Atmospheric Environment
journal homepage: www.elsevier.com/locate/atmosenv
h i g h l i g h t s g r a p h i c a l a b s t r a c t
a r t i c l e i n f o a b s t r a c t
Article history: In this paper, a new way to apportion the absorption coefcient (babs) of carbonaceous atmospheric
Received 1 August 2014 aerosols starting from a multi-wavelength optical analysis is shown. This methodology can disentangle
Received in revised form and quantify the contribution to total absorption of equivalent black carbon (EBC) emitted by wood
23 February 2015
burning (EBCWB) and fossil fuel (EBCFF) as well as brown carbon (BrC) due to incomplete combustion. The
Accepted 25 February 2015
Available online 26 February 2015
method uses the information gathered at ve different wavelengths in a renewed and upgraded version
of the approach usually referred to as Aethalometer model. Moreover, we present the results of an
apportionment study of carbonaceous aerosol sources performed in a rural area and in a coastal city, both
Keywords:
Carbonaceous aerosol
located in the North-West of Italy. Results obtained by the proposed approach are validated against
Light absorption independent measurements of levoglucosan and radiocarbon. At the rural site the EBCWB and EBCFF
Source apportionment relative contributions are about 40% and 60% in winter and 15% and 85% in summer, respectively. At the
coastal urban site, EBCWB and EBCFF are about 15% and 85% during fall. The OC contribution to the wood
* Corresponding author.
).
E-mail address: massabo@ge.infn.it (D. Massabo
http://dx.doi.org/10.1016/j.atmosenv.2015.02.058
1352-2310/ 2015 Elsevier Ltd. All rights reserved.
2 et al. / Atmospheric Environment 108 (2015) 1e12
D. Massabo
burning source at the rural site results approximately 50% in winter and 10% in summer and about 15% at
the coastal urban site in fall. The new methodology also provides a direct measurement of the absorption
ngstro m exponent of BrC (aBrC) which resulted aBrC 3.95 0.20.
2015 Elsevier Ltd. All rights reserved.
Fig. 2. Optical apportionment obtained at the rural site during wintertime 2014: (a) l 850 nm (IR) and (b) l 375 nm (UV).
Fig. 3. EC apportionment at the rural site (a) and the urban background site (b).
following the general relationship babs(l)fla, where a is different the absorbing aerosol as follows:
for BC and BrC (aBC and aBrC, respectively). Thus, Eq. (1) can be
written as:
!aFF !aWB
!aBC !aBrC babs;FF l l babs;WB l l
babs BC
l l1 babs BrC
l l1 (4)
1 1 (2) babs;FF lref lref babs;WB lref lref
babs BC
lref lref babs BrC
lref lref
where aFF and aWB are the AAE representative for FF and WB
where lref can be arbitrarily chosen. aerosol and lref can be arbitrarily chosen.
In the second case, the decomposition approach is the same as Moreover, the MWAA approach is based on the following
in the Aethalometer model: assumptions:
babs l babs;FF l babs;WB l (3) a) Wood burning is the only source of BrC;
b) BCFF and BCWB have the same AAE (aBC), disregarding the
where babs,FF and babs,WB are the contributions from FF and WB to emission source;
the total babs. This decomposition assumes that FF and WB are the c) BC and BrC have different spectral dependences, i.e. different
only sources of light absorbing species at the sampling site. In this AAE (aBC and aBrC, respectively);
6 et al. / Atmospheric Environment 108 (2015) 1e12
D. Massabo
FF (850 nm) only for samples with aexp z 1; (b) OC e OCFF vs. babs (407 nm) open squares refer to wintertime 2013 and full triangles to
Fig. 4. Rural site dataset: (a) OC versus babs, BC BrC
wintertime 2014; (c) OC e OCFF vs. bBrCabs (407 nm) for samples collected in the warm period.
et al. / Atmospheric Environment 108 (2015) 1e12
D. Massabo 7
Fig. 5. OC apportionment for the rural site (a) and the urban background site (b).
d) Fossil fuels are assumed not to contribute to BrC, thus AAE for e) aWB was set to a xed value as explained in the following.
FF aerosol is assumed to be the one for BC (aFF aBC). aFF
value was set as explained in the following; Equations (1) and (2) can be joined and rewritten as:
!aBC !aBrC
h i l h i l
BC BrC
babs l BCFF BCWB $MAClref BrC$MAClref
1 lref 1 2 lref 2
2 3 2 3
MAClref BC MAClref BrC
4BCFF BCWB $ aBC 5 laBC 4BrC$ aBrC 5 laBrC
1 2
lref 1 lref 2 (5)
|{z} |{z}
A B
h i h i
BCFF BCWB $sBC 0 laBC BrC$sBrC 0 laBrC
|{z} |{z}
A B
8 et al. / Atmospheric Environment 108 (2015) 1e12
D. Massabo
Table 1 With the same formalism introduced for Eq. (5), Eqs. (3) and (4)
Average EC and OC apportionment at the two sites. Values are given as percentages are joined and rewritten as:
of total measured EC and OC.
