Pérez,et al.  Interpretation of the variability of levels of regional background aerosols in the Western Mediterranean. , 2008, The Science of the total environment.

[49]  J. Putaud,et al.  Toward a standardized thermal-optical protocol for measuring atmospheric organic and elemental carbon: The EUSAAR protocol , 2008 .

[50]  M. Andreae,et al.  Black carbon or brown carbon? The nature of light-absorbing carbonaceous aerosols , 2006 .

[51]  Mar Viana,et al.  Influence of Sampling Artefacts on Measured PM, OC, and EC Levels in Carbonaceous Aerosols in an Urban Area , 2006 .

[52]  T. Bond,et al.  Light Absorption by Carbonaceous Particles: An Investigative Review , 2006 .

[53]  Thomas W. Kirchstetter,et al.  Evidence that the spectral dependence of light absorption by aerosols is affected by organic carbon , 2004 .

[54]  J. Jimenez,et al.  A generalised method for the extraction of chemically resolved mass spectra from aerodyne aerosol mass spectrometer data , 2004 .

[55]  Andreas Petzold,et al.  Multi-angle absorption photometry—a new method for the measurement of aerosol light absorption and atmospheric black carbon , 2004 .

[56]  X. Querol,et al.  Sources and processes affecting levels and composition of atmospheric aerosol in the western Mediterranean , 2002 .

[57]  Xavier Querol,et al.  PM10 and PM2.5 source apportionment in the Barcelona Metropolitan area, Catalonia, Spain , 2001 .

[58]  G. Kallos,et al.  Saharan dust contributions to PM10 and TSP levels in Southern and Eastern Spain , 2001 .

[59]  M. Jacobson Global direct radiative forcing due to multicomponent anthropogenic and natural aerosols , 2001 .

[60]  P. Paatero The Multilinear Engine—A Table-Driven, Least Squares Program for Solving Multilinear Problems, Including the n-Way Parallel Factor Analysis Model , 1999 .

[61]  P. Paatero,et al.  Positive matrix factorization: A non-negative factor model with optimal utilization of error estimates of data values† , 1994 .