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Tropospheric ozone lidars are well suited to measuring the high spatio-temporal variability of this important trace gas. Furthermore, lidar measurements in conjunction with balloon soundings, aircraft, and satellite observations provide substantial information about a variety of atmospheric chemical and physical processes. Examples of processes elucidated by ozone-lidar measurements are presented, and modeling studies using WRF-Chem, RAQMS, and DALES/LES models illustrate our current understanding and shortcomings of these processes.

NASA initiated an interagency ozone lidar observation network under the name TOLNet to promote cooperative multiple-station ozone-lidar observations to provide highly time-resolved (few minutes) tropospheric-ozone vertical profiles useful for air-quality studies, model evaluation, and satellite validation.

Ground-based lidars are suitable for long-term ozone monitoring as a complement to satellite and ozonesonde measurements. However, current ground-based lidars are unable to consistently measure ozone below 500 m above ground level (AGL) due to both engineering issues and high retrieval sensitivity to various measurement errors. In this paper, we present our instrument design, retrieval techniques, and preliminary results that focus on the high-temporal profiling of ozone within the atmospheric boundary layer (ABL) achieved by the addition of an inexpensive and compact mini-receiver to the previous system. For the first time, to the best of our knowledge, the lowest, consistently achievable observation height has been extended down to 125 m AGL for a ground-based ozone lidar system. Both the analysis and preliminary measurements demonstrate that this lidar measures ozone with a precision generally better than 10% at a temporal resolution of 10 min and a vertical resolution from 150 m at the bottom of the ABL to 550 m at the top. A measurement example from summertime shows that inhomogeneous ozone aloft was affected by both surface emissions and the evolution of ABL structures.

This paper presents ozone structures measured by a ground-based ozone lidar and ozonesonde at Huntsville, Alabama, on 27-29 April 2010 originating from a stratosphere-to-troposphere transport event associated with a cutoff cyclone and tropopause fold. In this case, the tropopause reached 6 km and the stratospheric intrusion resulted in a 2-km thick elevated ozone layer with values between 70 and 85 ppbv descending from the 306-K to 298-K isentropic surface at a rate of 5 km day1. The potential temperature was provided by a collocated microwave profiling radiometer. We examine the corresponding meteorological fields and potential vorticity (PV) structures derived from the analysis data from the North American Mesoscale model. The 2-PVU (PV unit) surface, defined as the dynamic tropopause, is able to capture the variations of the ozone tropopause estimated from the ozonesonde and lidar measurements. The estimated ozone/PV ratio, from the measured ozone and model derived PV, for the mixing layer between the troposphere and stratosphere is approximately 41 ppbv/PVU with an uncertainty of approximately 33%. Within two days, the estimated mass of ozone irreversibly transported from the stratospheric into the troposphere is between 0.07 Tg (0.9 10(exp33) molecules) and 0.11 Tg (1.3 10(exp33) molecules) with an estimated uncertainty of 59%. Tropospheric ozone exhibited enormous variability due to the complicated mixing processes. Low ozone and large variability were observed in the mid-troposphere after the stratospheric intrusion due to the westerly advection including the transition from a cyclonic system to an anticyclonic system. This study using high temporal and vertical-resolution measurements suggests that, in this case, stratospheric air quickly lost its stratospheric characteristics once it is irreversibly mixed down into the troposphere.

We report the use of a return-to- zero (RZPN) pseudo noise modulation technique for making range resolved measurements of CO2 within the planetary boundary layer (PBL) using commercial, off-the-shelf, components. Conventional, range resolved, DIAL measurements require laser pulse widths that are significantly shorter than the desired spatial resolution and necessitate using pulses whose temporal spacing is such that scattered returns from only a single pulse are observed by the receiver at any one time (for the PBL pulse separations must be greater than approximately 20 microseconds). This imposes significant operational limitations when using currently available fiber lasers because of the resulting low duty cycle (less than approximately 0.0005) and consequent low average laser output power. The RZPN modulation technique enables a fiber laser to operate at much higher duty cycles (approaching 0.04) thereby more effectively utilizing the amplifier's output. This increases the counts received by approximately two orders of magnitude. Our approach involves employing two distributed feedback lasers (DFB), each modulated by a different RPZN code, whose outputs are then amplified by a CW fiber amplifier. One laser is tuned to a CO2 absorption line; the other operates offline thereby permitting the simultaneous acquisition of both on and offline signals using independent RZPN codes. This minimizes the impact of atmospheric turbulence on the measurement. The on and offline signals are retrieved by deconvolving the return signal using the appropriate kernels.

