US Participation in the GOME and SCIAMACHY Projects

The research performed during this reporting period includes development and maintenance of scientific software for the GOME retrieval algorithms, consultation on operational software development for GOME, further sensitivity and instrument studies to help finalize the definition of the SCIAMACHY instrument, and consultation on optical and detector issues for both GOME and SCIAMACHY. The Global Ozone Monitoring Experiment was successfully launched on the ERS-2 satellite on April 20, 1995, during this reporting period, and is working in the expected fashion. The European Space Agency has made their selections from responses to the Announcement of Opportunity for GOME validation and science studies, part of the overall ERS AO. The Smithsonian Astrophysical Observatory (SAO) proposal has been selected. These proposals are primarily for access to the data; ESA does not provide research funding for the selected investigations. The SAO activities that are carried out as a result of selection by ESA are funded by the present grant, to the limit that can be accomplished at the present level of funding. SCIAMACHY is currently in Phase C/D. Instrument design is almost finalized and selection of infrared detectors from the initial production run has been made

Mapping isoprene emissions over North America using formaldehyde column observations from space

We present a methodology for deriving emissions of volatile organic compounds (VOC) using space-based column observations of formaldehyde (HCHO) and apply it to data from the Global Ozone Monitoring Experiment (GOME) satellite instrument over North America during July 1996. The HCHO column is related to local VOC emissions, with a spatial smearing that increases with the VOC lifetime. Isoprene is the dominant HCHO precursor over North America in summer, and its lifetime (≃1 hour) is sufficiently short that the smearing can be neglected. We use the Goddard Earth Observing System global 3-D model of tropospheric chemistry (GEOS-CHEM) to derive the relationship between isoprene emissions and HCHO columns over North America and use these relationships to convert the GOME HCHO columns to isoprene emissions. We also use the GEOS-CHEM model as an intermediary to validate the GOME HCHO column measurements by comparison with in situ observations. The GEOS-CHEM model including the Global Emissions Inventory Activity (GEIA) isoprene emission inventory provides a good simulation of both the GOME data (r2 = 0.69, n = 756, bias = +11%) and the in situ summertime HCHO measurements over North America (r2 = 0.47, n = 10, bias = −3%). The GOME observations show high values over regions of known high isoprene emissions and a day-to-day variability that is consistent with the temperature dependence of isoprene emission. Isoprene emissions inferred from the GOME data are 20% less than GEIA on average over North America and twice those from the U.S. EPA Biogenic Emissions Inventory System (BEIS2) inventory. The GOME isoprene inventory when implemented in the GEOS-CHEM model provides a better simulation of the HCHO in situ measurements than either GEIA or BEIS2 (r2 = 0.71, n = 10, bias = −10%)

Tunable far infrared studies of molecular parameters in support of stratospheric measurements

Lab studies were made in support of far infrared spectroscopy of the stratosphere using the Tunable Far InfraRed (TuFIR) method of ultrahigh resolution spectroscopy and, more recently, spectroscopic and retrieval calculations performed in support of satellite-based atmospheric measurement programs: the Global Ozone Monitoring Experiment (GOME), and the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY)

FACE TO FACE AGAIN - REPORT FROM THE DOCTORAL SYMPOSIUM IN ENGINEERING EDUCATION RESEARCH AT SEFI 2022

The 6th Doctoral Symposium at SEFI 2022 attracted 20 doctoral students and 17 senior researchers. After two years as an online event during the pandemic, it was organised as a fully in-person event. In preparation, the doctoral students wrote extended abstracts to introduce themselves and their PhD projects, while the seniorsprovided reading recommendations and advice. The intense, full-day program was based on group discussions and interactive plenary sessions. The Doctoral Symposium was concluded by a session in which each participant presented their take-home message. This paper outlines how the Doctoral Symposium was organised and summarizes some of the documentation

New retrieval of BrO from SCIAMACHY limb: an estimate of the stratospheric bromine loading during April 2008

We present a new retrieval of stratospheric BrO (bromine monoxide) from channel 2 SCIAMACHY (SCanning Imaging Absorption spectrometer for Atmospheric CHartographY) limb observations. Retrievals are shown to agree with independent balloon observations to within one standard deviation of the retrieval noise. We retrieve BrO profiles for all of April 2008, and apply simulated [BrO]/[Br_y] (bromine monoxide : stratospheric inorganic bromine) ratios to estimate the stratospheric Br_y loading. We find 23.5 ± 6 ppt Br, suggesting 7 ppt Br from short-lived bromocarbons to be at the high end of the current best estimate (3–8 ppt). The 6 ppt Br uncertainty estimate is dominated by the 21% uncertainty in the simulated [BrO] / [Br_y] ratio due to propagation of errors from the underlying chemical kinetics

