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    Photocurrent modelling and experimental confirmation for meteoric smoke particle detectors on board atmospheric sounding rockets
    (Katlenburg-Lindau : Copernicus, 2018-9-20) Giono, Gabriel; Strelnikov, Boris; Asmus, Heiner; Staszak, Tristan; Ivchenko, Nickolay; Lübken, Franz-Josef
    Characterising the photoelectron current induced by the Sun's UV radiation is crucial to ensure accurate daylight measurements from particle detectors. This article lays out the methodology used to address this problem in the case of the meteoric smoke particle detectors (MSPDs), developed by the Leibniz Institute of Atmospheric Physics in Kühlungsborn (IAP) and flown on board the PMWEs (Polar Mesosphere Winter Echoes) sounding rockets in April 2018. The methodology focuses on two complementary aspects: modelling and experimental measurements. A detailed model of the MSPD photocurrent was created based on the expected solar UV flux, the atmospheric UV absorption as a function of height by molecular oxygen and ozone, the photoelectric yield of the material coating the MSPD as a function of wavelength, the index of refraction of these materials as a function of wavelength and the angle of incidence of the illumination onto the MSPD. Due to its complex structure, composed of a central electrode shielded by two concentric grids, extensive ray-tracing calculations were conducted to obtain the incidence angles of the illumination on the central electrode, and this was done for various orientations of the MSPD in respect to the Sun. Results of the modelled photocurrent at different heights and for different materials, as well as for different orientations of the detector, are presented. As a pre-flight confirmation, the model was used to reproduce the experimental measurements conducted by Robertson et al. (2014) and agrees within an order of magnitude. An experimental setup for the calibration of the MSPD photocurrent is also presented. The photocurrent induced by the Lyman-alpha line from a deuterium lamp was recorded inside a vacuum chamber using a narrowband filter, while a UV-sensitive photodiode was used to monitor the UV flux. These measurements were compared with the model prediction, and also matched within an order of magnitude. Although precisely modelling the photocurrent is a challenging task, this article quantitatively improved the understanding of the photocurrent on the MSPD and discusses possible strategies to untangle the meteoric smoke particles (MSPs) current from the photocurrent recorded in-flight.
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    Intercomparison study and optical asphericity measurements of small ice particles in the CERN CLOUD experiment
    (Katlenburg-Lindau : Copernicus, 2017) Nichman, Leonid; Järvinen, Emma; Dorsey, James; Connolly, Paul; Duplissy, Jonathan; Fuchs, Claudia; Ignatius, Karoliina; Sengupta, Kamalika; Stratmann, Frank; Möhler, Ottmar; Schnaiter, Martin; Gallagher, Martin
    Optical probes are frequently used for the detection of microphysical cloud particle properties such as liquid and ice phase, size and morphology. These properties can eventually influence the angular light scattering properties of cirrus clouds as well as the growth and accretion mechanisms of single cloud particles. In this study we compare four commonly used optical probes to examine their response to small cloud particles of different phase and asphericity. Cloud simulation experiments were conducted at the Cosmics Leaving OUtdoor Droplets (CLOUD) chamber at European Organisation for Nuclear Research (CERN). The chamber was operated in a series of multi-step adiabatic expansions to produce growth and sublimation of ice particles at super- and subsaturated ice conditions and for initial temperatures of -30, -40 and -50°C. The experiments were performed for ice cloud formation via homogeneous ice nucleation. We report the optical observations of small ice particles in deep convection and in situ cirrus simulations. Ice crystal asphericity deduced from measurements of spatially resolved single particle light scattering patterns by the Particle Phase Discriminator mark 2 (PPD-2K, Karlsruhe edition) were compared with Cloud and Aerosol Spectrometer with Polarisation (CASPOL) measurements and image roundness captured by the 3View Cloud Particle Imager (3V-CPI). Averaged path light scattering properties of the simulated ice clouds were measured using the Scattering Intensity Measurements for the Optical detectioN of icE (SIMONE) and single particle scattering properties were measured by the CASPOL. We show the ambiguity of several optical measurements in ice fraction determination of homogeneously frozen ice in the case where sublimating quasi-spherical ice particles are present. Moreover, most of the instruments have difficulties of producing reliable ice fraction if small aspherical ice particles are present, and all of the instruments cannot separate perfectly spherical ice particles from supercooled droplets. Correlation analysis of bulk averaged path depolarisation measurements and single particle measurements of these clouds showed higher R2 values at high concentrations and small diameters, but these results require further confirmation. We find that none of these instruments were able to determine unambiguously the phase of the small particles. These results have implications for the interpretation of atmospheric measurements and parametrisations for modelling, particularly for low particle number concentration clouds.
