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The Earth's mesopause region between about 75 and 105 km is characterised by chemiluminescent emission from various lines of different molecules and atoms. This emission was and is important for the study of the chemistry and dynamics in this altitude region at nighttime. However, our understanding is still very limited with respect to molecular emissions with low intensities and high line densities that are challenging to resolve. Based on 10 years of data from the astronomical X-shooter echelle spectrograph at Cerro Paranal in Chile, we have characterised in detail this nightglow (pseudo-)continuum in the wavelength range from 300 to 1800 nm. We studied the spectral features, derived continuum components with similar variability, calculated climatologies, studied the response to solar activity, and even estimated the effective emission heights. The results indicate that the nightglow continuum at Cerro Paranal essentially consists of only two components, which exhibit very different properties. The main structures of these components peak at 595 and 1510 nm. While the former was previously identified as the main peak of the FeO "orange arc" bands, the latter is a new discovery. Laboratory data and theory indicate that this feature and other structures between about 800 and at least 1800 nm are caused by emission from the low-lying A′′ and A′ states of HO2. In order to test this assumption, we performed runs with the Whole Atmosphere Community Climate Model (WACCM) with modified chemistry and found that the total intensity, layer profile, and variability indeed support this interpretation, where the excited HO2 radicals are mostly produced from the termolecular recombination of H and O2. The WACCM results for the continuum component that dominates at visual wavelengths show good agreement for FeO from the reaction of Fe and O3. However, the simulated total emission appears to be too low, which would require additional mechanisms where the variability is dominated by O3. A possible (but nevertheless insufficient) process could be the production of excited OFeOH by the reaction of FeOH and O3. [ABSTRACT FROM AUTHOR]

This article begins with a review of important advances in the chemistry and related physics of the mesosphere and lower thermosphere (MLT) region of the atmosphere that have occurred over the past 2 decades, since the founding of Atmospheric Chemistry and Physics. The emphasis here is on chemistry, but we also discuss recent findings on atmospheric dynamics and forcings to the extent that these are important for understanding MLT composition and chemistry. Topics that are covered include observations, with satellite, rocket and ground-based techniques; the variability and connectedness of the MLT on various length scales and timescales; airglow emissions; the cosmic dust input and meteoric metal layers; and noctilucent/polar mesospheric ice clouds. The paper then concludes with a discussion of important unanswered questions and likely future directions for the field over the next decade. [ABSTRACT FROM AUTHOR]

The Earth's mesopause region between about 75 and 105 km is characterised by chemiluminescent emission from various lines of different molecules and atoms. This emission was and is important for the study of the chemistry and dynamics in this altitude region at nighttime. However, our understanding is still very limited with respect to molecular emissions with low intensities and high line densities that are challenging to resolve. Based on 10 years of data from the astronomical X-shooter echelle spectrograph at Cerro Paranal in Chile, we have characterised in detail this nightglow (pseudo-)continuum in the wavelength range from 300 to 1,800 nm. We studied the spectral features, derived continuum components with similar variability, calculated climatologies, studied the response to solar activity, and even estimated the effective emission heights. The results indicate that the nightglow continuum at Cerro Paranal essentially consists of only two components, which exhibit very different properties. The main structures of these components peak at 595 and 1,510 nm. While the former was previously identified as the main peak of the FeO 'orange arc' bands, the latter is a new discovery. Laboratory data and theory indicate that this feature and other structures between about 800 and at least 1,800 nm are caused by emission from the low-lying A'' and A' states of HO2. In order to test this assumption, we performed runs with the Whole Atmosphere Community Climate Model (WACCM) with modified chemistry and found that the total intensity, layer profile, and variability indeed support this interpretation, where the excited molecules HO2 are mostly produced from the termolecular recombination of H and O2. The WACCM results for the continuum component that dominates at visual wavelengths show good agreement for FeO from the reaction of Fe and O3. However, the simulated total emission appears to be too low, which would require additional mechanisms where the variability is dominated by O3. [ABSTRACT FROM AUTHOR]

