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Sara Lance, Jie Zhang, James J. Schwab, Paul Casson, Richard E. Brandt, David R. Fitzjarrald, Margaret J. Schwab, John Sicker, Cheng-Hsuan Lu, Sheng-Po Chen, Jeongran Yun, Jeffrey M. Freedman, Bhupal Shrestha, Qilong Min, Mark Beauharnois, Brian Crandall, Everette Joseph, Matthew J. Brewer, Justin R. Minder, Daniel Orlowski, Amy Christiansen, Annmarie G. Carlton, and Mary C. Barth

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.

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Xin-Zhong Liang, Min Xu, Xing Yuan, Tiejun Ling, Hyun I. Choi, Feng Zhang, Ligang Chen, Shuyan Liu, Shenjian Su, Fengxue Qiao, Yuxiang He, Julian X. L. Wang, Kenneth E. Kunkel, Wei Gao, Everette Joseph, Vernon Morris, Tsann-Wang Yu, Jimy Dudhia, and John Michalakes

The CWRF is developed as a climate extension of the Weather Research and Forecasting model (WRF) by incorporating numerous improvements in the representation of physical processes and integration of external (top, surface, lateral) forcings that are crucial to climate scales, including interactions between land, atmosphere, and ocean; convection and microphysics; and cloud, aerosol, and radiation; and system consistency throughout all process modules. This extension inherits all WRF functionalities for numerical weather prediction while enhancing the capability for climate modeling. As such, CWRF can be applied seamlessly to weather forecast and climate prediction. The CWRF is built with a comprehensive ensemble of alternative parameterization schemes for each of the key physical processes, including surface (land, ocean), planetary boundary layer, cumulus (deep, shallow), microphysics, cloud, aerosol, and radiation, and their interactions. This facilitates the use of an optimized physics ensemble approach to improve weather or climate prediction along with a reliable uncertainty estimate. The CWRF also emphasizes the societal service capability to provide impactrelevant information by coupling with detailed models of terrestrial hydrology, coastal ocean, crop growth, air quality, and a recently expanded interactive water quality and ecosystem model.

This study provides a general CWRF description and basic skill evaluation based on a continuous integration for the period 1979– 2009 as compared with that of WRF, using a 30-km grid spacing over a domain that includes the contiguous United States plus southern Canada and northern Mexico. In addition to advantages of greater application capability, CWRF improves performance in radiation and terrestrial hydrology over WRF and other regional models. Precipitation simulation, however, remains a challenge for all of the tested models.

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