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- ItemPhonon-Polaritonic Bowtie Nanoantennas: Controlling Infrared Thermal Radiation at the Nanoscale(Washington, DC : ACS Publications, 2017) Wang, Tao; Li, Peining; Chigrin, Dmitry N.; Giles, Alexander J.; Bezares, Francisco J.; Glembocki, Orest J.; Caldwell, Joshua D.; Taubner, ThomasA conventional thermal emitter exhibits a broad emission spectrum with a peak wavelength depending upon the operation temperature. Recently, narrowband thermal emission was realized with periodic gratings or single microstructures of polar crystals supporting distinct optical modes. Here, we exploit the coupling of adjacent phonon-polaritonic nanostructures, demonstrating experimentally that the nanometer-scale gaps can control the thermal emission frequency while retaining emission line widths as narrow as 10 cm-1. This was achieved by using deeply subdiffractional bowtie-shaped silicon carbide nanoantennas. Infrared far-field reflectance spectroscopy, near-field optical nanoimaging, and full-wave electromagnetic simulations were employed to prove that the thermal emission originates from strongly localized surface phonon-polariton resonances of nanoantenna structures. The observed narrow emission line widths and exceptionally small modal volumes provide new opportunities for the user-design of near- and far-field radiation patterns for advancements in infrared spectroscopy, sensing, signaling, communications, coherent thermal emission, and infrared photodetection. © 2017 American Chemical Society.
- ItemThiophene-Based Conjugated Acetylenic Polymers with Dual Active Sites for Efficient Co-Catalyst-Free Photoelectrochemical Water Reduction in Alkaline Medium(Weinheim : Wiley-VCH, 2021) Borrelli, Mino; Querebillo, Christine Joy; Pastoetter, Dominik L.; Wang, Tao; Milani, Alberto; Casari, Carlo; Khoa Ly, Hoang; He, Fan; Hou, Yang; Neumann, Christof; Turchanin, Andrey; Sun, Hanjun; Weidinger, Inez M.; Feng, XinliangAlthough being attractive materials for photoelectrochemical hydrogen evolution reaction (PEC HER) under neutral or acidic conditions, conjugated polymers still show poor PEC HER performance in alkaline medium due to the lack of water dissociation sites. Herein, we demonstrate that tailoring the polymer skeleton from poly(diethynylthieno[3,2-b]thiophene) (pDET) to poly(2,6-diethynylbenzo[1,2-b:4,5-b′]dithiophene (pBDT) and poly(diethynyldithieno[3,2-b:2′,3′-d]thiophene) (pDTT) in conjugated acetylenic polymers (CAPs) introduces highly efficient active sites for water dissociation. As a result, pDTT and pBDT, grown on Cu substrate, demonstrate benchmark photocurrent densities of 170 μA cm−2 and 120 μA cm−2 (at 0.3 V vs. RHE; pH 13), which are 4.2 and 3 times higher than that of pDET, respectively. Moreover, by combining DFT calculations and electrochemical operando resonance Raman spectroscopy, we propose that the electron-enriched Cβ of the outer thiophene rings of pDTT are the water dissociation active sites, while the −C≡C− bonds function as the active sites for hydrogen evolution. © 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH
- ItemThe acidity of atmospheric particles and clouds(Katlenburg-Lindau : EGU, 2020) Pye, Havala O.T.; Nenes, Athanasios; Alexander, Becky; Ault, Andrew P.; Barth, Mary C.; Clegg, Simon L.; Collett Jr, Jeffrey L.; Fahey, Kathleen M.; Hennigan, Christopher J.; Herrmann, Hartmut; Kanakidou, Maria; Kelly, James T.; Ku, I-Ting; McNeill, V. Faye; Riemer, Nicole; Schaefer, Thomas; Shi, Guoliang; Tilgner, Andreas; Walker, John T.; Wang, Tao; Weber, Rodney; Xing, Jia; Zaveri, Rahul A.; Zuend, AndreasAcidity, defined as pH, is a central component of aqueous chemistry. In the atmosphere, the acidity of condensed phases (aerosol particles, cloud water, and fog droplets) governs the phase partitioning of semivolatile gases such as HNO3, NH3, HCl, and organic acids and bases as well as chemical reaction rates. It has implications for the atmospheric lifetime of pollutants, deposition, and human health. Despite its fundamental role in atmospheric processes, only recently has this field seen a growth in the number of studies on particle acidity. Even with this growth, many fine-particle pH estimates must be based on thermodynamic model calculations since no operational techniques exist for direct measurements. Current information indicates acidic fine particles are ubiquitous, but observationally constrained pH estimates are limited in spatial and temporal coverage. Clouds and fogs are also generally acidic, but to a lesser degree than particles, and have a range of pH that is quite sensitive to anthropogenic emissions of sulfur and nitrogen oxides, as well as ambient ammonia. Historical measurements indicate that cloud and fog droplet pH has changed in recent decades in response to controls on anthropogenic emissions, while the limited trend data for aerosol particles indicate acidity may be relatively constant due to the semivolatile nature of the key acids and bases and buffering in particles. This paper reviews and synthesizes the current state of knowledge on the acidity of atmospheric condensed phases, specifically particles and cloud droplets. It includes recommendations for estimating acidity and pH, standard nomenclature, a synthesis of current pH estimates based on observations, and new model calculations on the local and global scale. © 2020 Author(s).
