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Sadegh Yazdi

Publications and source records attributed to Sadegh Yazdi.

8 recordsLinked to original sources

Atomic Alignment in PbS Nanocrystal Superlattices with Compact Inorganic Ligands via Reversible Oriented Attachment of Nanocrystals

Nanocrystals (NCs) serve as versatile building blocks for the creation of functional materials, with NC self-assembly offering opportunities to enable novel material properties. Here, we demonstrate that PbS NCs functionalized with strongly negatively charged metal chalcogenide complex (MCC) ligands, such as $Sn_2S_6^{4-}$ and $AsS_4^{3-}$, can self-assemble into all-inorganic superlattices with both long-range superlattice translational and atomic-lattice orientational order. Structural characterizations reveal that the NCs adopt unexpected edge-to-edge alignment, and numerical simulation clarifies that orientational order is thermodynamically stabilized by many-body ion correlations originating from the dense electrolyte. Furthermore, we show that the superlattices of $Sn_2S_6^{4-}$-functionalized PbS NCs can be fully disassembled back into the colloidal state, which is highly unusual for orientationally attached superlattices with atomic-lattice alignment. The reversible oriented attachment of NCs, enabling their dynamic assembly and disassembly into effectively single-crystalline superstructures, offers a pathway toward designing reconfigurable materials with adaptive and controllable electronic and optoelectronic properties.

cond-mat.mtrl-sci

Trion Formation Hampers Single Quantum Dot Performance in Silane-Coated FAPbBr3 Quantum Dots

We explore silane-coated formamidinium lead bromide (FAPbBr3) quantum dots as single photon emitters and compare them to FAPbBr3 quantum dots passivated with a phosphoethylammonium derivative (PEAC8C12), which represents current state-of-the-art in zwitterionic molecular surface ligand passivation. We compare properties including single-photon purity (g2(t)), linewidth, blinking, and photostability. We find that at room temperature, these silane-coated dots perform comparably to the PEAC8C12 passivation in terms of single-photon performance metrics, while exhibiting improvements in photostability. However, we find that at 4K, silane-coated FAPbBr3 quantum dots perform worse than the PEAC8C12-passivated samples, exhibiting faster blue-shifting and photobleaching under illumination. Analysis of fluorescence lifetime intensity distributions from the photon-counting data indicates increased efficiency of fast non-radiative processes in the silane-coated quantum dots at 4K. We propose a trion related degradation pathway at low temperatures that is consistent with the observed kinetics and estimate that at 4K with 6.1 uJ/cm2, 472 nm excitation the silane-coated quantum dots build up double the trion population of their PEAC8C12-passivated counterparts.

cond-mat.mtrl-sci

Emissive Surface Traps Lead to Asymmetric Photoluminescence Line Shape in Spheroidal CsPbBr3 Quantum Dots

The morphology of quantum dots plays an important role in governing their photophysics. Here, we explore the photoluminescence of spheroidal CsPbBr3 quantum dots synthesized via the room-temperature trioctlyphosphine oxide/PbBr2 method. Despite photoluminescence quantum yields nearing 100%, these spheroidal quantum dots exhibit an elongated red photoluminescence tail not observed in typical cubic quantum dots synthesized via hot injection. We explore this elongated red tail through structural and optical characterization including small-angle x-ray scattering, transmission electron microscopy and time-resolved, steady-state, and single quantum dot photoluminescence. From these measurements we conclude that the red tail originates from emissive surface traps. We hypothesize that these emissive surface traps are located on the (111) surfaces and show that the traps can be passivated by adding phenethyl ammonium bromide, resulting in a more symmetric line shape

cond-mat.mtrl-sci

Non-Destructive, High-Resolution, Chemically Specific, 3D Nanostructure Characterization using Phase-Sensitive EUV Imaging Reflectometry

Next-generation nano and quantum devices have increasingly complex 3D structure. As the dimensions of these devices shrink to the nanoscale, their performance is often governed by interface quality or precise chemical or dopant composition. Here we present the first phase-sensitive extreme ultraviolet imaging reflectometer. It combines the excellent phase stability of coherent high-harmonic sources, the unique chemical- and phase-sensitivity of extreme ultraviolet reflectometry, and state-of-the-art ptychography imaging algorithms. This tabletop microscope can non-destructively probe surface topography, layer thicknesses, and interface quality, as well as dopant concentrations and profiles. High-fidelity imaging was achieved by implementing variable-angle ptychographic imaging, by using total variation regularization to mitigate noise and artifacts in the reconstructed image, and by using a high-brightness, high-harmonic source with excellent intensity and wavefront stability. We validate our measurements through multiscale, multimodal imaging to show that this technique has unique advantages compared with other techniques based on electron and scanning-probe microscopies.

