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Article ; Online: Core-Shell Modeling of Light Scattering by Vesicles: Effect of Size, Contents, and Lamellarity.

Wang, Anna / Chan Miller, Christopher / Szostak, Jack W

2019 Volume 116, Issue 4, Page(s) 659–669

Abstract: Having a fast, reliable method for characterizing vesicles is vital for their use as model cell membranes in biophysics, synthetic biology, and origins of life studies. Instead of the traditionally used Rayleigh-Gans-Debye approximation, we use an exact ... ...

Abstract	Having a fast, reliable method for characterizing vesicles is vital for their use as model cell membranes in biophysics, synthetic biology, and origins of life studies. Instead of the traditionally used Rayleigh-Gans-Debye approximation, we use an exact extended Lorenz-Mie solution for how core-shell particles scatter light to model vesicle turbidity. This approach enables accurate interpretations of simple turbidimetric measurements and is able to accurately model highly scattering vesicles, such as larger vesicles, those with multiple layers, and those with encapsulated material. We uncover several surprising features, including that vesicle lamellarity has a larger effect on sample turbidity than vesicle size and that the technique can be used to measure the membrane thickness of vesicles. We also examine potential misinterpretations of turbidimetry and discuss when measurements are limited by forward and multiple scattering and by the geometry of the instrument.
MeSH term(s)	Light ; Lipid Bilayers/chemistry ; Models, Theoretical ; Oleic Acid/chemistry ; Phosphatidylcholines/chemistry ; Scattering, Radiation
Chemical Substances	Lipid Bilayers ; Phosphatidylcholines ; Oleic Acid (2UMI9U37CP) ; 1-palmitoyl-2-oleoylphosphatidylcholine (TE895536Y5)
Language	English
Publishing date	2019-01-10
Publishing country	United States
Document type	Journal Article ; Research Support, Non-U.S. Gov't ; Research Support, U.S. Gov't, Non-P.H.S.
ZDB-ID	218078-9
ISSN	1542-0086 ; 0006-3495
ISSN (online)	1542-0086
ISSN	0006-3495
DOI	10.1016/j.bpj.2019.01.006
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Book ; Online: Level0 to Level1B processor for MethaneAIR

Conway, Eamon K. / Souri, Amir H. / Benmergui, Joshua / Sun, Kang / Liu, Xiong / Staebell, Carly / Chan Miller, Christopher / Franklin, Jonathan / Samra, Jenna / Wilzewski, Jonas / Roche, Sebastien / Luo, Bingkun / Chulakadabba, Apisada / Sargent, Maryann / Hohl, Jacob / Daube, Bruce / Gordon, Iouli / Chance, Kelly / Wofsy, Steven

eISSN: 1867-8548

2024

Abstract: This work presents the development of the MethaneAIR Level0–Level1B processor, which converts raw L0 data to calibrated and georeferenced L1B data. MethaneAIR is the airborne simulator for MethaneSAT, a new satellite under development by MethaneSAT LLC, ... ...

Abstract	This work presents the development of the MethaneAIR Level0–Level1B processor, which converts raw L0 data to calibrated and georeferenced L1B data. MethaneAIR is the airborne simulator for MethaneSAT, a new satellite under development by MethaneSAT LLC, a subsidiary of the Environmental Defense Fund (EDF). MethaneSAT's goals are to precisely map over 80 % of the production sources of methane from oil and gas fields across the globe to an accuracy of 2–4 ppb on a 2 km 2 scale. Efficient algorithms have been developed to perform dark corrections, estimate the noise, radiometrically calibrate data, and correct stray light. A forward model integrated into the L0–L1B processor is demonstrated to retrieve wavelength shifts during flight accurately. It is also shown to characterize the instrument spectral response function (ISRF) changes occurring at each sampled spatial footprint. We demonstrate fast and accurate orthorectification of MethaneAIR data in a three-step process: (i) initial orthorectification of all observations using aircraft avionics, a simple camera model, and a medium-resolution digital elevation map; (ii) registration of oxygen (O 2 ) channel grayscale images to reference Multispectral Instrument (MSI) band 11 imagery via Accelerated-KAZE (A-KAZE) feature extraction and linear transformation, with similar co-registration of methane (CH 4 ) channel grayscale images to the registered O 2 channel images; and finally (iii) optimization of the aircraft position and attitude to the registered imagery and calculation of viewing geometry. This co-registration technique accurately orthorectifies each channel to the referenced MSI imagery. However, in the pixel domain, radiance data for each channel are offset by almost 150–200 across-track pixels (rows) and need to be aligned for the full-physics or proxy retrievals where both channels are simultaneously used. We leveraged our orthorectification tool to identify tie points with similar geographic locations in both CH 4 and O 2 images in order to produce shift ...
Subject code	333
Language	English
Publishing date	2024-02-29
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Article: Revisiting the effectiveness of HCHO/NO2 ratios for inferring ozone sensitivity to its precursors using high resolution airborne remote sensing observations in a high ozone episode during the KORUS-AQ campaign

