The treatment of raw data as well as cloud-screening was performed in the same way for both instruments. Afterwards, the two datasets of each instrument are merged in one homogeneous common “day&night” dataset. The AOD measurements are only available during cloud free time. Hence, there is also a clear-sky bias in the data evaluation. High aerosol events, which arrived during cloudy/rainy conditions, can therefore not be captured by photometer observations. Data of some months will be neglected due to the small number of measurement time, since a daily median is only calculated, if the measurement was at least 60 min long and the criterion of
Section 4.2 is extendet. A monthly median is only taken into account, if at least 5 daily median values exist. This criterion is much stricter than in other studies like [
27,
28] to obtain a more representative data set.
5.2. Monthly Changes of AOD
Figure 5 gives an overview of monthly median AOD observations over the entire measurement period 2004–2023. A detailed distribution for every month and year is provided in
Figure 6.
Winter (October to March), appears with heterogeneous monthly median AOD observations. The difference in median AOD between summer and winter exceeds 0.1 and the median AOD in winter is on average three times higher than in summer. During the time of the Arctic Haze in early spring (March and April), mean monthly median AOD is about 0.04 higher than during the summer (June to September). While these months show a low year-to-year variability, April and May show a broader variability, indicating less stable atmospheric conditions and an influence of different aerosol events occurring in Ny-Ålesund.
The months from March to September are generally characterised by a small variability between the years and a low AOD with small variability within a month. Some months and years with exceptional high AOD can still be found, but they indicate a single individual event, rather than a general trend. The exceptional high AOD in August 2019, which is already described in much detail by Xian et al. [
29].
Winters (October to February) have a pronounced increase in AOD, particularly in January, which is characterised by an elevated AOD in general and a high variability of it. The tendency shows that this season is increasingly polluted over the last two decades, with a year-to-year variability being more significant compared to summer. In the recent years, a noticeable increase in AOD was found from October to February, indicating that a change of aerosol load and/or properties has happened. The number of measurement days in October and November is sparse (see
Table 1), which is partially caused by an enhancement of arriving storms compared to other seasons by increasing the cloud cover. Even though the observational time is reduced in winter compared to summer. Our dataset reveals this enhancement of the AOD.
During the time of the Arctic Haze (March and April) the AOD is significantly reduced compared to winter, but is much higher than during summer.
Median AOD in summer (May to September) is in general lower than in winter, with less variability between adjacent years, with a yearly minimum in August. However, an extraordinary spike in AOD was observed in mid-July to early August 2019 due to wildfires and transported aerosols. This was not captured in our July data due to maintenance issues and is further discussed by Xian et al. [
29]. We did not observe a general increasing monthly AOD in the recent years (2004–2023). The difference is relatively small in summer, but large in winter. Due to many storms in autumn, the cloud cover is high (up to 80%) [
19], see
Table 1.
As a summary of the results’ analysis: Winter (October to February) is a highly polluted time of the year, what is surprising for the pristine environment of the Arctic. The importance of the Arctic Haze is clearly being reduced, since winter is the most polluted season, while simultaneously the amplitude between minimum and maximum of the median becomes larger and larger over the available measurement time. Several different reasons for this change will be discussed in the
Section 5.3 and
Section 5.7.
5.3. Trend Analysis for AOD
As already shown in
Figure 6, the AOD varies between years and months significantly. In the following, linear trends of the Arctic AOD are analysed by month (
Figure 7).
For a more substantial analysis of changes in AOD, a trend analysis is performed, first for the entire period of 2004–2023, afterwards for every decade separately. The results of the linear trend for each month and the corresponding standard deviation for this month are presented in
Table 2. The trend is calculated over the entire observation period and has the unit
. The
interval is used to determine the uncertainty of the trend analysis.