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    New particle formation and sub-10nm size distribution measurements during the A-LIFE field experiment in Paphos, Cyprus
    (Katlenburg-Lindau : EGU, 2020) Brilke, Sophia; Fölker, Nikolaus; Kandler, Konrad; Müller, Thomas; Gong, Xianda; Peischl, Jeff; Weinzierl, Bernadett; Winkler, Paul M.
    Atmospheric particle size distributions were measured in Paphos, Cyprus, during the A-LIFE (absorbing aerosol layers in a changing climate: ageing, lifetime and dynamics) field experiment from 3 to 30 April 2017. The newly developed differential mobility analyser train (DMAtrain) was deployed for the first time in an atmospheric environment for the direct measurement of the nucleation mode size range between 1.8 and 10 nm diameter. The DMA-train set-up consists of seven size channels, of which five are set to fixed particle mobility diameters and two additional diameters are obtained by alternating voltage settings in one DMA every 10 s. In combination with a conventional mobility particle size spectrometer (MPSS) and an aerodynamic particle sizer (APS) the complete atmospheric aerosol size distribution from 1.8 nm to 10 μ m was covered. The focus of the A-LIFE study was to characterize new particle formation (NPF) in the eastern Mediterranean region at a measurement site with strong local pollution sources. The nearby Paphos airport was found to be a large emission source for nucleation mode particles, and we analysed the size distribution of the airport emission plumes at approximately 500 m from the main runway. The analysis yielded nine NPF events in 27 measurement days from the combined analysis of the DMAtrain, MPSS and trace gas monitors. Growth rate calculations were performed, and a size dependency of the initial growth rate (< 10 nm) was observed for one event case. Fast changes of the sub-10 nm size distribution on a timescale of a few minutes were captured by the DMA-train measurement during early particle growth and are discussed in a second event case. In two cases, particle formation and growth were detected in the nucleation mode size range which did not exceed the 10 nm threshold. This finding implies that NPF likely occurs more frequently than estimated from studies where the lower nanometre size regime is not covered by the size distribution measurements. © 2020 Author(s).
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    Experimental assessment of a micro-pulse lidar system in comparison with reference lidar measurements for aerosol optical properties retrieval
    (Katlenburg-Lindau : European Geosciences Union, 2021) Córdoba-Jabonero, Carmen; Ansmann, Albert; Jiménez, Cristofer; Baars, Holger; López-Cayuela, María-Ángeles; Engelmann, Ronny
    Simultaneous observations of a polarized micro-pulse lidar (P-MPL) system and two reference European Aerosol Research Lidar Network lidars running at the Leipzig site Germany, 51.4g gN, 12.4g gE; 125gmga.s.l.) were performed during a comprehensive 2-month field intercomparison campaign in summer 2019. An experimental assessment regarding both the overlap (OVP) correction of the P-MPL signal profiles and the volume linear depolarization ratio (VLDR) analysis, together with its impact on the retrieval of the aerosol optical properties, is achieved; the experimental procedure used is also described. The optimal lidar-specific OVP function is experimentally determined, highlighting that the one delivered by the P-MPL manufacturer cannot be used long. Among the OVP functions examined, the averaged function between those obtained from the comparison of the P-MPL observations with those of the other two reference lidars seems to be the best proxy at both near- and far-field ranges. In addition, the impact of the OVP function on the accuracy of the retrieved profiles of the total particle backscatter coefficient (PBC) and the particle linear depolarization ratio (PLDR) is examined. The VLDR profile is obtained and compared with that derived from the reference lidar, showing that it needs to be corrected by a small offset value with good accuracy. Once P-MPL measurements are optimally (OVP, VLDR) corrected, both the PBC and PLDR profiles can be accurately derived and are in good agreement with reference aerosol retrievals. Overall, as a systematic requirement for lidar systems, an adequate OVP function determination and VLDR testing analysis needs to be performed on a regular basis to correct the P-MPL measurements in order to derive suitable aerosol products. A dust event observed in Leipzig in June 2019 is used for illustration.
