Satellite remote sensing of cloud properties in support of troposheric trace gas retrievals

Aben, E.A.A. [Promotor

Photopolarimetric Retrievals of Snow Properties

Polarimetric observations of snow surfaces, obtained in the 410-2264 nm range with the Research Scanning Polarimeter onboard the NASA ER-2 high-altitude aircraft, are analyzed and presented. These novel measurements are of interest to the remote sensing community because the overwhelming brightness of snow plagues aerosol and cloud retrievals based on airborne and spaceborne total reflection measurements. The spectral signatures of the polarized reflectance of snow are therefore worthwhile investigating in order to provide guidance for the adaptation of algorithms currently employed for the retrieval of aerosol properties over soil and vegetated surfaces. At the same time, the increased information content of polarimetric measurements allows for a meaningful characterization of the snow medium. In our case, the grains are modeled as hexagonal prisms of variable aspect ratios and microscale roughness, yielding retrievals of the grains' scattering asymmetry parameter, shape and size. The results agree with our previous findings based on a more limited data set, with the majority of retrievals leading to moderately rough crystals of extreme aspect ratios, for each scene corresponding to a single value of the asymmetry parameter

Aerosol Retrieval from Multiangle Multispectral Photopolarimetric Measurements: Importance of Spectral Range and Angular Resolution

We investigated the importance of spectral range and angular resolution for aerosol retrieval from multiangle photopolarimetric measurements over land. For this purpose, we use an extensive set of simulated measurements for different spectral ranges and angular resolutions and subsets of real measurements of the airborne Research Scanning Polarimeter (RSP) carried out during the PODEX and SEAC4RS campaigns over the continental USA. Aerosol retrievals performed from RSP measurements show good agreement with ground-based AERONET measurements for aerosol optical depth (AOD), single scattering albedo (SSA) and refractive index. Furthermore, we found that inclusion of shortwave infrared bands (1590 and/or 2250 nm) significantly improves the retrieval of AOD, SSA and coarse mode microphysical properties. However, accuracies of the retrieved aerosol properties do not improve significantly when more than five viewing angles are used in the retrieval

Retrieval of liquid water cloud properties from POLDER-3 measurements using a neural network ensemble approach

This paper describes a neural network algorithm for the estimation of liquid water cloud optical properties from the Polarization and Directionality of Earth's Reflectances-3 (POLDER-3) instrument aboard the Polarization &amp; Anisotropy of Reflectances for Atmospheric Sciences coupled with Observations from a Lidar (PARASOL) satellite. The algorithm has been trained on synthetic multi-angle, multi-wavelength measurements of reflectance and polarization and has been applied to the processing of 1 year of POLDER-3 data. Comparisons of the retrieved cloud properties with Moderate Resolution Imaging Spectroradiometer (MODIS) products show that the neural network algorithm has a low bias of around 2 in cloud optical thickness (COT) and between 1 and 2&thinsp;µm in the cloud effective radius. Comparisons with existing POLDER-3 datasets suggest that the proposed scheme may have enhanced capabilities for cloud effective radius retrieval, at least over land. An additional feature of the presented algorithm is that it provides COT and effective radius retrievals at the native POLDER-3 Level 1B pixel level.</p

Remote sensing of ice crystal asymmetry parameter using multi-directional polarization measurements &ndash; Part 1: Methodology and evaluation with simulated measurements

We present a new remote sensing technique to infer the average asymmetry parameter of ice crystals near cloud top from multi-directional polarization measurements. The method is based on previous findings that (a) complex aggregates of hexagonal crystals generally have scattering phase matrices resembling those of their components; and (b) scattering phase matrices systematically vary with aspect ratios of crystals and their degree of microscale surface roughness. Ice cloud asymmetry parameters are inferred from multi-directional polarized reflectance measurements by searching for the closest fit in a look-up table of simulated polarized reflectances computed for cloud layers that contain individual, randomly oriented hexagonal columns and plates with varying aspect ratios and roughness values. The asymmetry parameter of the hexagonal particle that leads to the best fit with the measurements is considered the retrieved value. For clouds with optical thickness less than 5, the cloud optical thickness must be retrieved simultaneously with the asymmetry parameter, while for optically thicker clouds the asymmetry parameter retrieval is independent of cloud optical thickness. Evaluation of the technique using simulated measurements based on the optical properties of a number of complex particles and their mixtures shows that the ice crystal asymmetry parameters are generally retrieved to within 5%, or about 0.04 in absolute terms. The retrieval scheme is largely independent of calibration errors, range and sampling density of scattering angles and random noise in the measurements. The approach can be applied to measurements of past, current and future airborne and satellite instruments that measure multi-directional polarized reflectances of ice-topped clouds

