arXiv subjects

Ilke Arslan

Publications and source records attributed to Ilke Arslan.

9 recordsLinked to original sources

arXiv2026

From Stacking Disorder to Cubic Order: Ice Crystallization from Deeply Supercooled Water

Crystallization far from equilibrium can generate morphologies that defy classical crystal habits, yet the microscopic mechanisms linking atomic-scale disorder to emergent macroscopic order remain elusive. Here we use in situ cryogenic transmission electron microscopy with a membrane-encapsulated microdroplet platform to directly visualize the freezing of deeply supercooled water at molecular resolution. We show that homogeneous nucleation produces stacking-disordered ice composed of mixed hexagonal and cubic sequences, in which cubic ice initially exists only as isolated monolayers. The gradual thickening of these cubic layers constitutes the key kinetic mechanism that governs the entire crystallization pathway. As thickening proceeds, nanoscale, defect-free cubic ice germs nucleate on the basal planes of the disordered lattice. These faceted cubic germs act as facet-registered kinetic seeds that enforce cubic twinning and sequentially multiply growth branches. This kinetic pathway reproducibly generates robust eight-branched dendrites with global cubic (octahedral) symmetry, even though each branch remains highly stacking-disordered. At later stages, latent heat release drives a crossover to the thermodynamically favored hexagonal phase; remarkably, the pre-established global cubic symmetry is retained. These results reveal how strong kinetic driving forces convert microscopic disorder into emergent macroscopic symmetry, providing a general framework for understanding and controlling rapid crystallization far from equilibrium.

cond-mat.mtrl-sci↗

arXiv2023

Nanosecond electron imaging of transient electric fields and material response

Electrical pulse stimulation drives many important physical phenomena in condensed matter as well as in electronic systems and devices. Often, nanoscopic and mesoscopic mechanisms are hypothesized, but methods to image electrically driven dynamics on both their native length and time scales have so far been largely undeveloped. Here, we present an ultrafast electron microscopy approach that uses electrical pulses to induce dynamics and records both the local time-resolved electric field and corresponding material behavior with nanometer-nanosecond spatiotemporal resolution. Quantitative measurement of the time-dependent field via the electron beam deflection is demonstrated by recording the field between two electrodes with single-ns temporal resolution. We then show that this can be applied in a material by correlating applied field with resulting dynamics in TaS$_{2}$. First, time-resolved electron diffraction is used to simultaneously record the electric field and crystal structure change in a selected region during a 20 ns voltage pulse, showing how a charge density wave transition evolves during and after the applied field. Then, time-resolved nanoimaging is demonstrated, revealing heterogeneous distortions that occur in the freestanding flake during a longer, lower amplitude pulse. Altogether, these results pave the way for future experiments that will uncover the nanoscale dynamics underlying electrically driven phenomena.

cond-mat.mes-hall↗

arXiv2022

Chiral Assemblies of Pinwheel Superlattices on Substrates

The unique topology and physics of chiral superlattices make their self-assembly from nanoparticles a holy grail for (meta)materials. Here we show that tetrahedral gold nanoparticles can spontaneously transform from a perovskite-like low-density phase with corner-to-corner connections into pinwheel assemblies with corner-to-edge connections and denser packing. While the corner-sharing assemblies are achiral, pinwheel superlattices become strongly mirror-asymmetric on solid substrates as demonstrated by chirality measures. Liquid-phase transmission electron microscopy and computational models show that van der Waals and electrostatic interactions between nanoparticles control thermodynamic equilibrium. Variable corner-to-edge connections among tetrahedra enable fine-tuning of chirality. The domains of the bilayer superlattices display strong chiroptical activity identified by photon-induced near-field electron microscopy and finite-difference time-domain simulations. The simplicity and versatility of the substrate-supported chiral superlattices facilitate manufacturing of metastructured coatings with unusual optical, mechanical and electronic characteristics.

cond-mat.mtrl-sci↗

arXiv2021

Ultrafast formation of transient 2D diamond-like structure in twisted bilayer graphene

Due to the absence of matching carbon atoms at honeycomb centers with carbon atoms in adjacent graphene sheets, theorists predicted that a sliding process is needed to form AA, AB, or ABC stacking when directly converting graphite into sp3 bonded diamond. Here, using twisted bilayer graphene, which naturally provides AA and AB stacking configurations, we report the ultrafast formation of a transient 2D diamond-like structure (which is not observed in aligned graphene) under femtosecond laser irradiation. This photo-induced phase transition is evidenced by the appearance of new bond lengths of 1.94A and 3.14A in the time-dependent differential pair distribution function using MeV ultrafast electron diffraction. Molecular dynamics and first principles calculation indicate that sp3 bonds nucleate at AA and AB stacked areas in moire pattern. This work sheds light on the direct graphite-to-diamond transformation mechanism, which has not been fully understood for more than 60 years.

