scholarly journals Parameterizing radiative transfer to convert MAX-DOAS dSCDs into near-surface box-averaged mixing ratios

2013 ◽  
Vol 6 (6) ◽  
pp. 1521-1532 ◽  
Author(s):  
R. Sinreich ◽  
A. Merten ◽  
L. Molina ◽  
R. Volkamer
Keyword(s):  
Boundary Layer ◽  
Radiative Transfer ◽  
Mexico City ◽  
Vertical Gradient ◽  
Radiative Transfer Model ◽  
Optical Absorption Spectroscopy ◽  
Transfer Model ◽  
Model Calculations ◽  
Near Surface ◽  
Mixing Ratios

Abstract. We present a novel parameterization method to convert multi-axis differential optical absorption spectroscopy (MAX-DOAS) differential slant column densities (dSCDs) into near-surface box-averaged volume mixing ratios. The approach is applicable inside the planetary boundary layer under conditions with significant aerosol load, and builds on the increased sensitivity of MAX-DOAS near the instrument altitude. It parameterizes radiative transfer model calculations and significantly reduces the computational effort, while retrieving ~ 1 degree of freedom. The biggest benefit of this method is that the retrieval of an aerosol profile, which usually is necessary for deriving a trace gas concentration from MAX-DOAS dSCDs, is not needed. The method is applied to NO2 MAX-DOAS dSCDs recorded during the Mexico City Metropolitan Area 2006 (MCMA-2006) measurement campaign. The retrieved volume mixing ratios of two elevation angles (1° and 3°) are compared to volume mixing ratios measured by two long-path (LP)-DOAS instruments located at the same site. Measurements are found to agree well during times when vertical mixing is expected to be strong. However, inhomogeneities in the air mass above Mexico City can be detected by exploiting the different horizontal and vertical dimensions probed by the MAX-DOAS and LP-DOAS instruments. In particular, a vertical gradient in NO2 close to the ground can be observed in the afternoon, and is attributed to reduced mixing coupled with near-surface emission inside street canyons. The existence of a vertical gradient in the lower 250 m during parts of the day shows the general challenge of sampling the boundary layer in a representative way, and emphasizes the need of vertically resolved measurements.

scholarly journals Parameterizing radiative transfer to convert MAX-DOAS dSCDs into near-surface box averaged mixing ratios and vertical profiles

2012 ◽  
Vol 5 (5) ◽  
pp. 7641-7673 ◽  
Author(s):  
R. Sinreich ◽  
A. Merten ◽  
L. Molina ◽  
R. Volkamer
Keyword(s):  
Boundary Layer ◽  
Radiative Transfer ◽  
Mexico City ◽  
Vertical Gradient ◽  
Trace Gas ◽  
Optical Absorption Spectroscopy ◽  
Transfer Model ◽  
Model Calculations ◽  
Near Surface ◽  
Mixing Ratios

Abstract. We present a novel parameterization method to convert Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) differential Slant Column Densities (dSCDs) into near-surface box averaged volume mixing ratios. The approach is applicable inside the planetary boundary layer under conditions with significant aerosol load, does not require a-priori assumptions about the trace gas vertical distribution and builds on the increased sensitivity of MAX-DOAS near the instrument altitude. It parameterizes radiative transfer model calculations and significantly reduces the computational effort. The biggest benefit of this method is that the retrieval of an aerosol profile, which usually is necessary for deriving a trace gas concentration from MAX-DOAS dSCDs, is not needed. The method is applied to NO2 MAX-DOAS dSCDs recorded during the Mexico City Metropolitan Area 2006 (MCMA-2006) measurement campaign. The retrieved volume mixing ratios of two elevation angles (1° and 3°) are compared to volume mixing ratios measured by two long-path (LP)-DOAS instruments located at the same site. Measurements are found to agree well during times when vertical mixing is expected to be strong. However, inhomogeneities in the air mass above Mexico City can be detected by exploiting the different horizontal and vertical dimensions probed by MAX-DOAS measurements at different elevation angles, and by LP-DOAS. In particular, a vertical gradient in NO2 close to the ground can be observed in the afternoon, and is attributed to reduced mixing coupled with near surface emission. The existence of a vertical gradient in the lower 250 m during parts of the day shows the general challenge of sampling the boundary layer in a representative way and emphasizes the need of vertically resolved measurements.