A tropospheric ozone Differential Absorption Lidar system, developed jointly by The University of Alabama in Huntsville and the National Aeronautics and Space Administration, is making regular observations of ozone vertical distributions between 1 and 8 km with two receivers under both daytime and nighttime conditions using lasers at 285 and 291 nm. This paper describes the lidar system and analysis technique with some measurement examples. An iterative aerosol correction procedure reduces the retrieval error arising from differential aerosol backscatter in the lower troposphere. Lidar observations with coincident ozonesonde flights demonstrate that the retrieval accuracy ranges from better than 10% below 4 km to better than 20% below 8 km with 750-m vertical resolution and 10-min 17 temporal integration.

Retrievals of CO2 profiles within the planetary boundary layer (PBL) are required to understand CO2 transport over regional scales and for validating the future space borne CO2 remote sensing instrument, such as the CO2 Laser Sounder, for the ASCENDS mission, We report the use of a return-to-zero (RZ) pseudo noise (PN) code modulation technique for making range resolved measurements of CO2 within the PBL using commercial, off-the-shelf, components. Conventional, range resolved, measurements require laser pulse widths that are s#rorter than the desired spatial resolution and have pulse spacing such that returns from only a single pulse are observed by the receiver at one time (for the PBL pulse separations must be greater than approximately 2000m). This imposes a serious limitation when using available fiber lasers because of the resulting low duty cycle (less than 0.001) and consequent low average laser output power. RZ PN code modulation enables a fiber laser to operate at much higher duty cycles (approaching 0.1) thereby more effectively utilizing the amplifier's output. This results in an increase in received counts by approximately two orders of magnitude. The approach involves employing two, back to back, CW fiber amplifiers seeded at the appropriate on and offline CO2 wavelengths (approximately 1572 nm) using distributed feedback diode lasers modulated by a PN code at rates significantly above 1 megahertz. An assessment of the technique, discussions of measurement precision and error sources as well as preliminary data will be presented.

A tropospheric ozone Differential Absorption Lidar (DIAL) system, developed jointly by the University of Alabama at Huntsville and NASA, is making regular observations of ozone vertical distributions between 1 and 8 km with two receivers under both daytime and nighttime conditions using lasers at 285 and 291 nm. This paper describes the lidar system and analysis technique with some measurement examples. An iterative aerosol correction procedure reduces the retrieval error arising from differential aerosol backscatter in the lower troposphere. Lidar observations with coincident ozonesonde flights demonstrate that the retrieval accuracy ranges from better than 10% below 4 km to better than 20% below 8 km with 750-m vertical resolution and 10-min temporal integration

A tropospheric ozone DIfferential Absorption Lidar (DIAL) system has been developed jointly by NASA and the University of Alabama at Huntsville (UAH). Two separated Nd:YAG pumped dye laser systems produce the laser pulses with wavelengths of 285 and 291 nm at 20 Hz frequency. The receiver is a Newtonian telescope with a 40 cm primary and a two-channel aft optics unit. The detection system currently uses photon counting to facilitate operations at the maximum achievable altitude. This lidar measures free-tropospheric ozone profiles between 4-10 km at Regional Atmospheric Profiling Laboratory for Discovery (RAPCD) in UAH campus (ASL 206 m) under both daytime and nighttime conditions. Frequent coincident ozonesonde flights and theoretical calculations provide evidence to indicate the retrieval accuracy ranges from approx.5% at 4 km to approx.60% at 10 km with 750-m vertical resolution and 30-minute integration. Three Hamamatsu 7400 PMTs and analog detection technique will be added on the current system to extend the measurement to approx.100 m above ground to monitor the PBL and lower tropospheric ozone variations.

A tropospheric ozone Differential Absorption Lidar (DIAL) system, developed jointly by NASA and the University of Alabama at Huntsville (UAH), measures free-tropospheric ozone profiles between 4-10 km. Located at 192 meters altitude in the Regional Atmospheric Profiling Laboratory for Discovery (RAPCD) on the UAH campus in Huntsville, AL, USA, this tropospheric ozone lidar operates under both daytime and nighttime conditions. Frequent coincident ozonesonde flights and theoretical calculations provide evidence to indicate the retrieval accuracy ranges from better than 8% at 4km to 40%-60% at 10 kin with 750-m vertical resolution and 30-minute integration. With anticipated improvements to allow retrievals at both higher and lower altitudes, this ozone lidar, along with co-located aerosol and Doppler Wind Lidars, will provide a unique 18 dataset for investigations of PBL and free-tropospheric chemical and dynamic processes.

A ground based differential absorption lidar is under development at NASA's Goddard Space Flight Center to make range resolved measurements of CO2 within the planetary boundary layer. This is a direct detection lidar designed for both photon counting and analog use. Technology being developed for this instrument will be discussed including efforts in fiber lasers, optical parametric amplifiers and both InGaAs and HgCdTe solid-state detectors. The capabilities of this system are investigated and preliminary results presented.

