Inverse Methods: a Powerful Tool for Evaluating Aerosol Data, Exemplified on Cases With Relevance for the Atmosphere and the Aerosol Climate Effect

For a complete description of a given aerosol, more than one parameter is necessary, e.g. parameters concerning size distribution, chemical composition, and particle morphology. On the other hand, most instruments measuring aerosol properties are sensitive mostly to one parameter, but cross-sensitive to others. These cross-sensitivities are often eliminated by assumptions during data evaluation, inducing systematic uncertainties in the results. The use of assumptions can be reduced by combining the information of several instruments on the same aerosol and using inverse methods for interpretation of the data. The presentation focuses on two application examples of these methods. The first example concerns a size distribution inversion algorithm that combines data from several instruments into one size distribution. The second example deals with an algorithm that retrieves the aerosol asymmetry parameter (with respect to particle scattering) from measurements of the aerosol absorption and spectral scattering and hemispheric backscattering coefficients, thereby providing a set of parameters that completely describes an aerosol with respect to its direct climate effect

Vibrational spectroscopy of an optogenetic rhodopsin: a biophysical study of molecular mechanisms

In this dissertation,the membrane protein channelrhodopsin-1 from the green flagellate algae Chlamydomonas agustae (CaChR1) is studied using a variety of spectroscopic techniques developed in the Rothschild Molecular Biophysics Laboratory at Boston University. Over the last decade, channelrhodopsins have proven to be effective optogenetic tools due to their ability to function as light-gated ion channels when expressed in neurons. This ability allows neuroscientists to optically activate an inward directed photocurrent which depolarizes the neuronal membranes and triggers an action potential. Although a variety of channelrhodopsins with different properties have been used, the underlying mechanisms of channelrhodopsin functionality is not yet fully understood. The protein studied here has several advantageous properties compared to the more extensively studied channelrhodopsin-2 from Chlamydomonas reinhardtii including a red shifted visible absorption and slower light inactivation despite having a lower channel current. Elucidating the internal molecular mechanisms underlying the function of CaChR1 provides critical insight into the large class of channelrhodopsin proteins leading toward improved bioengineering for specific optogenetic applications. Here near-IR pre-resonance Raman spectroscopy of CaChR1 provides information on the structure of the unphotolyzed (P0) retinal chromophore, the Schiff base protonation state, and presence of carboxylic acid residues interacting with the Schiff base. Low-temperature FTIR difference spectroscopy combined with site-directed mutagenesis and isotope labeling provide information on changes occurring in the retinal chromophore and protein during the primary phototransition (P0 to P1). This includes information about changes involving protonation state of binding-pocket residues, protein backbone structure, and internal water molecules. Further experiments combining low-temperature and time-resolved FTIR-difference spectroscopy reveal additional information about structural changes during the transition from the unphotolyzed state to the active (open channel) state of the protein (P0 to P2). This work has resulted in an initial model that describes key proton transfer events which occur between the Schiff base and carboxylic acid residues inside the active site of CaChR1. The model raises the possibility that ion channel gating and ion specificity is regulated by the protonation changes of two key residues (Glu 169 and Asp299) located near the Schiff base

Scientific Objectives, Measurement Needs, and Challenges Motivating the PARAGON Aerosol Initiative

Aerosols are involved in a complex set of processes that operate across many spatial and temporal scales. Understanding these processes, and ensuring their accurate representation in models of transport, radiation transfer, and climate, requires knowledge of aerosol physical, chemical, and optical properties and the distributions of these properties in space and time. To derive aerosol climate forcing, aerosol optical and microphysical properties and their spatial and temporal distributions, and aerosol interactions with clouds, need to be understood. Such data are also required in conjunction with size-resolved chemical composition in order to evaluate chemical transport models and to distinguish natural and anthropogenic forcing. Other basic parameters needed for modeling the radiative influences of aerosols are surface reflectivity and three-dimensional cloud fields. This large suite of parameters mandates an integrated observing and modeling system of commensurate scope. The Progressive Aerosol Retrieval and Assimilation Global Observing Network (PARAGON) concept, designed to meet this requirement, is motivated by the need to understand climate system sensitivity to changes in atmospheric constituents, to reduce climate model uncertainties, and to analyze diverse collections of data pertaining to aerosols. This paper highlights several challenges resulting from the complexity of the problem. Approaches for dealing with them are offered in the set of companion papers