US Participation in the GOME and SCIAMACHY Projects

This report summarizes research done under NASA Grant NAGW-2541 through September 30, 1997. The research performed under this grant includes development and maintenance of scientific software for the GOME retrieval algorithms, consultation on operational software development for GOME, sensitivity and instrument studies to define GOME and SCIAMACHY instruments, consultation on optical and detector issues for both GOME and SCIAMACHY, consultation and development for SCIAMACHY near-real-time (NRT) and off-line (OL) data products, and development of infrared line-by-line atmospheric modeling and retrieval capability for SCIAMACHY. The European Space Agency selected the SAO to participate in GOME validation and science studies, part of the overall ERS AO. This provided access to all GOME data; The SAO activities that are carried out as a result of selection by ESA were funded by the present grant. The Global Ozone Monitoring Experiment was successfully launched on the ERS- 2 satellite on April 20, 1995, and remains working in normal fashion. SCIAMACHY is currently scheduled for launch in early 2000. The first two European ozone monitoring instruments (OMI), to fly on the q series of operational meteorological satellites being planned by Eumetsat, have been selected to be GOME-type instruments (the first, in fact, will be the refurbished GOME flight spare). K. Chance is the U.S. member of the OMI Users Advisory Group

Improvement of OMI Ozone Profile Retrievals in the Troposphere and Lower Troposphere by the Use of the Tropopause-Based Ozone Profile Climatology

An advance algorithm based on the optimal estimation technique has beeen developed to derive ozone profile from GOME UV radiances and have adapted it to OMI UV radiances. OMI vertical resolution : 7-11 km in the troposphere and 10-14 km in the stratosphere. Satellite ultraviolet measurements (GOME, OMI) contain little vertical information for the small scale of ozone, especially in the upper troposphere (UT) and lower stratosphere (LS) where the sharp O3 gradient across the tropopause and large ozone variability are observed. Therefore, retrievals depend greatly on the a-priori knowledge in the UTL

Measuring the quantum efficiency of single radiating dipoles using a scanning mirror

Using scanning probe techniques, we show the controlled manipulation of the radiation from single dipoles. In one experiment we study the modification of the fluorescence lifetime of a single molecular dipole in front of a movable silver mirror. A second experiment demonstrates the changing plasmon spectrum of a gold nanoparticle in front of a dielectric mirror. Comparison of our data with theoretical models allows determination of the quantum efficiency of each radiating dipole.Comment: 4 pages, 4 figure

Global satellite analysis of the relation between aerosols and short-lived trace gases

The spatial and temporal correlations between concurrent satellite observations of aerosol optical thickness (AOT) from the Moderate Resolution Imaging Spectroradiometer (MODIS) and tropospheric columns of nitrogen dioxide (NO<sub>2</sub>), sulfur dioxide (SO<sub>2</sub>), and formaldehyde (HCHO) from the Ozone Monitoring Instrument (OMI) are used to infer information on the global composition of aerosol particles. When averaging the satellite data over large regions and longer time periods, we find significant correlation between MODIS AOT and OMI trace gas columns for various regions in the world. This shows that these enhanced aerosol and trace gas concentrations originate from common sources, such as fossil fuel combustion, biomass burning, and organic compounds released from the biosphere. This leads us to propose that satellite-inferred AOT to NO<sub>2</sub> ratios for regions with comparable photochemical regimes can be used as indicators for the relative regional pollution control of combustion processes. Indeed, satellites observe low AOT to NO<sub>2</sub> ratios over the eastern United States and western Europe, and high AOT to NO<sub>2</sub> ratios over comparably industrialized regions in eastern Europe and China. Emission databases and OMI SO<sub>2</sub> observations over these regions suggest a much stronger sulfur contribution to aerosol formation than over the well-regulated areas of the eastern United States and western Europe. Furthermore, satellite observations show AOT to NO<sub>2</sub> ratios are a factor 100 higher over biomass burning regions than over industrialized areas, reflecting the unregulated burning practices with strong primary particle emissions in the tropics compared to the heavily controlled combustion processes in the industrialized Northern Hemisphere. Simulations with a global chemistry transport model (GEOS-Chem) capture most of these variations, although on regional scales significant differences are found. Wintertime aerosol concentrations show strongest correlations with NO<sub>2</sub> throughout most of the Northern Hemisphere. During summertime, AOT is often (also) correlated with enhanced HCHO concentrations, reflecting the importance of secondary organic aerosol formation in that season. We also find significant correlations between AOT and HCHO over biomass burning regions, the tropics in general, and over industrialized regions in southeastern Asia. The distinct summertime maximum in AOT (0.4 at 550 nm) and HCHO over the southeastern United States strengthens existing hypotheses that local emissions of volatile organic compounds lead to the formation of secondary organic aerosols there. GEOS-Chem underestimates the AOT over the southeastern United States by a factor of 2, most likely due to too strong precipitation and too low SOA yield in the model

Photonic mode density effects on single-molecule fluorescence blinking

We investigated the influence of the photonic mode density (PMD) on the triplet dynamics of individual chromophores on a dielectric interface by comparing their response in the presence and absence of a nearby gold film. Lifetimes of the excited singlet state were evaluated in ordet to measure directly the PMD at the molecules position. Triplet state lifetimes were simultaneously determined by statistical analysis of the detection time of the fluorescence photons. The observed singlet decay rates are in agreement with the predicted PMD for molecules with different orientations. The triplet decay rate is modified in a fashion correlated to the singlet decay rate. These results show that PMD engineering can lead to an important suppression of the fluorescence, introducing a novel aspect of the physical mechanism to enhance fluorescence intensity in PMD-enhancing systems such as plasmonic devices