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Journal of Cultural Heritage 46 (2020) 207–217

Available online at

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Original article

Spatial variability of aerosols over Greek archaeological sites using


Space-Borne Remote Sensing
Arezina Sakka a , Evangelos Gerasopoulos b,c,∗ , Eleni Liakakou b,c ,
Iphigenia Keramitsoglou d , Nikolaos Zacharias a
a
University of the Peloponnese, Department of History, Archaeology & Cultural Resources Management, 24100 Kalamata, Greece
b
National Observatory of Athens, Institute for Environmental Research and Sustainable Development, 15236 P. Penteli, Athens, Greece
c
Navarino Environmental Observatory, Costa Navarino, Navarino Dunes, 24001 Messenia, Greece
d
National Observatory of Athens, Institute for Astronomy, Astrophysics, Space Applications & Remote Sensing, 15236 P. Penteli, Athens, Greece

i n f o a r t i c l e A b s t r a c t

Historique de l’article : Twenty-one archaeological sites in Greece were selected to study their exposure to particulate pollution,
Reçu le 6 janvier 2020 in terms of aerosol loading and chemical type, to infer on the potential impact on the structural mate-
Accepté le 9 juillet 2020 rials (specifically stone) of the monuments, using Space-Borne Remote Sensing instruments, MODIS and
Disponible sur Internet le 15 August 2020
CALIPSO. The analysis revealed three geographical distributed clusters, with higher loads in the northern
Greece, slightly lower values in the south-east corner of Greece and finally the lower values over an area
Keywords : that transverses Greece from its NW to its SE corners, with differences spanning from 15 to 20%. The most
Cultural heritage
dominant aerosol types in terms of occurrence were polluted dust (38%) followed by dust (28%), together
Monument
Stone
accounting for on average 66% of the time, while the sites located on islands showed increased exposure
Aerosol to clean marine aerosol (in the order of 25%). Polluted continental aerosol increased over continental
Air pollution areas at the north and west parts of Greece, while smoke contribution was as high as 35% in specific
Dust sites. Three distinct seasonal patterns were also revealed with respect to aerosol loadings, a summer
Smoke maximum cycle in the north part of Greece, a spring maximum along an arc-like path from the west
Remote sensing coastline towards the southern parts of Greece and a spring and summer plateau in different parts of the
MODIS Greek territory. During the last decade, an important decrease in aerosol levels was observed (on average
CALIPSO
15 ± 6% per decade), attributed to effective controlling and mitigating measures in Europe. In conclusion,
Preventive conservation
the exposure of antiquities to aerosols in Greece, varies in time, seasonal intensification and chemical
type, thus continuous monitoring of particulate pollution over cultural heritage (CH) sites is imperative
to support the selection and design of appropriate measures in the field of preventive conservation of
monuments, in order to mitigate corrosion and avoid further damage.
© 2020 Les Auteurs. Publié par Elsevier Masson SAS. Cet article est publié en Open Access sous licence
CC BY (http://creativecommons.org/licenses/by/4.0/).

1. Introduction pollution phenomena [1]. This process of deterioration by external


environmental factors is a multi-dimensional interaction of clima-
Cultural heritage (CH) monuments and sites are constantly tic, biological and chemical processes, resulting from the impact of
exposed to a multitude of environmental factors and the envi- contaminants and natural elements of the surrounding setting [2].
ronment in which monuments are located plays an important Air pollution, and specifically aerosols, is a principal environmen-
role on their long-term preservation. Building materials weather tal factor amongst others (moisture, temperature, solar radiation,
progressively in the natural environment and many factors may precipitation, chemical and biochemical attack) that influence CH
accelerate this procedure (e.g. air pollution). Materials degrade not materials [3].
only nearby high emission areas but also in unpolluted conditions, Aerosol is of major importance as a constituent of the Earth’s
as a result of a combined natural aging processes and transported atmosphere and has major impacts on climate, human health,
ecosystems, and materials [4]. They are found in solid or liquid
form in suspension in the atmosphere and they can block sun-
light via absorption or scattering. The amount of these particles
∗ Corresponding author at: National Observatory of Athens, Institute for Environ- in the atmospheric column is quantified by an optical measure, the
mental Research and Sustainable Development, 15236 P. Penteli, Athens, Greece. Aerosol Optical Depth (AOD) or Aerosol Optical Thickness (AOT)
Adresse e-mail : egera@noa.gr (E. Gerasopoulos).

https://doi.org/10.1016/j.culher.2020.07.001
1296-2074/© 2020 The Authors. Published by Elsevier Masson SAS. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
208 A. Sakka et al. / Journal of Cultural Heritage 46 (2020) 207–217