In order to address the problem of sources and sinks of CO2 measurements are needed on a global scale. Clearly a satellite is a promising approach to meeting this requirement. Unfortunately, most methods for making a CO2 measurement from space involve the whole column. Since sources and sinks at the surface represent a small perturbation to the total column one is faced with the need to measure the column with a precision better than 1%. No species has ever been measured from space at this level. We have developed over the last 3 years a small instrument based upon a Fabry-Perot interferometer that is very sensitive to atmospheric CO2 and has a high signal to noise ratio. We have tested this instrument in a ground based configuration and from aircraft platforms simulating operation from a satellite. We will present results from these tests and discuss ways that this promising new instrument could be used to improve our understanding of the global carbon budget.

This paper describes the development of a lidar transmitter using an optical parametric amplifier. It is designed for profiling gases of atmospheric interest at high spatial and temporal precision in the near-IR. Discussions on desirable characteristics for such a transmitter with specific reference to the case of CO, are made.

The interaction between local and regional pollution levels occurs at the interface of the Planetary Boundary Layer and the Free Troposphere. Measuring the vertical distribution of ozone, aerosols, and winds with high temporal and vertical resolution is essential to diagnose the nature of this interchange and ultimately for accurately forecasting ozone and aerosol pollution levels. The Regional Atmospheric Profiling Center for Discovery, RAPCD, was built and instrumented to address this critical issue. The ozone W DIAL lidar, Nd:YAG aerosol lidar, and 2.1 micron Doppler wind lidar, along with balloon- borne ECC ozonesondes form the core of the W C D instrumentation for addressing this problem. Instrumentation in the associated Mobile Integrated Profiling (MIPS) laboratory includes 91 5Mhz profiler, sodar, and ceilometer. The collocated Applied particle Optics and Radiometry (ApOR) laboratory hosts an FTIR along with MOUDI and optical particle counters. With MODELS-3 analysis by colleagues in the National Space Science and Technology Center on the UAH campus and the co- located National Weather Service Forecasting Office in Huntsville, AL we are developing a unique facility for advancing the state of the science of pollution forecasting.

A detailed mechanistic understanding of the sources and sinks of CO2 will be required to reliably predict future CO2 levels and climate. A commonly used technique for deriving information about CO2 exchange with surface reservoirs is to solve an 'inverse problem', where CO2 observations are used with an atmospheric transport model to find the optimal distribution of sources and sinks. Synthesis inversion methods are powerful tools for addressing this question, but the results are disturbingly sensitive to the details of the calculation. Studies done using different atmospheric transport models and combinations of surface station data have produced substantially different distributions of surface fluxes. Adjoint methods are now being developed that will more effectively incorporate diverse datasets in estimates of surface fluxes of CO2. In an adjoint framework, it will be possible to combine CO2 concentration data from longterm surface and aircraft monitoring stations with data from intensive field campaigns and with proposed future satellite observations. We have recently developed an adjoint for the GSFC 3-D Parameterized Chemistry and Transport Model (PCTM). Here, we will present results from a PCTM Adjoint study comparing the sampling footprints of tall tower, aircraft and potential future lidar observations of CO2. The vertical resolution and extent of the profiles and the observation frequency will be considered for several sites in North America.

The AROTAL instrument (Airborne Raman Ozone Temperature and Aerosol Lidar) - a collaboration between scientists at NASA Goddard Space Flight Center, and Langley Research Center - was flown on the NASA DC-8 during the SOLVE II Campaign during January and February, 2003. The flights were flown from the Arena Arctica in Kiruna, Sweden. We report measurements of temperature and ozone profiles showing approximately a 600 ppbv loss in ozone near 17.5 km, over the time frame of the aircraft campaign. Comparisons of ozone profiles from AROTAL are made with the SAGE III instrument.

We report on an active remote sensing approach using an erbium fiber amplifier based transmitter for atmospheric CO2 measurements in an overtone band near 1.57 microns and initial horizontal path measurements to less than 1% precision.

Ground-based LIDAR observations can potentially provide continuous profiles of CO2 through the planetary boundary layer and into the free troposphere. We will present initial atmospheric measurements from a prototype system that is based on components developed by the telecommunications industry. Preliminary measurements and instrument performance calculations indicate that an optimized differential absorption LIDAR (DIAL) system will be capable of providing continuous hourly averaged profiles with 250m vertical resolution and better than 1 ppm precision at 1 km. Precision increases (decreases) at lower (higher) altitudes and is directly proportional to altitude resolution and acquisition time. Thus, precision can be improved if temporal or vertical resolution is sacrificed. Our approach measures absorption by CO2 of pulsed laser light at 1.6 microns backscattered from atmospheric aerosols. Aerosol concentrations in the planetary boundary layer are relatively high and are expected to provide adequate signal returns for the desired resolution. The long-term goal of the project is to develop a rugged, autonomous system using only commercially available components that can be replicated inexpensively for deployment in a monitoring network.

