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We investigate regional sources contributing to CO during the Korea United States Air Quality (KORUS-AQ) campaign conducted over Korea (1 May to 10 June 2016) using 17 tagged CO simulations from the Community Atmosphere Model with chemistry (CAM-chem). The simulations use three spatial resolutions, three anthropogenic emission inventories, two meteorological fields, and nine emission scenarios. These simulations are evaluated against measurements from the DC-8 aircraft and Measurements Of Pollution In The Troposphere (MOPITT). Results show that simulations using bottom-up emissions are consistently lower (bias: −34 to −39%) and poorer performing (Taylor skill: 0.38–0.61) than simulations using alternative anthropogenic emissions (bias: −6 to −33%; Taylor skill: 0.48–0.86), particularly for enhanced Asian CO and volatile organic compound (VOC) emission scenarios, suggesting underestimation in modeled CO background and emissions in the region. The ranges of source contributions to modeled CO along DC-8 aircraft from Korea and southern (90°E to 123°E, 20°N to 29°N), middle (90°E to 123°E, 29°N to 38.5°N), and northern (90°E to 131.5°E, 38.5°N to 45°N) East Asia (EA) are 6–13%, ~5%, 16–28%, and 9–18%, respectively. CO emissions from middle and northern EA can reach Korea via transport within the boundary layer, whereas those from southern EA are transported to Korea mainly through the free troposphere. Emission contributions from middle EA dominate during continental outflow events (29–51%), while Korean emissions play an overall more important role for ground sites (up to 25–49%) and plumes within the boundary layer (up to 25–44%) in Korea. Finally, comparisons with four other source contribution approaches (FLEXPART 9.1 back trajectory calculations driven by Weather Research and Forecasting (WRF) WRF inert tracer, China signature VOCs, and CO to CO2 enhancement ratios) show general consistency with CAM-chem.

Nitryl chloride (ClNO2) is a radical reservoir species that releases chlorine radicals upon photolysis. An integrated analysis of the impact of ClNO2 on regional photochemistry in the Seoul metropolitan area (SMA) during the Korea-United States Air Quality Study (KORUS-AQ) 2016 field campaign is presented. Comprehensive multiplatform observations were conducted aboard the NASA DC-8 and at two ground sites (Olympic Park, OP; Taehwa Research Forest, TRF), representing an urbanized area and a forested suburban region, respectively. Positive correlations between daytime Cl2 and ClNO2 were observed at both sites, the slope of which was dependent on O3 levels. The possible mechanisms are explored through box model simulations constrained with observations. The overall diurnal variations in ClNO2 at both sites appeared similar but the nighttime variations were systematically different. For about half of the observation days at the OP site the level of ClNO2 increased at sunset but rapidly decreased at around midnight. On the other hand, high levels were observed throughout the night at the TRF site. Significant levels of ClNO2 were observed at both sites for 4-5 h after sunrise. Airborne observations, box model calculations, and back-trajectory analysis consistently show that these high levels of ClNO2 in the morning are likely from vertical or horizontal transport of air masses from the west. Box model results show that chlorine-radical-initiated chemistry can impact the regional photochemistry by elevating net chemical production rates of ozone by 25% in the morning.

Abstract. Nitryl chloride (ClNO2) is a radical reservoir species that releases chlorine radicals upon photolysis. An integrated analysis of the impact of ClNO2 on regional photochemistry in the Seoul Metropolitan Area (SMA) during the Korean-United States-Air Quality (KORUS-AQ) 2016 field campaign is presented. Comprehensive multiplatform observations were conducted aboard the NASA DC-8 and at two ground sites (Olympic Park, OP; Taehwa Research Forest, TRF), representing an urbanized area and a forested region downwind, respectively. The overall diurnal variations of ClNO2 in both sites appeared similar but the night time variation were systematically different. For about half of the observation days at the OP site the level of ClNO2 increased at sunset but rapidly decreased at around midnight. On the other hand, high levels were sustained throughout the night at the TRF site. Significant levels of ClNO2 were sustained at both sites for 4–5 hours after sunrise. Airborne observations, box model calculations, and back trajectory analysis consistently show that this high levels of ClNO2 in the morning is likely due to the transport of air masses within the boundary layer. Box model results show that chlorine radical initiated chemistry can impact the regional photochemistry by elevating net ozone production rate up to ~ 25 % in the morning.