Over the entire observation time (2004–2023), the months April to June and especially May became clearer with a reduction in up to
, while the AOD in October and November increased with up to
. In agreement with
Figure 5, the standard deviation is larger for winter and smaller for summer with values around 0.02 (June), indicating that the monthly median AOD in summer changed less from year to year than in winter (0.09 in February). A significant decrease in AOD can be found in January and February. When also taking
Figure 6 into account, it can be seen, that this trend happened until the year 2020. Afterwards, a constant increasing of AOD is observed. Therefore, this linear trend only reflects roughly real changes. Generally, it can be seen that autumn becomes more polluted, while a small decrease in AOD can be found during spring.
We also tried to investigate the trend over one decade (2004–2013 and 2014–2023, respectively), but the large variability between two consecutive years of the same month does not allow a trend analysis. Hence, we stick to a twenty year long trend analysis.
5.4. Case Study: Polar Stratospheric Clouds
Polar Stratospheric Clouds (PSC) can occur in the Arctic lower stratosphere, when the temperature drops below 195 K. PSCs provide the surface, on which chemical reaction can take place to form free chlorine radicals, which directly destroy ozone molecules. Due to the required low temperatures of the atmosphere, they are typically observed in Ny-Ålesund between December and February [
30]. While the global temperature in the troposphere increases significantly due to climate change, the stratosphere cools down at the same time [
31]. This effect enhances the probability of PSC formation. Therefore, it is not trivial to directly transfer older studies like [
32,
33] to today’s occurrence probabilities of PSCs. Since these stratospheric clouds occur above Ny-Ålesund only during winter, when in parallel the AOD is significantly higher than during summer time, we estimate the possible impact of a PSC to star photometer observations. To obtain a height-dependent information about the PSC, we use additional Raman Lidar data. By measuring the back-scattering coefficient of aerosol and cloud layers, distinct and different layers can be identified. The presented ground-based observations (
Figure 8) by the Raman Lidar KARL (Koldewey Aerosol Raman Lidar), which is operated manually from Ny-Ålesund, shows one exemplary day with a thick and persistent PSC in February 2020. The temporal resolution is 10 min with a spatial resolution of 60 m. More information about the Raman Lidar KARL can be found at Hoffmann [
34]. A rough estimation of the AOD can be obtained from the extinction coefficient measured of a Raman Lidar. More information about the calculation of the AOD are described by Herrmann et al. [
35].
Figure 8 shows an example of a PSC in around 17 km to 20 km on 9 February 2020. As Massoli et al. [
33] showed, the temperature in the lower stratosphere can change rapidly from day to day, which immediately can stop the formation of PSCs or shift it into higher/lower altitudes. Generally, it can be seen in
Figure 8 the lower troposphere is quite polluted, indicated by high back-scatter values. This also supports the observations by the star photometer, which generally see a high aerosol load during the entire winter (see
Figure 6) with comparably large particles (later discussed in
Section 5.5).
Regularisation methods are used to retrieve the optical depth of this PSC. An optical depth of the PSC by Lidar is estimated to for the time period 5:09 UT to 6:40 UT. Parallel star photometer measurements with the star Merak reveal a mean aerosol optical depth for the entire atmospheric column of . Merak had during this measurement an elevation between 62°43′ and 58°31′. The Sun moved during this measurement from an elevation of about −18° to −13°.
The above described PSC dominates the back-scatter coefficient of the low stratosphere, but its contribution to the AOD measured by the star photometer is only an offset of
. Even if we correct the complete winter AOD dataset from this
PSC offset, supposing a PSC cover of 100 %, the winter months would still have higher AOD values than the summer months (see
Figure 5). As Maturilli et al. [
32] have shown, polar stratospheric clouds do not occur constantly in the Arctic winter stratosphere. Hence, the enhancement of AOD in winter cannot be caused by PSC-contamination in star photometer data, but is rather caused by aerosol layers.
