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Rapid growth of new atmospheric particles by nitric acid and ammonia condensation 期刊论文
NATURE, 2020, 581 (7807) : 184-+
作者:  Liang, Guanxiang;  Zhao, Chunyu;  Zhang, Huanjia;  Mattei, Lisa;  Sherrill-Mix, Scott;  Bittinger, Kyle;  Kessler, Lyanna R.;  Wu, Gary D.;  Baldassano, Robert N.;  DeRusso, Patricia;  Ford, Eileen;  Elovitz, Michal A.;  Kelly, Matthew S.;  Patel, Mohamed Z.;  Mazhani, Tiny;  Gerber, Jeffrey S.;  Kelly, Andrea;  Zemel, Babette S.;  Bushman, Frederic D.
收藏  |  浏览/下载:17/0  |  提交时间:2020/05/20

A list of authors and their affiliations appears at the end of the paper New-particle formation is a major contributor to urban smog(1,2), but how it occurs in cities is often puzzling(3). If the growth rates of urban particles are similar to those found in cleaner environments (1-10 nanometres per hour), then existing understanding suggests that new urban particles should be rapidly scavenged by the high concentration of pre-existing particles. Here we show, through experiments performed under atmospheric conditions in the CLOUD chamber at CERN, that below about +5 degrees Celsius, nitric acid and ammonia vapours can condense onto freshly nucleated particles as small as a few nanometres in diameter. Moreover, when it is cold enough (below -15 degrees Celsius), nitric acid and ammonia can nucleate directly through an acid-base stabilization mechanism to form ammonium nitrate particles. Given that these vapours are often one thousand times more abundant than sulfuric acid, the resulting particle growth rates can be extremely high, reaching well above 100 nanometres per hour. However, these high growth rates require the gas-particle ammonium nitrate system to be out of equilibrium in order to sustain gas-phase supersaturations. In view of the strong temperature dependence that we measure for the gas-phase supersaturations, we expect such transient conditions to occur in inhomogeneous urban settings, especially in wintertime, driven by vertical mixing and by strong local sources such as traffic. Even though rapid growth from nitric acid and ammonia condensation may last for only a few minutes, it is nonetheless fast enough to shepherd freshly nucleated particles through the smallest size range where they are most vulnerable to scavenging loss, thus greatly increasing their survival probability. We also expect nitric acid and ammonia nucleation and rapid growth to be important in the relatively clean and cold upper free troposphere, where ammonia can be convected from the continental boundary layer and nitric acid is abundant from electrical storms(4,5).


  
Ionic solids from common colloids 期刊论文
NATURE, 2020, 580 (7804) : 487-+
作者:  Delord, T.;  Huillery, P.;  Nicolas, L.;  Hetet, G.
收藏  |  浏览/下载:6/0  |  提交时间:2020/07/03

Oppositely charged colloidal particles are assembled in water through an approach that allows electrostatic interactions to be precisely tuned to generate macroscopic single crystals.


From rock salt to nanoparticle superlattices, complex structure can emerge from simple building blocks that attract each other through Coulombic forces(1-4). On the micrometre scale, however, colloids in water defy the intuitively simple idea of forming crystals from oppositely charged partners, instead forming non-equilibrium structures such as clusters and gels(5-7). Although various systems have been engineered to grow binary crystals(8-11), native surface charge in aqueous conditions has not been used to assemble crystalline materials. Here we form ionic colloidal crystals in water through an approach that we refer to as polymer-attenuated Coulombic self-assembly. The key to crystallization is the use of a neutral polymer to keep particles separated by well defined distances, allowing us to tune the attractive overlap of electrical double layers, directing particles to disperse, crystallize or become permanently fixed on demand. The nucleation and growth of macroscopic single crystals is demonstrated by using the Debye screening length to fine-tune assembly. Using a variety of colloidal particles and commercial polymers, ionic colloidal crystals isostructural to caesium chloride, sodium chloride, aluminium diboride and K4C60 are selected according to particle size ratios. Once fixed by simply diluting out solution salts, crystals are pulled out of the water for further manipulation, demonstrating an accurate translation from solution-phase assembly to dried solid structures. In contrast to other assembly approaches, in which particles must be carefully engineered to encode binding information(12-18), polymer-attenuated Coulombic self-assembly enables conventional colloids to be used as model colloidal ions, primed for crystallization.