[5]. It is a dimensionless quantity that measures, usually verti- Table 1


Types of crust according to their composition and environment.
cally, the extinction of solar radiation by aerosols [6,7]. Atmospheric
aerosols can have very complex chemical composition due to the Types of crust Formation
various sources and transformations they undertake [8]. Sulphates,
nitrates, ammonium, organic material, crustal species, sea salt, Black crusts • Hard black crust Gypsum, recrystallized
(cities/industrial • Loose particulate deposit calcium carbonate,
metal oxides and hydrogen ions are among the species compo-
areas) carbon particulate
sing aerosols of different particle sizes [9,10]. The aforementioned matter (sheltered
substances, which consist a polluted atmosphere, combined with areas).
various external environmental factors, like humidity and tempe- Carbonaceous Salts deposit in the surface
rature, affect the structural materials of CH monuments [11]. crusts (natural from the interior. Integration
environment) of elemental and biological
Aerosols are continuously present in the atmosphere in quite particles.
variable concentrations, due to the very large heterogeneity of their Salt crusts Soluble salts (presence of high
sources and their moderately short residence time. They are trans- salt levels) formed by wet and
ported by winds, so continental aerosol can be seen over oceans dry cycles.
and vice versa, marine aerosol over land. Their spatial and tem-
poral variability depends on the distribution of sources and sinks
from local to regional and global scales and transport processes. Dry solution which reacts with calcareous materials (CaCO3 ) to pro-
and wet deposition are the two major sinks of aerosols [10]. The duce gypsum. The repeated deposition of gypsum and the formed
presence of aerosol in Greece may vary significantly in space and porous crust has little or no attachment to the stone and as a result
time. Northern Greece is mainly influenced by long and mid-range the stone exfoliates [25,28,29]. If the stone is exposed, the reaction
transport from Eastern Europe and the Balkan countries, princi- products are washed away with rain and the surface of the stone
pally during summertime, as well as from local sources [12]. In the progressively recedes, but if the stone is in a moderately sheltered
southern parts of the country, the frequency of dust transportation position, the reaction products accumulate and form dense black
from N. Africa, mainly during the transition seasons (spring and crusts. Sea spray, salt solutions of marine origin, are transferred by
autumn) is well documented, whereas in urban areas local pollu- the wind and deposited on vertical surfaces. Containing chloride
tion is superposed over regional background [13]. In coastal areas, acids and fly ashes they are amongst the most destructive particles.
the occurrence of marine aerosol (can be classified as primary, deri- The growth of salt crystals and their evaporation within the pores
ved from the mechanical process of bubble bursting, and secondary, of a stone, generates stresses that are sufficient to turn the stone
derived through ocean emission of precursor biogenic VOCs) in the into a powder (crystallization) [15,25]. On the other hand, dust par-
form of sea spray, mobilized by winds, is also widely evidenced ticles have no direct impact on the stone, but may have harmful
[14–18]. mechanical effects through abrasion (gradual loss of material of
There are limited studies dealing with the effect of specific the surface by the constant exposure to environmental elements)
aerosol types on cultural heritage monuments. The interest of the and soiling (surface blackening which reduce the artistic appeal,
scientists has been mainly concentrated in basic gaseous pollutants caused by alterations, deposition and biological colonization) [30].
(e.g. SO2 , NOx), which are however precursors of specific aerosol Dust particles may also carry corrosive chemicals (e.g. sulphates,
components. Most of the studies are focused on urban sites and the nitrates and chlorides) through c̈oatingp̈rocesses, which create an
identification and formation of black crusts or on marine areas and oxidative environment on the surface of the stone [2,28,31]. In
the investigation of salts’ crystallization on stone surfaces. A new general, atmospheric particles and dust play a catalytic role, acting
analytical method of the chemical composition of powder deposits as a transitional layer for the deposition of air pollutants and for
on the dolomitic stone used in the Richini courtyard, a masterpiece the subsequent chemically reactions.
of Lombard Baroque, placed in Milan [19], supports the fact that The systematic monitoring of air quality is a requirement in
in urban environments, EC (elemental carbon) is one of the main most of the heritage conservation plans, since CH monuments and
particles responsible for the blackening of the surfaces and the for- sites are constantly endangered by both anthropogenic and natural
mation of black crusts [20], studying the marbles of the Demeter threats (e.g. earthquakes, floods, fires, urbanization) [32,33]. Howe-
Sanctuary in Eleusis, Greece, demonstrated that particles contai- ver, in relation to other environmental parameters such as humidity
ning Si, Fe, Al and Cu explain the rusty-yellow color of washed-out and temperature, air pollution is less often monitored [34]. Satellite
marble surfaces, and fly ash particles play significant role on surface remote sensing applications on ambient air quality investigation
encrustations. The presence of non-carbonate carbon (NCC) aero- has dramatically evolved over the last decade and satellite data can
sols and their role on surface blackening and soiling has been the be efficiently used to monitor air pollution and its potential effects
subject of investigation at the Florence Baptistery [21]. The wea- [35], opening up new horizons also for the science of archaeo-
thering mechanism of marbles, granites and sandstones exposed logy. However, relevant studies are limited and mainly focus on
to marine environments has been the focus of two studies, one urban areas [33–37]. Despite the fact that satellite remote sensing
at Delos archaeological site, where dissolution and crystallization is an expensive technique for mapping small areas and requires
of salts, occurring in cycles, was shown [22], and the other at the specialized training for analyzing data [38], it may prevail over
sandstone surfaces of the Medieval Wall in Rhodes [23]. other conventional methods due to the frequency and quickness of
Stone, as the principal structural element of monuments, is the data acquisition over large areas. Moreover, remote sensing tech-
main concern of scientists regarding air pollution impacts. There nologies, as innovative, non-destructive techniques, have shown a
are many studies that demonstrate that the main deterioration great potential for the monitoring and protection of monuments
pattern of stones due to aerosol action is the formation of crusts and sites, facilitating systematic data and information gathering
(Table 1) [24,25]. Crusts are formed via reactions of materials with [39,40]. The identification of polluted cultural heritage sites and
air pollutants deposited on their surface, and their composition and the documentation of the way cultural heritage sites is affected by
form differs depending on the type of the stone, the composition of air pollution, as seen from space, is still limited. The knowledge of
airborne particles and the climate of the area [26–28]. The mecha- aerosol types and their concentration in the atmosphere, combined
nisms of stone deterioration also differ according to the attacking with their known effect on materials, can undoubtedly contribute
aerosol or precursor agent. Sulfur oxides, nitrogen oxides, and car- to better understanding the corrosion mechanisms of materials and
bon dioxide are capable of dissolving in water and creating an acidic hence to the most suitable selection of conservation strategies.
A. Sakka et al. / Journal of Cultural Heritage 46 (2020) 207–217 209