5.5. Ångström Exponent
The Ångström Exponent is a very important parameter to determine the effective size of aerosols. The evaluation of the Ångström Exponent is only performed for cloud-screened data. It is defined according to Ångström [
36] as followed:
In this work, has been calculated as a linear fit of and considering at least six wavelengths in the range between 413 nm and 862 nm (before 2013) and 381 nm to 779 nm (after 2013) for the sun photometer. For the star photometer, the Ångström Exponent is calculated with seven wavelengths between 381 nm and 861 nm (before 2006), with eight wavelengths until 2010 (413 nm to 861 nm) and from 2010 onwards between 450 nm and 862 nm with ten wavelengths.
Similar to
Figure 4 (for AOD),
Figure 9 shows the daily median Ångström Exponent for both instruments from 2004–2023. As can be seen, most of the
values concentrate within the range of
. Some exceptions are recorded for values
.
Figure 10 gives a relative overview about the density of AOD versus
, where yellow indicates a high density of combination and blue colors a low one for the two photometer data sets separately for a resolution of 1 min.
For the sun photometer data, most observations accumulate in a very small range of AOD- and
-values with
and corresponding
. A band of small aerosols and low AOD is found (
). The AOD in this regime is very low, which results in a large uncertainty. This error propagates through the calculation of the Ångström Exponent, and hence, these values cannot fully be trusted. Individual events with high AOD and comparably large
are also found. Since no averaging was applied to the data displayed in
Figure 10, much more points are visible compared to
Figure 9.
The situation is different for the star photometer. As already seen in
Figure 5, the AOD is much larger than during solar measurements, with a corresponding lower
. Typical combinations for the star photometer are
and
.
A more detailed overview of monthly median
values is given in
Figure 11 for the entire measurement period in grey. In orange over all these 20 years the lines for median (solid) and mean (dashed) are plotted. A more detailed distribution characteristics of the Ångström Exponent is presented in
Figure 12. Generally, aerosols in the atmosphere above Ny-Ålesund are larger in winter times with a corresponding higher AOD than in summer times. The same result was also found by Gogoi et al. [
37], who measured scattering coefficients at the surface.
For the entire measurement period, it can be said that summers usually have a smaller monthly variability than winters. A generally increased
in April and May compared to other months of the same year cannot clearly be seen in the data, which would be expected for a clear Arctic Haze season. The exceptionally low AE values, and therefore large particles, in August correspond to a wildfire event the year 2019 [
29].
Summer exhibits smaller particles, with monthly median values typically between 1.2 and 1.7 (July), indicating a shift towards smaller aerosol sizes. The variability within a month reaches its maximum in July with low values, which indicate small particles on average. A small year-to-year variability evolves from June onwards with increasing tendency towards autumn and winter. The transition from summer to winter in September shows a gradual increase in particle size and variability.
After the polar day is over, a clear change in Ångström Exponent can be observed. Winters (October to February) are characterised by large particles with close to 1. There is significant diversity in the monthly median , with values in November ranging from 0.5 to 2.1. This is due to a wide variation in particle size during winter and especially in November. From November to January, a decreasing tendency in values is observed, indicating that particles became larger with decreasing variability from 2019 to 2023. The overall pattern suggests that aerosols arriving in the Arctic during winter, become more homogeneous (smaller spreading within a month) over time, with a consistent increase in AOD. When the mean AOD is high () and reduced with smaller . This indicates that large particles are transported into the Arctic, resulting in a local increase of the optical depth there.
Spring (March and April) shows a relatively small year-to-year variability and monthly variation in aerosol sizes. However, an expected increase in during April, indicative of the Arctic Haze season, is not clearly observed, but rather a smooth transition from winter to summer.
5.6. Trend Analysis for Ångström Exponent
For every month, the mean
value was calculated to deseasonalize the Ångström Exponent. With this deseasonalized
, the deviation between every single monthly median and its corresponding monthly mean value are calculated. The result is shown in
Figure 13.
