Aditya Kulkarni

High charge mobility in two-dimensional percolative networks of PbSe quantum dots connected by atomic bonds

Two-dimensional networks of quantum dots connected by atomic bonds have an electronic structure that is distinct from that of arrays of quantum dots coupled by ligand molecules. We prepared atomically coherent two-dimensional percolative networks of PbSe quantum dots connected via atomic bonds. Here, we show that photoexcitation leads to generation of free charges that eventually decay via trapping. The charge mobility probed with an AC electric field increases with frequency from 150±15 cm2 V−1 s−1 at 0.2 terahertz to 260±15 cm2 V−1 s−1 at 0.6 terahertz. Gated four-probe measurements yield a DC electron mobility of 13±2 cm2 V−1 s−1. The terahertz mobilities are much higher than for arrays of quantum dots coupled via surface ligands and are similar to the highest DC mobilities reported for PbSe nanowires. The terahertz mobility increases only slightly with temperature in the range of 15–290 K. The extent of straight segments in the two-dimensional percolative networks limits the mobility, rather than charge scattering by phonons.

Sequential Analysis of Trans-SNARE Formation in Intracellular Membrane Fusion

SM proteins stabilize cis-SNARE complexes leading to a specific preferred topology for trans-SNARE formation.

Dynamin-SNARE interactions control trans-SNARE formation in intracellular membrane fusion.

The fundamental processes of membrane fission and fusion determine size and copy numbers of intracellular organelles. While SNARE proteins and tethering complexes mediate intracellular membrane fusion, fission requires the presence of dynamin or dynamin-related proteins. Here we study these reactions in native yeast vacuoles and find that the yeast dynamin homolog Vps1 is not only an essential part of the fission machinery, but also controls membrane fusion by generating an active Qa SNARE- tethering complex pool, which is essential for trans-SNARE formation. Our findings provide new insight into the role of dynamins in membrane fusion by directly acting on SNARE proteins.

Photogeneration and Mobility of Charge Carriers in Atomically Thin Colloidal InSe Nanosheets Probed by Ultrafast Terahertz Spectroscopy

The implementation of next generation ultrathin electronics by applying highly promising dimensionality-dependent physical properties of two-dimensional (2D) semiconductors is ever increasing. In this context, the van der Waals layered semiconductor InSe has proven its potential as photodetecting material with high charge carrier mobility. We have determined the photogeneration charge carrier quantum yield and mobility in atomically thin colloidal InSe nanosheets (inorganic layer thickness 0.8-1.7 nm, mono/double-layers, ≤ 5 nm including ligands) by ultrafast transient terahertz (THz) spectroscopy. A near unity quantum yield of free charge carriers is determined for low photoexcitation density. The charge carrier quantum yield decreases at higher excitation density due to recombination of electrons and holes, leading to the formation of neutral excitons. In the THz frequency domain, we probe a charge mobility as high as 20 ± 2 cm2/(V s). The THz mobility is similar to field-effect transistor mobilities extracted from unmodified exfoliated thin InSe devices. The current work provides the first results on charge carrier dynamics in ultrathin colloidal InSe nanosheets.

A dynamin homolog promotes the transition from hemifusion to content mixing in intracellular membrane fusion.

The convergence of the antagonistic reactions of membrane fusion and fission at the hemifusion/hemifission intermediate has generated a captivating enigma of whether Soluble N‐ethylmaleimide sensitive factor Attachment Protein Receptor (SNAREs) and dynamin have unusual counter‐functions in fission and fusion, respectively. SNARE‐mediated fusion and dynamin‐driven fission are fundamental membrane flux reactions known to occur during ubiquitous cellular communication events such as exocytosis, endocytosis and vesicle transport. Here we demonstrate the influence of the dynamin homolog Vps1 (Vacuolar protein sorting 1) on lipid mixing and content mixing properties of yeast vacuoles, and on the incorporation of SNAREs into fusogenic complexes. We propose a novel concept that Vps1, through its oligomerization and SNARE domain binding, promotes the hemifusion‐content mixing transition in yeast vacuole fusion by increasing the number of trans‐SNAREs.

Efficient Steplike Carrier Multiplication in Percolative Networks of Epitaxially Connected PbSe Nanocrystals

Carrier multiplication (CM) is a process in which a single photon excites two or more electrons. CM is of interest to enhance the efficiency of a solar cell. Until now, CM in thin films and solar cells of semiconductor nanocrystals (NCs) has been found at photon energies well above the minimum required energy of twice the band gap. The high threshold of CM strongly limits the benefits for solar cell applications. We show that CM is more efficient in a percolative network of directly connected PbSe NCs. The CM threshold is at twice the band gap and increases in a steplike fashion with photon energy. A lower CM efficiency is found for a solid of weaker coupled NCs. This demonstrates that the coupling between NCs strongly affects the CM efficiency. According to device simulations, the measured CM efficiency would significantly enhance the power conversion efficiency of a solar cell.

A tethering complex dimer catalyzes trans-SNARE complex formation in intracellular membrane fusion.

SNARE complexes mediate membrane fusion in the endomembrane system. They consist of coiled-coil bundles of four helices designated as Qa, Qb, Qc and R. A critical intermediate in the fusion pathway is the trans-SNARE complex generated by the assembly of SNAREs residing in opposing membranes. Mechanistic details of trans-SNARE complex formation and topology in a physiological system remain largely unresolved. Our studies on native yeast vacuoles revealed that SNAREs alone are insufficient to form trans-SNARE complexes and that additional factors, potentially tethering complexes and Rab GTPases, are required for the process. Here we report a novel finding that a HOPS tethering complex dimer catalyzes Rab GTPase-dependent formation of a topologically preferred QbQcR-Qa trans-SNARE complex.

Ultrafast charge cooling and carrier multiplication in semiconductor nanocrystals and superlattices

We studied charge carrier photogeneration, cooling, carrier multiplication (CM) and charge mobility and decay in: a) isolated PbSe nanocrystals in solution, b) films of PbSe nanocrystals coupled by organic ligands, and c) 2D percolative networks of epitaxially connected PbSe nanocrystals. The studies were performed using ultrafast pump-probe spectroscopy with optical or terahertz/microwave conductivity detection. The effects of electronic coupling between the nanocrystals on charge mobility were characterized by frequency-resolved microwave and terahertz photoconductivity measurements. Reducing the size of ligand molecules between nanocrystals in a film strongly increases the charge mobility. Direct connection of nanocrystals in a percolative network yielded a sum of electron and hole mobilities as high as 270±10 cm2V-1s-1. We found that a high mobility is essential for multiple electron-hole pairs formed via CM to escape from recombination. The coupling between the nanocrystals was found to strongly affect the competition between cooling of hot charges by phonon emission and CM. In percolative networks of connected nanocrystals CM is much more efficient than in films with ligands between the nanocrystals. In the e networks CM occurs in a step-like fashion with threshold near the minimum photon energy of twice the band gap.