arXiv subjects

Leslie Schoop

Publications and source records attributed to Leslie Schoop.

11 recordsLinked to original sources

arXiv2026

Mechanochemical Nano-Writing of an Atomically Thin Metal

Mechanical energy accelerates many physicochemical processes, including materials syntheses that are hard to produce with thermal energy alone. However, physical understanding connecting applied mechanical forces with internal stresses and ensuing reaction mechanisms is lacking. Here we demonstrate mechanical force-enabled synthesis and nanoscale patterning to metallize a two-dimensional (2D) material, producing an atomically-thin superconducting material. Localized force applied by atomic force microscope tips to van der Waals (vdW) encapsulated stacks of 2D bilayer MoTe2 and adjacent source Pd guides 2D Pd7MoTe2 growth with 50 nm lateral resolution. Force accelerates reaction kinetics exponentially per Eyring's stress-assisted thermal activation model, reducing synthesis temperatures from ~200 °C to near-room temperature. Finite element simulations, density functional theory, and ab-initio grand canonical Monte Carlo calculations show that tip-induced compression facilitates Pd chemisorption to tensile-strained MoTe2 that converts to uniform Pd7MoTe2. This demonstrates a new, generalizable paradigm for nanoscale synthesis of quantum materials, and high-precision engineering of superconductivity.

cond-mat.mes-hall↗

arXiv2025

Visualizing the internal structure of the charge-density-wave state in CeSbTe

The collective reorganization of electrons into a charge density wave has long served as a textbook example of an ordered phase in condensed matter physics. Two-dimensional square lattices with $p$ electrons are well-suited to the realization of charge density waves, due to the anisotropy of the $p$ orbitals and the resulting one dimensionality of the electronic structure. In spite of a long history of study of charge density waves in square-lattice systems, few reports have recognized the significance of a hidden orbital degree of freedom. The degeneracy of $p_x$ and $p_y$ electrons may give rise to orbital patterns in real space that endow the charge density wave with additional broken symmetries or unusual order parameters. Here, we use scanning tunneling microscopy to visualize the internal structure of the charge-density-wave state of CeSbTe, which contains Sb square lattices with 5$p$ electrons. We image atomic-sized, anisotropic lobes of charge density with periodically modulating anisotropy, which we interpret in terms of a superposition of $p_x$ and $p_y$ bond density waves. Our results support the fact that delocalized $p$ orbitals can reorganize into emergent electronic states of matter.

cond-mat.mes-hall↗

arXiv2024

Direct evidence for efficient carrier multiplication in the topological insulator Bi$_2$Se$_3$

Carrier multiplication (CM), where the absorption of a single photon results in the generation of several electron-hole pairs via impact ionization, plays a pivotal role in the quest for enhancing the performance of solar cells beyond the Shockley-Queisser limit. The combination of its narrow bandgap relative to the photon energy of visible light, along with its low phonon frequencies that hinder efficient energy dissipation into phonons, makes the topological insulator Bi$_2$Se$_3$ an optimal candidate material for efficient CM. Here we use time- and angle-resolved photoemission spectroscopy (trARPES) to trace the number of electron-hole pairs after photoexcitation of Bi$_2$Se$_3$ with visible pump pulses at $\hbarω=2$ eV. We find that both the number of electrons inside the conduction band as well as the number of holes inside the valence band keep increasing long after the pump pulse is gone, providing direct evidence for CM. We also analyze the transient band structure as well as the hot carrier dynamics inside the conduction band, providing a complete picture of the non-equilibrium carrier dynamics in photoexcited Bi$_2$Se$_3$ which can now serve as a basis for novel optoelectronic applications.

cond-mat.mtrl-sci↗

arXiv2022

Photoinduced Band Renormalization Effects in ZrSiS Topological Nodal-line Semimetal

Out-of-equilibrium effects provide an elegant pathway to probing and understanding the underlying physics of topological materials. Creating exotic states of matter using ultrafast optical pulses in particular has shown promise towards controlling electronic band structure properties. Of recent interest is band renormalization in Dirac and Weyl semimetals as it leads to direct physical observables through the enhancement of the effective mass, or, in the shift of resonant energies. Here we provide experimental and theoretical signatures of photo-induced renormalization of the electronic band structure in a topological nodal line semimetal ZrSiS. Specifically, we show how the change of the transient reflectivity spectra under femtosecond optical excitations is induced by out-of-equilibrium effects that renormalize the kinetic energy of electrons. We associate the observed spectral shift to an enhancement of the effective mass and to a red-shift of the resonant frequency as a function of pump field strength. Finally, we show that the transient relaxation dynamics of the reflectivity is primarily an electronic effect with negligible phononic contribution. Our study presents the modifications of electronic properties in ZrSiS using ultrashort pulses, and demonstrates the potential of this approach in creating photo-induced phases in topological quantum mater through an all-optical route.

cond-mat.mtrl-sci↗

arXiv2020

A systematic study of stacked square nets: from Dirac fermions to material realizations

Non-symmorphic symmetries protect Dirac line nodes in square net materials. This phenomenon has been most prominently observed in ZrSiS. Here, we systematically study the symmetry-protected nodal fermions that result from different ways of embedding the square net into a larger unit cell. Surprisingly, we find that a nonsymmorphic space group is not a necessary condition for a filling enforced semimetal: symmorphic space groups can also host nodal fermions that are enforced by band folding and electron count, that is, a combination of a particular structural motif combined with electron filling. We apply the results of this symmetry analysis to define an algorithm, which we utilize to find square net materials with nodal fermions in specific symmorphic space groups. We highlight one result of this search, the compound ThGeSe, which has not been discussed before in the context of nodal fermions. Finally, we discuss how band folding can impose constraints on band connectivity beyond the connectivity of single elementary band representations.