For months with
, the observed aerosols had above-average effective sizes, for cases with
vice-versa. The variability of
was large at the beginning of the observation time. But is decreasing from year to year (for all 12 months). The trend of the monthly mean
, the Std (standard deviation of this parameter), and the
confidence interval (uncertainty of the linear trend) are shown in
Table 3.
A trend analysis is only possible to be performed with a 20-year-long data set, because the variability (indicated by the standard deviation and the 2
confidence interval) is so large, that a potential trend is hidden behind it. The uncertainty parameters (Std and
) are very large; therefore, trends of the parameter
have to be analysed carefully. Positive trends in the parameter
(see
Table 3) mean that the particle size of the aerosols is decreasing. Negative trends in the parameter
mean, that there is an increasing particle size. This occurs mostly in winter. The interpretation is that the particles transported over Ny-Ålesund in this season are getting larger from year to year.
In winter (November to February), aerosols tend to become larger, while a slight decrease in aerosol size is observed over the two decades in June to August. This trend needs to be considered with caution since for these months, the uncertainty parameters (Std and
) are the highest. As already concluded in
Section 5.2, the particles are more heterogeneous in winter, which can be supported by the analysis of the Ångström Exponent as well. The increase in AOD in autumn and early winter is caused by particles, which become larger over time. The effective particle size increases not only in the winter, but also in March and April. Therefore, we do not conclude that the time of the Arctic Haze is shifted to earlier times. Rather we interpret that there is a general trend of increasing AOD and increasing particle size (decrease in
) throughout the entire winter.
5.7. Duration of Events
With autocorrelation analysis a typical length of AOD events shall be determined for every month individually.
Figure 14 shows the autocorrelations for each month in grey,
, and the median of the different years in green. An autocorrelation analysis was performed for a month, which fulfils the requirements discussed already in
Section 4.3. For calculating the autocorrelation no interpolation was applied for measurement gaps.
Lags of 1 h and 1 day are each indicated by the black vertical lines. For all months, the variability between different years of one month is large as well as between adjacent months. For all months, the correlation coefficient decreases to
within the duration length of several hours. For every month, the vertex of the median curve (black diamond of
Figure 14) is determined. This duration estimates a typical aerosol event of this month. The vertexes of in all months have a corresponding correlation coefficient in all cases > 0.47. The different time lags are shown in
Table 4.
It can be seen that the duration is longest during the time between May and October and shortest throughout winter and spring (November to April). Generally a low variability occurs on minute time-scales. This indicates that aerosol events change significantly within usually about 3 h to 7 h. September and October have different patterns with a high variability within minute-scale, but this is due to the low data coverage (see
Table 1). On time-scales of several days the correlation coefficient varies strongly, between −1 and +1. At that point, the atmosphere has no memory of previous events. Therefore, we conclude the observed events are all different from each other, especially during winter, the autocorrelation becomes noisy. However, for some months, a small positive correlation coefficient can be observed by 1.2 to 1.5 days with
. A similar peak in
is also observed with a lower intensity in July to August with a similar length.
The more rapid decline of the median curve of the correlation coefficient between 1 h and 1 day in winter (November to March) indicates that consecutive aerosol events within one month are very diverse and no projection or forecast of their length or intensity can be made. These events also change rapidly. Sudden jumps in the correlation coefficient indicate larger gaps in the measurements, especially obviously in early winter. A smoother transition between consecutive aerosol events occur more often in summer, in which the decline of
happens on larger time scales, which indicates a smoother transition from low aerosol load to an event. The obtained duration of aerosol events agrees with the study by Dada et al. [
38], who analysed aerosol events caused by warm air mass intrusions. Overall the duration of a single event of depends strongly on the atmospheric conditions [
39].