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    Polarization lidar: An extended three-signal calibration approach
    (Katlenburg-Lindau : Copernicus, 2019) Jimenez, Cristofer; Ansmann, Albert; Engelmann, Ronny; Haarig, Moritz; Schmidt, Jörg; Wandinger, Ulla
    We present a new formalism to calibrate a threesignal polarization lidar and to measure highly accurate height profiles of the volume linear depolarization ratios under realistic experimental conditions. The methodology considers elliptically polarized laser light, angular misalignment of the receiver unit with respect to the main polarization plane of the laser pulses, and cross talk among the receiver channels. A case study of a liquid-water cloud observation demonstrates the potential of the new technique. Long-term observations of the calibration parameters corroborate the robustness of the method and the long-term stability of the three-signal polarization lidar. A comparison with a second polarization lidar shows excellent agreement regarding the derived volume linear polarization ratios in different scenarios: A biomass burning smoke event throughout the troposphere and the lower stratosphere up to 16 km in height, a dust case, and also a cirrus cloud case. © Author(s) 2019.
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    Modelling winter organic aerosol at the European scale with CAMx: Evaluation and source apportionment with a VBS parameterization based on novel wood burning smog chamber experiments
    (Katlenburg-Lindau : EGU, 2017) Ciarelli, Giancarlo; Aksoyoglu, Sebnem; El Haddad, Imad; Bruns, Emily A.; Crippa, Monica; Poulain, Laurent; Äijälä, Mikko; Carbone, Samara; Freney, Evelyn; O'Dowd, Colin; Baltensperger, Urs; Prévôt, André S. H.
    We evaluated a modified VBS (volatility basis set) scheme to treat biomass-burning-like organic aerosol (BBOA) implemented in CAMx (Comprehensive Air Quality Model with extensions). The updated scheme was parameterized with novel wood combustion smog chamber experiments using a hybrid VBS framework which accounts for a mixture of wood burning organic aerosol precursors and their further functionalization and fragmentation in the atmosphere. The new scheme was evaluated for one of the winter EMEP intensive campaigns (February-March 2009) against aerosol mass spectrometer (AMS) measurements performed at 11 sites in Europe. We found a considerable improvement for the modelled organic aerosol (OA) mass compared to our previous model application with the mean fractional bias (MFB) reduced from -61 to -29 %. We performed model-based source apportionment studies and compared results against positive matrix factorization (PMF) analysis performed on OA AMS data. Both model and observations suggest that OA was mainly of secondary origin at almost all sites. Modelled secondary organic aerosol (SOA) contributions to total OA varied from 32 to 88% (with an average contribution of 62 %) and absolute concentrations were generally under-predicted. Modelled primary hydrocarbon-like organic aerosol (HOA) and primary biomass-burning-like aerosol (BBPOA) fractions contributed to a lesser extent (HOA from 3 to 30 %, and BBPOA from 1 to 39 %) with average contributions of 13 and 25 %, respectively. Modelled BBPOA fractions were found to represent 12 to 64% of the total residential-heating-related OA, with increasing contributions at stations located in the northern part of the domain. Source apportionment studies were performed to assess the contribution of residential and non-residential combustion precursors to the total SOA. Non-residential combustion and road transportation sector contributed about 30-40% to SOA formation (with increasing contributions at urban and near industrialized sites), whereas residential combustion (mainly related to wood burning) contributed to a larger extent, around 60-70 %. Contributions to OA from residential combustion precursors in different volatility ranges were also assessed: our results indicate that residential combustion gas-phase precursors in the semivolatile range (SVOC) contributed from 6 to 30 %, with higher contributions predicted at stations located in the southern part of the domain. On the other hand, the oxidation products of higher-volatility precursors (the sum of intermediate-volatility compounds (IVOCs) and volatile organic compounds (VOCs)) contribute from 15 to 38% with no specific gradient among the stations. Although the new parameterization leads to a better agreement between model results and observations, it still underpredicts the SOA fraction, suggesting that uncertainties in the new scheme and other sources and/or formation mechanisms remain to be elucidated. Moreover, a more detailed characterization of the semivolatile components of the emissions is needed.
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    Time-reversal symmetry breaking type-II Weyl state in YbMnBi2
    (London : Nature Publishing Group, 2019) Borisenko, S.; Evtushinsky, D.; Gibson, Q.; Yaresko, A.; Koepernik, K.; Kim, T.; Ali, M.; van den Brink, J.; Hoesch, M.; Fedorov, A.; Haubold, E.; Kushnirenko, Y.; Soldatov, I.; Schäfer, R.; Cava, R.J.