2. Research aim Table 2


Basic statistics of AOD observations for all the archaeological sites of interest
(monthly average values for the time period 2002–2016).
The present work attempts to shed light on the potential
contribution of remote sensing on understanding the ambient envi- Avg Stdev Min Max Median
ronment that affects cultural heritage values at risk. The loading 1MR 0.217 0.058 0.095 0.410 0.219
and type of aerosols, their geographical distribution, their seaso- 2AV 0.216 0.062 0.087 0.368 0.216
nality, and trends during the last fifteen years over Greece, were 3FL 0.174 0.088 0.038 0.434 0.161
4WT 0.247 0.088 0.069 0.453 0.239
used as proxies of the exposure of well-known CH monuments
5VR 0.219 0.086 0.060 0.410 0.218
and sites spread in the Hellenic territory. The study of the impact 6LS 0.185 0.079 0.039 0.378 0.186
of aerosols on ancient and historical monuments, using Space- 7DD 0.205 0.082 0.064 0.396 0.203
Borne Remote sensing, is a relatively new direction in the field 8NC 0.187 0.072 0.062 0.372 0.180
9MS 0.200 0.052 0.105 0.332 0.197
of CH science. Unambiguously, it can serve as a useful instrument
10PL 0.204 0.057 0.094 0.347 0.206
to better understand chemical weathering mechanisms of mate- 11DE 0.186 0.071 0.055 0.346 0.186
rials, enforcing decision making towards efficient antipollution and 12AC 0.201 0.054 0.088 0.333 0.206
preventive conservation measures, targeting at mitigating further 13MC 0.180 0.056 0.072 0.333 0.178
formation of deterioration patterns, in a geospatially disaggregated 14OL 0.199 0.055 0.092 0.331 0.197
15IR 0.198 0.047 0.100 0.342 0.196
manner.
16ME 0.190 0.058 0.077 0.350 0.189
17DL 0.191 0.048 0.099 0.373 0.183
18ST 0.187 0.046 0.097 0.326 0.183
3. Materials and methods
19RH 0.203 0.056 0.090 0.353 0.207
20FS 0.204 0.053 0.109 0.376 0.204
Twenty-one archaeological sites in Greece (Table S1, Fig. 1) were 21KN 0.200 0.049 0.095 0.314 0.200
selected to study their exposure to particulate air pollution and
the potential impact on the structural materials of the monuments,
using Space-Borne Remote Sensing. Table S1 (see Supplementary On the other hand, CALIPSO is a LIDAR mission developed by
material online) contains the examined archaeological sites, their NASA and it mostly aims to improve the understanding of the role
geographical designation and their main building material [41–52]. that clouds and atmospheric aerosols play in regulating the Earth’s
The selection of the CH sites was based on the following criteria: climate and air quality, by providing the vertical structure and pro-
perties of aerosols [58–60]. CALIPSO data are available through the
• Full and dense geographical coverage of Greece in latitude and LIVAS (Lidar climatology of Vertical Aerosol Structure) project that
longitude, to obtain a representative picture at the national level, provides a global and extensive aerosol and cloud optical database
• Acquisition and study of data for different environmental [61,62]. In particular, the LIVAS climatology is a three-dimensional
conditions, with emphasis on the micro-climate and dominant global aerosol and cloud optical database, based on CALIPSO obser-
pollution sources, namely urban, remote and coastal sites, vations at 532 and 1064 nm. The final LIVAS global dataset includes
• Constant exposure to the external environmental conditions, time-averaged CALIPSO/CALIOP observations on a uniform grid of