scholarly journals Determination of tropospheric vertical columns of NO<sub>2</sub> and aerosol optical properties in a rural setting using MAX-DOAS

2011 ◽  
Vol 11 (23) ◽  
pp. 12475-12498 ◽  
Author(s):  
J. D. Halla ◽  
T. Wagner ◽  
S. Beirle ◽  
J. R. Brook ◽  
K. L. Hayden ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Radiative Transfer ◽  
Urban Areas ◽  
Source Region ◽  
Time Of Day ◽  
Rural Setting ◽  
Radiative Transfer Model ◽  
Optical Absorption Spectroscopy ◽  
Transfer Model ◽  
Vertical Column

Abstract. Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements were performed in a rural location of southwestern Ontario during the Border Air Quality and Meteorology Study. Slant column densities (SCDs) of NO2 and O4 were determined using the standard DOAS technique. Using a radiative transfer model and the O4 SCDs, aerosol optical depths were determined for clear sky conditions and compared to OMI, MODIS, AERONET, and local PM2.5 measurements. This aerosol information was input to a radiative transfer model to calculate NO2 air mass factors, which were fit to the measured NO2 SCDs to determine tropospheric vertical column densities (VCDs) of NO2. The method of determining NO2 VCDs in this way was validated for the first time by comparison to composite VCDs derived from aircraft and ground-based measurements of NO2. The new VCDs were compared to VCDs of NO2 determined via retrievals from the satellite instruments SCIAMACHY and OMI, for overlapping time periods. The satellite-derived VCDs were higher, with a mean bias of +0.5–0.9×1015 molec cm−2. This last finding is different from previous studies whereby MAX-DOAS geometric VCDs were higher than satellite determinations, albeit for urban areas with higher VCDs. An effective boundary layer height, BLHeff, is defined as the ratio of the tropospheric VCD and the ground level concentration of NO2. Variations of BLHeff can be linked to time of day, source region, stability of the atmosphere, and the presence or absence of elevated NOx sources. In particular, a case study is shown where a high VCD and BLHeff were observed when an elevated industrial plume of NOx and SO2 was fumigated to the surface as a lake breeze impacted the measurement site. High BLHeff values (~1.9 km) were observed during a regional smog event when high winds from the SW and high convection promoted mixing throughout the boundary layer. During this event, the regional line flux of NO2 through the region was estimated to be greater than 112 kg NO2 km−1 h−1.

scholarly journals The CU 2-dimensional MAX-DOAS instrument – Part 1: Retrieval of NO<sub>2</sub> in 3 dimensions and azimuth dependent OVOC ratios

2014 ◽  
Vol 7 (11) ◽  
pp. 11653-11709 ◽  
Author(s):  
I. Ortega ◽  
T. Koenig ◽  
R. Sinreich ◽  
D. Thomson ◽  
R. Volkamer
Keyword(s):  
Boundary Layer ◽  
Trace Gases ◽  
Elevation Angle ◽  
Tropospheric Chemistry ◽  
Radiative Transfer Model ◽  
Optical Absorption Spectroscopy ◽  
Transfer Model ◽  
High Time Resolution ◽  
Vertical Profiles ◽  
Near Surface

