Indium phosphide quantum dots have become an industrially relevant material for solid-state lighting and wide color gamut displays. The synthesis of indium from carboxylates tris(trimethylsilyl)phosphine (P(SiMe3)3) is understood to proceed through the formation magic-sized clusters, with In37P20(O2CR)51 being key isolable intermediate. reactivity cluster a vital parameter in controlling conversion dots. Herein, we report structural perturbations clusters induced by tuning steric properties...

We create defects for quantum technologies by using high temperatures and pressures to convert molecularly doped carbon diamond.

The discovery of magic-sized clusters as intermediates in the synthesis colloidal quantum dots has allowed for insight into formation pathways and provided atomically precise molecular platforms studying structure surface chemistry those materials. monodisperse InAs been developed through use indium carboxylate As(SiMe3)3 precursors documented to proceed intermediates. Herein, we report synthesis, isolation, single-crystal X-ray diffraction an nanocluster that is ubiquitous across reports...

Diamonds approaching the nanoscale have potential for use as probe materials their optical properties can be sensitive to optical/electric fields, mechanical stress/pressure, and configuration of nuclear spins. The surface nanodiamonds impacts sensing capabilities, examining nanodiamond through X-ray absorption give insights into molecular structures. Here, quantum dot models with varying amounts carbon passivation are prepared, optimized, compared. loss diamond sp3 lattice is examined by...

Developing interfacial probes of ligand-nanocluster interactions is crucial for understanding and tailoring the optoelectronic properties these emerging nanomaterials. Using transient IR spectroscopy, we demonstrate that ligand vibrational modes oleate-capped 1.3 nm InP nanoclusters report on photogenerated exciton. The exciton induces an intensity change in asymmetric carboxylate stretching mode by 57% while generating no appreciable shift frequency. Thus, observed difference signal...

Magnetic circular dichroism (MCD) spectra are able to provide insights into the geometric, electronic, and magnetic properties of chemical systems. However, they can be challenging understand simulate given need simultaneously treat both finite optical fields. Thus, efficient simulations desired resolve molecular electronic states. Real-time dynamics used widely in simulation spectroscopies such as absorption well dichroism, but simulating MCD with real-time is technically theoretically...

This paper describes coinage-metal-doped InP quantum dots (QDs) as a platform for enhanced electron transfer to molecular acceptors relative undoped QDs. A synthetic strategy is developed prepare doped InP/ZnSe First-principles DFT calculations show that Ag+ and Cu+ dopants localize photoexcited holes while leaving electrons delocalized. charge carrier wave function modulation leveraged enhance by up an order of magnitude. Examination photoluminescence quenching data suggests larger...

The presence of midgap states introduced by localized defects in wide-band-gap-doped semiconductors can strongly affect the electronic structure and optical properties materials, generating a wide range applications. Silicon-divacancy diamond have been recently proposed for probing high-resolution pressure changes performing quantum cryptography, making them good candidates to substitute more common nitrogen-vacancy centers. Using group-theory ab initio methods, molecular origin states,...

We demonstrate fine-tuning of the atomic composition InP/ZnSe quantum dots (QDs) at core/shell interface. Specifically, we control stoichiometry both anions (P, As, S, and Se) cations (In Zn) interface correlate these changes with resultant steady-state time-resolved optical properties nanocrystals. The use reactive trimethylsilyl reagents results in surface-limited reactions that shift nanocrystal to anion-rich improve epitaxial growth shell layer. In general, anion deposition on InP QD...

Chromium iodide monolayers, which have different magnetic properties in comparison to the bulk chromium iodide, been shown form skyrmionic states applied electromagnetic fields or Janus-layer devices. In this work, we demonstrate that spin-canted solutions can be induced into monolayer by select substitution of atoms with isovalent impurities. Several concentrations and spatial configurations halide substitutional defects are selected probe coupling between local defect-induced geometric...

Fluorescent nanodiamonds, that is, those containing optically active defects, have attracted interest for their ability to be used as qubits; in vivo imaging; and sensors spin, stress, temperature. One of the most commonly studied nanodiamond color centers is nitrogen vacancy. However, there strong discovering other impurity provide localized midband gap transitions. Noble gas atoms garnered attention since they been discovered within nanodiamonds produced through...

