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Performance-limiting nanoscale trap clusters at grain junctions in halide perovskites 期刊论文
NATURE, 2020, 580 (7803) : 360-+
作者:  van den Brink, Susanne C.;  Alemany, Anna;  van Batenburg, Vincent;  Moris, Naomi;  Blotenburg, Marloes;  Vivie, Judith;  Baillie-Johnson, Peter;  Nichols, Jennifer;  Sonnen, Katharina F.;  Arias, Alfonso;  van Oudenaarden, Alexander
收藏  |  浏览/下载:27/0  |  提交时间:2020/07/03

Halide perovskite materials have promising performance characteristics for low-cost optoelectronic applications. Photovoltaic devices fabricated from perovskite absorbers have reached power conversion efficiencies above 25 per cent in single-junction devices and 28 per cent in tandem devices(1,2). This strong performance (albeit below the practical limits of about 30 per cent and 35 per cent, respectively(3)) is surprising in thin films processed from solution at low-temperature, a method that generally produces abundant crystalline defects(4). Although point defects often induce only shallow electronic states in the perovskite bandgap that do not affect performance(5), perovskite devices still have many states deep within the bandgap that trap charge carriers and cause them to recombine non-radiatively. These deep trap states thus induce local variations in photoluminescence and limit the device performance(6). The origin and distribution of these trap states are unknown, but they have been associated with light-induced halide segregation in mixed-halide perovskite compositions(7) and with local strain(8), both of which make devices less stable(9). Here we use photoemission electron microscopy to image the trap distribution in state-of-the-art halide perovskite films. Instead of a relatively uniform distribution within regions of poor photoluminescence efficiency, we observe discrete, nanoscale trap clusters. By correlating microscopy measurements with scanning electron analytical techniques, we find that these trap clusters appear at the interfaces between crystallographically and compositionally distinct entities. Finally, by generating time-resolved photoemission sequences of the photo-excited carrier trapping process(10,11), we reveal a hole-trapping character with the kinetics limited by diffusion of holes to the local trap clusters. Our approach shows that managing structure and composition on the nanoscale will be essential for optimal performance of halide perovskite devices.


  
Observations of grain-boundary phase transformations in an elemental metal 期刊论文
NATURE, 2020, 579 (7799) : 375-+
作者:  Valente, Luis;  Phillimore, Albert B.;  Melo, Martim;  Warren, Ben H.;  Clegg, Sonya M.;  Havenstein, Katja;  Tiedemann, Ralph;  Illera, Juan Carlos;  Thebaud, Christophe;  Aschenbach, Tina;  Etienne, Rampal S.
收藏  |  浏览/下载:17/0  |  提交时间:2020/07/03

Atomic-resolution observations combined with simulations show that grain boundaries within elemental copper undergo temperature-induced solid-state phase transformation to different structures  grain boundary phases can also coexist and are kinetically trapped structures.


The theory of grain boundary (the interface between crystallites, GB) structure has a long history(1) and the concept of GBs undergoing phase transformations was proposed 50 years ago(2,3). The underlying assumption was that multiple stable and metastable states exist for different GB orientations(4-6). The terminology '  complexion'  was recently proposed to distinguish between interfacial states that differ in any equilibrium thermodynamic property(7). Different types of complexion and transitions between complexions have been characterized, mostly in binary or multicomponent systems(8-19). Simulations have provided insight into the phase behaviour of interfaces and shown that GB transitions can occur in many material systems(20-24). However, the direct experimental observation and transformation kinetics of GBs in an elemental metal have remained elusive. Here we demonstrate atomic-scale GB phase coexistence and transformations at symmetric and asymmetric [111 over bar ] tilt GBs in elemental copper. Atomic-resolution imaging reveals the coexistence of two different structures at sigma 19b GBs (where sigma 19 is the density of coincident sites and b is a GB variant), in agreement with evolutionary GB structure search and clustering analysis(21,25,26). We also use finite-temperature molecular dynamics simulations to explore the coexistence and transformation kinetics of these GB phases. Our results demonstrate how GB phases can be kinetically trapped, enabling atomic-scale room-temperature observations. Our work paves the way for atomic-scale in situ studies of metallic GB phase transformations, which were previously detected only indirectly(9,15,27-29), through their influence on abnormal grain growth, non-Arrhenius-type diffusion or liquid metal embrittlement.