Abstract. We present an innovative instrument telescope, and describe a retrieval method to probe 3-D distributions of atmospheric trace gases that are relevant to air pollution and tropospheric chemistry. The University of Colorado (CU) two dimensional (2-D) Multi-AXis-Differential Optical Absorption Spectroscopy (CU 2D-MAX-DOAS) instrument measures nitrogen dioxide (NO2), formaldehyde (HCHO), glyoxal (CHOCHO), oxygen dimer (O2-O2, or O4) and water vapor (H2O); also nitrous acid (HONO), bromine monoxide (BrO), iodine monoxide (IO) among other gases can in principle be measured. Information about aerosols is derived through coupling with a radiative transfer model (RTM). The 2-D telescope has 3 modes of operation: (mode 1) measures solar scattered photons from any pair of elevation angle (−20° < EA < +90° or zenith; zero is to the horizon) and azimuth angle (−180° < AA < +180°; zero being North), (mode 2) measures any set of AA at constant EA (almucantar scans); and (mode 3) tracks the direct solar beam via a separate view port. Vertical profiles of trace gases are measured, and used to estimate planetary boundary layer height (PBL). Horizontal distributions are then derived using PBL and parameterization of RTM (Sinreich et al., 2013). NO2 is evaluated at different wavelengths (350, 450, and 560 nm), exploiting the fact that the effective path length varies systematically with wavelength. The area probed is constrained by O4 observations at nearby wavelengths, and has an effective radius of 7.5 to 20 km around the instrument location; i.e., up to 1250 km2 can be sampled near-instantaneously, and with high time resolution. The instrument was deployed as part of the Multi Axis DOAS Comparison campaign for Aerosols and Trace gases (MAD-CAT) in Mainz, Germany from 7 June to 6 July 2013. We present first measurements (modes 1 and 2 only) and describe a four-step retrieval to derive (a) boundary layer vertical profiles of NO2 and PBL; (b) near-surface horizontal distributions of NO2; (c) range resolved NO2 horizontal distribution measurements using an "onion peeling" approach; and (d) the ratios HCHO-to-NO2 (RFN), CHOCHO-to-NO2 (RGN), and CHOCHO-to-HCHO (RGF) at 14 pre-set azimuth angles distributed over a 360° view. 2D-MAX-DOAS provides an innovative, regional perspective about trace gases, their spatial and temporal concentration gradients, and maximizes information to compare near-surface observations with atmospheric models and satellites.

scholarly journals Determination of tropospheric vertical columns of NO<sub>2</sub> and aerosol optical properties in a rural setting using MAX-DOAS

2011 ◽  
Vol 11 (4) ◽  
pp. 13035-13097 ◽  
Author(s):  
J. D. Halla ◽  
T. Wagner ◽  
S. Beirle ◽  
J. R. Brook ◽  
K. L. Hayden ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Radiative Transfer ◽  
Urban Areas ◽  
Source Region ◽  
Time Of Day ◽  
Rural Setting ◽  
Radiative Transfer Model ◽  
Optical Absorption Spectroscopy ◽  
Transfer Model ◽  
Vertical Column

Abstract. Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements were performed in a rural location of southwestern Ontario during the Border Air Quality and Meteorology Study. Slant column densities (SCDs) of NO2 and O4 were determined using the standard DOAS technique. Using a radiative transfer model and the O4 SCDs, aerosol optical depths were determined for clear sky conditions and compared to OMI, MODIS, AERONET, and local PM2.5 measurements. This aerosol information was input to a radiative transfer model to calculate NO2 air mass factors, which were fit to the measured NO2 SCDs to determine tropospheric vertical column densities (VCDs) of NO2. The method of determining NO2 VCDs in this way was validated by comparison to composite VCDs derived from aircraft and ground-based measurements of NO2. The new VCDs were compared to VCDs of NO2 determined via the satellite instruments SCIAMACHY and OMI, for overlapping time periods. The satellite-derived VCDs were higher by 50%, with a mean positive error of 0.5–0.9 × 1015 molec cm−2. This last finding is different from previous studies whereby MAX-DOAS geometric VCDs were higher than satellite determinations, albeit for urban areas with higher VCDs. An effective boundary layer height, BLeff, is defined as the ratio of the tropospheric VCD and the ground level concentration of NO2. Variations of BLeff can be linked to time of day, source region, stability of the atmosphere, and the presence or absence of elevated NOx sources. In particular, a case study is shown where a high VCD and BLeff were observed when an elevated industrial plume of NOx and SO2 was fumigated to the surface as a lake breeze front impacted the measurement site. High BLeff values (~1.9 km) were observed during a regional smog event when high winds from the SW and high convection promoted mixing throughout the boundary layer. During this event, the regional line flux of NO2 through the region was estimated to be greater than 112 kg NO2 km−1 h−1.

Polar  Stratospheric Clouds detection at Belgrano II Antarctic station from DOAS measurements

2021 ◽  
Author(s):  
Laura Gómez Martín ◽  
Daniel Toledo ◽  
Margarita Yela ◽  
Cristina Prados-Román ◽  
José Antonio Adame ◽  
...  
Keyword(s):  
Radiative Transfer ◽  
Color Index ◽  
Radiative Transfer Model ◽  
Optical Absorption Spectroscopy ◽  
Transfer Model ◽  
Meteorological Model ◽  
Weather Forecasts ◽  
Stratospheric Temperature ◽  
Stratospheric Clouds