    Spectroscopic detection of Dirac and Weyl fermions in real materials is vital for both, promising applications and fundamental bridge between high-energy and condensed-matter physics. While the presence of Dirac and noncentrosymmetric Weyl fermions is well established in many materials, the magnetic Weyl semimetals still escape direct experimental detection. In order to find a time-reversal symmetry breaking Weyl state we design two materials and present here experimental and theoretical evidence of realization of such a state in one of them, YbMnBi2. We model the time-reversal symmetry breaking observed by magnetization and magneto-optical microscopy measurements by canted antiferromagnetism and find a number of Weyl points. Using angle-resolved photoemission, we directly observe two pairs of Weyl points connected by the Fermi arcs. Our results not only provide a fundamental link between the two areas of physics, but also demonstrate the practical way to design novel materials with exotic properties.
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    Pressure-tuning the quantum spin Hamiltonian of the triangular lattice antiferromagnet Cs2CuCl4
    ([London] : Nature Publishing Group UK, 2019) Zvyagin, S.A.; Graf, D.; Sakurai, T.; Kimura, S.; Nojiri, H.; Wosnitza, J.; Ohta, H.; Ono, T.; Tanaka, H.
    Quantum triangular-lattice antiferromagnets are important prototype systems to investigate numerous phenomena of the geometrical frustration in condensed matter. Apart from highly unusual magnetic properties, they possess a rich phase diagram (ranging from an unfrustrated square lattice to a quantum spin liquid), yet to be confirmed experimentally. One major obstacle in this area of research is the lack of materials with appropriate (ideally tuned) magnetic parameters. Using Cs2CuCl4 as a model system, we demonstrate an alternative approach, where, instead of the chemical composition, the spin Hamiltonian is altered by hydrostatic pressure. The approach combines high-pressure electron spin resonance and r.f. susceptibility measurements, allowing us not only to quasi-continuously tune the exchange parameters, but also to accurately monitor them. Our experiments indicate a substantial increase of the exchange coupling ratio from 0.3 to 0.42 at a pressure of 1.8 GPa, revealing a number of emergent field-induced phases.
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    Computational design and optimization of electro-physiological sensors
    ([London] : Nature Publishing Group UK, 2021) Nittala, Aditya Shekhar; Karrenbauer, Andreas; Khan, Arshad; Kraus, Tobias; Steimle, Jürgen
    Electro-physiological sensing devices are becoming increasingly common in diverse applications. However, designing such sensors in compact form factors and for high-quality signal acquisition is a challenging task even for experts, is typically done using heuristics, and requires extensive training. Our work proposes a computational approach for designing multi-modal electro-physiological sensors. By employing an optimization-based approach alongside an integrated predictive model for multiple modalities, compact sensors can be created which offer an optimal trade-off between high signal quality and small device size. The task is assisted by a graphical tool that allows to easily specify design preferences and to visually analyze the generated designs in real-time, enabling designer-in-the-loop optimization. Experimental results show high quantitative agreement between the prediction of the optimizer and experimentally collected physiological data. They demonstrate that generated designs can achieve an optimal balance between the size of the sensor and its signal acquisition capability, outperforming expert generated solutions.
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    Enantio-sensitive unidirectional light bending
    ([London] : Nature Publishing Group UK, 2021) Ayuso, David; Ordonez, Andres F.; Decleva, Piero; Ivanov, Misha; Smirnova, Olga
    Structured light, which exhibits nontrivial intensity, phase, and polarization patterns in space, has key applications ranging from imaging and 3D micromanipulation to classical and quantum communication. However, to date, its application to molecular chirality has been limited by the weakness of magnetic interactions. Here we structure light’s local handedness in space to introduce and realize an enantio-sensitive interferometer for efficient chiral recognition without magnetic interactions, which can be seen as an enantio-sensitive version of Young’s double slit experiment. Upon interaction with isotropic chiral media, such chirality-structured light effectively creates chiral emitters of opposite handedness, located at different positions in space. We show that if the distribution of light’s handedness breaks left-right symmetry, the interference of these chiral emitters leads to unidirectional bending of the emitted light, in opposite directions in media of opposite handedness, even if the number of the left-handed and right-handed emitters excited in the medium is exactly the same. Our work introduces the concepts of polarization of chirality and chirality-polarized light, exposes the immense potential of sculpting light’s local chirality, and offers novel opportunities for efficient chiral discrimination, enantio-sensitive optical molecular fingerprinting and imaging on ultrafast time scales.