- ItemSingle-photon emission from isolated monolayer islands of InGaN(London : Nature Publishing Group, 2020) Sun, Xiaoxiao; Wang, Ping; Wang, Tao; Chen, Ling; Chen, Zhaoying; Gao, Kang; Aoki, Tomoyuki; Li, Mo; Zhang, Jian; Schulz, Tobias; Albrecht, Martin; Ge, Weikun; Arakawa, Yasuhiko; Shen, Bo; Holmes, Mark; Wang, XinqiangWe identify and characterize a novel type of quantum emitter formed from InGaN monolayer islands grown using molecular beam epitaxy and further isolated via the fabrication of an array of nanopillar structures. Detailed optical analysis of the characteristic emission spectrum from the monolayer islands is performed, and the main transmission is shown to act as a bright, stable, and fast single-photon emitter with a wavelength of ~400 nm. © 2020, The Author(s).
- ItemThe 2020 UV emitter roadmap(Bristol : IOP Publ., 2020) Amano, Hiroshi; Collazo, Ramón; De Santi, Carlo; Einfeldt, Sven; Funato, Mitsuru; Glaab, Johannes; Hagedorn, Sylvia; Hirano, Akira; Hirayama, Hideki; Ishii, Ryota; Kashima, Yukio; Kawakami, Yoichi; Kirste, Ronny; Kneissl, Michael; Martin, Robert; Mehnke, Frank; Meneghini, Matteo; Ougazzaden, Abdallah; Parbrook, Peter J.; Rajan, Siddharth; Reddy, Pramod; Römer, Friedhard; Friedhard, Jan; Sarkar, Biplab; Scholz, Ferdinand; Schowalter, Leo J; Shields, Philip; Sitar, Zlatko; Sulmoni, Luca; Wang, Tao; Wernicke, Tim; Weyers, Markus; Witzigmann, Bernd; Wu, Yuh-Renn; Wunderer, Thomas; Zhang, YueweiSolid state UV emitters have many advantages over conventional UV sources. The (Al,In,Ga)N material system is best suited to produce LEDs and laser diodes from 400 nm down to 210 nm - due to its large and tuneable direct band gap, n- and p-doping capability up to the largest bandgap material AlN and a growth and fabrication technology compatible with the current visible InGaN-based LED production. However AlGaN based UV-emitters still suffer from numerous challenges compared to their visible counterparts that become most obvious by consideration of their light output power, operation voltage and long term stability. Most of these challenges are related to the large bandgap of the materials. However, the development since the first realization of UV electroluminescence in the 1970s shows that an improvement in understanding and technology allows the performance of UV emitters to be pushed far beyond the current state. One example is the very recent realization of edge emitting laser diodes emitting in the UVC at 271.8 nm and in the UVB spectral range at 298 nm. This roadmap summarizes the current state of the art for the most important aspects of UV emitters, their challenges and provides an outlook for future developments. © 2020 IOP Publishing Ltd.