5.8. Possible Aerosol Sources and Sinks
To investigate potential sources and sinks for high and low aerosol events in the Arctic, ten different potential contributors were investigated on their impact to the photometer observations. Therefore, a multiple linear regression analysis is performed using the implemented MATLAB-routine “regress.m”. Note that the linear independence of these parameters was not checked. After the multiple linear regression analysis was performed, an artificial AOD was reconstructed, based on the result. This reconstructed AOD was afterwards correlated with the measured one for comparison. We used the following parameters:
PNA- (Pacific-North American teleconnection pattern) and
NAO-Index (North Atlantic Oscillation) by the
Climate Prediction Center (last accessed on 6 June 2024): The NAO- and PNA-Indices are calculated daily and are based on Rotated Principal Component Analysis and are applied to monthly standardised 500 mbar height anomalies
Fire Radiative Power (FRP) by
MODIS–Moderate Resolution Imaging Spectroradiometer (last accessed on 6 June 2024): MODIS is a NASA satellite-based radiometer. It is designed for Earth observations across 36 different spectral bands, ranging from 0.4 μm to 14.4 μm in wavelength. Depending on the selected specific bands, MODIS offers a spatial resolution of 0.25° × 0.25° and a temporal resolution of approximately two days. MODIS detects wildfires by analysing the 4 μm and 11 μm bands, identifying temperature anomalies relative to the background and absolute temperatures. This study uses the Fire Radiative Power (FRP) from the two satellites Aqua and Terra, with a gridded spatial resolution of 1 km. For more information about MODIS and its data products, visit the official website:
MODIS–Moderate Resolution Imaging Spectroradiometer (last accessed on 3 October 2024)
Arctic Sea Ice Extend by
Meereisportal [
40] (Data received by authors on 19 January 2024): The sea ice extend is a product of several, homogenised data sets from different passive microwave sensors of satellite observations with horizontal resolutions between 5 km to 50 km. More information can be found at
Online Sea-Ice Knowledge and Data Platform (last accessed on 3 October 2024)
Radiosonde products (temperature (T), pressure (P), wind speed (Wind Speed) and water vapour mixing ration (water vapour)) are described in detail by Maturilli and Kayser [
41], Maturilli [
42]. At AWIPEV, one radiosonde is launched at 11 UT every day. The altitude, in which the wind is less perturbed by orography is at about 700 m as it is shown by Graßl et al. [
43] using Wind Lidar measurements. For taking local weather effects into account, we used these radiosonde observations
Precipitation observations are taken from
Met Norway (last accessed on 3 October 2024). A day with precipitation was chosen, if the daily cumulative amount was ≥1 mm.
The North Atlantic Oscillation depends on the strength and positions of Iceland Low and Azores High. In the positive phase both pressure systems are well evolved and the large-scale weather systems pass quickly. The meridional transport is weaker in the North Atlantic sector, which also prevents aerosols reaching the Arctic over this pathway. In a negative phase, both pressure systems are weak, blocking occurs. Continuously cold Arctic air reaches the midlatitudes or warm Atlantic air penetrates into the Arctic.
The PNA has a big influence on the extratropics on the Northern Hemisphere. The positive phase is associated with an enhanced East Asian jet stream with its exit over the western part of the USA with precipitation anomalies, including above-average amounts in the Gulf of Alaska to the Pacific Northwestern USA, while the negative phase is associated with blocking activity over the high latitudes of the North pacific and a strong split-flow over the central North Pacific.
In the frame of a case study by Graßl and Ritter [
9], we tested the hypothesis with a longer time series that sea ice prevents removal processes of aerosols from the lower atmosphere. Another explanation for a positive correlation between sea ice extend and AOD could be the erosion of ice crystals by wind. These ice crystals are then further transported and measured in Ny-Ålesund. To test this hypothesis, depolarisation measurements of aerosols are be needed. This information is not available with both photometers of this study and therefore has to be performed in future studies.