  
Assessing the Kinetics and Pore-Scale Characteristics of Biological Calcium Carbonate Precipitation in Porous Media using a Microfluidic Chip Experiment 期刊论文
WATER RESOURCES RESEARCH, 2020, 56 (2)
作者:  Kim, Daehyun H.;  Mahabadi, Nariman;  Jang, Jaewon;  van Paassen, Leon A.
收藏  |  浏览/下载:13/0  |  提交时间:2020/07/02
urea hydrolysis  MICP  EICP  image processing  precipitation kinetics  microfluidic chip  
Fast oxidation of sulfur dioxide by hydrogen peroxide in deliquesced aerosol particles 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2020, 117 (3) : 1354-1359
作者:  Liu, Tengyu;  Clegg, Simon L.;  Abbatt, Jonathan P. D.
收藏  |  浏览/下载:11/0  |  提交时间:2020/05/13
air pollution  Chinese haze  sulfate aerosol  multiphase chemistry  aerosol kinetics  
Activation of the GLP-1 receptor by a non-peptidic agonist 期刊论文
NATURE, 2020, 577 (7790) : 432-+
作者:  Zhao, Peishen;  Liang, Yi-Lynn;  Belousoff, Matthew J.;  Deganutti, Giuseppe;  Fletcher, Madeleine M.;  Willard, Francis S.;  Bell, Michael G.;  Christe, Michael E.;  Sloop, Kyle W.;  Inoue, Asuka;  Truong, Tin T.;  Clydesdale, Lachlan;  Furness, Sebastian G. B.;  Christopoulos, Arthur;  Wang, Ming-Wei;  Miller, Laurence J.;  Reynolds, Christopher A.;  Danev, Radostin;  Sexton, Patrick M.;  Wootten, Denise
收藏  |  浏览/下载:9/0  |  提交时间:2020/07/03

Class B G-protein-coupled receptors are major targets for the treatment of chronic diseases, including diabetes and obesity(1). Structures of active receptors reveal peptide agonists engage deep within the receptor core, leading to an outward movement of extracellular loop 3 and the tops of transmembrane helices 6 and 7, an inward movement of transmembrane helix 1, reorganization of extracellular loop 2 and outward movement of the intracellular side of transmembrane helix 6, resulting in G-protein interaction and activation(2-6). Here we solved the structure of a non-peptide agonist, TT-OAD2, bound to the glucagon-like peptide-1 (GLP-1) receptor. Our structure identified an unpredicted non-peptide agonist-binding pocket in which reorganization of extracellular loop 3 and transmembrane helices 6 and 7 manifests independently of direct ligand interaction within the deep transmembrane domain pocket. TT-OAD2 exhibits biased agonism, and kinetics of G-protein activation and signalling that are distinct from peptide agonists. Within the structure, TT-OAD2 protrudes beyond the receptor core to interact with the lipid or detergent, providing an explanation for the distinct activation kinetics that may contribute to the clinical efficacy of this compound series. This work alters our understanding of the events that drive the activation of class B receptors.


  
Kinetic Control on the Depth Distribution of Superdeep Diamonds 期刊论文
GEOPHYSICAL RESEARCH LETTERS, 2019, 46 (4) : 1984-1992
作者:  Zhu, Feng;  Li, Jie;  Liu, Jiachao;  Lai, Xiaojing;  Chen, Bin;  Meng, Yue
收藏  |  浏览/下载:7/0  |  提交时间:2019/04/09
superdeep diamond  slab-mantle interaction  redox reaction  reaction kinetics  
Shear Rate-Dependent Disequilibrium Rheology and Dynamics of Basalt Solidification 期刊论文
GEOPHYSICAL RESEARCH LETTERS, 2018, 45 (13) : 6466-6475
作者:  Kolzenburg, S.;  Giordano, D.;  Hess, K. U.;  Dingwell, D. B.
收藏  |  浏览/下载:5/0  |  提交时间:2019/04/09
magma rheology  shear rate  advection  viscometry  crystallization kinetics  disequilibrium processes  
Observed NO/NO2 Ratios in the Upper Troposphere Imply Errors in NO-NO2-O-3 Cycling Kinetics or an Unaccounted NOx Reservoir 期刊论文
GEOPHYSICAL RESEARCH LETTERS, 2018, 45 (9) : 4466-4474
作者:  Silvern, R. F.;  Jacob, D. J.;  Travis, K. R.;  Sherwen, T.;  Evans, M. J.;  Cohen, R. C.;  Laughner, J. L.;  Hall, S. R.;  Ullmann, K.;  Crounse, J. D.;  Wennberg, P. O.;  Peischl, J.;  Pollack, I. B.
收藏  |  浏览/下载:9/0  |  提交时间:2019/04/09
NOx  upper troposphere  SEAC(4)RS  GEOS-Chem  kinetics  
Pulsating dissolution of crystalline matter 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2018, 115 (5) : 897-902
作者:  Fischer, Cornelius;  Luttge, Andreas
收藏  |  浏览/下载:7/0  |  提交时间:2019/11/27
surface reactivity  kinetics  dissolution  fluid-solid interaction  rate spectra  
Evaporation Kinetics of Polyol Droplets: Determination of Evaporation Coefficients and Diffusion Constants 期刊论文
JOURNAL OF GEOPHYSICAL RESEARCH-ATMOSPHERES, 2017, 122 (22)
作者:  Su, Yong-Yang;  Marsh, Aleksandra;  Haddrell, Allen E.;  Li, Zhi-Ming;  Reid, Jonathan P.
收藏  |  浏览/下载:11/0  |  提交时间:2019/04/09
evaporation kinetics  polyol droplets  electrodynamic balance (EDB)  evaporation coefficients  diffusion constants