We offer a comprehensive approach to determine how physical confinement can affect the water formation reaction. By using free-standing crystalline SiO2 bilayer supported on Ru(0001) as a model system, we studied the water formation reaction under confinement in situ and in real time. Low-energy electron microscopy reveals that the reaction proceeds via the formation of reaction fronts propagating across the Ru(0001) surface. The Arrhenius analyses of the front velocity yield apparent activation energies (Eaapp) of 0.32 eV for the confined and 0.59 eV for the nonconfined reaction. DFT simulations indicate that the rate-determining step remains unchanged upon confinement, therefore ruling out the widely accepted transition state effect. Additionally, H2O accumulation cannot explain the change in Eaapp for the confined cases studied because its concentration remains low. Instead, numerical simulations of the proposed kinetic model suggest that the H2 adsorption process plays a decisive role in reproducing the Arrhenius plots.
Our understanding of how rapid Arctic warming and permafrost thaw affect global climate dynamics is restricted by limited spatiotemporal data coverage due to logistical challenges and the complex landscape of Arctic regions. It is therefore crucial to make best use of the available observations, including the integrated data analysis across disciplines and observational platforms. To alleviate the data compilation process for syntheses, cross-scale analyses, Earth system models, and remote sensing applications, we introduce the ARctic greenhouse Gas Observation metadata version 1 (ARGO), a new meta-dataset comprised of greenhouse gas observations from various observational platforms across the Arctic and boreal biomes within the polar region of the Northern Hemisphere. ARGO provides a centralised repository for metadata on carbon dioxide (CO2), methane (CH4), and nitrous oxide (N2O) measurements and is linked to an interactive online tool (https://www.bgc-jena.mpg.de/argo/, last access: 6 May 2025). This tool offers prompt metadata visualisation for the research community. Here, we present the structure and features of ARGO, underscoring its role as a valuable resource for advancing Arctic climate research and guiding synthesis efforts in the face of rapid environmental change in northern regions. The ARGO meta-dataset is openly available for download at Zenodo (https://doi.org/10.5281/zenodo.13870389; Vogt et al., 2024 a ).
14 September 2024 in Journal of Geophysical Research: Atmospheres
Arctic permafrost thaw holds the potential to drastically alter the Earth's surface in Northern high latitudes. We utilize high‐resolution large eddy simulations to investigate the impact of the changing surfaces onto the neutrally stratified atmospheric boundary layer (ABL). A stochastic surface model based on Gaussian Random Fields modeling typical permafrost landscapes is established in terms of two land cover classes: grass land and open water bodies, which exhibit different surface roughness length and surface sensible heat flux. A set of experiments is conducted where two parameters, the lake areal fraction and the surface correlation length, are varied to study the sensitivity of the boundary layer with respect to surface heterogeneity. Our key findings from the simulations are the following: The lake areal fraction has a substantial impact on the aggregated sensible heat flux at the blending height where surface heterogeneities become horizontally homogenized. The larger the lake areal fraction, the smaller the sensible heat flux. This result gives rise to a potential feedback mechanism. When the Arctic dries due to climate heating, the interaction with the ABL may accelerate permafrost thaw. Furthermore, the blending height shows significant dependency on the correlation length of the surface features. A longer surface correlation length causes an increased blending height. This finding is of relevance for land surface models concerned with Arctic permafrost as they usually do not consider a heterogeneity metric comparable to the surface correlation length.
Wentzel–Kramers–Brillouin theory was employed by Grimshaw (Geophys. Fluid Dyn., vol. 6, 1974, pp. 131–148) and Achatz et al. (J. Fluid Mech., vol. 210, 2010, pp. 120–147) to derive modulation equations for non-hydrostatic internal gravity wave packets in the atmosphere. This theory allows for wave packet envelopes with vertical extent comparable to the pressure scale height and for large wave amplitudes with wave-induced mean-flow speeds comparable to the local fluctuation velocities. Two classes of exact travelling wave solutions to these nonlinear modulation equations are derived here. The first class involves horizontally propagating wave packets superimposed over rather general background states. In a co-moving frame of reference, examples from this class have a structure akin to stationary mountain lee waves. Numerical simulations corroborate the existence of nearby travelling wave solutions under the pseudo-incompressible model and reveal better than expected convergence with respect to the asymptotic expansion parameter. Travelling wave solutions of the second class also feature a vertical component of their group velocity but exist under isothermal background stratification only. These waves include an interesting nonlinear wave–mean-flow interaction process: a horizontally periodic wave packet propagates vertically while draining energy from the mean wind aloft. In the process it decelerates the lower-level wind. It is shown that the modulation equations apply equally to hydrostatic waves in the limit of large horizontal wavelengths. Aside from these results of direct physical interest, the new nonlinear travelling wave solutions provide a firm basis for subsequent studies of nonlinear internal wave instability and for the design of subtle test cases for numerical flow solvers.
1 February 2019 in Mathematics of Climate and Weather Forecasting
We apply spectral stability theory to investigate nonlinear gravity waves in the atmosphere. These waves are determined by modulation equations that result from Wentzel-Kramers-Brillouin theory. First, we establish that plane waves, which represent exact solutions to the inviscid Boussinesq equations, are spectrally stable with respect to their nonlinear modulation equations under the same conditions as what is known as modulational stability from weakly nonlinear theory. In contrast to Boussinesq, the pseudo-incompressible regime does fully account for the altitudinal varying background density. Second,we show for the first time that upward-traveling non-plane wave fronts solving the inviscid nonlinear modulation equations, that compare to pseudo-incompressible theory, are unconditionally unstable. Both inviscid regimes turn out to be ill-posed as the spectra allow for arbitrarily large instability growth rates. Third, a regularization is found by including dissipative effects. The corresponding nonlinear traveling wave solutions have localized amplitude. As a consequence of the nonlinearity, envelope and linear group velocity, as given by the derivative of the frequency with respect to wavenumber, do not coincide anymore. These waves blow up unconditionally by embedded eigenvalue instabilities but the instability growth rate is bounded from above and can be computed analytically. Additionally, all three types of nonlinear modulation equations are solved numerically to further investigate and illustrate the nature of the analytic stability results.
The traditional approximation neglects the cosine components of the Coriolis acceleration, and this approximation has been widely used in the study of geophysical phenomena. However, the justification of the traditional approximation is questionable under a few circumstances. In particular, dynamics with substantial vertical velocities or geophysical phenomena in the tropics have non-negligible cosine Coriolis terms. Such cases warrant investigations with the non-traditional setting, i.e. the full Coriolis acceleration. In this manuscript, we study the effect of the non-traditional setting on an isothermal, hydrostatic and compressible atmosphere assuming a meridionally homogeneous flow. Employing linear stability analysis, we show that, given appropriate boundary conditions, i.e. a bottom boundary condition that allows for a vertical energy flux and non-reflecting boundary at the top, the atmosphere at rest becomes prone to a novel unstable mode. The validity of assuming a meridionally homogeneous flow is investigated via scale analysis. Numerical experiments were conducted, and Rayleigh damping was used as a numerical approximation for the non-reflecting top boundary. Our three main results are as follows: (i) experiments involving the full Coriolis terms exhibit an exponentially growing instability, yet experiments subjected to the traditional approximation remain stable; (ii) the experimental instability growth rate is close to the theoretical value; (iii) a perturbed version of the unstable mode arises even under sub-optimal bottom boundary conditions. Finally, we conclude our study by discussing the limitations, implications and remaining open questions. Specifically, the influence on numerical deep-atmosphere models and possible physical interpretations of the unstable mode are discussed.