Fig. 6. Rural site high volume samples: (a) fNF vs. levoglucosan/TC; (b) fNF vs. TC e TCFF obtained by the optical approach (TCFF ECFF OCFF).
et al. / Atmospheric Environment 108 (2015) 1e12
D. Massabo 9
Fig. 7. (a) OCWB vs. levoglucosan and (b) ECWB vs. levoglucosan. In the case of OCWB two different OCWB to levoglucosan ratios were found for Propata (open squares) and Genoa (full
triangles).
into account the previous considerations, in this study we xed 400 and 700 nm (Lack and Langridge, 2013; and references
aFF 1.0 (see further discussion at x4). therein). The values obtained in this work are in good agreement
In the case of woodsmoke, aWB values are generally in the range with the ndings of Yang et al. (2009) who reported aBrC 3.5 (for
of 0.9e2.2 (Harrison et al., 2013; and therein cited literature) wavelength pairs 470 and 660 nm).
depending on several factors as air mass aging and the type of wood Considering Eqs. (5) and (6), the following relations can be
burnt as well as the specic wavelength range where the aWB derived:
values are calculated. In this work, we xed aWB 1.8 which gave a 8
fairly good agreement with independent 14C measurements (see > 0 BC
< A A BCWB s0
discussion at x4). Once aBC, aFF, and aWB have been set, the system is 0 BC
A BCFF s0
numerically solved by tting the two Eqs. (5) and (6) separately and >
:
B BrC sBC
0
using a MINUIT c2 minimization routine (James, 1978) home-
written as a C program (ROOT package; Brun and Rademakers, and the corresponding l dependences lead to:
1997). The minimization program ts the 5-l babs measurements
performed by MWAA following Eqs. (5) and (6) to obtain A, B, A0 , B0 8
BC aBC
> BC
< babs;WB l BCWB s0 l A A0 laBC
and aBrC for each sample. It is noteworthy the multi-l measure-
BC aBC
ments allow to run the proposed model and provide an accurate
BC
babs;FF l BCFF s0 l A0 laBC (7)
>
: BrC aBrC
tting. The mean aBrC values extracted for the Propata and Genoa
BrC
babs l BrC s0 l BlaBrC
datasets are 3.89 0.18 and 4.02 0.19, respectively (quoted un-
certainties are the standard deviation of the two distributions). thus the source-dependent (FF or WB) light absorption contribu-
Values of aBrC up to 9.5 have been reported for wavelength pairs FF (l), babs, WB(l), and babs (l)) can be
tions to BC and BrC (babs, BC BC BrC
10 et al. / Atmospheric Environment 108 (2015) 1e12
D. Massabo
obtained from the results of the minimization algorithm. Please light-absorbing carbon as well as non-combustion components
note that BrC is assumed to be emitted only by WB, thus the source (OCNC) such as spores, pollen, etc. can contribute to OC. The OC
indication is omitted in bBrC
abs . values determined by the TOT analysis can be thus expressed as:
In Fig. 1, the mean babs(l) source apportionment at the rural site
of Propata is shown. Moreover, the optical apportionment for the OC OCFF OCWB OCNC (13)
Propata winter campaign is shown as an example in Fig. 2 at
In the following, all the biogenic compounds are considered as
l 850 nm and l 375 nm. As expected, the Figures show that bBrC abs
not optically active and they are summed up in the OCNC term.
is very low at the infrared (IR) wavelength whereas it explains up to
Moreover, BrC is assumed to be produced only by the WB source;
50% of the total light absorption in the case of UV. Although
this is actually conrmed by the inter-comparison discussed in x4
bBrC
abs (850 nm) is generally low, it varies greatly from one day to
(see also Zheng et al., 2013).
another reaching values up to 11% of the total babs(850 nm).