Souri, Amir H / Abad, Gonzalo González / Blake, Donald R / Chan Miller, Christopher E / Chance, Kelly / Diskin, Glenn S / Fried, Alan / Janz, Scott J / Lamsal, Lok N / Liu, Xiong / Nowlan, Caroline R / Weinheimer, Andrew J / Wolfe, Glenn M

Elsevier Ltd Atmospheric environment. 2020 Mar. 01, v. 224

2020

Abstract: The nonlinear chemical processes involved in ozone production (P(O3)) have necessitated using proxy indicators to convey information about the primary dependence of P(O3) on volatile organic compounds (VOCs) or nitrogen oxides (NOx). In particular, the ... ...

Abstract	The nonlinear chemical processes involved in ozone production (P(O3)) have necessitated using proxy indicators to convey information about the primary dependence of P(O3) on volatile organic compounds (VOCs) or nitrogen oxides (NOx). In particular, the ratio of remotely sensed columns of formaldehyde (HCHO) to nitrogen dioxide (NO2) has been widely used for studying O3 sensitivity. Previous studies found that the errors in retrievals and the incoherent relationship between the column and the near-surface concentrations are a barrier in applying the ratio in a robust way. In addition to these obstacles, we provide calculational-observational evidence, using an ensemble of 0-D photochemical box models constrained by DC-8 aircraft measurements on an ozone event during the Korea-United States Air Quality (KORUS-AQ) campaign over Seoul, to demonstrate the chemical feedback of NO2 on the formation of HCHO is a controlling factor for the transition line between NOx-sensitive and NOx-saturated regimes. A fixed value (~2.7) of the ratio of the chemical loss of NOx (LNOx) to the chemical loss of HO2+RO2 (LROx) perceptibly differentiates the regimes. Following this value, data points with a ratio of HCHO/NO2 less than 1 can be safely classified as NOx-saturated regime, whereas points with ratios between 1 and 4 fall into one or the other regime. We attribute this mainly to the HCHO-NO2 chemical relationship causing the transition line to occur at larger (smaller) HCHO/NO2 ratios in VOC-rich (VOC-poor) environments. We then redefine the transition line to LNOx/LROx~2.7 that accounts for the HCHO-NO2 chemical relationship leading to HCHO = 3.7 × (NO2 – 1.14 × 1016 molec.cm−2). Although the revised formula is locally calibrated (i.e., requires for readjustment for other regions), its mathematical format removes the need for having a wide range of thresholds used in HCHO/NO2 ratios that is a result of the chemical feedback. Therefore, to be able to properly take the chemical feedback into consideration, the use of HCHO = a × (NO2 – b) formula should be preferred to the ratio in future works. We then use the Geostationary Trace gas and Aerosol Sensor Optimization (GeoTASO) airborne instrument to study O3 sensitivity in Seoul. The unprecedented spatial (250 × 250 m2) and temporal (~every 2 h) resolutions of HCHO and NO2 observations form the sensor enhance our understanding of P(O3) in Seoul; rather than providing a crude label for the entire city, more in-depth variabilities in chemical regimes are observed that should be able to inform mitigation strategies correspondingly.
Keywords	aerosols ; air quality ; atmospheric chemistry ; formaldehyde ; models ; nitrites ; nitrogen dioxide ; ozone ; photochemistry ; remote sensing ; volatile organic compounds
Language	English
Dates of publication	2020-0301
Publishing place	Elsevier Ltd
Document type	Article
ZDB-ID	216368-8
ISSN	0004-6981 ; 1352-2310
ISSN	0004-6981 ; 1352-2310
DOI	10.1016/j.atmosenv.2020.117341
Database	NAL-Catalogue (AGRICOLA)