  
General synthesis of two-dimensional van der Waals heterostructure arrays 期刊论文
NATURE, 2020: 368-+
作者:  Bloch, Joel S.;  Pesciullesi, Giorgio;  Boilevin, Jeremy;  Nosol, Kamil;  Irobalieva, Rossitza N.;  Darbre, Tamis;  Aebi, Markus;  Kossiakoff, Anthony A.;  Reymond, Jean-Louis;  Locher, Kaspar P.
收藏  |  浏览/下载:63/0  |  提交时间:2020/07/03

Two-dimensional van der Waals heterostructures (vdWHs) have attracted considerable interest(1-4). However, most vdWHs reported so far are created by an arduous micromechanical exfoliation and manual restacking process(5), which-although versatile for proof-of-concept demonstrations(6-16) and fundamental studies(17-30)-is clearly not scalable for practical technologies. Here we report a general synthetic strategy for two-dimensional vdWH arrays between metallic transition-metal dichalcogenides (m-TMDs) and semiconducting TMDs (s-TMDs). By selectively patterning nucleation sites on monolayer or bilayer s-TMDs, we precisely control the nucleation and growth of diverse m-TMDs with designable periodic arrangements and tunable lateral dimensions at the predesignated spatial locations, producing a series of vdWH arrays, including VSe2/WSe2, NiTe2/WSe2, CoTe2/WSe2, NbTe2/WSe2, VS2/WSe2, VSe2/MoS2 and VSe2/WS2. Systematic scanning transmission electron microscopy studies reveal nearly ideal vdW interfaces with widely tunable moire superlattices. With the atomically clean vdW interface, we further show that the m-TMDs function as highly reliable synthetic vdW contacts for the underlying WSe2 with excellent device performance and yield, delivering a high ON-current density of up to 900 microamperes per micrometre in bilayer WSe2 transistors. This general synthesis of diverse two-dimensional vdWH arrays provides a versatile material platform for exploring exotic physics and promises a scalable pathway to high-performance devices.


A general strategy for the synthesis of two-dimensional van der Waals heterostructure arrays is used to produce high-performance electronic devices, showing the potential of this scalable approach for practical technologies.


  
Antagonistic cooperativity between crystal growth modifiers 期刊论文
NATURE, 2020, 577 (7791) : 497-+
作者:  Ma, Wenchuan;  Lutsko, James F.;  Rimer, Jeffrey D.;  Vekilov, Peter G.
收藏  |  浏览/下载:9/0  |  提交时间:2020/07/03

Inhibitor pairs that suppress the crystallization of haematin, which is a part of malaria parasites'  physiology, show unexpected antagonism due to attenuation of step pinning by kink blockers.


Ubiquitous processes in nature and the industry exploit crystallization from multicomponent environments(1-5)  however, laboratory efforts have focused on the crystallization of pure solutes(6,7) and the effects of single growth modifiers(8,9). Here we examine the molecular mechanisms employed by pairs of inhibitors in blocking the crystallization of haematin, which is a model organic compound with relevance to the physiology of malaria parasites(10,11). We use a combination of scanning probe microscopy and molecular modelling to demonstrate that inhibitor pairs, whose constituents adopt distinct mechanisms of haematin growth inhibition, kink blocking and step pinning(12,13), exhibit both synergistic and antagonistic cooperativity depending on the inhibitor combination and applied concentrations. Synergism between two crystal growth modifiers is expected, but the antagonistic cooperativity of haematin inhibitors is not reflected in current crystal growth models. We demonstrate that kink blockers reduce the line tension of step edges, which facilitates both the nucleation of crystal layers and step propagation through the gates created by step pinners. The molecular viewpoint on cooperativity between crystallization modifiers provides guidance on the pairing of modifiers in the synthesis of crystalline materials. The proposed mechanisms indicate strategies to understand and control crystallization in both natural and engineered systems, which occurs in complex multicomponent media(1-3,8,9). In a broader context, our results highlight the complexity of crystal-modifier interactions mediated by the structure and dynamics of the crystal interface.


  
New Particle Formation in the Atmosphere: From Molecular Clusters to Global Climate 期刊论文
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2019, 124 (13) : 7098-7146
作者:  Lee, Shan-Hu;  Gordon, Hamish;  Yu, Huan;  Lehtipalo, Katrianne;  Haley, Ryan;  Li, Yixin;  Zhang, Renyi
收藏  |  浏览/下载:13/0  |  提交时间:2019/11/27
new particle formation  nucleation and growth  CCN  sulfuric acid  ammonia  HOMs  
Organic-mineral interfacial chemistry drives heterogeneous nucleation of Sr-rich (Ba-x, Sr1-x)SO4 from undersaturated solution 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2019, 116 (27) : 13221-13226
作者:  Deng, Ning;  Stack, Andrew G.;  Weber, Juliane;  Cao, Bo;  De Yoreo, James J.;  Hu, Yandi
收藏  |  浏览/下载:7/0  |  提交时间:2019/11/27
Sr-rich marine barite  organic-mineral interactions  solid solution  nucleation and growth  paleoenvironments  
Organic–mineral interfacial chemistry drives heterogeneous nucleation of Sr-rich (Bax, Sr1−x)SO4 from undersaturated solution 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2019, 116 (27) : 13221-13226
作者:  Ning Deng;  Andrew G. Stack;  Juliane Weber;  Bo Cao;  James J. De Yoreo;  and Yandi Hu
收藏  |  浏览/下载:6/0  |  提交时间:2019/11/27
Sr-rich marine barite  organic–mineral interactions  solid solution  nucleation and growth  paleoenvironments