- ItemEvolution of Ozone Pollution in China: What Track Will It Follow?(Columbus, Ohio : American Chemical Society, 2022) Guo, Jia; Zhang, Xiaoshan; Gao, Yi; Wang, Zhangwei; Zhang, Meigen; Xue, Wenbo; Herrmann, Hartmut; Brasseur, Guy Pierre; Wang, Tao; Wang, ZheIncreasing surface ozone (O3) concentrations has emerged as a key air pollution problem in many urban regions worldwide in the last decade. A longstanding major issue in tackling ozone pollution is the identification of the O3 formation regime and its sensitivity to precursor emissions. In this work, we propose a new transformed empirical kinetic modeling approach (EKMA) to diagnose the O3 formation regime using regulatory O3 and NO2 observation datasets, which are easily accessible. We demonstrate that mapping of monitored O3 and NO2 data on the modeled regional O3-NO2 relationship diagram can illustrate the ozone formation regime and historical evolution of O3 precursors of the region. By applying this new approach, we show that for most urban regions of China, the O3 formation is currently associated with a volatile organic compound (VOC)-limited regime, which is located within the zone of daytime-produced O3 (DPO3) to an 8h-NO2 concentration ratio below 8.3 ([DPO3]/[8h-NO2] ≤ 8.3). The ozone production and controlling effects of VOCs and NOx in different cities of China were compared according to their historical O3-NO2 evolution routes. The approach developed herein may have broad application potential for evaluating the efficiency of precursor controls and further mitigating O3 pollution, in particular, for regions where comprehensive photochemical studies are unavailable.
- ItemSignificant concentrations of nitryl chloride sustained in the morning: Investigations of the causes and impacts on ozone production in a polluted region of northern China(München : European Geopyhsical Union, 2016) Tham, Yee Jun; Wang, Zhe; Li, Qinyi; Yun, Hui; Wang, Weihao; Wang, Xinfeng; Xue, Likun; Lu, Keding; Ma, Nan; Bohn, Birger; Li, Xin; Kecorius, Simonas; Größ, Johannes; Shao, Min; Wiedensohler, Alfred; Zhang, Yuanhang; Wang, TaoNitryl chloride (ClNO2) is a dominant source of chlorine radical in polluted environment, and can significantly affect the atmospheric oxidative chemistry. However, the abundance of ClNO2 and its exact role are not fully understood under different environmental conditions. During the summer of 2014, we deployed a chemical ionization mass spectrometer to measure ClNO2 and dinitrogen pentoxide (N2O5) at a rural site in the polluted North China Plain. Elevated mixing ratios of ClNO2 (> 350 pptv) were observed at most of the nights with low levels of N2O5 (< 200 pptv). The highest ClNO2 mixing ratio of 2070 pptv (1 min average) was observed in a plume from a megacity (Tianjin), and was characterized with a faster N2O5 heterogeneous loss rate and ClNO2 production rate compared to average conditions. The abundant ClNO2 concentration kept increasing even after sunrise, and reached a peak 4 h later. Such highly sustained ClNO2 peaks after sunrise are discrepant from the previously observed typical diurnal pattern. Meteorological and chemical analysis shows that the sustained ClNO2 morning peaks are caused by significant ClNO2 production in the residual layer at night followed by downward mixing after breakup of the nocturnal inversion layer in the morning. We estimated that ∼ 1.7–4.0 ppbv of ClNO2 would exist in the residual layer in order to maintain the observed morning ClNO2 peaks at the surface site. Observation-based box model analysis show that photolysis of ClNO2 produced chlorine radical with a rate up to 1.12 ppbv h−1, accounting for 10–30 % of primary ROx production in the morning hours. The perturbation in total radical production leads to an increase of integrated daytime net ozone production by 3 % (4.3 ppbv) on average, and with a larger increase of 13 % (11 ppbv) in megacity outflow that was characterized with higher ClNO2 and a relatively lower oxygenated hydrocarbon (OVOC) to non-methane hydrocarbon (NMHC) ratio.