We demonstrate colloidal, layer-by-layer growth of metal oxide shells on InP quantum dots (QDs) at room temperature. show with computational modeling that native QD surface oxides give rise to nonradiative pathways due the presence surface-localized dark states near band edges. Replacing indium zinc form a ZnO shell results in reduced decay and density valence edge resembles defect-free, stoichiometric InP. then developed synthetic strategy using amounts common atomic layer deposition...

Defects within nanodiamonds have enabled a variety of quantum sensors based on optical properties that are sensitive to pressure, optical/electric fields, and the configuration both electronic nuclear spins. The presence dopants can introduce midgap states influencing their properties. Complex defects nitrogen aggregates been shown form in nitrogen-containing diamonds; as such, it is important differentiate these systems from pure diamond single vacancy (NV) systems. Here we report effect...

Indium phosphide quantum dots have become an industrially relevant material for solid-state lighting and wide color gamut displays. The synthesis of indium from carboxylates tris(trimethylsilyl)phosphine (P(SiMe3)3) is understood to proceed through the formation magic-sized clusters, with In37P20(O2CR)51 being key isolable intermediate. reactivity cluster a vital parameter in controlling conversion dots. Here, we report structural perturbations clusters induced by tuning steric properties...

This paper describes coinage-metal-doped InP quantum dots (QDs) as a platform for enhanced electron transfer to molecular acceptors relative undoped QDs. A versatile synthesis strategy is developed prepare high quality doped InP/ZnSe First principles DFT calculations show that Ag+ and Cu+ dopants localize photoexcited holes while leaving electrons delocalized. charge carrier wavefunction modulation leveraged enhance by up an order of magnitude. Examination photoluminescence quenching data...

This paper describes coinage-metal-doped InP quantum dots (QDs) as a platform for enhanced electron transfer to molecular acceptors relative undoped QDs. A synthetic strategy is developed prepare doped InP/ZnSe First principles DFT calculations show that Ag+ and Cu+ dopants localize photoexcited holes while leaving electrons delocalized. charge carrier wavefunction modulation leveraged enhance by up an order of magnitude. Examination photoluminescence quenching data suggests larger...

The discovery of magic sized clusters as intermediates in the synthesis colloidal quantum dots has allowed for insight into formation pathways and provided atomically precise, molecular platforms studying structure surface chemistry those materials. monodisperse InAs been developed through use indium carboxylate As(SiMe3)3 precursors documented to proceed magic-sized intermediates. Herein, we report synthesis, isolation, single-crystal X-ray diffraction an nanocluster that is ubiquitous...

Hysteresis in the fifth loading cycle has been measured for a series of polyurethane-ureas based on polytetramethylene glycol (PTMEG), toluene diisocyanate (TDI), and two different amine chain extenders/curatives, methylenebisortho chloroanaline (MBOCA) dimethylthio diamine (Ethacure 300, Ethyl Corp.). was seen to increase with strain temperature all samples. However, hysteresis limited by crosslinking hard domains these materials also showed decreased dependence at higher temperatures....

Recent experiments have shown that exfoliated few-layer CrI3, a prototypical van der Waals magnet, undergoes phase transition from the high-temperature monoclinic structure to low-temperature rhombohedral under pressure. To understand how magnetism of CrI3 responds these structural changes, we perform ab initio density functional theory simulations on bilayer CrI3. We simulate interlayer lateral shift-dependent potential energy surface examine stability and as function external Using hybrid...

We demonstrate fine-tuning of the atomic composition InP/ZnSe QDs at core/shell interface. Specifically, we control stoichiometry both anions (P, As, S, and Se) cations (In, Zn) correlate these changes with resultant steady-state time-resolved optical properties nanocrystals. Anion deposition on InP QD surface results in a redshift absorption, quenching excitonic photoluminescence, relative increase intensity broad trap-based consistent delocalization exciton wavefunction relaxation...

We demonstrate colloidal, layer-by-layer growth of metal oxide shells on InP quantum dots (QDs) at room temperature. First, computational modeling demonstrates that native surface oxides give rise to increased nonradiative pathways due the presence surface-localized dark states near band edges. Replacing indium with zinc form a ZnO shell results in reduced decay and density valence maximum resembles defect-free, stoichiometric InP. Motivated by these findings, we developed synthetic strategy...