Brian J. Drouin

Validation of the Aura Microwave Limb Sounder middle atmosphere water vapor and nitrous oxide measurements

[1] The quality of the version 2.2 (v2.2) middle atmosphere water vapor and nitrous oxide measurements from the Microwave Limb Sounder (MLS) on the Earth Observing System (EOS) Aura satellite is assessed. The impacts of the various sources of systematic error are estimated by a comprehensive set of retrieval simulations. Comparisons with correlative data sets from ground-based, balloon and satellite platforms operating in the UV/visible, infrared and microwave regions of the spectrum are performed. Precision estimates are also validated, and recommendations are given on the data usage. The v2.2 H2O data have been improved over v1.5 by providing higher vertical resolution in the lower stratosphere and better precision above the stratopause. The single-profile precision is � 0.2–0.3 ppmv (4–9%), and the vertical resolution is � 3–4 km in the stratosphere. The precision and vertical resolution become worse with increasing height above the stratopause. Over the pressure range 0.1–0.01 hPa the precision degrades from 0.4 to 1.1 ppmv (6–34%), and the vertical resolution degrades to � 12–16 km. The accuracy is estimated to be 0.2–0.5 ppmv (4–11%) for the pressure range 68–0.01 hPa. The scientifically useful range of the H2O data is from 316 to 0.002 hPa, although only the 82–0.002 hPa pressure range is validated here. Substantial improvement has been achieved in the v2.2 N2O data over v1.5 by reducing a significant low bias in the stratosphere and eliminating unrealistically high biased mixing ratios in the polar regions. The single-profile precision is � 13–25 ppbv (7–38%), the vertical resolution is � 4–6 km and the accuracy is estimated to be 3–70 ppbv (9–25%) for the pressure range 100–4.6 hPa. The scientifically useful range of the N2O data is from 100 to 1 hPa.

Validation of Aura Microwave Limb Sounder stratospheric ozone measurements

[1] The Earth Observing System (EOS) Microwave Limb Sounder (MLS) aboard the Aura satellite has provided essentially daily global measurements of ozone (O3) profiles from the upper troposphere to the upper mesosphere since August of 2004. This paper focuses on validation of the MLS stratospheric standard ozone product and its uncertainties, as obtained from the 240 GHz radiometer measurements, with a few results concerning mesospheric ozone. We compare average differences and scatter from matched MLS version 2.2 profiles and coincident ozone profiles from other satellite instruments, as well as from aircraft lidar measurements taken during Aura Validation Experiment (AVE) campaigns. Ozone comparisons are also made between MLS and balloon-borne remote and in situ sensors. We provide a detailed characterization of random and systematic uncertainties for MLS ozone. We typically find better agreement in the comparisons using MLS version 2.2 ozone than the version 1.5 data. The agreement and the MLS uncertainty estimates in the stratosphere are often of the order of 5%, with values closer to 10% (and occasionally 20%) at the lowest stratospheric altitudes, where small positive MLS biases can be found. There is very good agreement in the latitudinal distributions obtained from MLS and from coincident profiles from other satellite instruments, as well as from aircraft lidar data along the MLS track.

Application of cascaded frequency multiplication to molecular spectroscopy

Laboratory molecular spectroscopy provides the basis for interpretation of atmospheric, planetary, and astrophysical data gathered by remote sensing. Laboratory studies of atomic and molecular signatures across the electromagnetic spectrum provide high-precision, quantitative data used to interpret the observed environment from remote measurements. Historically, the region of the spectrum above 500 GHz has been relatively unexplored due to atmospheric absorption and technical difficulties generating and detecting radiation. Laboratory spectroscopy at these frequencies has traditionally involved measurement of one or two absorption features and relied on fitting of models to the limited data. We report a new spectrometer built around a computer-controlled commercial synthesizer and millimeter-wave module driving a series of amplifiers followed by a series of wide-bandwidth frequency doublers and triplers. The spectrometer provides the ability to rapidly measure large pieces of frequency space with higher resolution, accuracy, and sensitivity than with Fourier transform infrared techniques. The approach is simple, modular, and requires no custom-built electronics or high voltage and facilitates the use of infrared data analysis techniques on complex submillimeter spectra.