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Book ; Online: Methane retrieval from MethaneAIR using the CO2 Proxy Approach

eISSN:

A demonstration for the upcoming MethaneSAT mission

2023

Abstract: Reducing methane (CH 4 ) emissions from the oil and gas (O&G) sector is key to mitigating climate change in the near-term. MethaneSAT is an upcoming satellite mission designed to monitor basin-wide O&G emissions globally, providing estimates of emission ... ...

Abstract	Reducing methane (CH 4 ) emissions from the oil and gas (O&G) sector is key to mitigating climate change in the near-term. MethaneSAT is an upcoming satellite mission designed to monitor basin-wide O&G emissions globally, providing estimates of emission rates and helping identify the underlying processes leading to methane release to the atmosphere. MethaneSAT data will help advocacy and policy efforts to help track methane reduction commitments and targets made by countries and industry. Here we introduce the CH 4 retrieval algorithm for MethaneSAT based on the CO 2 proxy method. We apply the algorithm to observations from the maiden campaign of MethaneAIR, an airborne precursor to the satellite with similar instrument specifications. The campaign was conducted during winter 2019 and summer 2021 over three major US oil and gas basins. Analysis of the MethaneAIR data shows that measurement precision is typically better than 2 % for 20 × 20 m 2 pixel resolution, with no strong dependence on geophysical variables such as surface reflectance. We show that detector focus drifts over the course of each flight likely due to thermal gradients that develop across the optical bench. The impacts of this drift on retrieved CH 4 can mostly be mitigated by including a parameter that squeezes the laboratory tabulated instrument spectral response function in the spectral fit. Validation against coincident EM27/SUN retrievals shows that MethaneAIR values are generally within 1 %. MethaneAIR retrievals were also intercompared with those of TROPOMI; the latitudinal gradients for the two datasets are in good agreement, with a 2.5 ppb mean bias between instruments. We evaluate the accuracy of MethaneAIR estimates of point source emissions using observations made over the Permian O&G basin, based on the integrated mass enhancement approach coupled with a plume-masking algorithm based on total variational denoising. We estimate that the median point source detection threshold is 100–150 kg h −1 at the aircraft’s nominal ...
Subject code	333
Language	English
Publishing date	2023-10-06
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Book ; Online: Methane point source quantification using MethaneAIR

Chulakadabba, Apisada / Sargent, Maryann / Lauvaux, Thomas / Benmergui, Joshua S. / Franklin, Jonathan E. / Chan Miller, Christopher / Wilzewski, Jonas S. / Roche, Sébastien / Conway, Eamon / Souri, Amir H. / Sun, Kang / Luo, Bingkun / Hawthrone, Jacob / Samra, Jenna / Daube, Bruce C. / Liu, Xiong / Chance, Kelly / Li, Yang / Gautam, Ritesh /

Omara, Mark / Rutherford, Jeff S. / Sherwin, Evan D. / Brandt, Adam / Wofsy, Steven C.

eISSN: 1867-8548

a new airborne imaging spectrometer

2023

Abstract: The MethaneSAT satellite instrument and its aircraft precursor, MethaneAIR, are imaging spectrometers designed to measure methane concentrations with wide spatial coverage, fine spatial resolution, and high precision compared to currently deployed remote ...

