ATP-dependent Force Generation and Membrane Scission by ESCRT-III and Vps4
2018
The endosomal sorting complexes required for transport (ESCRTs) catalyze reverse-topology scission from the inner face of membrane necks in HIV budding, multivesicular endosome biogenesis, cytokinesis, and other pathways. We encapsulated ESCRT-III subunits Snf7, Vps24, and Vps2 and the AAA...
3D Covalent Organic Frameworks of Interlocking 1D Square Ribbons
2018
A new mode of mechanical entanglement in extended structures is described where 1D organic ribbons of corner-sharing squares are mutually interlocked to form 3D woven covalent organic framework-500, COF-500. Reaction of aldehyde-functionalized tetrahedral Cu(PDB)2...
Bioinspired Metal-Organic Framework Catalysts for Selective Methane Oxidation to Methanol
2018
Particulate methane monooxygenase (pMMO) is an enzyme that oxidizes methane to methanol with high activity and selectivity. Limited success has been achieved in incorporating biologically relevant ligands for the formation of such active site in a synthetic system. Here, we report the...
Studying rare nonadiabatic dynamics with transition path sampling quantum jump trajectories
2018
We present a method to study rare nonadiabatic dynamics in open quantum systems using transition path sampling and quantum jump trajectories. As with applications of transition path sampling to classical dynamics, the method does not rely on prior knowledge of transition states or reactive...
Nonlinear transport coefficients from large deviation functions
2018
Nonlinear response occurs naturally when a strong perturbation takes a system far from equilibrium. Despite of its omnipresence in nanoscale systems, it is difficult to predict in a general and efficient way. Here we introduce a way to compute arbitrarily high order transport coefficients...
Design Principles for Trap-Free CsPbX3 Nanocrystals: Enumerating and Eliminating Surface Halide Vacancies with Softer Lewis Bases
2018
We introduce a general surface passivation mechanism for cesium lead halide perovskite materials (CsPbX3, X = Cl, Br, I) that is supported by a combined experimental and theoretical study of the nanocrystal surface chemistry. A variety of spectroscopic methods are...
Elucidating CO2 Chemisorption in Diamine-Appended Metal-Organic Frameworks
2018
The widespread deployment of carbon capture and sequestration as a climate change mitigation strategy could be facilitated by the development of more energy-efficient adsorbents. Diamine-appended metal–organic frameworks of the type diamine–M2(dobpdc) (M = Mg, Mn...
Molecular Weaving of Covalent Organic Frameworks for Adaptive Guest Inclusion
2018
The synthesis of new isoreticular non-interpenetrated woven covalent organic frameworks (COFs) was achieved by linking aldehyde-functionalized copper(I) bisphenanthroline complexes with benzidine linkers in the presence of a bulky anion, diphenylphosphinate (PO2Ph...
Local Electronic Structure of Molecular Heterojunctions in a Single‐Layer 2D Covalent Organic Framework
2018
The synthesis of a single‐layer covalent organic framework (COF) with spatially modulated internal potentials provides new opportunities for manipulating the electronic structure of molecularly defined materials. Here, the fabrication and electronic characterization of COF‐420: a single‐...
Molecular Mechanics Simulations and Improved Tight-Binding Hamiltonians for Artificial Light Harvesting Systems: Predicting Geometric Distributions, Disorder, and Spectroscopy of Chromophores in a Protein Environment
2018
We present molecular mechanics and spectroscopic calculations on prototype artificial light harvesting systems consisting of chromophores attached to a tobacco mosaic virus (TMV) protein scaffold. These systems have been synthesized and characterized spectroscopically, but information...
Identification of the Strong Brønsted Acid Site in a Metal–Organic Framework Solid Acid Catalyst
2018
It remains difficult to understand the surface of solid acid catalysts at the molecular level, despite their importance for industrial catalytic applications. A sulfated zirconium-based metal–organic framework, MOF-808-SO4, was previously shown to be a strong...
Identification of the Bronsted Acid Catalytic Site in Sulfated MOF-808
2018
It remains difficult to understand the surface of solid acid catalysts at the molecular level, despite their importance for industrial catalytic applications. A sulfated zirconium-based metal–organic framework, MOF-808-SO4, was previously shown to be a strong solid Brønsted acid material.
...Leveraging Continuous Material Averaging for Inverse Electromagnetic Design
2018
Inverse electromagnetic design has emerged as a way of efficiently designing active and passive electromagnetic devices. This maturing strategy involves optimizing the shape or topology of a device in order to improve a figure of merit–a process which typically requires that we compute the...
Incarceration of Iodine in a Pyrene-Based Metal-Organic Framework
2018
A pyrene‐based metal‐organic framework (MOF) SION‐8 captured iodine (I2) vapor with a capacity of 460 and 250 mg g−1MOF at room temperature and 75 °C, respectively. Single‐crystal X‐ray diffraction...
Urea-Linked Covalent Organic Frameworks
2018
2D covalent organic frameworks (COFs) with flexible urea linkages have been synthesized by condensation of 1,3,5-triformylphloroglucinol (TFP) with 1,4-phenylenediurea (BDU) or 1,1′-(3,3′-dimethyl-[1,1′-biphenyl]-4,4′-diyl)diurea (DMBDU). The resulting COF-117 and COF-118 undergo...