Validation of the Aura Microwave Limb Sounder ClO measurements

We assess the quality of the version 2.2 (v2.2) ClO measurements from the Microwave Limb Sounder (MLS) on the Earth Observing System Aura satellite. The MLS v2.2 ClO data are scientifically useful over the range 100 to 1 hPa, with a single- profile precision of similar to 0.1 ppbv throughout most of the vertical domain. Vertical resolution is similar to 3-4 km. Comparisons with climatology and correlative measurements from a variety of different platforms indicate that both the amplitude and the altitude of the peak in the ClO profile in the upper stratosphere are well determined by MLS. The latitudinal and seasonal variations in the ClO distribution in the lower stratosphere are also well determined, but a substantial negative bias is present in both daytime and nighttime mixing ratios at retrieval levels below (i. e., pressures larger than) 22 hPa. Outside of the winter polar vortices, this negative bias can be eliminated by subtracting gridded or zonal mean nighttime values from the individual daytime measurements. In studies for which knowledge of lower stratospheric ClO mixing ratios inside the winter polar vortices to better than a few tenths of a ppbv is needed, however, day - night differences are not recommended and the negative bias must be corrected for by subtracting the estimated value of the bias from the individual measurements at each affected retrieval level.

Validation of Aura Microwave Limb Sounder Ozone by ozonesonde and lidar measurements

We present validation studies of MLS version 2.2 upper tropospheric and stratospheric ozone profiles using ozonesonde and lidar data as well as climatological data. Ozone measurements from over 60 ozonesonde stations worldwide and three lidar stations are compared with coincident MLS data. The MLS ozone stratospheric data between 150 and 3 hPa agree well with ozonesonde measurements, within 8% for the global average. MLS values at 215 hPa are biased high compared to ozonesondes by A`20% at middle to high latitude, although there is a lot of variability in this altitude region. Comparisons between MLS and ground-based lidar measurements from Mauna Loa, Hawaii, from the Table Mountain Facility, California, and from the Observatoire de Haute-Provence, France, give very good agreement, within A`5%, for the stratospheric values. The comparisons between MLS and the Table Mountain Facility tropospheric ozone lidar show that MLS data are biased high by A`30% at 215 hPa, consistent with that indicated by the ozonesonde data. We obtain better global average agreement between MLS and ozonesonde partial column values down to 215 hPa, although the average MLS values at low to middle latitudes are higher than the ozonesonde values by up to a few percent. MLS v2.2 ozone data agree better than the MLS v1.5 data with ozonesonde and lidar measurements. MLS tropical data show the wave one longitudinal pattern in the upper troposphere, with similarities to the average distribution from ozonesondes. High upper tropospheric ozone values are also observed by MLS in the tropical Pacific from June to November.

Demonstration of a room temperature 2.48–2.75 THz coherent spectroscopy source

We report the first demonstration of a continuous wave coherent source covering 2.48-2.75 THz, with greater than 10% instantaneous tuning bandwidth and having 1-14 μW of output power at room temperature. This source is based on a 91.8-101.8 GHz synthesizer followed by a power amplifier and three cascaded frequency triplers. It demonstrates for the first time that purely electronic solid-state sources can generate a useful amount of power in a region of the electromagnetic spectrum where lasers (solid state or gas) were previously the only available coherent sources. The bandwidth, agility, and operability of this THz source have enabled wideband, high resolution spectroscopic measurements of water, methanol, and carbon monoxide with a resolution and signal-to-noise ratio unmatched by any other existing system, providing new insight in the physics of these molecules. Furthermore, the power and optical beam quality are high enough to observe the Lamb-dip effect in water. The source frequency has an absolute accuracy better than 1 part in 10(12) and the spectrometer achieves sub-Doppler frequency resolution better than 1 part in 10(8). The harmonic purity is better than 25 dB. This source can serve as a coherent signal for absorption spectroscopy, a local oscillator for a variety of heterodyne systems and can be used as a method for precision control of more powerful but much less frequency agile quantum mechanical terahertz sources.