&lt;p&gt;&lt;span&gt;Ground-based zenith DOAS (Differential Optical Absorption Spectroscopy) measurements have been used to detect and estimate the altitude of PSCs over Belgrano II Antarctic station during the polar sunrise seasons of 2018 and 2019. The method used in this work studies the evolution of the color index (CI) during twilights. The CI has been defined here as the ratio of the recorded signal at 520 and 420 nm. In the presence of PSCs, the CI shows a maximum at a given solar zenith angle (SZA). The value of such SZA depends on the altitude of the PSC. By using a spherical Monte Carlo radiative transfer model (RTM), the method has been validated and a function relating the SZA of the CI maximum and the PSC altitude has been calculated. Model simulations also show that PSCs can be detected and their altitude can be estimated even in presence of optically thin tropospheric clouds or aerosols. Our results are in good agreement with the stratospheric temperature evolution obtained through the ERA5 data reanalysis from the global meteorological model ECMWF (European Centre for Medium Range Weather Forecasts) and the PSCs observations from CALIPSO (Cloud-Aerosol-Lidar and Infrared Pathfinder Satellite Observations).&lt;/span&gt;&lt;/p&gt;&lt;p&gt;&lt;span&gt;The methodology used in this work could also be applied to foreseen and/or historical measurements obtained with ground-based spectrometers such e. g. the DOAS instruments dedicated to trace gas observation in Arctic and Antarctic sites. This would also allow to investigate the presence and long-term evolution of PSCs.&lt;/span&gt;&lt;/p&gt;&lt;p&gt;&lt;span&gt;&lt;strong&gt;Keywords: &lt;/strong&gt;Polar stratospheric clouds; color index; radiative transfer model; visible spectroscopy.&lt;/span&gt;&lt;/p&gt;

scholarly journals Validating the MYSTIC three-dimensional radiative transfer model with observations from the complex topography of Arizona's Meteor Crater

2010 ◽  
Vol 10 (5) ◽  
pp. 13373-13405 ◽  
Author(s):  
B. Mayer ◽  
S. W. Hoch ◽  
C. D. Whiteman
Keyword(s):  
Monte Carlo ◽  
Radiative Transfer ◽  
Three Dimensional ◽  
Longwave Radiation ◽  
Horizontal Resolution ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
Deep Basin ◽  
Near Surface ◽  
Radiation Fields

Abstract. The MYSTIC three-dimensional Monte-Carlo radiative transfer model has been extended to simulate solar and thermal irradiances with a rigorous consideration of topography. Forward as well as backward Monte Carlo simulations are possible for arbitrarily oriented surfaces and we demonstrate that the backward Monte Carlo technique is superior to the forward method for applications involving topography, by greatly reducing the computational demands. MYSTIC is used to simulate the short- and longwave radiation fields during a clear day and night in and around Arizona's Meteor Crater, a bowl-shaped, 165-m-deep basin with a diameter of 1200 m. The simulations are made over a 4 by 4 km domain using a 10-m horizontal resolution digital elevation model and meteorological input data collected during the METCRAX (Meteor Crater Experiment) field experiment in 2006. Irradiance (or radiative flux) measurements at multiple locations inside the crater are then used to evaluate the simulations. MYSTIC is shown to realistically model the complex interactions between topography and the radiative field, resolving the effects of terrain shading, terrain exposure, and longwave surface emissions. The effects of surface temperature variations and of temperature stratification within the crater atmosphere on the near-surface longwave irradiance are then evaluated with additional simulations.

scholarly journals Inter-comparison of MAX-DOAS measurements of tropospheric HONO slant column densities and vertical profiles during the CINDI-2 Campaign

2020 ◽  
Author(s):  
Yang Wang ◽  
Arnoud Apituley ◽  
Alkiviadis Bais ◽  
Steffen Beirle ◽  
Nuria Benavent ◽  
...  
Keyword(s):  
Radiative Transfer ◽  
Estimation Method ◽  
Optimal Estimation ◽  
Early Morning ◽  
Radiative Transfer Model ◽  
Measuring Instruments ◽  
Transfer Model ◽  
Vertical Profiles ◽  
Near Surface ◽  
Profile Inversion