• Historical and archaeological significance of the monuments. 1◦ × 1◦ horizontal resolution and with the original vertical resolu-
tion of CALIPSO [63]. In the framework of the present study, LIVAS
mean extinction coefficient profiles at 532 nm are implemented,
Two satellite remote sensing instruments were used to map air
for the LIVAS classified aerosol-subtypes [64].
pollution over the areas of interest, MODIS (Moderate Resolution
It is noted here that the resolution of 1◦ × 1◦ provided by GIO-
Imaging Spectro – radiometer) for the period 2002–2016 (14 years)
VANNI and LIVAS does not allow for explicit information extraction
and CALIPSO (Cloud-Aerosol Lidar and Infrared Pathfinder Satellite
over urban centers (3 out of 21 sites in this study), however it
Observation) for the partially overlapping period of 2008–2011 (4
has been used here for homogeneity purposes with respect to
years).
remote/rural sites, and also to promote ready to use, universal
In the present study, the Aerosol Optical Depth at 550 nm obtai-
approaches, versus demanding retrievals of raw data that is not
ned by MODIS has been processed. MODIS, flying onboard the
yet automated.
Terra and Aqua polar-orbit satellites, provides columnar AODs
at high accuracy [53,54] and due to its wide viewing swath,
a global coverage is achieved almost on a daily basis. AOD is 4. Results
derived via the implementation of different retrieval algorithms
applied over vegetated land and maritime areas, relying on the 4.1. Exposure of CH monuments to aerosol levels and types:
Dark Target (DT) approach [55] with varying assumptions depen- general characteristics
ding on the underlying surface type, as well as over deserts
and low-covered vegetated surfaces, relying on the Deep Blue Satellite based, times series of AOD monthly average values,
(DB) approach [56]. Here, the monthly MODIS-Aqua DT AOD550 for the time period 2002–2016 from MODIS and vertical pro-
data, derived by the latest version (Collection 6.1, C061) of files of aerosols types from CALIPSO, averaged for the time span
the applied retrieval algorithms and available at 1◦ × 1◦ spatial 2008–2011, were produced. In Figs. 2 and 3, selected sites are
resolution (Level 3, L3), has been utilized. The aforementioned presented being indicative of the geographical coverage and of
dataset has been acquired through GIOVANNI (Goddard Interactive different types (or combination of types) of aerosol (e.g. higher
Online Visualization and Analysis Infrastructure) web application percentage occurrence), respectively.
(http://giovanni.gsfc.nasa.gov/giovanni/), developed by the GES Basic statistics for all the sites are included in Table 2. The
DISC (NASA Goddard Earth Sciences Data and Information Ser- geographical distribution of the average AOD values reveals the
vices Center), which provides a simple way to explore interactively, existence of specific patterns in exposure. In particular, the inten-
visualize and analyze vast amounts of atmospheric data from satel- sity of exposure to particulate pollution is higher in north Greece
lites. Data derived from MODIS observations through GIOVANNI (average 0.225 ± 0.015, Maronia, Avdira, White Tower, Vergina).
can be used also by non-experts to study processes and trends on The next distinct cluster reveals slightly lower values in south
local to global scales [57]. Greece (average 0.202 ± 0.002, Falassarna, Knossos, Rhodes). Simi-
210 A. Sakka et al. / Journal of Cultural Heritage 46 (2020) 207–217