Abstract	The MethaneSAT satellite instrument and its aircraft precursor, MethaneAIR, are imaging spectrometers designed to measure methane concentrations with wide spatial coverage, fine spatial resolution, and high precision compared to currently deployed remote sensing instruments. At 12 960 m cruise altitude above ground (13 850 m above sea level), MethaneAIR datasets have a 4.5 km swath gridded to 10 m × 10 m pixels with 17–20 ppb standard deviation on a flat scene. MethaneAIR was deployed in the summer of 2021 in the Permian Basin to test the accuracy of the retrieved methane concentrations and emission rates using the algorithms developed for MethaneSAT. We report here point source emissions obtained during a single-blind volume-controlled release experiment, using two methods. (1) The modified integrated mass enhancement (mIME) method estimates emission rates using the total mass enhancement of methane in an observed plume combined with winds obtained from Weather Research Forecast driven by High-Resolution Rapid Refresh meteorological data in Large Eddy Simulations mode (WRF-LES-HRRR). WRF-LES-HRRR simulates winds in stochastic eddy-scale (100–1000 m) variability, which is particularly important for low-wind conditions and informing the error budget. The mIME can estimate emission rates of plumes of any size that are detectable by MethaneAIR. (2) The divergence integral (DI) method applies Gauss's theorem to estimate the flux divergence fields through a series of closed surfaces enclosing the sources. The set of boxes grows from the upwind side of the plume through the core of each plume and downwind. No selection of inflow concentration, as used in the mIME, is required. The DI approach can efﬁciently determine ﬂuxes from large sources and clusters of sources but cannot resolve small point emissions. These methods account for the effects of eddy-scale variation in different ways: the DI averages across many eddies, whereas the mIME re-samples many eddies from the LES simulation. The DI directly uses HRRR winds, ...
Subject code	333
Language	English
Publishing date	2023-12-01
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Book ; Online: Methane Point Source Quantification Using MethaneAIR

Omara, Mark / Rutherford, Jeff S. / Sherwin, Evan D. / Brandt, Adam / Wofsy, Steven C.

eISSN:

A New Airborne Imaging Spectrometer

2023

Abstract	The MethaneSAT satellite instrument and its aircraft precursor, MethaneAIR, are imaging spectrometers designed to measure methane concentrations with wide spatial coverage, fine spatial resolution, and high precision compared to currently deployed remote sensing instruments. At 12 960 m cruise altitude above ground (13 850 m above sea level), MethaneAIR datasets have a 4.5 km swath gridded to 10 m × 10 m pixels with 17–20 ppb standard deviation on a flat scene. MethaneAIR was deployed in the summer of 2021 in the Permian Basin to test the accuracy of the retrieved methane concentrations and emission rates using the algorithms developed for MethaneSAT. We report here point source emissions obtained during a single-blind volume-controlled release experiment, using two methods. (1) The modified integrated mass enhancement (mIME) method estimates emission rates using the total mass enhancement of methane in an observed plume combined with winds obtained from Weather Research Forecast driven by High-Resolution Rapid Refresh meteorological data in Large Eddy Simulations mode (WRF-LES-HRRR). WRF-LES-HRRR simulates winds in stochastic eddy-scale (100–1000 m) variability, which is particularly important for low-wind conditions and informing the error budget. The mIME can estimate emission rates of plumes of any size that are detectable by MethaneAIR. (2) The divergence integral (DI) method applies Gauss's theorem to estimate the flux divergence fields through a series of closed surfaces enclosing the sources. The set of boxes grows from the upwind side of the plume through the core of each plume and downwind. No selection of inflow concentration, as used in the mIME, is required. The DI approach can efﬁciently determine ﬂuxes from large sources and clusters of sources but cannot resolve small point emissions. These methods account for the effects of eddy-scale variation in different ways: the DI averages across many eddies, whereas the mIME re-samples many eddies from the LES simulation. The DI directly uses HRRR winds, ...
Subject code	333
Language	English
Publishing date	2023-12-01
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Book ; Online: Hotspot of glyoxal over the Pearl River delta seen from the OMI satellite instrument

Chan Miller, Christopher / Jacob, Daniel J. / González Abad, Gonzalo / Chance, Kelly

eISSN: 1680-7324

implications for emissions of aromatic hydrocarbons

2016

Abstract: The Pearl River delta (PRD) is a densely populated hub of industrial activity located in southern China. OMI (Ozone Monitoring Instrument) satellite observations reveal a large hotspot of glyoxal (CHOCHO) over the PRD that is almost twice as large as any ...

