Water vapour line assignments in the 9250-26 000 cm (-1) frequency range

Line parameters for water vapour in natural abundance have recently been determined for the 9250-13 000 cm(-1) region [M.-F. Wrienne, A. Jenouvrier, C. Hermans, A.C. Vandaele, M. Carleer, C. Clerbaux, P.-F. Coheur, R. Colin, S. Fally, M. Bach, J. Quant. Spectrosc. Radiat. Transfer 82 (2003) 99] and the 13 000-26 000 cm(-1) region [P.-F. Coheur, S. Fally, M. Carleer, C. Clerbaux, R. Colin, A. Jenouvrier, M.-F. Wrienne, C. Hermans, A.C. Vandaele, J. Quant. Spectrosc. Radial. Transfer 74 (2002) 493] using a high-resolution Fourier-transform spectrometer with a long-path absorption cell. These spectra are analysed using several techniques including variational line lists and assignments made. In total, over 15 000 lines were assigned to transitions involving more than 150 exited vibrational states of (H2O)-O-16. Twelve new vibrational band origins are determined and estimates for a further 16 are presented. (c) 2005 Elsevier Inc. All rights reserved

Decoherence of matter waves by thermal emission of radiation

Emergent quantum technologies have led to increasing interest in decoherence - the processes that limit the appearance of quantum effects and turn them into classical phenomena. One important cause of decoherence is the interaction of a quantum system with its environment, which 'entangles' the two and distributes the quantum coherence over so many degrees of freedom as to render it unobservable. Decoherence theory has been complemented by experiments using matter waves coupled to external photons or molecules, and by investigations using coherent photon states, trapped ions and electron interferometers. Large molecules are particularly suitable for the investigation of the quantum-classical transition because they can store much energy in numerous internal degrees of freedom; the internal energy can be converted into thermal radiation and thus induce decoherence. Here we report matter wave interferometer experiments in which C70 molecules lose their quantum behaviour by thermal emission of radiation. We find good quantitative agreement between our experimental observations and microscopic decoherence theory. Decoherence by emission of thermal radiation is a general mechanism that should be relevant to all macroscopic bodies.Comment: 5 pages, 4 figure

First space-based derivation of the global atmospheric methanol emission fluxes

This study provides improved methanol emission estimates on the global scale, in particular for the largest methanol source, the terrestrial biosphere, and for biomass burning. To this purpose, one complete year of spaceborne measurements of tropospheric methanol columns retrieved for the first time by the thermal infrared sensor IASI aboard the MetOp satellite are compared with distributions calculated by the IMAGESv2 global chemistry-transport model. Two model simulations are performed using a priori biogenic methanol emissions either from the new MEGANv2.1 emission model, which is fully described in this work and is based on net ecosystem flux measurements, or from a previous parameterization based on net primary production by Jacob et al. (2005). A significantly better model performance in terms of both amplitude and seasonality is achieved through the use of MEGANv2.1 in most world regions, with respect to IASI data, and to surface- and air-based methanol measurements, even though important discrepancies over several regions are still present. As a second step of this study, we combine the MEGANv2.1 and the IASI column abundances over continents in an inverse modelling scheme based on the adjoint of the IMAGESv2 model to generate an improved global methanol emission source. The global optimized source totals 187 Tg yr−1 with a contribution of 100 Tg yr−1 from plants, only slightly lower than the a priori MEGANv2.1 value of 105 Tg yr−1. Large decreases with respect to the MEGANv2.1 biogenic source are inferred over Amazonia (up to 55 %) and Indonesia (up to 58 %), whereas more moderate reductions are recorded in the Eastern US (20-25 %) and Central Africa (25-35 %). On the other hand, the biogenic source is found to strongly increase in the arid and semi-arid regions of Central Asia (up to a factor of 5) and Western US (factor of 2), probably due to a source of methanol specific to these ecosystems which is unaccounted for in the MEGANv2.1 inventory. The most significant error reductions achieved by the optimization concern the derived biogenic emissions over the Amazon and over the Former Soviet Union. The robustness of the derived fluxes to changes in convective updraft fluxes, in methanol removal processes, and in the choice of the biogenic a priori inventory is assessed through sensitivity inversions. Detailed comparisons of the model with a number of aircraft and surface observations of methanol, as well as new methanol measurements in Europe and in the Reunion Island show that the satellite-derived methanol emissions improve significantly the agreement with the independent data, giving thus credence to the IASI dataset. © 2011 Author(s)

Atmospheric impacts of COVID-19 on NOx and VOC levels over China based on TROPOMI and IASI satellite data and modeling

202307 bcchVersion of RecordRGCOthersBIRA-IASB; BRAIN-be; Belgian Research Action; Copernicus Atmosphere Monitoring Service; ESA-BELSPO; ESRIN; German Aerospace Centre; IASI; ICOVAC, (2020-2021); TROVA-E2, (2019-2023); National Science Foundation; National Center for Atmospheric Research; European Commission; European Space Agency; Fonds De La Recherche Scientifique; Belgian Federal Science Policy Office, BELSPO, (2019-2021); Centre National d’Etudes Spatiales; Deutsches Zentrum für Luft- und RaumfahrtPublishe

Using Thermal Infrared Absorption and Emission to Determine Trace Gases

International audienceThe light emerging from the top of the atmosphere in the greater part of the infrared region is thermal radiation from the Earth's surface. The resultant spectra obtained depend on the temperature difference between the emitting feature and absorbing gas. In this region the greenhouse gases, carbon dioxide, CO2, methane, CH4, ozone, O3, and water, H2O, are observed as well as carbon monoxide, CO, a product indicative of fossil fuel combustion, methanol, CH3OH, from biomass burning, and ammonia, NH3, from agriclulture. Chapter 3 describes the techniques for retrieving atmospheric abundances of these and other species from a number of satellite instruments, and concludes with suggestions for future developments

Application of renormalized coupled-cluster methods to potential function of water

Abstract The goal of this paper is to examine the performance of the conventional and renormalized single-reference coupled-cluster (CC) methods in calculations of the potential energy surface of the water molecule. A comparison with the results of the internally contracted multi-reference configuration interaction calculations including the quasi-degenerate Davidson correction (MRCI(Q)) and the spectroscopically accurate potential energy surface of water resulting from the use of the energy switching (ES) approach indicates that the relatively inexpensive completely renormalized (CR) CC methods with singles (S), doubles (D), and a non-iterative treatment of triples (T) or triples and quadruples (TQ), such as CR-CCSD(T), CR-CCSD(TQ), and the recently developed rigorously size extensive extension of CR-CCSD(T), termed CR-CC(2,3), provide substantial improvements in the results of conventional CCSD(T) and CCSD(TQ) calculations at larger internuclear separations. It is shown that the CR-CC(2,3) results corrected for the effect of quadruply excited clusters through the CR-CC(2,3)+Q approach can compete with the highly accurate MRCI(Q) data. The excellent agreement between the CR-CC(2,3)+Q and MRCI(Q) results suggests ways of improving the global potential energy surface of water resulting from the use of the ES approach in the regions of intermediate bond stretches and intermediate energies connecting the region of the global minimum with the asymptotic regions