This Opinion article begins with a review of important advances in the science of the Mesosphere and Lower Thermosphere (MLT) region of the atmosphere that have occurred over the past two decades since the founding of Atmospheric Chemistry and Physics. The emphasis is on chemistry (although, of course, this cannot be decoupled from discussion of atmospheric physics and dynamics), and the primary focus is on work during the past 10 years. Topics that are covered include: observations (satellite, rocket and ground-based techniques); the variability and connectedness of the MLT on various length- and time-scales; airglow emissions; the cosmic dust input and meteoric metal layers; and noctilucent (or polar mesospheric) ice clouds. The paper then concludes with a discussion of important unanswered questions and likely future directions for the field over the next decade. [ABSTRACT FROM AUTHOR]

Emissions from the OH Meinel bands are routinely used to determine rotational temperatures that are considered proxies for the kinetic temperature near the mesopause region. Previous observations determined OH rotational temperatures that show a dependence on the vibrational level, with the temperature rising overall as the OH vibrational quantum number v increases. The source of this trend is not well understood and has generally been attributed to deviations from thermodynamic equilibrium. This technical note demonstrates that the existence of bimodal OH rotational population distributions is an inherent feature of rotational relaxation in gases and can provide an explanation for the previously reported temperature trend. The use of only a few lines from rotational transitions involving low rotational quantum numbers to determine rotational temperatures does not account for the bimodality of the OH rotational population distributions and leads to systematic errors overestimating the OH rotational temperature. This note presents selected examples, discusses the relevant implications, and considers strategies that could lead to more reliable OH rotational temperature determination. [ABSTRACT FROM AUTHOR]

Emission from the OH Meinel bands is routinely used to determine rotational temperatures that are considered proxies for the kinetic temperature near the mesopause region. Previous observations determined OH rotational temperatures that show a dependence on the vibrational level, with the temperature rising overall as the OH vibrational quantum number v increases. The source of this trend is not well understood and has generally been attributed to deviations from thermodynamic equilibrium. This Technical Note demonstrates that the existence of bimodal OH rotational population distributions is an inherent feature of rotational relaxation in gases and can provide an explanation for the previously reported temperature trend. The use of only a few lines from rotational transitions involving low rotational quantum numbers to determine rotational temperatures does not account for the bimodality of the OH rotational population distributions and leads to systematic errors overestimating the OH rotational temperature. This Note presents selected examples, discusses the relevant implications, and considers strategies that could lead to more reliable OH rotational temperature determination. [ABSTRACT FROM AUTHOR]

The question of whether mesospheric OH(v) rotational population distributions are in equilibrium with the local kinetic temperature has been debated over several decades. Despite several indications for the existence of non-equilibrium effects, the general consensus has been that emissions originating from low rotational levels are thermalized. Sky spectra simultaneously observing several vibrational levels demonstrated reproducible trends in the extracted OH(v) rotational temperatures as a function of vibrational excitation. Laboratory experiments provided information on rotational energy transfer and direct evidence for fast multi-quantum OH(high-v) vibrational relaxation by O atoms. We examine the relationship of the new relaxation pathways with the behavior exhibited by OH(v) rotational population distributions. Rapid OH(high-v) + O multi-quantum vibrational relaxation connects high and low vibrational levels and enhances the hot tail of the OH(low-v) rotational distributions. The effective rotational temperatures of mesospheric OH(v) are found to deviate from local thermodynamic equilibrium for all observed vibrational levels. Dedicated to Tom G. Slanger in celebration of his 5 decades of research in aeronomy. [ABSTRACT FROM AUTHOR]

