A5065081943- Quantum Dots Synthesis And Properties
- Chalcogenide Semiconductor Thin Films
- Advanced Chemical Physics Studies
- Nanocluster Synthesis and Applications
- Metal-Organic Frameworks: Synthesis and Applications
- Electrocatalysts for Energy Conversion
- Crystallography and molecular interactions
- Catalytic Processes in Materials Science
- Genetics, Bioinformatics, and Biomedical Research
- Crystallization and Solubility Studies
- Asymmetric Hydrogenation and Catalysis
- X-ray Diffraction in Crystallography
- Semiconductor Quantum Structures and Devices
- Various Chemistry Research Topics
- Protein Structure and Dynamics
- Machine Learning in Materials Science
- Green IT and Sustainability
- Covalent Organic Framework Applications
- Magnetic and transport properties of perovskites and related materials
- Catalysis and Hydrodesulfurization Studies
- Optical properties and cooling technologies in crystalline materials
- Perovskite Materials and Applications
- Inorganic Fluorides and Related Compounds
- Carbon Dioxide Capture Technologies
- Gold and Silver Nanoparticles Synthesis and Applications
Lawrence Berkeley National Laboratory
2023-2024
Massachusetts Institute of Technology
2014-2024
University of California, Berkeley
2023-2024
University of Iowa
2019
University of Chicago
2014-2017
IIT@MIT
2014
We report here the design of BINAP-based metal–organic frameworks and their postsynthetic metalation with Rh complexes to afford highly active enantioselective single-site solid catalysts for asymmetric cyclization reactions 1,6-enynes. Robust, chiral, porous Zr-MOFs UiO topology, BINAP-MOF (I) or BINAP-dMOF (II), were prepared using purely BINAP-derived dicarboxylate linkers by mixing unfunctionalized linkers, respectively. Upon Rh(nbd)2BF4 [Rh(nbd)Cl]2/AgSbF6, MOF precatalysts I·Rh(BF4)...
Water splitting by artificial catalysts is a critical process in the production of hydrogen gas as an alternative fuel. In this paper, we examine essential role theoretical calculations, with particular focus on density functional theory (DFT), understanding water-splitting reaction these catalysts. First, present overview DFT thermochemical calculations catalysts, addressing how are adapted to condensed phases and room temperature. We show DFT-derived chemical descriptors reactivity can be...
Carbon capture can mitigate point-source carbon dioxide (CO 2 ) emissions, but hurdles remain that impede the widespread adoption of amine-based technologies. Capturing CO at temperatures closer to those many industrial exhaust streams (>200°C) is interest, although metal oxide absorbents operate these typically exhibit sluggish absorption kinetics and instability cycling. Here, we report a porous metal–organic framework featuring terminal zinc hydride sites reversibly bind above...
The first chiral rhodium-diene-based metal–organic frameworks are highly active and enantioselective catalysts for C–C bond formation reactions.
Colloidal CdSe nanocrystals (NCs) have shown promise in applications ranging from LED displays to medical imaging. Their unique photophysics depend sensitively on the presence or absence of surface defects. Using simulations, we show that NCs are inherently defective; even for stoichiometric with perfect ligand passivation and no vacancies defects, still observe low energy spectrum is dominated by dark, surface-associated excitations, which more numerous larger NCs. Surface structure...
Lead halide perovskite nanocrystals (LHP NCs) are an emerging materials system with broad potential applications, including as emitters of quantum light. We apply design principles aimed at the structural optimization surface ligand species for CsPbBr3 NCs, leading us to study LHP NCs dicationic quaternary ammonium bromide ligands. Through selection linking groups and aliphatic backbones guided by experiments computational support, we demonstrate consistently narrow photoluminescence line...
The widespread application of III–V colloidal quantum dots (QDs) as nontoxic, highly tunable emitters is stymied by their high density trap states. Here, we utilize functional theory (DFT) to investigate state formation in a diverse set realistically passivated core-only InP and GaP QDs. Through orbital localization techniques, deconvolute the dense manifold states allow for detailed assignment surface defects. We find that three-coordinate species dominate trapping QDs identify features...
As luminescence applications of colloidal semiconductor nanocrystals push toward higher excitation flux conditions, there is an increased need to both understand and potentially control emission from multiexciton states. We develop a spectrally resolved correlation method study the triply excited state that enables direct measurements recombination pathway for triexciton, rather than relying on indirect extraction rates. demonstrate that, core–shell CdSe–CdS nanocrystals, triexciton arises...
Colloidal semiconductor nanocrystals have attracted much interest due to their unique optical properties, with applications ranging from displays biomedical imaging. Nanocrystal properties depend on the structure of surface, where defects can lead traps. CdSe undergo surface reorganization, or self-healing, eliminate defects, removing midgap traps band structure. However, effect this process spectrum is not well studied. Here, we show that self-healing only eliminates but also brightens and...
The pseudopotential (PP) approximation is one of the most common techniques in computational chemistry. Despite its long history, development custom PPs has not tracked with explosion different density functional approximations (DFAs). As a result, use exchange/correlation models for which they were developed widespread, although this practice known to be theoretically unsound. extent PP inconsistency errors (PPIEs) associated been systematically explored across types energy differences...
We explore an alternative to twist averaging in order obtain more cost-effective and accurate extrapolations the thermodynamic limit (TDL) for coupled cluster doubles (CCD) calculations. seek a single angle perform calculations at, instead of integrating over many random points or grid. introduce concept connectivity, quantity derived from nonzero four-index integrals MP2 calculation. This allows us find special that provides appropriate connectivity energy equation, which yields results...
We examine the 1-electron reduction of manganese porphyrin complexes Mn(iii) and TDE-2-ImP5+, which have attracted recent interest due to their properties as superoxide dismutase mimics. perform a series electronic structure calculations using variational 2-electron reduced density matrix (2-RDM) method with large [30,30] active space that represents wavefunction 1019 variables, well more traditional complete self-consistent field (CASSCF) [14,14] space. show larger 2-RDM calculation,...
Computational screens for oxygen evolution reaction (OER) catalysts based on Sabatier analysis have seen great success in recent years; however, the concept of using chemical descriptors to form a coordinate has not been put under scrutiny complex systems. In this paper, we examine critically use as method conducting catalytic screens. Applying density functional theory calculations two-center metal oxide model system, show that is quite successful predicting activities and capturing...
Organic light-emitting diodes (OLEDs) are promising candidates for solid-state lighting but suffer from decreased efficiency at the high current density required applications. This is called roll-off, and its cause remains subject of much debate. Here, a combination targeted experiments novel modeling used to quantify importance different microscopic processes in OLED roll-off. study utilizes new formalism—mean-field steady-state kinetics—that can rapidly simulate macroscopic device...
The widespread application of III-V colloidal quantum dots (QDs) as non-toxic, highly tunable emitters is stymied by their high density trap states. Here, we utilize functional theory (DFT) to investigate state formation in a diverse set realistically passivated core-only InP and GaP QDs. Through orbital localization techniques, deconvolute the dense manifold states allow for detailed assignment surface defects. We find that three-coordinate species dominate trapping QDs identify features...
Abstract Review: 91 refs
Abstract BINAP‐based metal‐organic frameworks and their postsynthetic metalation with Rh‐complexes are designed used as highly active enantioselective single‐site solid catalysts for the reductive cyclization Alder‐ene cycloisomerization of 1,6‐enynes well Pauson—Khand reactions between cinnamaldehyde CO source.