Abstract. We present the inter-comparison of delta slant column densities (SCDs) and vertical profiles of nitrous acid (HONO) derived from measurements of different MAX-DOAS instruments and using different inversion algorithms during the Second Cabauw Inter-comparison campaign for Nitrogen Dioxide measuring Instruments (CINDI-2), in September 2016, at Cabauw, The Netherlands (51.97° N, 4.93° E). Systematic discrepancies of HONO delta SCDs are observed in the range of ±0.3 × 1015 molecules cm−2, which is half of the typical random discrepancy of 0.6 × 1015 molecules cm−2. For a typical high HONO delta SCD of 2 × 1015 molecules cm−2, the relative systematic and random discrepancies are about 15 % and 30 %, respectively. The inter-comparison of HONO profiles shows that both systematic and random discrepancies of HONO VCDs and near-surface volume mixing ratios (VMRs) are mostly in the range of ~ ±0.5 × 1015 molecules cm−2 and ~ ±0.1 ppb (typically ~ 20 %). Further we find that the discrepancies of the retrieved HONO profiles are dominated by discrepancies of the HONO delta SCDs. The profile retrievals only contribute to the discrepancies of the HONO profiles by ~ 5 %. However, some data sets with substantial larger discrepancies than the typical values indicate that inappropriate implementations of profile inversion algorithms and configurations of radiative transfer models in the profile retrievals can also be an important uncertainty source. In addition, estimations of measurement uncertainties of HONO dSCDs, which can significantly impact profile retrievals using the optimal estimation method, need to consider not only DOAS fit errors, but also atmospheric variability, especially for an instrument with a DOAS fit error lower than ~ 3 × 1015 molecules cm−2. The MAX-DOAS results during the CINDI-2 campaign indicate that the peak HONO levels (e.g. near-surface VMRs of ~ 0.4 ppb) often appeared in the early morning and below 0.2 km. The near-surface VMRs retrieved from the MAX-DOAS observations are compared with those measured using a co-located long-path DOAS instrument. The systematic differences are smaller than 0.15 ppb and 0.07 ppb during early morning and around noon, respectively. Since true HONO values at high altitudes are not known in the absence of real measurements, in order to evaluate the abilities of profile inversion algorithms to respond to different HONO profile shapes, we performed sensitivity studies using synthetic HONO delta SCDs simulated by a radiative transfer model with assumed HONO profiles. The tests indicate that the profile inversion algorithms based on the optimal estimation method with proper configurations can well reproduce the different HONO profile shapes. Therefore we conclude that the feature of HONO accumulated near the surface derived from MAX-DOAS measurements are expected to well represent the ambient HONO profiles.

Process-Based Decomposition of the Decadal Climate Difference between 2002–13 and 1984–95

2017 ◽  
Vol 30 (12) ◽  
pp. 4373-4393 ◽  
Author(s):  
Xiaoming Hu ◽  
Yana Li ◽  
Song Yang ◽  
Yi Deng ◽  
Ming Cai
Keyword(s):  
Radiative Transfer ◽  
Heat Storage ◽  
Decomposition Analysis ◽  
Arctic Region ◽  
The Arctic ◽  
Radiative Transfer Model ◽  
Transfer Model ◽  
Model Calculations ◽  
Surface Warming ◽  
Decadal Climate

This study examines at the process level the climate difference between 2002–13 and 1984–95 in ERA-Interim. A linearized radiative transfer model is used to calculate the temperature change such that its thermal radiative cooling would balance the energy flux perturbation associated with the change of an individual process, without regard to what causes the change of the process in the first place. The global mean error of the offline radiative transfer model calculations is 0.09 K, which corresponds to the upper limit of the uncertainties from a single term in the decomposition analysis. The process-based decomposition indicates that the direct effect of the increase of CO2 (0.15 K) is the largest contributor to the global warming between the two periods (about 0.27 K). The second and third largest contributors are the cloud feedback (0.14 K) and the combined effect of the oceanic heat storage and evaporation terms (0.11 K), respectively. The largest warming associated with the oceanic heat storage term is found in the tropical Pacific and Indian Oceans, with relatively weaker warming over the tropical Atlantic Ocean. The increase in atmospheric moisture adds another 0.1 K to the global surface warming, but the enhancement in tropical convections acts to reduce the surface warming by 0.17 K. The ice-albedo and atmospheric dynamical feedbacks are the two leading factors responsible for the Arctic polar warming amplification (PWA). The increase of atmospheric water vapor over the Arctic region also contributes substantially to the Arctic PWA pattern.

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