Fig. 1. Map of Greece indicating the location of each site followed by its code name (see Table S1). The seasonality (color of the large boxes) and the dominant aerosol types
(color of the internal squares) are also presented, shorted vertically according to their percentage of occurrence. The codes of the aerosol types in the label correspond to
clean marine (CM), dust (D), polluted continental (PC), clean continental (CC), polluted dust (PD) and smoke (S). (For interpretation of the references to colour in this figure
legend, the reader is referred to the web version of this article.)

lar values are found in the central-north Aegean Sea (average at the north and west parts of Greece, where continental pollution
0.200 ± 0.003, Sanctuary of Messa, Palamari, Ireon), which toge- mainly from central Europe and the Balkans takes place [65]. Clean
ther with the previous cluster cover the south-east corner of Greece. continental aerosol is the less frequently occurring aerosol type
Finally, two more clusters are formed, one with sites in Peloponnese with an average of 2% occurrence. The highest polluted dust occur-
and Cyclades (Olympia, Messene, Delos, Ancient Thira) with values rence is bounded at the sites in northern Greece, ranging within
in the range 0.186–0.203, and another in west and central Greece 40–50%, while 3 more sites (Mycenae, Ireon and Rhodes) also suf-
(Dodoni, Larissa, Nicopolis, Delphi, Mycenae, Acropolis) with values fer from high contributions, probably due to mixtures of dust and
in the range 0.180–0.0.199. Again, these two clusters constitute an pollution received from urban agglomerations (like Athens and Tur-
area that transverses Greece from its NW to its SE corners. The dif- kish cities e.g. Izmir) located upwind from the sites. Finally, smoke,
ference of those less polluted clusters from those which exhibit the which appears on average during 12% of the time, can reach contri-
highest levels at the north is in the order of 15–20%. butions more than 20% (mostly in central-west Greece) and up to
In Table S2, the aerosol subtype occurrence for each archaeolo- 35%, the latter in the case of Filippoi.
gical site is presented. In general, the most dominant aerosol type is
polluted dust (38%) followed by dust (28%). As expected, the higher
contributions of clean marine aerosol (in the order of 25% or higher 4.2. Seasonal patterns of exposure
compared to the average of 11%) are encountered in sites located
at islands in the Aegean Sea, including Crete island, unless ano- In order to study the seasonality of aerosol loadings, plots of
ther aerosol type is extensively dominant to mask the contribution the AOD monthly averaged values were created for each site (not
of marine sea salt. Over the same geographical area, the highest shown) and distinct annual patterns were revealed with maximum
percentages of dust (in the range 30–40%) are also revealed, cha- values observed mostly during summer or spring. After cluste-
racteristic of the southernmost sites of this analysis (Falassarna, ring the sites according to the season when the maximum value
Knossos, Rhodes), where the most intense impact of Saharan dust was found, three distinct patterns were formed: a seasonal cycle
is found. This is also the case in the central Aegean, probably reflec- with summer maximum, a seasonal cycle with spring maximum
ting the significant contribution of dust to such a relatively pristine and a cycle forming a plateau during spring and summer (denoted
environment. Polluted continental aerosol is observed on average as SUM MAX, SPR MAX and SPR-SUM MAX respectively in Fig. 1).
during 8% of the time, with maximum values over continental areas Sites falling within the same pattern were aggregated and the ave-
A. Sakka et al. / Journal of Cultural Heritage 46 (2020) 207–217 211

Fig. 2. Time series of area averaged Aerosol Optical Depth at 550 nm for land (corrected): monthly MODIS-Aqua DT AOD550 data, derived by the latest version (Collection
6.1, C061) over July 2002–June 2016.