physics.optics

Direct observation of enhanced electron-phonon coupling in copper nanoparticles in the warm-dense matter regime

Warm-dense matter (WDM) is a highly-excited state that lies at the confluence of solids, plasmas, and liquids and that cannot be described by equilibrium theories. The transient nature of this state when created in a laboratory, as well as the difficulties in probing the strongly-coupled interactions between the electrons and the ions, make it challenging to develop a complete understanding of matter in this regime. In this work, by exciting isolated ~8 nm nanoparticles with a femtosecond laser below the ablation threshold, we create uniformly-excited WDM. We then use photoelectron spectroscopy to track the instantaneous electron temperature and directly extract the strongest electron-ion coupling observed experimentally to date. By directly comparing with state-of-the-art theories, we confirm that the superheated nanoparticles lie at the boundary between hot solids and plasmas, with associated strong electron-ion coupling. This is evidenced both by the fast energy loss of electrons to ions, as well as a strong modulation of the electron temperature by acoustic oscillations in the nanoparticle. This work demonstrates a new route for experimental exploration and theoretical validation of the exotic properties of WDM.

physics.plasm-ph

Direct observation of 3D topological spin textures and their interactions using soft x-ray vector ptychography

Magnetic topological defects are energetically stable spin configurations characterized by symmetry breaking. Vortices and skyrmions are two well-known examples of 2D spin textures that have been actively studied for both fundamental interest and practical applications. However, experimental evidence of the 3D spin textures has been largely indirect or qualitative to date, due to the difficulty of quantitively characterizing them within nanoscale volumes. Here, we develop soft x-ray vector ptychography to quantitatively image the 3D magnetization vector field in a frustrated superlattice with 10 nm spatial resolution. By applying homotopy theory to the experimental data, we quantify the topological charge of hedgehogs and anti-hedgehogs as emergent magnetic monopoles and probe their interactions inside the frustrated superlattice. We also directly observe virtual hedgehogs and anti-hedgehogs created by magnetically inert voids. We expect that this new quantitative imaging method will open the door to study 3D topological spin textures in a broad class of magnetic materials. Our work also demonstrates that magnetically frustrated superlattices could be used as a new platform to investigate hedgehog interactions and dynamics and to exploit optimized geometries for information storage and transport applications.

cond-mat.str-el

Origins of size effects in initially dislocation-free single-crystal metallic micro- and nanocubes

We report phenomenal yield strengths, up to one fourth of the theoretical strength of silver, recorded in microcompression testing of initially dislocation free silver micro and nanocubes synthesized from a multistep seed growth process. These high strengths and the massive strain bursts that occur upon yield are results of the initially dislocation free single crystal structure of the pristine samples that yield through spontaneous nucleation of dislocations. When the pristine samples are exposed to a focused ion beam to fabricate pillars and then compressed, the dramatic strain burst does not occur, and they yield at a quarter of the strength of their pristine counterparts. Regardless of the defect state of the samples prior to testing, a size effect is apparent, where the yield strength increases as the sample size decreases. Since dislocation starvation and the single arm source mechanisms cannot explain a size effect on yield strength in dislocation free samples, we investigate the dislocation nucleation mechanisms controlling the size effect through careful experimental observations and molecular statics simulations. We find that intrinsic or extrinsic symmetry breakers such as surface defects, edge roundness, external sample shape, or a high vacancy concentration can influence dislocation nucleation, and thus contribute to the size effect on yield strength in initially dislocation-free samples.

cond-mat.mtrl-sci

Creation of high mobility two-dimensional electron gases via strain induced polarization at an otherwise nonpolar complex oxide interface

The discovery of two-dimensional electron gases (2DEGs) in SrTiO3-based heterostructures provides new opportunities for nanoelectronics. Herein, we create a new type of oxide 2DEG by the epitaxial-strain-induced polarization at an otherwise nonpolar perovskite-type interface of CaZrO3/SrTiO3. Remarkably, this heterointerface is atomically sharp, and exhibits a high electron mobility exceeding 60,000 cm2V-1s-1 at low temperatures. The 2DEG carrier density exhibits a critical dependence on the film thickness, in good agreement with the polarization induced 2DEG scheme.

cond-mat.mtrl-sci