2009, Grygalashvyly, M., Sonnemann, G.R., Hartogh, P.

We investigate the influence the rising concentrations of methane, nitrous oxide and carbon dioxide which have occurred since the pre-industrial era, have had on the chemistry of the mesosphere. For this investigation we use our global 3-D-model COMMA-IAP which was designed for the exploration of the MLT-region and in particular the extended mesopause region. Assumptions and approximations for the trends in the Lyman-flux (needed for the water vapor dissociation rate), methane and the water vapor mixing ratio at the hygropause are necessary to accomplish this study. To approximate the solar Lyman-α flux back to the pre-industrial time, we derived a quadratic fit using the sunspot number record which extends back to 1749 and is the only solar proxy available for the Lyman-α flux prior to 1947. We assume that methane increases with a constant growth rate from the pre-industrial era to the present. An unsolved problem for the model calculations consists of how the water vapor mixing ratio at the hygropause should be specified during this period. We assume that the hygropause was dryer during pre-industrial times than the present. As a consequence of methane oxidation, the model simulation indicates that the middle atmosphere has become more humid as a result of the rising methane concentration, but with some dependence on height and with a small time delay of few years. The solar influence on the water vapor mixing ratio is insignificant below about 80 km in summer high latitudes, but becomes increasingly more important above this altitude. The enhanced water vapor concentration increasesthe hydrogen radical concentration and reduces the mesospheric ozone. A second region of stronger ozone decrease is located in the vicinity of the stratopause. Increases in CO2 concentration enhance slightly the concentration of CO in the mesosphere. However, its influence upon the chemistry is small and its main effect is connected with a cooling of the upper atmosphere. The long-term behavior of water vapor is discussed in particular with respect to its impact on the NLC region.

2009, Sonnemann, G.R., Hartogh, P.

Ozone measurements taken with a ground based microwave instrument at Lindau (51.66° N, 10.13° E) over some years showed strong ozone decrease events within the stratopause region, particularly during the winter half-year. These events are characterized by a marked drop of the ozone mixing ratio from two to three ppmv to less than half a ppmv in extreme cases. Simultaneous water vapor measurements at the same place, also carried out by a microwave instrument, showed a strong increase of its mixing ratio and the temperature was also enhanced during these episodes. The theoretical analysis brought evidence that these events result from a positive feedback in the complex radiatively-chemical system between the ozone column density and the ozone dissociation rate.

2015, Sonnemann, G.R., Hartogh, P., Berger, U., Grygalashvyly, M.

The layer of vibrationally excited hydroxyl (OH*) near the mesopause in Earth's atmosphere is widely used to derive the temperature at this height and to observe dynamical processes such as gravity waves. The concentration of OH* is controlled by the product of atomic hydrogen, with ozone creating a layer of enhanced concentration in the mesopause region. However, the basic influences on the OH* layer are atomic oxygen and temperature. The long-term monitoring of this layer provides information on a changing atmosphere. It is important to know which proportion of a trend results from anthropogenic impacts on the atmosphere and which proportion reflects natural variations. In a previous paper (Grygalashvyly et al., 2014), the trend of the height of the layer and the trend in temperature were investigated particularly in midlatitudes on the basis of our coupled dynamic and chemical transport model LIMA (Leibniz Institute Middle Atmosphere). In this paper we consider the trend for the number density between the years 1961 and 2009 and analyze the reason of the trends on a global scale. Further, we consider intra-annual variations. Temperature and wind have the strongest impacts on the trend. Surprisingly, the increase in greenhouse gases (GHGs) has no clear influence on the chemistry of OH*. The main reason for this lies in the fact that, in the production term of OH*, if atomic hydrogen increases due to increasing humidity of the middle atmosphere by methane oxidation, ozone decreases. The maximum of the OH* layer is found in the mesopause region and is very variable. The mesopause region is a very intricate domain marked by changeable dynamics and strong gradients of all chemically active minor constituents determining the OH* chemistry. The OH* concentration responds, in part, very sensitively to small changes in these parameters. The cause for this behavior is given by nonlinear reactions of the photochemical system being a nonlinear enforced chemical oscillator driven by the diurnal-periodic solar insolation. At the height of the OH* layer the system operates in the vicinity of chemical resonance. The solar cycle is mirrored in the data, but the long-term behavior due to the trend in the Lyman-α radiation is very small. The number density shows distinct hemispheric differences. The calculated OH* values show sometimes a step around a certain year. We introduce a method to find out the date of this step and discuss a possible reason for such behavior.

2004, von Zahn, U., Baumgarten, G., Berger, U., Fiedler, J., Hartogh, P.

The topic of this paper is the sensitivity of the brightness of noctilucent clouds (NLC) on the ambient water vapour mixing ratio f(H2O). Firstly, we use state-of-the-art models of NLC layer formation to predict NLC brightness changes in response to changes in the 80km mixing ratio f(H2O) for the two cases of ground-based 532nm lidar observations at 69° N and for hemispheric satellite SBUV observations at 252nm wavelength. In this study, we include a re-evaluation of the sensitivity of NLC brightness to changes in solar Lyman α flux. Secondly, we review observations of episodic changes in f(H2O) and those in NLC brightness, the former being available since 1992, the latter since 1979. To this review, we add a new series of observations of f(H2O), performed in the Arctic summer at the ALOMAR observatory. The episodic change exhibited by the Arctic summer means of f(H2O) turns out to be quite different from all those derived from annual means of f(H2O). The latter indicate that since 1996 a significant reduction of annually averaged upper mesospheric water vapour has occurred at low, mid, and high latitudes. These decreases of f(H2O) have been observed over the same time period in which a slow increase of SBUV NLC albedo has occurred. From this scenario and additional arguments we conclude that the cause for the observed long-term increase in NLC albedo remains to be identified. We close with comments on the very different character of decadal variations in NLC brightness and occurrence rate.