Spitzer Mapping of PAHs and H2 in Photodissociation Regions

The mid-infrared (MIR) spectra of dense photodissociation regions (PDRs) are typically dominated by emission from polycyclic aromatic hydrocarbons (PAHs) and the lowest pure rotational states of molecular hydrogen (H2); two species which are probes of the physical properties of gas and dust in intense UV radiation fields. We utilize the high angular resolution of the Infrared Spectrograph on the Spitzer Space Telescope to construct spectral maps of the PAH and H2 features for three of the best studied PDRs in the galaxy, NGC 7023, NGC 2023 and IC 63. We present spatially resolved maps of the physical properties, including the H2 ortho-to-para ratio, temperature, and G_o/n_H. We also present evidence for PAH dehydrogenation, which may support theories of H2 formation on PAH surfaces, and a detection of preferential self-shielding of ortho-H2. All PDRs studied exhibit average temperatures of ~500 - 800K, warm H2 column densities of ~10^20 cm^-2, G_o/n_H ~ 0.1 - 0.8, and ortho-to-para ratios of ~ 1.8. We find that while the average of each of these properties is consistent with previous single value measurements of these PDRs, when available, the addition of spatial resolution yields a diversity of values with gas temperatures as high as 1500 K, column densities spanning ~ 2 orders of magnitude, and extreme ortho-to-para ratios of 3.Comment: 14 figure

When an old star smolders: On the detection of hydrocarbon emission from S-type AGB stars

Polycyclic aromatic hydrocarbons (PAHs) produce characteristic infrared emission bands that have been observed in a wide range of astrophysical environments, where carbonaceous material is subjected to ultraviolet (UV) radiation. Although PAHs are expected to form in carbon-rich AGB stars, they have up to now only been observed in binary systems where a hot companion provides a hard radiation field. In this letter, we present low-resolution infrared spectra of four S-type AGB stars, selected from a sample of 90 S-type AGB stars observed with the infrared spectrograph aboard the Spitzer satellite. The spectra of these four stars show the typical infrared features of PAH molecules. We confirm the correlation between the temperature of the central star and the centroid wavelength of the 7.9 {\mu}m feature, present in a wide variety of stars spanning a temperature range from 3 000 to 12 000 K. Three of four sources presented in this paper extend this relation towards lower temperatures. We argue that the mixture of hydrocarbons we see in these S-stars has a rich aliphatic component. The fourth star, BZ CMa, deviates from this correlation. Based on the similarity with the evolved binary TU Tau, we predict that BZ CMa has a hot companion as well.Comment: 5 pages, 2 figures, 2 table

Simultaneous Polarimeter Retrievals of Microphysical Aerosol and Ocean Color Parameters from the MAPP Algorithm with Comparison to High Spectral Resolution Lidar Aerosol and Ocean Products