cond-mat.mtrl-sci↗

arXiv2021

Atomistic Evidence of Nucleation Mechanism for the Direct Graphite-to-Diamond Transformation

The direct graphite-to-diamond transformation mechanism has been a subject of intense study and remains debated concerning the initial stages of the conversion, the intermediate phases, and their transformation pathways. Here, we successfully recover samples at early conversion stage by tuning high-pressure/high-temperature conditions and reveal direct evidence supporting the nucleation-growth mechanism. Atomistic observations show that intermediate orthorhombic graphite phase mediates the growth of diamond nuclei. Furthermore, we observe that quenchable orthorhombic and rhombohedra graphite are stabilized in buckled graphite at lower temperatures. These intermediate phases are further converted into hexagonal and cubic diamond at higher temperatures following energetically favorable pathways in the order: graphite -> orthorhombic graphite -> hexagonal diamond, graphite -> orthorhombic graphite -> cubic diamond, graphite -> rhombohedra graphite -> cubic diamond. These results significantly improve our understanding of the transformation mechanism, enabling the synthesis of different high-quality forms of diamond from graphite.

cond-mat.mtrl-sci↗

arXiv2020

Large anomalous Nernst and inverse spin-Hall effects in epitaxial thin films of Kagome semimetal Mn$_3$Ge

Synthesis of crystallographically well-defined thin films of topological materials is important for unraveling their mesoscale quantum properties and for device applications. Mn$_3$Ge, an antiferromagnetic Weyl semimetal with a chiral magnetic structure on a Kagome lattice, is expected to have enhanced Berry curvature around Weyl nodes near the Fermi energy, leading to large anomalous Hall / Nernst effects and a large spin-Hall effect. Using magnetron sputtering, we have grown epitaxial thin films of hexagonal D0$_{19}$ Mn$_3$Ge that are flat and continuous. Large anomalous Nernst and inverse spin-Hall effects are observed in thermoelectric and spin-pumping devices. The anomalous Nernst signal in our Mn$_3$Ge films is estimated to be 0.1 $μ$V / K, and is comparable to that in ferromagnetic Fe, despite Mn$_3$Ge having a weak magnetization of ~3.5 m$μ_B$ at room temperature. The spin mixing conductance is 90.5 nm$^{-2}$ at the Py / Mn$_3$Ge interface, and the spin-Hall angle in Mn$_3$Ge is estimated to be about 8 times of that in Pt.

cond-mat.mtrl-sci↗

arXiv2018

Enhanced Superconducting Transition Temperature in Electroplated Rhenium

We show that electroplated Re films in multilayers with noble metals such as Cu, Au, and Pd have an enhanced superconducting critical temperature relative to previous methods of preparing Re. The dc resistance and magnetic susceptibility indicate a critical temperature of approximately 6 K. Magnetic response as a function of field at 1.8 K demonstrates type-II superconductivity, with an upper critical field on the order of 2.5 T. Critical current densities greater than 10^7 A/m^2 were measured above liquid-helium temperature. Low-loss at radio frequency was obtained below the critical temperature for multilayers deposited onto resonators made with Cu traces on commercial circuit boards. These electroplated superconducting films can be integrated into a wide range of standard components for low-temperature electronics.

cond-mat.supr-con↗

arXiv2017

Tunable Low Density Palladium Nanowire Foams

Nanostructured palladium foams offer exciting potential for applications in diverse fields such as catalyst, fuel cell, and particularly hydrogen storage technologies. We have fabricated palladium nanowire foams using a cross-linking and freeze-drying technique. These foams have a tunable density down to 0.1% of the bulk, and a surface area to volume ratio of up to 1,540,000:1. They exhibit highly attractive characteristics for hydrogen storage, in terms of loading capacity, rate of absorption and heat of absorption. The hydrogen absorption/desorption process is hysteretic in nature, accompanied by substantial lattice expansion/contraction as the foam converts between Pd and PdHx.

cond-mat.mtrl-sci↗

arXiv2017

Recovering Fine Details from Under-Resolved Electron Tomography Data using HOTV Regularization

Over the last decade or so, reconstruction methods using $\ell_1$ regularization, often categorized as compressed sensing (CS) algorithms, have significantly improved the capabilities of high fidelity imaging in electron tomography. The most popular $\ell_1$ regularization approach within electron tomography has been total variation (TV) regularization. In addition to reducing unwanted noise, TV regularization encourages a piecewise constant solution with sparse boundary regions. In this paper we propose an alternative $\ell_1$ regularization approach for electron tomography based on higher order total variation (HOTV). Like TV, the HOTV approach promotes solutions with sparse boundary regions. In smooth regions however, the solution is not limited to piecewise constant behavior. We demonstrate that this allows for more accurate reconstruction of a broader class of images -- even those for which TV was designed for -- particularly when dealing with pragmatic tomographic sampling patterns and very fine image features. We develop results for an electron tomography data set as well as a phantom example, and we also make comparisons with discrete tomography approaches.

math.NA↗