Aerosol Data Sources and Their Roles within PARAGON

We briefly but systematically review major sources of aerosol data, emphasizing suites of measurements that seem most likely to contribute to assessments of global aerosol climate forcing. The strengths and limitations of existing satellite, surface, and aircraft remote sensing systems are described, along with those of direct sampling networks and ship-based stations. It is evident that an enormous number of aerosol-related observations have been made, on a wide range of spatial and temporal sampling scales, and that many of the key gaps in this collection of data could be filled by technologies that either exist or are expected to be available in the near future. Emphasis must be given to combining remote sensing and in situ active and passive observations and integrating them with aerosol chemical transport models, in order to create a more complete environmental picture, having sufficient detail to address current climate forcing questions. The Progressive Aerosol Retrieval and Assimilation Global Observing Network (PARAGON) initiative would provide an organizational framework to meet this goal

Reply to ''Comments on 'Why Hasn't Earth Warmed as much as Expected?'''

In response to our article, Why Hasnt Earth Warmed as Much as Expected? (2010), Knutti and Plattner (2012) wrote a rebuttal. The term climate sensitivity is usually defined as the change in global mean surface temperature that is produced by a specified change in forcing, such as a change in solar heating or greenhouse gas concentrations. We had argued in the 2010 paper that although climate models can reproduce the global mean surface temperature history over the past century, the uncertainties in these models, due primarily to the uncertainty in climate forcing by airborne particles, mean that the models lack the confidence to actually constrain the climate sensitivity within useful limits for climate prediction. Knutti and Plattner are climate modelers, and they argued essentially that because the models could reproduce the surface temperature history, the issue we raised was moot. Our response amounts to straightening out this confusion; for the models to be constraining, they must be able to reproduce the surface temperature history with sufficient confidence, not just to match the measurements, but to exclude alternative histories. As before, we concluded that if we can actually make the aerosol measurements using currently available, state-of-the-art techniques, we can determine the aerosol climate forcing to the degree required to constrain that aspect of model climate sensitivity. A technical issue relating to the timescale over which a change in CO2 emissions would be equilibrated in the environmental energy balance was also discussed, again, a matter of differences in terminology

Evaluation of Daytime Measurements of Aerosols and Water Vapor made by an Operational Raman Lidar over the Southern Great Plains

Raman lidar water vapor and aerosol extinction profiles acquired during the daytime over the Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) site in northern Oklahoma (36.606 N, 97.50 W, 315 m) are evaluated using profiles measured by in situ and remote sensing instruments deployed during the May 2003 Aerosol Intensive Operations Period (IOP). The automated algorithms used to derive these profiles from the Raman lidar data were first modified to reduce the adverse effects associated with a general loss of sensitivity of the Raman lidar since early 2002. The Raman lidar water vapor measurements, which are calibrated to match precipitable water vapor (PWV) derived from coincident microwave radiometer (MWR) measurements were, on average, 5-10% (0.3-0.6 g/m(exp 3) higher than the other measurements. Some of this difference is due to out-of-date line parameters that were subsequently updated in the MWR PWV retrievals. The Raman lidar aerosol extinction measurements were, on average, about 0.03 km(exp -1) higher than aerosol measurements derived from airborne Sun photometer measurements of aerosol optical thickness and in situ measurements of aerosol scattering and absorption. This bias, which was about 50% of the mean aerosol extinction measured during this IOP, decreased to about 10% when aerosol extinction comparisons were restricted to aerosol extinction values larger than 0.15 km(exp -1). The lidar measurements of the aerosol extinction/backscatter ratio and airborne Sun photometer measurements of the aerosol optical thickness were used along with in situ measurements of the aerosol size distribution to retrieve estimates of the aerosol single scattering albedo (omega(sub o)) and the effective complex refractive index. Retrieved values of omega(sub o) ranged from (0.91-0.98) and were in generally good agreement with omega(sub o) derived from airborne in situ measurements of scattering and absorption. Elevated aerosol layers located between about 2.6 and 3.6 km were observed by the Raman lidar on May 25 and May 27. The airborne measurements and lidar retrievals indicated that these layers, which were likely smoke produced by Siberian forest fires, were primarily composed of relatively large particles (r(sub eff) approximately 0.23 micrometers), and that the layers were relatively nonabsorbing (omega(sub o) approximately 0.96-0.98). Preliminary results show that major modifications that were made to the Raman lidar system during 2004 have dramatically improved the sensitivity in the aerosol and water vapor channels and reduced random errors in the aerosol scattering ratio and water vapor retrievals by an order of magnitude