We present an optimal estimation based retrieval framework, the Microphysical Aerosol Properties from Polarimetry (MAPP) algorithm, designed for simultaneous retrieval of aerosol microphysical properties and ocean color bio-optical parameters using multi-angular polarized radiances. Polarimetric measurements from the airborne NASA Research Scanning Polarimeter (RSP) were inverted by MAPP to produce atmosphere and ocean products. The RSP MAPP results are compared with co-incident lidar measurements made by the NASA High Spectral Resolution Lidar HSRL-1 and HSRL-2 instruments. Comparisons are made of the aerosol optical depth (AOD) at 355 and 532 nm, lidar column-averaged measurements of the aerosol lidar ratio and ngstrm exponent, and lidar ocean measurements of the particulate hemispherical backscatter coefficient and the diffuse attenuation coefficient. The measurements were collected during the 2012 Two-Column Aerosol Project (TCAP) campaign and the 2014 Ship-Aircraft Bio-Optical Research (SABOR) campaign. For the SABOR campaign, 73% RSP MAPP retrievals fall within 0.04 AOD at 532 nm as measured by HSRL-1, with an R value of 0.933 and root-mean-square deviation of 0.0372. For the TCAP campaign, 53% of RSP MAPP retrievals are within 0.04 AOD as measured by HSRL-2, with an R value of 0.927 and root-mean-square deviation of 0.0673. Comparisons with HSRL-2 AOD at 355 nm during TCAP result in an R value of 0.959 and a root-mean-square deviation of also 0.0694. The RSP retrievals using the MAPP optimal estimation framework represent a key milestone on the path to a combined lidar + polarimeter retrieval using both HSRL and RSP measurements

Confronting the Challenge of Modeling Cloud and Precipitation Microphysics

In the atmosphere, microphysics refers to the microscale processes that affect cloud and precipitation particles and is a key linkage among the various components of Earth\u27s atmospheric water and energy cycles. The representation of microphysical processes in models continues to pose a major challenge leading to uncertainty in numerical weather forecasts and climate simulations. In this paper, the problem of treating microphysics in models is divided into two parts: (i) how to represent the population of cloud and precipitation particles, given the impossibility of simulating all particles individually within a cloud, and (ii) uncertainties in the microphysical process rates owing to fundamental gaps in knowledge of cloud physics. The recently developed Lagrangian particle‐based method is advocated as a way to address several conceptual and practical challenges of representing particle populations using traditional bulk and bin microphysics parameterization schemes. For addressing critical gaps in cloud physics knowledge, sustained investment for observational advances from laboratory experiments, new probe development, and next‐generation instruments in space is needed. Greater emphasis on laboratory work, which has apparently declined over the past several decades relative to other areas of cloud physics research, is argued to be an essential ingredient for improving process‐level understanding. More systematic use of natural cloud and precipitation observations to constrain microphysics schemes is also advocated. Because it is generally difficult to quantify individual microphysical process rates from these observations directly, this presents an inverse problem that can be viewed from the standpoint of Bayesian statistics. Following this idea, a probabilistic framework is proposed that combines elements from statistical and physical modeling. Besides providing rigorous constraint of schemes, there is an added benefit of quantifying uncertainty systematically. Finally, a broader hierarchical approach is proposed to accelerate improvements in microphysics schemes, leveraging the advances described in this paper related to process modeling (using Lagrangian particle‐based schemes), laboratory experimentation, cloud and precipitation observations, and statistical methods

[SiPAH]+ pi-Complexes in the Interstellar Medium

We investigate the presence of silicon atoms adsorbed on the surface of interstellar polycyclic aromatic hydrocarbons (PAHs) to form SiPAH pi-complexes. We use quantum chemistry calculations to obtain structural, thermodynamic and mid-IR properties of neutral and cationic SiPAH complexes. The binding energy was found to be at least 1.5 eV for [SiPAH]+ complexes whereas it is roughly 0.5 eV for their neutral counterparts. From the spectral analysis of the calculated IR spectra, we found that the coordination of silicon to PAH+ does not strongly affect the intensities of the PAH+ spectra, but systematically introduces blueshifts of the C-C in-plane and the C-H out-of-plane bands. The thermodynamic data calculated for [SiPAH]+ complexes show that these species are stable and can be easily formed by radiative association of Si+ and PAH species that are known to be abundant in photodissociation regions. Their mid-IR fingerprints show features induced by the coordination of silicon that could account for (i) the blueshifted position of the 6.2 micron AIB and (ii) the presence of satellite bands observed on the blue side of the 6.2 and 11.2 micron AIBs. From such an assignment, we can deduce that typically 1% of the cosmic silicon appears to be attached to PAHs.Comment: Accepted for publication in Astronomy and Astrophysic