Abstract	The Pearl River delta (PRD) is a densely populated hub of industrial activity located in southern China. OMI (Ozone Monitoring Instrument) satellite observations reveal a large hotspot of glyoxal (CHOCHO) over the PRD that is almost twice as large as any other in Asia. Formaldehyde (HCHO) and NO 2 observed by OMI are also high in the PRD but no more than in other urban/industrial areas of China. The CHOCHO hotspot over the PRD can be explained by industrial paint and solvent emissions of aromatic volatile organic compounds (VOCs), with toluene being a dominant contributor. By contrast, HCHO in the PRD originates mostly from VOCs emitted by combustion (principally vehicles). By applying a plume transport model to wind-segregated OMI data, we show that the CHOCHO and HCHO enhancements over the PRD observed by OMI are consistent with current VOC emission inventories. Prior work using CHOCHO retrievals from the SCIAMACHY satellite instrument suggested that emission inventories for aromatic VOCs in the PRD were too low by a factor of 10–20; we attribute this result in part to bias in the SCIAMACHY data and in part to underestimated CHOCHO yields from oxidation of aromatics. Our work points to the importance of better understanding CHOCHO yields from the oxidation of aromatics in order to interpret space-based CHOCHO observations in polluted environments.
Subject code	551
Language	English
Publishing date	2016-04-13
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Book ; Online: Validation of satellite formaldehyde (HCHO) retrievals using observations from 12 aircraft campaigns

Zhu, Lei / González Abad, Gonzalo / Nowlan, Caroline R. / Chan Miller, Christopher / Chance, Kelly / Apel, Eric C. / DiGangi, Joshua P. / Fried, Alan / Hanisco, Thomas F. / Hornbrook, Rebecca S. / Hu, Lu / Kaiser, Jennifer / Keutsch, Frank N. / Permar, Wade / Clair, Jason M. / Wolfe, Glenn M.

eISSN: 1680-7324

2020

Abstract: Formaldehyde (HCHO) has been measured from space for more than two decades. Owing to its short atmospheric lifetime, satellite HCHO data are used widely as a proxy of volatile organic compounds (VOCs; please refer to Appendix A for abbreviations and ... ...

Abstract	Formaldehyde (HCHO) has been measured from space for more than two decades. Owing to its short atmospheric lifetime, satellite HCHO data are used widely as a proxy of volatile organic compounds (VOCs; please refer to Appendix A for abbreviations and acronyms), providing constraints on underlying emissions and chemistry. However, satellite HCHO products from different satellite sensors using different algorithms have received little validation so far. The accuracy and consistency of HCHO retrievals remain largely unclear. Here we develop a global validation platform for satellite HCHO retrievals using in situ observations from 12 aircraft campaigns with a chemical transport model (GEOS-Chem) as the intercomparison method. Application to the NASA operational OMI HCHO product indicates slight biases (−30.9 % to +16.0 %) under high-HCHO conditions partially caused by a priori shape factors used in the retrievals, while high biases (+113.9 % to +194.6 %) under low-HCHO conditions due mainly to slant column fitting and radiance reference sector correction. By providing quick assessment to systematic biases in satellite products over large domains, the platform facilitates, in an iterative process, optimization of retrieval settings and the minimization of retrieval biases. It is also complementary to localized validation efforts based on ground observations and aircraft spirals.
Subject code	551
Language	English
Publishing date	2020-01-13
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Book ; Online: Validation of satellite formaldehyde (HCHO) retrievals using observations from 12 aircraft campaigns

eISSN: 1680-7324

2020

Abstract: Formaldehyde (HCHO) has been measured from space for more than 2 decades. Owing to its short atmospheric lifetime, satellite HCHO data are used widely as a proxy of volatile organic compounds (VOCs; please refer to Appendix A for abbreviations and ... ...