The Virtual Atomic and Molecular Data Centre (VAMDC) Consortium

The Virtual Atomic and Molecular Data Centre (VAMDC) Consortium is a worldwide consortium which federates atomic and molecular databases through an e-science infrastructure and an organisation to support this activity. About 90% of the inter-connected databases handle data that are used for the interpretation of astronomical spectra and for modelling in many fields of astrophysics. Recently the VAMDC Consortium has connected databases from the radiation damage and the plasma communities, as well as promoting the publication of data from Indian institutes. This paper describes how the VAMDC Consortium is organised for the optimal distribution of atomic and molecular data for scientific research. It is noted that the VAMDC Consortium strongly advocates that authors of research papers using data cite the original experimental and theoretical papers as well as the relevant databases.

Acetone: Laboratory Assignments and Predictions through 620 GHZ for the Vibrational-Torsional Ground State

The acetone molecule has a complex rotational spectrum arising from the internal rotation of two methyl tops and their interaction with each other and the rigid-body rotation of the molecule. Here we report the measurement and assignment of a large number of new rotational-torsional transitions of acetone in the vibrational-torsional ground state at frequencies of up to 620 GHz. The newly measured lines have been combined with previously measured transition frequencies and fitted by a procedure used successfully for dimethyl ether. From the fit to the global data set, we have extracted parameters that have enabled us to predict accurately the frequencies and intensities of over 10,000 lines of possible astronomical importance at frequencies of up to 620 GHz. The detection of interstellar acetone was first reported by Combes et al. based on two transitions with partially resolved internal rotation structure. The present work will aid further interstellar studies to verify acetone as an interstellar constituent.

Submillimeter-wave and far-infrared spectroscopy of high-J transitions of the ground and ν2=1 states of ammonia

Complete and reliable knowledge of the ammonia spectrum is needed to enable the analysis and interpretation of astrophysical and planetary observations. Ammonia has been observed in the interstellar medium up to J=18 and more highly excited transitions are expected to appear in hot exoplanets and brown dwarfs. As a result, there is considerable interest in observing and assigning the high J (rovibrational) spectrum. In this work, numerous spectroscopic techniques were employed to study its high J transitions in the ground and ν(2)=1 states. Measurements were carried out using a frequency multiplied submillimeter spectrometer at Jet Propulsion Laboratory (JPL), a tunable far-infrared spectrometer at University of Toyama, and a high-resolution Bruker IFS 125 Fourier transform spectrometer (FTS) at Synchrotron SOLEIL. Highly excited ammonia was created with a radiofrequency discharge and a dc discharge, which allowed assignments of transitions with J up to 35. One hundred and seventy seven ground state and ν(2)=1 inversion transitions were observed with microwave accuracy in the 0.3-4.7 THz region. Of these, 125 were observed for the first time, including 26 ΔK=3 transitions. Over 2000 far-infrared transitions were assigned to the ground state and ν(2)=1 inversion bands as well as the ν(2) fundamental band. Of these, 1912 were assigned using the FTS data for the first time, including 222 ΔK=3 transitions. The accuracy of these measurements has been estimated to be 0.0003-0.0006 cm(-1). A reduced root mean square error of 0.9 was obtained for a global fit of the ground and ν(2)=1 states, which includes the lines assigned in this work and all previously available microwave, terahertz, far-infrared, and mid-infrared data. The new measurements and predictions reported here will support the analyses of astronomical observations by high-resolution spectroscopy telescopes such as Herschel, SOFIA, and ALMA. The comprehensive experimental rovibrational energy levels reported here will permit further refinement of the potential energy surface to improve ammonia ab initio calculations and facilitate assignment of new high-resolution spectra of hot ammonia.

Rotational Spectrum of the Formyl Cation, HCO+, to 1.2 THz

A variety of high-quality spectroscopic studies have contributed to knowledge of the formyl cation, HCO+, and its rare isotopologues, but technical limitations have previously limited precise determinations of the far-infrared, or terahertz spectrum. This study extends the microwave, millimeter, and submillimeter spectroscopy of HCO+ into the terahertz range. The resulting measurements and predictions are of sufficient coverage to adequately address astrophysical questions about this species using the Herschel Space Observatory or the Atacama Large Millimeter Array.