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1. Contrasting Local and Long-Range Transported Warm Ice-Nucleating Particles During an Atmospheric River in Coastal California, USA

   https://doi.org/10.5194/acp-2018-702  

   Martin, Andrew C. ; Cornwell, Gavin ; Beall, Charlotte Marie ; Cannon, Forest ; Reilly, Sean ; Schaap, Bas ; Lucero, Dolan ; Creamean, Jessie ; Ralph, F. Martin ; Mix, Hari T. ; et al ( July 2018 , Atmospheric Chemistry and Physics Discussions)

   Abstract. Ice nucleating particles (INP) have been found to influence the amount, phase, and efficiency of precipitation from winter storms, including atmospheric rivers. Warm INP, those that initiate freezing at temperatures warmer than −10°C, are thought to be particularly impactful because they can create primary ice in mixed-phase clouds, enhancing precipitation efficiency. The dominant sources of warm INP during atmospheric rivers, the role of meteorology in modulating transport and injection of warm INP into atmospheric river clouds and the impact of warm INP on mixed-phase cloud properties are not well-understood. Time-resolved precipitation samples were collected during an atmospheric river in Northern California, USA during winter 2016. Precipitation was collected at two sites, one coastal and one inland, that are separated by less than 35km. The sites are sufficiently close that airmass sources during this storm were almost identical, but the inland site was exposed to terrestrial sources of warm INP while the coastal site was not. Warm INP were more numerous in precipitation at the inland site by an order of magnitude. Using FLEXPART dispersion modelling and radar-derived cloud vertical structure, we detected influence from terrestrial INP sources at the inland site, but did not find clear evidence of marine warm INP at either site. We episodically detected warm INP from long-range transported sources at both sites. By extending the FLEXPART modelling using a meteorological reanalysis, we demonstrate that long-range transported warm INP are observed only when the upper tropospheric jet provided transport to cloud tops. Using radar-derived hydrometeor classifications, we demonstrate that hydrometeors over the terrestrially-influenced inland site were more likely to be in the ice phase for cloud temperatures between 0°C and −10°C. We thus conclude that terrestrial and long-range transported aerosol were important sources of warm INP during this atmospheric river. Meteorological details such as transport mechanism and cloud structure were important in determining warm INP source strength and injection temperature, and ultimately the impact of warm INP on mixed phase cloud properties.

    

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2. Threshold Fluence Measurement for Laser Liftoff of InP Thin Films by Selective Absorption

   https://doi.org/10.1002/adem.201700624  

   Jan, Antony ; Reeves, Benjamin A. ; van de Burgt, Yoeri ; Hayes, Garrett J. ; Clemens, Bruce M. ( September 2017 , Advanced Engineering Materials)

   We explore conditions for achieving laser liftoff in epitaxially grown heterojunctions, in which single crystal thin films can be separated from their growth substrates using a selectively absorbing buried intermediate layer. Because this highly non‐linear process is subject to a variety of process instabilities, it is essential to accurately characterize the parameters resulting in liftoff. Here, we present an InP/InGaAs/InP heterojunction as a model system for such characterization. We show separation of InP thin films from single crystal InP growth substrates, wherein a ≈10 ns, Nd:YAG laser pulse selectively heats a coherently strained, buried InGaAs layer. We develop a technique to measure liftoff threshold fluences within an inhomogeneous laser spatial profile, and apply this technique to determine threshold fluences of the order 0.5 J cm⁻²for our specimens. We find that the fluence at the InGaAs layer is limited by non‐linear absorption and InP surface damage at high powers, and measure the energy transmission in an InP substrate from 0 to 8 J cm⁻². Characterization of the ejected thin films shows crack‐free, single crystal InP. Finally, we present evidence that the hot InGaAs initiates a liquid phase front that travels into the InP substrate during liftoff.

    

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3. Surface passivation extends single and biexciton lifetimes of InP quantum dots

   https://doi.org/10.1039/D0SC01039A  

   Yang, Wenxing ; Yang, Yawei ; Kaledin, Alexey L. ; He, Sheng ; Jin, Tao ; McBride, James R. ; Lian, Tianquan ( June 2020 , Chemical Science)

   Indium phosphide quantum dots (InP QDs) are nontoxic nanomaterials with potential applications in photocatalytic and optoelectronic fields. Post-synthetic treatments of InP QDs are known to be essential for improving their photoluminescence quantum efficiencies (PLQEs) and device performances, but the mechanisms remain poorly understood. Herein, by applying ultrafast transient absorption and photoluminescence spectroscopies, we systematically investigate the dynamics of photogenerated carriers in InP QDs and how they are affected by two common passivation methods: HF treatment and the growth of a heterostructure shell (ZnS in this study). The HF treatment is found to improve the PLQE up to 16–20% by removing an intrinsic fast hole trapping channel ( τ h,non = 3.4 ± 1 ns) in the untreated InP QDs while having little effect on the band-edge electron decay dynamics ( τ e = 26–32 ns). The growth of the ZnS shell, on the other hand, is shown to improve the PLQE up to 35–40% by passivating both electron and hole traps in InP QDs, resulting in both a long-lived band-edge electron ( τ e > 120 ns) and slower hole trapping lifetime ( τ h,non > 45 ns). Furthermore, both the untreated and the HF-treated InP QDs have short biexciton lifetimes ( τ xx ∼ 1.2 ± 0.2 ps). The growth of an ultra-thin ZnS shell (∼0.2 nm), on the other hand, can significantly extend the biexciton lifetime of InP QDs to 20 ± 2 ps, making it a passivation scheme that can improve both the single and multiple exciton lifetimes. Based on these results, we discuss the possible trap-assisted Auger processes in InP QDs, highlighting the particular importance of trap passivation for reducing the Auger recombination loss in InP QDs. 