rage cycles were calculated (Fig. 4). In the SUM MAX cluster, the the main continental axis of Greece (Dodoni, Delphi, Mycenae),
maximum value is found in August with about 2.5 times higher where none of the above two pollution sources does not appear
value compared to the winter background level encountered in to be dominant with respect to the control of their seasonality. The
December. In Fig. 1, it is shown that these site (red squares) are plateau of the values spans the period from April to August, and
located in the north part of Greece (Avdira, Filippoi, White Tower, only a slight decrease in June is distinguished. As in the case of the
Vergina, Larissa) and this summer maximum reflects the trans- SPR MAX cluster, the maximum to minimum ratio is around 2.
port of pollution from the Balkans and Eastern Europe [65,66], Similarly, the seasonal variation is also depicted in the extinction
which is intensified during summer time due the dominance of the vertical distribution of typical sites falling in the different clusters
well-established northerly, etesian winds [67,68]. In the SPR MAX (Fig. 5). Since the AOD refers to the columnar loading of aerosols
cluster, the maximum is observed during April and it is two-fold the over the sites, in order to infer on the seasonality of monuments’
minimum value, once more encountered in December. The distri- exposure, one could also look into the near surface aerosol seaso-
bution of these sites (green squares in Fig. 1) forms an arc covering nal patterns. However, it should be taken into account that certain
the west coastline and the southern parts of Greece (Nicopolis, limitations exist when focusing on the analysis near the surface.
Olympia, Messene, Falassarna, Knossos), these areas being the first The LIVAS vertical resolution within the Planetary Boundary Layer
to be exposed to dust outbreaks from N. Africa according to the (PBL) is of 60 m resolution, as it follows CALIPSO Level 2 (L2) aero-
three identified pathways of Saharan dust transport over the Eas- sol and cloud profile products. Considering that the aerosol subtype
tern Mediterranean [65]. It also covers the Aegean Sea (Ancient classification algorithm is applied to L2 products, no finer vertical
Thera, Sanctuary of Messa, Ireon, Palamari, Delos), including Acro- resolution than the 60 m can be achieved, leading to aerosol obser-
polis in Athens, where the relative contribution of dust is still high vations at heights even closer to the CH sites. Furthermore, the
in spring. Finally, the remaining cluster SPR-SUM MAX includes effort of studying aerosol properties close to the surface is constrai-
five sites spread in different parts of Greece, from the north, eas- ned by several factors, such as (a) the non-ideal recovery of the
ternmost (Maronia), to the south, easternmost (Rhodes), and along CALIOP 532 nm photomultiplier tubes (PMTs) after interaction with
212 A. Sakka et al. / Journal of Cultural Heritage 46 (2020) 207–217

Fig. 3. Vertical column of aerosol type observations (aerosol extinction at 532 nm per type) over the selected monuments (from LIVAS database). (For interpretation of the
references to colour in this figure legend, the reader is referred to the web version of this article.)

Table 3
Seasonal aspects of CH monuments’ exposure.

Code Seasonal maximum

Columnar Near surface

1MR SPR-SUM ALL


2AV SUM SUM*
3FL SUM ALL*
4WT SUM WIN
5VR SUM WIN
6LS SUM WIN
7DD SPR-SUM SPR-SUM-AUT
8NC SPR SPR-SUM-AUT
9MS SPR ALL
10PL SPR WIN
Fig. 4. Annual cycles of AOD at 550 nm (monthly average values for each month
11DE SPR-SUM ALL*
for the period 2002–2016) over the three clusters of sites with similar seasonal
12AC SPR WIN
patterns. (For interpretation of the references to colour in this figure legend, the
13MC SPR-SUM WIN*
reader is referred to the web version of this article.)
14OL SPR WIN
15IR SPR WIN
16ME SPR WIN
17DL SPR WIN-AUT dissipates smoothly above this height and up to about 4 km. Bet-
18ST SPR WIN ween 2 and 4 km the dominance of the summer time aerosol is clear
19RH SPR-SUM AUT and this drives the columnar summer maximum pattern. When loo-
20FS SPR WIN-AUT
king at the 1st km from the surface, the winter component becomes
21KN SPR WIN
more pronounced, which, given the limitations described, indicates
SPR = spring, SUM = summer, AUT = autumn, WIN = winter, ALL = year round, * = spiky the combination of more anthropogenic activities (e.g. residential
profiles.
heating) and a lower mixing height, as a result of colder condi-
tions. This near surface difference is less pronounced at non-urban
strong backscattering targets (e.g. Earth’s surface, Oceans, clouds, sites. With respect to the SPR MAX cluster, the spring columnar
even dense aerosol layers [69]; (b) misclassified gaps of clear-air values appear larger (e.g. Fig. 5b), not necessarily being the case
between Earth’s surface and the base of detected aerosol layers near the surface, where in most of the cases (see Table 3) winter
[70]; (c) layer detection errors due to low Signal-to-Noise Ratio aerosol appears again more dominant, in few cases also together
(SNR) or algorithm classification errors; (d) surface returns; (e) with autumn profiles, always keeping in mind the constraints of
representativeness/weighting effects of the computed climatolo- near surface values retrieval. Finally, the SPR-SUM MAX cluster is
gical profiles due to topographic/orographic effects [61,71]. Table 3 characterized by similar profiles in spring and summer, in most
summarizes the seasonal patterns information at the column and cases there is no seasonal pattern near the surface and spiky profiles
near the surface, for each site. are indicative of the different type of high load events, at several
The SUM MAX cluster, as evident in the case of White Tower heights. Given the significant contribution of Saharan dust mainly
(Fig. 5a), is driven by an elevated mixing layer of aerosol (up to during spring, but also summer, it should be noted that in spring
3 km), and has a relatively homogeneous vertical distribution that time dust transport is evidenced as homogeneous layers travelling
A. Sakka et al. / Journal of Cultural Heritage 46 (2020) 207–217 213