On a regular basis, wildfires occur in the Northern Hemisphere throughout the entire year and are a big source for aerosols, which can be lifted by several processes into the free troposphere or even stratosphere, where they are able to be transported over long distances [
44,
45,
46]. Since Russia and North America represent the two major land masses, where large wildfires on the Northern Hemisphere occur, these regions are represented in the rectangular fields by the geographical coordinates 77°N 31°E and 48°N 180°E for “Russia” and by 71°N 170°W and 48°N 52°W for “North America” (NA).
Assuming that aerosols are a good tracer of wind fields, the altitude of 700 m is used to compare the photometer data with local atmospheric conditions. For this study, monthly mean profiles were taken and compared with monthly mean AOD measurements. Temperature and pressure are taken into account, since they are good tracers for pressure systems moving over Ny-Ålesund but also warm air intrusions, which might also affect the aerosol budget.
As Schmale et al. [
14] has already shown, the Arctic aerosol budget is influenced by several different parameters. Hence, a correlation analysis between each independent parameter and the measured AOD would lead to wrong conclusions. The obtained parameters are then used to construct an AOD, which is expected to be measured, if the chosen ten parameters are responsible for the aerosol budget. A correlation analysis afterwards shows how well the artificially obtained AOD matches to the observations. Monthly median values of NAO, PNA, pressure, temperature and wind speed at 700 m altitude, integrated water vapour over the entire troposphere, sea ice cover of the Arctic, precipitation days and wildfires in North America and Russia.
The parameter coefficients for the above-mentioned parameters of the multiple linear regression are shown in
Table 5. Since sea ice cover is in the order of magnitude of
but NAO- or PNA-indices are usually <2, a normalisation was applied before calculating the regression parameters. The normalisation factors of each parameter are also given, as well as the upper and lower confidence intervals.
As shown in
Table 5, the coefficients of the multiple linear regression analysis are different for each chosen period. Early spring (March and April) are in direct comparison still a bit different, which also agrees with the previous findings of our study. The negative sign for fire radiative power (FRP) for North America and Russia might be a bit counter intuitive. We think, the highly polluted air by boreal wildfires either has no trajectories into the European Arctic or the aerosol is dry or wet removed before arriving at Svalbard. The positive coefficient between sea ice cover and AOD agrees to the study by Graßl and Ritter [
9] with a significantly larger data set. With these coefficients of
Table 5, we conclude that the measured aerosol load throughout the time period 2004–2023 is a superposition of different sources and sinks as well as different pathways into the Arctic. A clear correlation between an AOD event and a source or pathway was not found.
Figure 15 shows the measured AOD median and the reconstructed AOD based on the above-mentioned parameters after performing a multiple linear regression.
The observed and the reconstructed AOD-curves are further correlated with each other to obtain an estimation about the alignment between each other. The chosen parameters for the multiple linear regression analysis represent different seasons with a different signs and order of magnitude for the selected months or in total.
Figure 15 shows a good reconstruction for years without extreme AOD events, such as from 2009 to 2014. In other years with exceptional high AOD values, this simulation does not provide a good reconstruction. In these cases, the measured AOD is much higher than the reconstructed one.
For all months, a correlation coefficient
(
p-value:
) was found. By just looking at individual time periods the situation is different: while March and April can be reconstructed well (
,
p-value:
), summer is poorer represented with a correlation
(
p-value:
). Winter is close to the annual correlation
(
p-value:
). The small p-values in all seasons and the entire year indicate that the used set of possible sources and sinks do not span a full orthogonal basis, on which the multiple linear regression analysis is calculated because the correlation is not significant. A high correlation between the reconstructed and observed AOD indicates a large contribution by the chosen parameters to the aerosol budget at Ny-Ålesund. With this set of different parameters, the observed AOD cannot be represented entirely. This can be caused by the presence of more local sources and agrees with in situ measurements by Tunved et al. [
47]. Generally speaking, the full annual cycle can partially be explained by the chosen parameters and the correlation could be improved by using slightly different variables, with which the AOD is reconstructed.