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Abstract
Central to the aerosol indirect effect on climate is the relationship between cloud droplet concentrations Nd and cloud condensation nuclei (CCN) concentrations. There are valid reasons to expect a sublinear relationship between measured Nd and CCN, and such relationships have been observed for clouds in a variety of locations. However, a measurement artifact known as “coincidence” can also produce a sublinear trend. The current paper shows that two commonly used instruments, the cloud droplet probe (CDP) and the cloud and aerosol spectrometer (CAS), can be subject to significantly greater coincidence errors than are typically recognized, with an undercounting bias of at least 27% and an oversizing bias of 20%–30% on average at Nd = 500 cm−3, and with an undercounting bias of as much as 44% at Nd = 1000 cm−3. This type of systematic error may have serious implications for interpretation of in situ cloud observations. It is shown that a simple optical modification of the CDP dramatically reduces oversizing and undercounting biases due to coincidence. Guidance is provided for diagnosing coincidence errors in CAS and CDP instruments.
Abstract
Central to the aerosol indirect effect on climate is the relationship between cloud droplet concentrations Nd and cloud condensation nuclei (CCN) concentrations. There are valid reasons to expect a sublinear relationship between measured Nd and CCN, and such relationships have been observed for clouds in a variety of locations. However, a measurement artifact known as “coincidence” can also produce a sublinear trend. The current paper shows that two commonly used instruments, the cloud droplet probe (CDP) and the cloud and aerosol spectrometer (CAS), can be subject to significantly greater coincidence errors than are typically recognized, with an undercounting bias of at least 27% and an oversizing bias of 20%–30% on average at Nd = 500 cm−3, and with an undercounting bias of as much as 44% at Nd = 1000 cm−3. This type of systematic error may have serious implications for interpretation of in situ cloud observations. It is shown that a simple optical modification of the CDP dramatically reduces oversizing and undercounting biases due to coincidence. Guidance is provided for diagnosing coincidence errors in CAS and CDP instruments.
Abstract
It has been known that aerosol particles act as nuclei for ice formation for over a century and a half (see Dufour). Initial attempts to understand the nature of these ice nucleating particles were optical and electron microscope inspection of inclusions at the center of a crystal (see Isono; Kumai). Only within the last few decades has instrumentation to extract ice crystals from clouds and analyze the residual material after sublimation of condensed-phase water been available (see Cziczo and Froyd). Techniques to ascertain the ice nucleating potential of atmospheric aerosols have only been in place for a similar amount of time (see DeMott et al.). In this chapter the history of measurements of ice nucleating particles, both in the field and complementary studies in the laboratory, are reviewed. Remaining uncertainties and artifacts associated with measurements are described and suggestions for future areas of improvement are made.
Abstract
It has been known that aerosol particles act as nuclei for ice formation for over a century and a half (see Dufour). Initial attempts to understand the nature of these ice nucleating particles were optical and electron microscope inspection of inclusions at the center of a crystal (see Isono; Kumai). Only within the last few decades has instrumentation to extract ice crystals from clouds and analyze the residual material after sublimation of condensed-phase water been available (see Cziczo and Froyd). Techniques to ascertain the ice nucleating potential of atmospheric aerosols have only been in place for a similar amount of time (see DeMott et al.). In this chapter the history of measurements of ice nucleating particles, both in the field and complementary studies in the laboratory, are reviewed. Remaining uncertainties and artifacts associated with measurements are described and suggestions for future areas of improvement are made.
Abstract
Aqueous chemical processing within cloud and fog water is thought to be a key process in the production and transformation of secondary organic aerosol mass, found abundantly and ubiquitously throughout the troposphere. Yet, significant uncertainty remains regarding the organic chemical reactions taking place within clouds and the conditions under which those reactions occur, owing to the wide variety of organic compounds and their evolution under highly variable conditions when cycled through clouds. Continuous observations from a fixed remote site like Whiteface Mountain (WFM) in New York State and other mountaintop sites have been used to unravel complex multiphase interactions in the past, particularly the conversion of gas-phase emissions of SO2 to sulfuric acid within cloud droplets in the presence of sunlight. These scientific insights led to successful control strategies that reduced aerosol sulfate and cloud water acidity substantially over the following decades. This paper provides an overview of observations obtained during a pilot study that took place at WFM in August 2017 aimed at obtaining a better understanding of Chemical Processing of Organic Compounds within Clouds (CPOC). During the CPOC pilot study, aerosol cloud activation efficiency, particle size distribution, and chemical composition measurements were obtained below-cloud for comparison to routine observations at WFM, including cloud water composition and reactive trace gases. Additional instruments deployed for the CPOC pilot study included a Doppler lidar, sun photometer, and radiosondes to assist in evaluating the meteorological context for the below-cloud and summit observations.
Abstract
Aqueous chemical processing within cloud and fog water is thought to be a key process in the production and transformation of secondary organic aerosol mass, found abundantly and ubiquitously throughout the troposphere. Yet, significant uncertainty remains regarding the organic chemical reactions taking place within clouds and the conditions under which those reactions occur, owing to the wide variety of organic compounds and their evolution under highly variable conditions when cycled through clouds. Continuous observations from a fixed remote site like Whiteface Mountain (WFM) in New York State and other mountaintop sites have been used to unravel complex multiphase interactions in the past, particularly the conversion of gas-phase emissions of SO2 to sulfuric acid within cloud droplets in the presence of sunlight. These scientific insights led to successful control strategies that reduced aerosol sulfate and cloud water acidity substantially over the following decades. This paper provides an overview of observations obtained during a pilot study that took place at WFM in August 2017 aimed at obtaining a better understanding of Chemical Processing of Organic Compounds within Clouds (CPOC). During the CPOC pilot study, aerosol cloud activation efficiency, particle size distribution, and chemical composition measurements were obtained below-cloud for comparison to routine observations at WFM, including cloud water composition and reactive trace gases. Additional instruments deployed for the CPOC pilot study included a Doppler lidar, sun photometer, and radiosondes to assist in evaluating the meteorological context for the below-cloud and summit observations.
