Abstract. We present a dynamic twin-cuvette system for quantifying the trace-gas exchange fluxes between plants and the atmosphere under controlled temperature, light, and humidity conditions. Compared with a single-cuvette system, the twin-cuvette system is insensitive to disturbing background effects such as wall deposition. In combination with a climate chamber, we can perform flux measurements under constant and controllable environmental conditions. With an Automatic Temperature Regulated Air Humidification System (ATRAHS), we are able to regulate the relative humidity inside both cuvettes between 40 and 90 % with a high precision of 0.3 %. Thus, we could demonstrate that for a cuvette system operated with a high flow rate (> 20 L min −1 ), a temperature-regulated humidification system such as ATRAHS is an accurate method for air humidification of the flushing air. Furthermore, the fully automatic progressive fill-up of ATRAHS based on a floating valve improved the performance of the entire measurement system and prevented data gaps. Two reactive gas species, ozone (O 3 ) and peroxyacetyl nitrate (PAN), were used to demonstrate the quality and performance of the twin-cuvette system. O 3 and PAN exchange with Quercus ilex was investigated over a 14 day measurement period under controlled climate chamber conditions. By using O 3 mixing ratios between 32 and 105 ppb and PAN mixing ratios between 100 and 350 ppt, a linear dependency of the O 3 flux as well as the PAN flux in relation to its ambient mixing ratio could be observed. At relative humidity (RH) of 40 %, the deposition velocity ratio of O 3 and PAN was determined to be 0.45. At that humidity, the deposition of O 3 to the plant leaves was found to be only controlled by the leaf stomata. For PAN, an additional resistance inhibited the uptake of PAN by the leaves. Furthermore, the formation of water films on the leaf surface of plants inside the chamber could be continuously tracked with our custom built leaf wetness sensors. Using this modified leaf wetness sensor measuring the electrical surface conductance on the leaves, an exponential relationship between the ambient humidity and the electrical surface conductance could be determined.

Nitrogen oxide (NOx) pollution is emerging as a primary environmental concern across Europe. While some large European metropolitan areas are already in breach of EU safety limits for NO2, this phenomenon does not seem to be only restricted to large industrialized areas anymore. Many smaller scale populated agglomerations including their surrounding rural areas are seeing frequent NO2 concentration violations. The question of a quantitative understanding of different NOx emission sources is therefore of immanent relevance for climate and air chemistry models as well as air pollution management and health. Here we report simultaneous eddy covariance flux measurements of NOx, CO2, CO and non methane volatile organic compound tracers in a city that might be considered representative for Central Europe and the greater Alpine region. Our data show that NOx fluxes are largely at variance with modelled emission projections, suggesting an appreciable underestimation of the traffic related atmospheric NOx input in Europe, comparable to the weekend-weekday effect, which locally changes ozone production rates by 40%.

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Abstract. In the present study a Relaxed Eddy Accumulation (REA) system for the quantification of vertical fluxes of nitrous acid (HONO) was developed and tested. The system is based on a three-channel-LOPAP instrument, for which two channels are used for the updrafts and downdrafts, respectively, and a third one for the correction of chemical interferences. The instrument is coupled to a REA gas inlet, for which an ultrasonic anemometer controls two fast magnetic valves to probe the two channels of the LOPAP instrument depending on the vertical wind direction. A software (PyREA) was developed, which controls the valves and measurement cycles, which regularly alternates between REA-, zero- and parallel ambient measurements. In addition, the assignment of the updrafts and downdrafts to the physical LOPAP channels is periodically alternated, to correct for differences in the interferences of the different air masses. During the study, only small differences of the interferences were identified for the updrafts and downdrafts excluding significant errors when using only one interference channel. In laboratory experiments, high precision of the two channels and the independence of the dilution corrected HONO concentrations on the length of the valve switching periods were demonstrated. A field campaign was performed in order to test the new REA-LOPAP system at the TROPOS monitoring station in Melpitz, Germany. HONO fluxes in the range of −4·1013 molecules m−2 s−1 (deposition) to +1.0·1014 molecules m−2 s−1 (emission) were obtained. A typical diurnal variation of the HONO fluxes was observed with low, partly negative fluxes during night-time and higher positive fluxes around noon. After an intensive rain period the positive HONO emissions during daytime were continuously increasing, which was explained by the drying of the upper most ground surfaces. Similar to other campaigns, the highest correlation of the HONO flux was observed with the product of the NO2 photolysis frequency and the NO2 concentration (J(NO2)·[NO2]), which implies a HONO formation by photosensitized conversion of NO2 on organic surfaces, like e.g. humic acids. Other postulated HONO formation mechanisms are also discussed, but are ranked being of minor importance for the present field campaign.