NASA Goddard Space Flight Center's Airborne Raman Ozone, Temperature and Aerosol Lidar (AROTEL) measured extremely cold temperatures during all three deployments (December 1-16, 1999, January 14-29, 2000 and February 27-March 15, 2000) of the Sage III Ozone Loss and Validation Experiment (SOLVE). Temperatures were significantly below values observed in previous years with large regions regularly below 191 K and frequent temperature retrievals yielding values at or below 187 K. Temperatures well below the saturation point of type I polar stratospheric clouds (PSCs) were regularly encountered but their presence was not well correlated with PSCs observed by the NASA Langley Research Center's Aerosol Lidar co-located with AROTEL. Temperature measurements by meteorological sondes launched within areas traversed by the DC-8 showed minimum temperatures consistent in time and vertical extent with those derived from AROTEL data. Calculations to establish whether PSCs could exist at measured AROTEL temperatures and observed mixing ratios of nitric acid and water vapor showed large regions favorable to PSC formation. On several occasions measured AROTEL temperatures up to 10 K below the NAT saturation temperature were insufficient to produce PSCs even though measured values of nitric acid and water were sufficient for their formation.

The Airborne Raman Ozone, Temperature and Aerosol Lidar (AROTEL) participated in the recent Sage III Ozone Loss and Validation Experiment (SOLVE) by providing profiles of aerosols, polar stratospheric clouds (PSCs), ozone and temperature with high vertical and horizontal resolution. Temperatures were derived from just above the aircraft to approximately 60 kilometers geometric altitude with a reported vertical resolution of between 0.5 and 1.5 km. The horizontal footprint varied from 4 to 70 km. This paper explores the measurement uncertainties associated with the temperature retrievals and makes comparisons with independent, coincident, measurements of temperature. Measurement uncertainties range from 0.1 K to approximately 4 K depending on altitude and integration time. Comparisons between AROTEL and balloon sonde temperatures retrieved under clear sky conditions using both Rayleigh and Raman scattered data showed AROTEL approximately 1 K colder than sonde values. Comparisons between AROTEL and the Meteorological Measurement System (MMS) on NASA's ER-2 show AROTEL being from 2-3 K colder for altitudes ranging from 14 to 18 km. Temperature comparisons between AROTEL and the United Kingdom Meteorological Office's model showed differences of approximately 1 K below approximately 25 km and a very strong cold bias of approximately 12 K at altitudes between 30 and 35 km.

Ozone observations from ozonesondes, the lidars aboard the DC-8, in situ ozone measurements from the ER-2, and satellite ozone measurements from Polar Ozone and Aerosol Measurement III (POAM) were used to assess ozone loss during the Sage III Ozone Loss and Validation Experiment (SOLVE) 1999-2000 Arctic campaign. Two methods of analysis were used. In the first method a simple regression analysis is performed on the ozonesonde and POAM measurements within the vortex. In the second method, the ozone measurements from all available ozone data were injected into a free running diabatic trajectory model and carried forward in time from December 1 to March 15. Vortex ozone loss was then estimated by comparing the ozone values of those parcels initiated early in the campaign with those parcels injected later in the campaign. Despite the variety of observational techniques used during SOLVE, the measurements provide a fairly consistent picture. Over the whole vortex, the largest ozone loss occurs between 550 and 400 K potential temperatures (approximately 23-16 km) with over 1.5 ppmv lost by March 15, the end of the SOLVE mission period. An ozone loss rate of 0.04-0.05 ppmv/day was computed for March 15. Ozonesondes launched after March 15 suggest that an additional 0.5 ppmv or more ozone was lost between March 15 and April 1. The small disagreement between ozonesonde and POAM analysis of January ozone loss is found to be due to biases in vortex sampling. POAM makes most of its solar occultation measurements at the vortex edge during January 2000 which bias samples toward air parcels that have been exposed to sunlight and likely do experience ozone loss. Ozonesonde measurements and the trajectory technique use observations that are more distributed within the interior of the vortex. Thus the regression analysis of the POAM measurements tends to overestimate mid-winter vortex ozone loss. Finally, our loss calculations are broadly consistent with other loss computations using ER-2 tracer data and MLS satellite data, but we find no evidence for the 1992 high mid-January loss reported using the Match technique.