To perform the OC apportionment, it is assumed a linear rela-
tionship between BCFF and OCFF as well as between BrC and OCWB
4.2. Mass apportionment: equivalent black carbon (EBC) (i.e. BCFF and BrC are used as tracers for FF and WB sources,
The MWAA approach described so far quanties the three main respectively). Moreover, the linear relationship between BCFF and
contributors to total babs (babs, BC BC BrC
FF , babs, WB, and babs,) at ve different BrC and their absorption coefcients allows re-writing Eq. (13) as:
l, so that:
OC k1 $babs;FF BC 850nm k2 $babs BrC 407nm OCNC (14)
babs l babs;FF BC l babs;WB BC l babs BrC l (8) |{z} |{z}
OCFF OCWB
Moreover, following the approach in Eq. (5) a wavelength-
dependent mass-absorption cross-section for BC can be intro- where:
aBC 1
duced as MACBC l sBC
0 l sBC
0 l . This allows the evaluation
of the equivalent black carbon in atmosphere (EBC) as the sum of OC is the organic carbon concentration in [mg m3] measured by
EBC from FF and WB (EBCFF and EBCWB, respectively): TOT analysis;
BC
babs, FF (850 nm) in [Mm1] is the contribution to the BCFF ab-
babs;FF BC l babs;WB BC l sorption @ l 850 nm;
EBC EBCFF EBCWB (9) 1
MAC BC l bBrC
abs (407 nm) in [Mm ] is the contribution to the BrC absorp-
tion @ l 407 nm;
With the further assumption of equivalence between the EBC in
k1 is a constant coefcient in [g m2] related to the
atmosphere and the EC determined by thermal-optical analysis
MACBC(850 nm) and to OCFF/BCFF;
(EBCFF ECFF and EBCWB ECWB), the following relationships hold
k2 is a constant coefcient in [g m2] related to the BrC MAC @
at every l:
l 407 nm and to OCWB/BrC;
! OCNC is expressed in [mg m3].
ECWB babs;WB BC
ECFF EC ECWB EC 1 EC 1
EC babs BC The absorption coefcient determined at l 850 nm and
407 nm where chosen as starting points for OCFF and OCWB deter-
! !
babs;WB BC babs babs BrC babs;WB BC mination. The choice of l 407 nm as reference for the evaluation
EC 1 EC of BrC contribution is related to the unavailability of the laser diode
babs babs BrC babs babs BrC with l 375 nm during the rst winter campaign.
(10) With our approach, both k1 and k2 are directly determined by
the experimental optical data. In samples where the aexp is close to
Focusing on the IR range where BrC contribution to total babs is
1.0 (i.e. the measured babs(l) approximately follows l1) bBrC abs is
minimized (thus reducing uncertainties on the denominator eval-
negligible, thus Eq. (14) reduces to:
uation) we obtain:
0.43 0.02 (R2 0.97). In this analysis, transition days between The model results depend on the choice of aBC, aFF, and aWB
cold and warm periods are not taken into account. Once deter- values in Eqs. (4) and (5): in the present study, they have been xed
mined k1 and k2, OCFF and OCWB are calculated for each sample and according to the recent literature and validated against indepen-
OCNC is obtained by Eq. (13). In Propata, OCWB concentration values dent techniques (aBC aFF 1.0; aWB 1.8). Although these values
are typically high during wintertime and especially during late fall in principle can be site-dependent and modied in future works,
2013 (Fig. 5a). The OCFF fraction is similar all over the year with a the data reduction approach here proposed remains valid. The
percentage increase in early springtime. OCNC concentration values optical apportionment is based on the assumption that the
are mostly negligible during the cold periods while they increase to absorbing species in aerosols are related to FF and WB only. In case
a mean <OCNC> (0.44 0.10) mg m3 during late spring and of signicant dust intrusions, this might be not true and could lead
summer. In Genoa, the OCFF fraction is dominant during the whole to inaccurate source apportionment. The possible optical activity of
campaign accounting for about 70% of total OC (Fig. 5b). In Table 1 a biogenic compounds is also neglected in this work but this issue
summary of the apportionment results for the two sites is reported. merits a further investigation. Despite of the mentioned limita-
tions, in this paper we introduce a new methodology which pro-
5. Comparison with independent techniques duces sounding results both at a rural site and in a large coastal city
in Italy.
The reliability of the optical mass apportionment was checked
by independent levoglucosan and 14C measurements. The com- Acknowledgements
parison between parallel determinations (please note that radio-
carbon measurements have been performed on 4 samples only, see This work was partially nanced by the National Institute of
x2) is shown in Fig. 6a. Nuclear Physics (INFN) in the frame of the MANIA experiment and
A very good agreement between fNF by radiocarbon measure- by the Amministrazione Provinciale di Genova. The authors
ments and levoglucosan/TC is found (slope 4.38, R2 0.99). The acknowledge Vincenzo Ariola, Franco Parodi, and Francesco Safoti
intercept value (55%) can be probably attributed to local back- (INFN-Genova) for technical support in the MWAA development
ground secondary organic aerosol, as the possible biogenic contri- and Maria Teresa Zannetti and Federico Manni (Amministrazione
bution seems to be negligible according to the optical Provinciale di Genova) for the collaboration during sampling.
apportionment (Fig. 5a).
The best agreement between the results obtained by our optical
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