Photoinduced intermolecular charge transfer (PICT) determines the voltage loss in bulk heterojunction (BHJ) organic photovoltaics (OPVs), and this voltage loss can be minimized by inducing efficient PICT, which requires energy‐state matching between the donor and acceptor at the BHJ interfaces. Thus, both geometrically and energetically accessible delocalized state matching at the hot energy level is crucial for achieving efficient PICT. In this study, an effective method for quantifying the hot state matching of OPVs was developed. The degree of energy‐state matching between the electron donor and acceptor at BHJ interfaces was quantified using a mismatching factor (MF) calculated from the modified optical density of the BHJ. Furthermore, the correlation between the open‐circuit voltage (Voc) of the OPV device and energy‐state matching at the BHJ interface was investigated using the calculated MF. The OPVs with small absolute MF values exhibited high Voc values. This result clearly indicates that the energy‐state matching between the donor and acceptor is crucial for achieving a high Voc in OPVs. Because the MF indicates the degree of energy‐state matching, which is a critical factor for suppressing energy loss, it can be used to estimate the Voc loss in OPVs. [ABSTRACT FROM AUTHOR]

In the present study, we developed an effective encapsulation method for highly stable perovskite solar cells (PeSCs). By simultaneously introducing UV absorbers with biomimetic textures on the backside of the FTO substrate and a heat-extraction composite layer composed of reduced graphene oxide (rGO) and commercially available Norland Optical Adhesive (NOA) on the Au electrode, we successfully demonstrated highly efficient and stable PeSCs. The UV-absorbing layer with micro- and nano-hierarchical structures effectively cut UV light while increasing the transmittance of visible light, resulting in enhanced device stability without sacrificing the photocurrent caused by cutting the incident UV light. In addition, the introduction of a composite layer comprising rGO and NOA on the Au electrode offers superior protection, attributed to the hydrophobic nature of epoxy and the increased complexity of the oxygen or water diffusion pathway. Additionally, the outstanding thermal conductivity of rGO facilitated efficient heat dissipation through the encapsulation layer. The encapsulated PeSCs reproducibly maintained their performance during a long-term operation, even after a series of rigorous aging tests over 2 months. [ABSTRACT FROM AUTHOR]

Perovskite solar cells (PeSCs) using FAPbI3 perovskite films often exhibit unfavorable phase transitions and defect‐induced nonradiative interfacial recombination, resulting in considerable energy loss and impairing the performance of PeSCs in terms of efficiency, stability, and hysteresis. In this work, a facile interface engineering strategy to control the surface structure and energy‐level alignment of perovskite films by tailoring the interface between the FAPbI3 film and hole‐transporting layer using 4‐hydroxypicolinic acid (4HPA) is reported. According to density functional theory studies, 4HPA has prominent electron delocalization distribution properties that enable it to anchor to the perovskite film surface and facilitate charge transfer at the interface. By enabling multiple bonding interactions with the perovskite layer, including hydrogen bonds, PbO, and PbN dative bonds, 4HPA passivation significantly reduces the trap density and efficiently suppresses nonradiative recombination. The obtained perovskite films exhibit superior optoelectronic properties with improved crystallinity, pure α‐phase FAPbI3, and favorable energy band bending. Following this strategy, 4HPA post‐treatment PeSCs achieve a champion power conversion efficiency of 23.28% in 0.12 cm2 cells and 19.26% in 36 cm2 modules with excellent environmental and thermal stabilities. [ABSTRACT FROM AUTHOR]

In this study, organic thin‐film transistors (OTFTs) are investigated as a promising platform for cost‐effective, reconfigurable, and strong electronic physically unclonable functions (PUFs) for highly secure cryptography primitives. Simple spin‐casting of solution‐processable small‐molecule organic semiconductors forms unique and unclonable fingerprint thin films with randomly distributed polycrystalline structures ranging from nanoscale molecular orientations to microcrystalline orientations, which provides a stochastic entropy source of device‐to‐device variations for OTFT arrays. Blending organic semiconductors with polymer materials is a promising strategy to improve the reliability of OTFT‐based PUFs. Studies on the relationship between the phase‐separated polycrystalline microstructure of organic semiconductor/polymer blend films and PUF characteristics reveal that the 2D mosaic microcrystalline structure of organic semiconductors in the vertically phase‐separated trilayered structure enables the implementation of OTFT‐based PUFs that simultaneously satisfy the requirements of being unclonable and unpredictable, with reliable cryptographic properties. The inherent multiscale randomness of the crystalline structure allows random distribution in OTFT‐based PUFs even with various channel dimensions. The secret bit stream generated from the OTFT‐based PUF developed in this study is reconfigurable by simply changing the gate bias, demonstrating the potential to counter evolving security attack threats. [ABSTRACT FROM AUTHOR]