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4. Best practices for precipitation sample storage for offline studies of ice nucleation in marine and coastal environments

   https://doi.org/10.5194/amt-13-6473-2020  

   Beall, Charlotte M. ; Lucero, Dolan ; Hill, Thomas C. ; DeMott, Paul J. ; Stokes, M. Dale ; Prather, Kimberly A. ( January 2020 , Atmospheric Measurement Techniques)

   null (Ed.)

   Abstract. Ice-nucleating particles (INPs) are efficiently removed fromclouds through precipitation, a convenience of nature for the study of thesevery rare particles that influence multiple climate-relevant cloudproperties including ice crystal concentrations, size distributions andphase-partitioning processes. INPs suspended in precipitation can be used toestimate in-cloud INP concentrations and to infer their originalcomposition. Offline droplet assays are commonly used to measure INPconcentrations in precipitation samples. Heat and filtration treatmentsare also used to probe INP composition and size ranges. Many previousstudies report storing samples prior to INP analyses, but little is knownabout the effects of storage on INP concentration or their sensitivity totreatments. Here, through a study of 15 precipitation samples collected at acoastal location in La Jolla, CA, USA, we found INP concentration changes upto > 1 order of magnitude caused by storage to concentrations ofINPs with warm to moderate freezing temperatures (−7 to−19 ∘C). We compared four conditions: (1) storage at roomtemperature (+21–23 ∘C), (2) storage at +4 ∘C, (3) storage at −20 ∘C and (4) flash-freezing samples with liquid nitrogen prior to storage at −20 ∘C. Results demonstrate that storage can lead to bothenhancements and losses of greater than 1 order of magnitude, withnon-heat-labile INPs being generally less sensitive to storage regime, butsignificant losses of INPs smaller than 0.45 µm in all tested storageprotocols. Correlations between total storage time (1–166 d) and changesin INP concentrations were weak across sampling protocols, with theexception of INPs with freezing temperatures ≥ −9 ∘C in samples stored at room temperature. We provide thefollowing recommendations for preservation of precipitation samples fromcoastal or marine environments intended for INP analysis: that samples bestored at −20 ∘C to minimize storage artifacts, thatchanges due to storage are likely an additional uncertainty in INPconcentrations, and that filtration treatments be applied only to freshsamples. At the freezing temperature −11 ∘C, average INPconcentration losses of 51 %, 74 %, 16 % and 41 % were observed foruntreated samples stored using the room temperature, +4, −20 ∘C, and flash-frozen protocols, respectively.Finally, the estimated uncertainties associated with the four storage protocolsare provided for untreated, heat-treated and filtered samples for INPsbetween −9 and −17 ∘C. 

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5. Aerosol–Ice Formation Closure: A Southern Great Plains Field Campaign

   https://doi.org/10.1175/BAMS-D-20-0151.1  

   Knopf, D. A. ; Barry, K. R. ; Brubaker, T. A. ; Jahl, L. G. ; Jankowski, K. A. ; Li, J. ; Lu, Y. ; Monroe, L. W. ; Moore, K. A. ; Rivera-Adorno, F. A. ; et al ( October 2021 , Bulletin of the American Meteorological Society)

   Abstract Prediction of ice formation in clouds presents one of the grand challenges in the atmospheric sciences. Immersion freezing initiated by ice-nucleating particles (INPs) is the dominant pathway of primary ice crystal formation in mixed-phase clouds, where supercooled water droplets and ice crystals coexist, with important implications for the hydrological cycle and climate. However, derivation of INP number concentrations from an ambient aerosol population in cloud-resolving and climate models remains highly uncertain. We conducted an aerosol–ice formation closure pilot study using a field-observational approach to evaluate the predictive capability of immersion freezing INPs. The closure study relies on collocated measurements of the ambient size-resolved and single-particle composition and INP number concentrations. The acquired particle data serve as input in several immersion freezing parameterizations, which are employed in cloud-resolving and climate models, for prediction of INP number concentrations. We discuss in detail one closure case study in which a front passed through the measurement site, resulting in a change of ambient particle and INP populations. We achieved closure in some circumstances within uncertainties, but we emphasize the need for freezing parameterization of potentially missing INP types and evaluation of the choice of parameterization to be employed. Overall, this closure pilot study aims to assess the level of parameter details and measurement strategies needed to achieve aerosol–ice formation closure. The closure approach is designed to accurately guide immersion freezing schemes in models, and ultimately identify the leading causes for climate model bias in INP predictions. 

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