Abstract. We present a dynamic twin-cuvette system for quantifying the trace gas exchange fluxes between plants and the atmosphere under controlled temperature, light and humidity conditions. Compared with a single cuvette system, the twin-cuvette system is insensitive for disturbing background effects such as wall deposition. In combination with a climate chamber we can perform flux measurements under constant and controllable environmental conditions. With an Automatic Temperature Regulated Air Humidification System (ATRAHS) we are able to regulate the relative humidity inside both cuvettes between 40 to 90 % with a high precision of 0.3 %. Thus, we could demonstrate that for a cuvette system operated with a high flow rate (> 20 L min−1) such a temperature regulated humidification system as ATRAHS is an accurate method for air humidification of the flushing air. Furthermore, the fully automatic progressive fill-up of ATRAHS based on a floating valve improved the performance of the entire measurement system and prevented data gaps. Two reactive gas species, ozone (O3) and peroxyacetyl nitrate (PAN), were used to demonstrate the quality and performance of the twin-cuvette system. O3 and PAN exchange with Quercus ilex was investigated over a 14 day measurement period under controlled climate chamber conditions. By using O3 mixing ratios between 32–105 ppb and PAN mixing ratios between 100–350 ppt a linear dependency of the O3 flux as well as the PAN flux in relation to its ambient mixing ratio could be observed. At relative humidity (RH) of 40 %, the deposition velocity ratio of O3 and PAN was determined to be 0.45. At that humidity, the deposition of O3 to the plant leaves was found to be only controlled by the leaf stomata. For PAN an additional resistance inhibited the uptake of PAN by the leaves. Furthermore, the formation of water films on the leaf surface of plants inside the chamber could be continuously tracked with our custom built leaf wetness sensors. Using this modified leaf wetness sensor measuring the electrical surface conductance on the leaves, an exponential relationship between the ambient humidity and the electrical surface conductance could be determined.

Abstract. In the present study a relaxed eddy accumulation (REA) system for the quantification of vertical fluxes of nitrous acid (HONO) was developed and tested. The system is based on a three-channel long-path absorption photometer (LOPAP) instrument, for which two channels are used for the updrafts and downdrafts, respectively, and a third one for the correction of chemical interferences. The instrument is coupled to a REA gas inlet, for which an ultrasonic anemometer controls two fast magnetic valves to probe the two channels of the LOPAP instrument depending on the vertical wind direction. A software (PyREA) was developed, which controls the valves and measurement cycles, which regularly alternates between REA, zero and parallel ambient measurements. In addition, the assignment of the updrafts and downdrafts to the physical LOPAP channels is periodically alternated, to correct for differences in the interferences of the different air masses. During the study, only small differences of the interferences were identified for the updrafts and downdrafts excluding significant errors when using only one interference channel. In laboratory experiments, high precision of the two channels and the independence of the dilution-corrected HONO concentrations on the length of the valve switching periods were demonstrated. A field campaign was performed in order to test the new REA-LOPAP system at the TROPOS monitoring station in Melpitz, Germany. HONO fluxes in the range of -4×1013 molecules m−2 s−1 (deposition) to +1.0×1014 molecules m−2 s−1 (emission) were obtained. A typical diurnal variation of the HONO fluxes was observed with low, partly negative fluxes during night-time and higher positive fluxes around noon. After an intensive rain period the positive HONO emissions during daytime were continuously increasing, which was explained by the drying of the uppermost ground surfaces. Similar to other campaigns, the highest correlation of the HONO flux was observed with the product of the NO2 photolysis frequency and the NO2 concentration (J(NO2)⋅[NO2]), which implies a HONO formation by photosensitized conversion of NO2 on organic surfaces, such as humic acids. Other postulated HONO formation mechanisms are also discussed but are tentatively ranked being of minor importance for the present field campaign.

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