Fig. 5. Vertical column of aerosol seasonal observations (aerosol extinction at 532 nm per season) over selected monuments. The digital elevation map (DEM) used by CALIPSO
(LIVAS product), provides the maximum surface elevation over the CALIPSO overpass for the grid cell of interest. (For interpretation of the references to colour in this figure
legend, the reader is referred to the web version of this article.)

from near the surface and up to some height, whereas in sum- Similarly, Fig. 6b depicts that the western parts present slightly
mer the case of elevated dust layers, especially over the south and less exposure to aerosols (in the order of 1% per degree longitude).
central parts of the country, is also observed [72]. This can be attributed to the regional climate differentiation intro-
duced by the Pindos mountain range, which operates as a blockage
4.3. Geographical and temporal trends for meteorological systems from the west, leading to more rain over
western Greece and thus cleaner atmosphere [74]. On the other
In addition to the seasonal patterns of monument’s exposure hand, the eastern part is slightly more exposed to aerosol as it is
to pollution, inter-annual trends and north-south, west-east gra- under the influence of Istanbul’s plume [75,76], but also due to
dients were also investigated. biomass burning from the Black Sea [65,66].
In Fig. 6, the average AOD levels are displayed by latitude and During the last decade, an important decrease in AOD levels is
longitude. Taking into account the errors associated with the AOD observed in most of the sites, as seen in Fig. 7. This is attributed to
levels at each site, Fig. 6a shows clearly that in north and south measures taken at the European level for controlling and mitigating
Greece there is greater exposure of the sites to aerosols compa- aerosol emissions. A negative trend of AODs is observed during the
red to central regions, attributed to two distinct processes and period of study over the selected Greek sites, on average 15 ± 6%
emission sources in the Eastern Mediterranean. The sites located per decade. The largest decrease is found over Filippoi and Delos
in the northern part of Greece are influenced by transported pollu- (−25%). Percentage trends higher than 20% per decade present an
tion from the industrialized Central and Eastern Europe (including uncertainty in the order of 25% (i.e. the trend in Filippoi is 25 ± 6%
the Balkans), while the southern parts are frequently influenced per decade), trends in the range 10–20% have an uncertainty in the
by dust outbreaks from Saharan desert [65,66,73]. The geogra- order of 30%, and finally trends lower than 10% can have an uncer-
phical overlap of these two distinct influences drives the v-shape tainty as high as 150%, on average. On top of the general declining
look of the points in Fig. 6a, and two linear regression curves trend over Greece, geographical patterns can be distinguished but
were fitted to each one of the branches to facilitate the estima- need to be treated with caution given the magnitude of uncertain-
tion of trends. The trend is in the order of 4% (7%) per degree ties. In Fig. 7a, with the exception of Delos, the higher reductions are
latitude, from south (north) to central Greece and this finding is observed at the south and north of Greece, where the higher AODs
fully aligned with the three seasonality patterns revealed in Section are also encountered, and in the same line Acropolis also stands
4.2. out with a reduction >20%, being situated in a highly urbanized
214 A. Sakka et al. / Journal of Cultural Heritage 46 (2020) 207–217

Fig. 6. Geographical distribution (a. latitude, b. longitude) of AOD annual values for the period 2002–2016 of all sites (excluding cities). The continuous lines are the regression
lines between the data points and the error bars correspond to the standard error of the respective annual AOD means.