Abstract	Formaldehyde (HCHO) has been measured from space for more than 2 decades. Owing to its short atmospheric lifetime, satellite HCHO data are used widely as a proxy of volatile organic compounds (VOCs; please refer to Appendix A for abbreviations and acronyms), providing constraints on underlying emissions and chemistry. However, satellite HCHO products from different satellite sensors using different algorithms have received little validation so far. The accuracy and consistency of HCHO retrievals remain largely unclear. Here we develop a validation platform for satellite HCHO retrievals using in situ observations from 12 aircraft campaigns with a chemical transport model (GEOS-Chem) as the intercomparison method. Application to the NASA operational OMI HCHO product indicates negative biases ( −44.5 % to −21.7 %) under high-HCHO conditions, while it indicates high biases ( +66.1 % to +112.1 %) under low-HCHO conditions. Under both conditions, HCHO a priori vertical profiles are likely not the main driver of the biases. By providing quick assessment of systematic biases in satellite products over large domains, the platform facilitates, in an iterative process, optimization of retrieval settings and the minimization of retrieval biases. It is also complementary to localized validation efforts based on ground observations and aircraft spirals.
Subject code	551
Language	English
Publishing date	2020-10-29
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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Book ; Online: Adjoint inversion of Chinese non-methane volatile organic compound emissions using space-based observations of formaldehyde and glyoxal

Cao, Hansen / Fu, Tzung-May / Zhang, Lin / Henze, Daven K. / Chan Miller, Christopher / Lerot, Christophe / González Abad, Gonzalo / Smedt, Isabelle / Zhang, Qiang / Roozendael, Michel / Chance, Kelly / Li, Jie / Zheng, Junyu / Zhao, Yuanhong

eISSN: 1680-7324

2018

Abstract: We used the GEOS-Chem model and its adjoint to quantify Chinese non-methane volatile organic compound (NMVOC) emissions for the year 2007, using the vertical column concentrations of formaldehyde and glyoxal observed by the Global Ozone Monitoring ... ...

Abstract	We used the GEOS-Chem model and its adjoint to quantify Chinese non-methane volatile organic compound (NMVOC) emissions for the year 2007, using the vertical column concentrations of formaldehyde and glyoxal observed by the Global Ozone Monitoring Experiment-2A (GOME-2A) instrument and the Ozone Monitoring Instrument (OMI) as constraints. We conducted a series of inversion experiments using different combinations of satellite observations to explore the impacts on top-down emission estimates due to different satellite retrievals. Our top-down estimates for Chinese annual total NMVOC emission was 23.4 to 35.4 (average 30.8) Tg C y −1 , including 13.5 to 19.7 (average 17.0) Tg C y −1 from anthropogenic sources, 8.9 to 14.8 (average 12.6) Tg C y −1 from biogenic sources, and 1.1 to 1.5 (average 1.2) Tg C y −1 from biomass burning. In comparison, the most widely-used bottom-up estimate for Chinese annual total NMVOC emission was 27.4 Tg C y −1 , including 15.5 Tg C y −1 from anthropogenic sources, 10.8 Tg C y −1 from biogenic sources, and 1.1 Tg C y −1 from biomass burning. The simultaneous use of glyoxal and formaldehyde observations helped distinguish the NMVOC species from different sources and was essential in constraining anthropogenic emissions. Our four inversions consistently showed that the emissions of Chinese anthropogenic NMVOC precursors of glyoxal were larger than the a priori estimates. Our top-down estimates for the Chinese annual emission of anthropogenic aromatics (benzene, toluene, and xylene) ranged from 5.0 to 7.3 Tg C y −1 , 2 % to 49 % larger than the estimate of the bottom-up inventory (4.9 Tg C y −1 ). Model simulations using the average of our top-down NMVOC emission estimates showed that surface afternoon ozone concentrations over northern and central China increased 5–12 ppb in June and decreased 5–13 ppb in December relative to the simulations using the a priori emissions and were in better agreement with measurements. We concluded that the satellite observations of glyoxal and formaldehyde together provided quantitative constraints on the emissions and source types of NMVOCs over China and improved our understanding on regional chemistry.
Subject code	333
Language	English
Publishing date	2018-01-15
Publishing country	de
Document type	Book ; Online
Database	BASE - Bielefeld Academic Search Engine (life sciences selection)

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