Time series are presented of radiocarbon and 13C contents in atmospheric carbon dioxide over eastern Europe (southern Poland), covering the periods 1983–1994 and 2000–2004. The carbon isotope composition was measured in biweekly composite samples of atmospheric CO2, collected about 20 m above the local ground level. The data for 2 observational sites are presented: i) city of Kraków (50°04′N, 19°55′E; 220 m asl; for 1983–1994 and 2000–2004); and ii) Kasprowy Wierch, Tatra Mountains (49°14′N, 19°56′E; 1989 m asl; for 2000–2004). The latter site is considered a regional reference station, relatively free of anthropogenic influences. During the period 1983–1994, observations in the Kraków area revealed a gradual decrease of 14C content with a broad minimum around 1991 and a small increase by about 10% in the subsequent years. δ13C also changes with time, showing a decreasing trend from approximately −9.6% in 1983, with a slope of −0.02%/yr. The observed trends for both isotopes coincide well with a substantial reduction of coal consumption in Poland and partial replacement of coal by natural gas, especially in urban regions. After 2000, the δ13C slightly increases, reaching a mean value of −10% in 2004, while Δ14C is below the reference level by ∼3.5%. Observations at Kasprowy Wierch (regional reference station) also reflect a diminishing input of fossil carbon into the regional atmosphere. The fossil component in atmospheric CO2, calculated with the aid of 14C data available for the 2 study periods, shows a reduction of anthropogenic input by a factor of 2, which is confirmed by annual statistics of coal consumption.
Regular measurements of atmospheric CO (2) mixing ratios and their carbon isotope composition ((13)C/(12)C and (14)C/(12)C ratios) performed between 2005 and 2009 at two sites of contrasting characteristics (Krakow and the remote mountain site Kasprowy Wierch) located in southern Poland were used to derive fossil fuel-related and biogenic contributions to the total CO (2) load measured at both sites. Carbon dioxide present in the atmosphere, not coming from fossil fuel and biogenic sources, was considered 'background' CO (2). In Krakow, the average contribution of fossil fuel CO (2) was approximately 3.4%. The biogenic component was of the same magnitude. Both components revealed a distinct seasonality, with the fossil fuel component reaching maximum values during winter months and the biogenic component shifted in phase by approximately 6 months. The partitioning of the local CO (2) budget for the Kasprowy Wierch site revealed large differences in the derived components: the fossil fuel component was approximately five times lower than that derived for Krakow, whereas the biogenic component was negative in summer, pointing to the importance of photosynthetic sink associated with extensive forests in the neighbourhood of the station. While the presented study has demonstrated the strength of combined measurements of CO (2) mixing ratios and their carbon isotope signature as efficient tools for elucidating the partitioning of local atmospheric CO (2) loads, it also showed the important role of the land cover and the presence of the soil in the footprint of the measurement location, which control the net biogenic surface CO (2) fluxes.
Anthropogenic emissions of carbon dioxide (CO 2) and methane (CH 4) in the atmosphere constitute an important component of the related carbon budget. The main source of anthropogenic CO 2 is burning of fossil fuels, especially in densely populated areas. Similar emissions of CH 4 are associated with the agricultural sector, coal mining, and other human activities, such as waste management and storage and natural gas networks supplying methane to large urban, industrial centers. We discuss several methods aimed at characterizing and quantifying atmospheric loads and fluxes of CO 2 and CH 4 in Krakow, the second largest city in Poland. The methods are based on atmospheric observations of mixing ratios as well as isotopic composition of the investigated gases. Atmospheric mixing ratios of CO 2 and CH 4 were measured using gas chromatography (GC) and cavity ring-down spectroscopy (CRDS). The isotopic composition of CO 2 and CH 4 was analyzed using isotope ratio mass spectrometry (IRMS), accelerator mass spectrometry (AMS), and CRDS techniques. These data, combined with auxiliary information characterizing the intensity of vertical mixing in the lower atmosphere (height of the nocturnal boundary layer [NBL] and atmospheric 222 Rn concentration), were further used to quantify emission rates of CO 2 and CH 4 in the urban atmosphere of Krakow. These methods provide an efficient way of quantifying surface emissions of major greenhouse gases originating from distributed sources, thus complementing the widely used bottom-up methodology based on emission statistics.
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