- ItemHeterogeneous N2O5 uptake coefficient and production yield of ClNO2 in polluted northern China: Roles of aerosol water content and chemical composition(Katlenburg-Lindau : EGU, 2018) Tham, Yee Jun; Wang, Zhe; Li, Qinyi; Wang, Weihao; Wang, Xinfeng; Lu, Keding; Ma, Nan; Yan, Chao; Kecorius, Simonas; Wiedensohler, Alfred; Zhang, Yuanhang; Wang, TaoHeterogeneous uptake of dinitrogen pentoxide (N2O5) and production of nitryl chloride (ClNO2) are important nocturnal atmospheric processes that have significant implications for the production of secondary pollutants. However, the understanding of N2O5 uptake processes and ClNO2 production remains limited, especially in China. This study presents a field investigation of the N2O5 heterogeneous uptake coefficient (γ(N2O5)) and ClNO2 production yield (ϕ) in a polluted area of northern China during the summer of 2014. The N2O5 uptake coefficient and ClNO2 yield were estimated by using the simultaneously measured ClNO2 and total nitrate in 10 selected cases, which have concurrent increases in the ClNO2 and nitrate concentrations and relatively stable environmental conditions. The determined γ(N2O5) and ϕ values varied greatly, with an average of 0.022 for γ(N2O5) (±0.012, standard deviation) and 0.34 for ϕ (±0.28, standard deviation). The variations in γ(N2O5) could not be fully explained by the previously derived parameterizations of N2O5 uptake that consider nitrate, chloride, and the organic coating. Heterogeneous uptake of N2O5 was found to have a strong positive dependence on the relative humidity and aerosol water content. This result suggests that the heterogeneous uptake of N2O5 in Wangdu is governed mainly by the amount of water in the aerosol, and is strongly water limited, which is different from most of the field observations in the US and Europe. The ClNO2 yield estimated from the parameterization was also overestimated comparing to that derived from the observation. The observation-derived ϕ showed a decreasing trend with an increasing ratio of acetonitrile to carbon monoxide, an indicator of biomass burning emissions, which suggests a possible suppressive effect on the production yield of ClNO2 in the plumes influenced by biomass burning in this region. The findings of this study illustrate the need to improve our understanding and to parameterize the key factors for γ(N2O5) and ϕ to accurately assess photochemical and haze pollution.
- ItemChemical characteristics of cloud water and the impacts on aerosol properties at a subtropical mountain site in Hong Kong SAR(Katlenburg-Lindau : EGU, 2020) Li, Tao; Wang, Zhe; Wang, Yaru; Wu, Chen; Liang, Yiheng; Xia, Men; Yu, Chuan; Yun, Hui; Wang, Weihao; Wang, Yan; Guo, Jia; Herrmann, Hartmut; Wang, TaoTo investigate the cloud water chemistry and the effects of cloud processing on aerosol properties, comprehensive field observations of cloud water, aerosols, and gasphase species were conducted at a mountaintop site in Hong Kong SAR in October and November 2016. The chemical composition of cloud water including water-soluble ions, dissolved organic matter (DOM), carbonyl compounds (refer to aldehydes and acetone), carboxylic acids, and trace metals was quantified. The measured cloud water was very acidic with a mean pH of 3.63, as the ammonium (174 μeq L-1) was insufficient for neutralizing the dominant sulfate (231 μeq L-1) and nitrate (160 μeq L-1). Substantial DOM (9.3 mgC L-1) was found in cloud water, with carbonyl compounds and carboxylic acids accounting for 18% and 6% in carbon molar concentrations, respectively. Different from previous observations, concentrations of methylglyoxal (19.1 μM; μM is equal to μmol L-1) and glyoxal (6.72 μM) were higher than that of formaldehyde (1.59 μM). The partitioning of carbonyls between cloud water and the gas phase was also investigated. The measured aqueous fractions of dicarbonyls were comparable to the theoretical estimations, while significant aqueous-phase supersaturation was found for less soluble monocarbonyls. Both organics and sulfate were significantly produced in cloud water, and the aqueous formation of organics was more enhanced by photochemistry and under less acidic conditions. Moreover, elevated sulfate and organics were measured in the cloudprocessed aerosols, and they were expected to contribute largely to the increase in droplet-mode aerosol mass fraction. This study demonstrates the significant role of clouds in altering the chemical compositions and physical properties of aerosols via scavenging and aqueous chemical processing, providing valuable information about gas-cloud-aerosol interactions in subtropical and coastal regions. © 2020 Author(s). This work is distributed under the Creative Commons Attribution 4.0 License.