In the 1970s, the mechanism of vibrational energy transfer from chemically produced OH(ν) in the nighttime mesosphere to the CO2(ν3) vibration, OH(ν)⇒N2(ν)⇒ CO2(ν3), was proposed. In later studies it was shown that this "direct" mechanism for simulated nighttime 4.3 μm emissions of the mesosphere is not sufficient to explain space observations. In order to better simulate these observations, an additional enhancement is needed that would be equivalent to the production of 2.8-3N2(1) molecules instead of one N2(1) molecule in each quenching reaction of OH(ν)+N2(0). Recently a new "indirect" channel of the OH(ν) energy transfer to N2(ν) vibrations, OH(ν)⇒O(1D)⇒N2(ν), was suggested and then confirmed in a laboratory experiment, where its rate for OH(ν = 9)+O(3P) was measured. We studied in detail the impact of the "direct" and "indirect" mechanisms on CO2(ν3) and OH(ν) vibrational level populations and emissions. We also compared our calculations with (a) the SABER/TIMED nighttime 4.3 μm CO2 and OH 1.6 and 2.0 μm limb radiances of the mesosphere-lower thermosphere (MLT) and (b) with ground- and space-based observations of OH(ν) densities in the nighttime mesosphere. We found that the new "indirect" channel provides a strong enhancement of the 4.3 μm CO2 emission, which is comparable to that obtained with the "direct" mechanism alone but assuming an efficiency that is 3 times higher. The model based on the "indirect" channel also produces OH(ν) density distributions which are in good agreement with both SABER limb OH emission observations and ground and space measurements. This is, however, not true for the model which relies on the "direct" mechanism alone. This discrepancy is caused by the lack of an efficient redistribution of the OH(ν) energy from higher vibrational levels emitting at 2.0 μm to lower levels emitting at 1.6 μm. In contrast, the new "indirect" mechanism efficiently removes at least five quanta in each OH(ν ⩾ 5)+O(3P) collision and provides the OH(ν) distributions which agree with both SABER limb OH emission observations and ground- and space-based OH(ν) density measurements. This analysis suggests that the important mechanism of the OH(ν) vibrational energy relaxation in the nighttime MLT, which was missing in the emission models of this atmospheric layer, has been finally identified. [ABSTRACT FROM AUTHOR]

Since 2002, SABER (Sounding of the Atmosphere using Broadband Emission Radiometry)/TIMED (Thermosphere, Ionosphere, Mesosphere, Energetics and Dynamics) has been continuously measuring the day- and nighttime infrared limb radiances of the mesosphere and lower thermoshere (MLT) in ten broadband channels. Recently, the MLT daytime temperature/pressure and CO2 densities have been obtained self-consistently from SABER 15 μm and 4.3 μm emission observations. However, similar nighttime data remain unprocessed due to a lack of understanding of the 4.3 μm emission generating mechanisms. A previous study suggested the "direct" transfer OH(v)) ↑ N2(v)) ↑ CO2(v3)) ↑ 4.3 μm of vibrational excitation from OH(v) to CO2 in the nighttime mesosphere. However, accounting for this excitation mechanism alone leads to significant under-prediction (by up to 80 %) of observed 4.3 μm limb radiances. Recently, theoretical and laboratory studies have suggested an additional "indirect" nighttime channel OH(v)) ↑ O(¹D)) ↑ N2(v)) ↑ CO2(v3)) ↑ 4.3 μm of this energy transfer. We implemented this new channel in our non-LTE (non-Local Thermodynamic Equilibrium) model and show that, for various latitudinal and seasonal scenarios, including this additional channel brings differences between simulated and measured nighttime SABER 4.3 μm limb radiances to (-20, +30) %. These results confirm the important role of the new mechanism as a source of the nighttime 4.3 μm emission. This finding creates new opportunities for the application of CO2 4.3 μm observations in the study of the energetics and dynamics of the nighttime MLT. [ABSTRACT FROM AUTHOR]

Emission from the OH Meinel bands is routinely used to determine rotational temperatures that are considered proxies for the kinetic temperature near the mesopause region. Previous observations determined OH rotational temperatures that show a dependence on the vibrational level, with the temperature rising overall as the OH vibrational quantum number v increases. The source of this trend is not well understood and has generally been attributed to deviations from thermodynamic equilibrium.This report shows the existence of bimodal OH rotational population distributions is an inherent feature of rotational relaxation in gases and can provide an explanation for the previously reported temperature trend. The use of only a few lines from rotational transitions involving low rotational quantum numbers to determine rotational temperatures does not account for the bimodality of the OH rotational population distributions and leads to systematic errors overestimating the OH rotational temperature. We will report selected examples, discuss the relevant implications, and consider strategies that could lead to more reliable OH rotational temperature determination [1].[1] K. S. Kalogerakis, Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-1047 (2018). [ABSTRACT FROM AUTHOR]