The Atmospheric Radiation Measurement Program May 2003 Intensive Operations Period Examining Aerosol Properties and Radiative Influences: Preface to Special Section

Atmospheric aerosols influence climate by scattering and absorbing radiation in clear air (direct effects) and by serving as cloud condensation nuclei, modifying the microphysical properties of clouds, influencing radiation and precipitation development (indirect effects). Much of present uncertainty in forcing of climate change is due to uncertainty in the relations between aerosol microphysical and optical properties and their radiative influences (direct effects) and between microphysical properties and their ability to serve as cloud condensation nuclei at given supersaturations (indirect effects). This paper introduces a special section that reports on a field campaign conducted at the Department of Energy Atmospheric Radiation Measurement site in North Central Oklahoma in May, 2003, examining these relations using in situ airborne measurements and surface-, airborne-, and space-based remote sensing

Cloud-Driven Changes in Aerosol Optical Properties - Final Technical Report

The optical properties of aerosol particles are the controlling factors in determining direct aerosol radiative forcing. These optical properties depend on the chemical composition and size distribution of the aerosol particles, which can change due to various processes during the particles’ lifetime in the atmosphere. Over the course of this project we have studied how cloud processing of atmospheric aerosol changes the aerosol optical properties. A counterflow virtual impactor was used to separate cloud drops from interstitial aerosol and parallel aerosol systems were used to measure the optical properties of the interstitial and cloud-scavenged aerosol. Specifically, aerosol light scattering, back-scattering and absorption were measured and used to derive radiatively significant parameters such as aerosol single scattering albedo and backscatter fraction for cloud-scavenged and interstitial aerosol. This data allows us to demonstrate that the radiative properties of cloud-processed aerosol can be quite different than pre-cloud aerosol. These differences can be used to improve the parameterization of aerosol forcing in climate models

Cloud Scavenging Effects on Aerosol Radiative and Cloud-nucleating Properties - Final Technical Report

The optical properties of aerosol particles are the controlling factors in determining direct aerosol radiative forcing. These optical properties depend on the chemical composition and size distribution of the aerosol particles, which can change due to various processes during the particles’ lifetime in the atmosphere. Over the course of this project we have studied how cloud processing of atmospheric aerosol changes the aerosol optical properties. A counterflow virtual impactor was used to separate cloud drops from interstitial aerosol and parallel aerosol systems were used to measure the optical properties of the interstitial and cloud-scavenged aerosol. Specifically, aerosol light scattering, back-scattering and absorption were measured and used to derive radiatively significant parameters such as aerosol single scattering albedo and backscatter fraction for cloud-scavenged and interstitial aerosol. This data allows us to demonstrate that the radiative properties of cloud-processed aerosol can be quite different than pre-cloud aerosol. These differences can be used to improve the parameterization of aerosol forcing in climate models