area. Similarly, longitude-wise (Fig. 7b) the trends are lower at the • The exposure of CH monuments to particulate pollution revealed
eastern and westernmost parts of Greece (with the exception of three geographical distributed clusters, with higher loads in the
Nicopolis), and markedly the three lowest values are found in east- northern Greece, slightly lower values in the south-east corner of
north east sites, probably under the influence of emissions from Greece and finally the lower values over an area that transverses
urban agglomerations in Turkey, potentially reflecting inefficient Greece from its NW to its SE corners. The difference between the
mitigation measures. most and less polluted clusters is in the order of 15–20%, with
pollution from the Balkans and eastern Europe on one hand and
Sahara dust from N. Africa being the main sources of the aerosol
5. Conclusions and discussion burden.
• The most dominant aerosol types in terms of occurrence are pol-
CH monuments have been exposed to natural components of luted dust (38%) followed by dust (28%), together accounting for
pollution (e.g. dust from desert areas) for hundreds to thousands on average 66% of the time. The higher contribution of dust is
years now. The anthropogenic pollution has been rising mostly encountered in the southernmost sites of this analysis (up to
after the industrial revolution and has been emerging among the 40%) due to Saharan dust transport, while, as expected, the sites
most serious environmental problems of the planet, also giving located in the Aegean Sea islands showed the major exposure to
rise to climate change due to the emission of Green House Gases clean marine aerosol (in the order of 25%). Polluted continental
(GHGs). Any instrumental exploration of the exposure of monu- aerosol makes its presence noticed over continental areas at the
ments to atmospheric pollution refers to this latter era, when north and west parts of Greece, while in certain sites the average
human’s intervention has been maximized, and the attempts are contribution from smoke can be as high as 35%.
driven massively by technological advancements. Satellite remote • Three distinct and geographically delimited seasonal patterns
sensing has been used in this study to quantify and investigate the were revealed with respect to aerosol loadings. A summer maxi-
geographical aspects of the exposure of CH materials to particu- mum cycle (max in August) in the north part of Greece, reflecting
late pollution in Greece, both in terms of absolute exposure and the transport of pollution from the Balkans and Eastern Europe,
pollutant type. The intention was an analysis to cover the whole a spring maximum (max in April) forming an arc from the west
Greek territory, for long time periods, and to map the background coastline towards the southern parts of Greece, areas first expo-
pollution condition that triggers the respective corrosion mecha- sed to dust outbreaks from N. Africa, including parts of the Aegean
nisms of monuments, in support of decisions and the design of more Sea, and finally a unimodal cycle with a spring and summer
appropriate conservation plans. plateau, spread in different parts of the Greek territory. The maxi-
The major conclusions are summarized in the following points: mum annual values are 2–2.5 times higher compared to the
A. Sakka et al. / Journal of Cultural Heritage 46 (2020) 207–217 215

Fig. 7. Negative trends of AODs monthly average values per decade by a. latitude, b. longitude.

minimum; the latter encountered during December. Given the are considered to further affect the Mediterranean by more aero-
constraints and uncertainty accompanying the near Earth’s sur- sol washout related to higher precipitation. However, the impact
face retrievals, a constant exposure is found in winter, despite the of more precipitation can also have reverse to atmospheric clea-
minimum columnar values in this season, which is probably indi- ning effects, as water presence is a significant proxy for material
cative of the increased anthropogenic combustion activities this corrosion, and the balance between the two processes is not yet
season and the entrapment of pollution within a lower Planetary understood.
Boundary Layer (PBL). The contribution of remote sensing techniques for monitoring
• During the last decade, an important decrease in aerosol levels is the pollution levels and other relevant parameters in a methodical
observed in most of the sites (on average 15 ± 6% per decade), way and global coverage, is certainly a new and promising field,
attributed to effective controlling and mitigating measures in especially after the launch of the new generation of Sentinel-5p
Europe. The higher reductions are observed where the higher satellite. Given the accompanying uncertainties and the limited
levels are found (north and south of Greece), with the highly spatial resolution (e.g. for urban scales) of the satellite measure-
urbanized site of Acropolis standing out with a reduction >20%. ments, as well as the spatio-temporal variability of aerosols, the
combination of satellite remote sensing with ground sampling
In a changing environment due to global development, urbani- seems the way forward [80,81], to effectively exploit Earth obser-
zation and climate change, it is imperative that pollution is closely vation techniques in Cultural Heritage policies.
monitored to evaluate its additive impacts on monuments. Des- The European Union through the European Environment
pite the general reduction in anthropogenic aerosol noted in many Agency, collects air quality data (e.g. ‘Air quality in Europe — 2018
parts of the world, known as global brightening [77] and attri- report’ EEA report No 12/2018) in an effort to review the progress
buted to reduced anthropogenic emissions [78,79], the levels of made towards meeting the air quality standards. However, a link
particulate pollutants are still considerable and their effect can between CH sites and environmental factors/pollution remains to
be disproportionate to this decrease due to existing deterioration be seen as an established European policy.
of the materials and memory effects [28]. Hemispheric or global The continuous monitoring of particulate pollution over CH sites
scale circulation patterns, such as the North Atlantic Oscillation can unambiguously support the selection and design of appropriate
(one of the most prominent modes of variability in the Northern measures in the field of preventive conservation of monuments, in
Hemisphere characterized by a meridional displacement of atmos- order to avoid further damage. As shown in this study, the expo-
pheric mass over the North Atlantic) and El Niño (a major source sure of antiquities to aerosols in Greece, varies in time, seasonal
of seasonal to interdecadal variability in the global atmosphere), intensification and chemical composition. Given that the basic buil-
216 A. Sakka et al. / Journal of Cultural Heritage 46 (2020) 207–217

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