cond-mat.mes-hall↗

arXiv2018

Chemical Principles of Topological Semimetals

Initiated by the discovery of topological insulators, topologically non-trivial materials have attracted immense interest in the physics community in the past decade. One of the latest additions to the field, the material class of topological semimetals, has grown at an extremely fast rate . While the prototype of a topological semimetal, graphene, has been known for a while, the first 3D analogues of graphene have only been discovered recently. This review, written from a chemistry perspective, intends to make the growing field of topological semimetals accessible to the wider community of materials scientists and scholars from related disciplines. To this end, we describe key features of topological semimetals, embedded in their electronic structure, and how they can be achieved based on chemical principles. We introduce the different classes of topological semimetals and review their salient representatives. Finally, selected properties and potential applications of these materials are discussed.

cond-mat.mtrl-sci↗

arXiv2017

Ir d-band Derived Superconductivity in the Lanthanum-Iridium System LaIr3

The electronic properties of the heavy metal superconductor LaIr3 are reported. The estimated superconducting parameters obtained from physical properties measurements indicate that LaIr3 is a BCS-type superconductor. Electronic band structure calculations show that Ir d- states dominate the Fermi level. A comparison of electronic band structures of LaIr3 and LaRh3 shows that the Ir-compound has a strong spin-orbit-coupling effect, which creates a complex Fermi surface.

cond-mat.supr-con↗

arXiv2015

Breakdown of Three-dimensional Dirac Semimetal State in pressurized Cd3As2

We report the first observation of a pressure-induced breakdown of the 3D-DSM state in Cd3As2, evidenced by a series of in-situ high-pressure synchrotron X-ray diffraction (XRD) and single crystal transport measurements. We find that Cd3As2 undergoes a structural phase transition from a metallic tetragonal (T) phase in space group I41/acd to a semiconducting monoclinic (M) phase in space group P21/c at critical pressure 2.57 GPa, above this pressure, an activation energy gap appears, accompanied by distinct switches in Hall resistivity slope and electron mobility. These changes of crystal symmetry and corresponding transport properties manifest the breakdown of the 3D-DSM state in pressurized Cd3As2.

cond-mat.supr-con↗

arXiv2015

Correlation of Crystal Quality and Extreme Magnetoresistance of WTe$_2$

High quality single crystals of WTe$_2$ were grown using a Te flux followed by a cleaning step involving self-vapor transport. The method is reproducible and yields consistently higher quality single crystals than are typically obtained via halide assisted vapor transport methods. Magnetoresistance (MR)values at 9 Tesla and 2 Kelvin as high as 1.75 million \%, nearly an order of magnitude higher than previously reported for this material, were obtained on crystals with residual resistivity ratio (RRR) of approximately 1250. The MR follows a near B$^2$ law (B = 1.95(1)) and, assuming a semiclassical model, the average carrier mobility for the highest quality crystal was found to be ~167,000 cm$^2$/Vs at 2 K. A correlation of RRR, MR ratio and average carrier mobility ($μ_{avg}$) is found with the cooling rate during the flux growth.

cond-mat.mtrl-sci↗

arXiv2014

Titanic Magnetoresistance in WTe2

Magnetoresistance is the change of a material's electrical resistance in response to an applied magnetic field. In addition to its intrinsic scientific interest, it is a technologically important property, placing it in "Pasteur's quadrant" of research value: materials with large magnetorsistance have found use as magnetic sensors 1, in magnetic memory 2, hard drives 3, transistors 4, and are the subject of frequent study in the field of spintronics 5, 6. Here we report the observation of an extremely large one-dimensional positive magnetoresistance (XMR) in the layered transition metal dichalcogenide (TMD) WTe2; 452,700 percent at 4.5 Kelvin in a magnetic field of 14.7 Tesla, and 2.5 million percent at 0.4 Kelvin in 45 Tesla, with no saturation. The XMR is highly anisotropic, maximized in the crystallographic direction where small pockets of holes and electrons are found in the electronic structure. The determination of the origin of this effect and the fabrication of nanostructures and devices based on the XMR of WTe2 will represent a significant new direction in the study and uses of magnetoresistivity. *The published version of the paper includes co-authors Tian Liang and Max Hirschberger. **This paper has been published with new MR data to 60T where the MR of WTe2 reaches 13 million percent (at 0.5K) and still shows no signs of saturation. We also have new electron diffraction patterns to lower temperature (10K). We discuss the possible origin of the MR as coming from an electron-hole 'resonance' condition established by a perfect n/p ratio of 1 (more details in a new "extended data" section). This makes WTe2, possibly, the first realization of a perfectly balanced semimetal. ***The paper is published as "Large non-saturating magnetoresistance in WTe2" in Nature (2014), DOI:10.1038/nature13763

cond-mat.mtrl-sci↗

arXiv2013

Superconductivity in the Cu(Ir1-xPtx)2Se4 Spinel

We report the observation of superconductivity in the CuIr2Se4 spinel induced by partial substitution of Pt for Ir. The optimal doping level for superconductivity in Cu(Ir1-xPtx)2Se4 is x = 0.2, where Tc is 1.76 K. A superconducting Tc vs. composition dome is established between the metallic, normal conductor CuIr2Se4 and semiconducting CuIrPtSe4. Electronic structure calculations show that the optimal Tc occurs near the electron count of a large peak in the calculated electronic density of states and that CuIrPtSe4 is a band-filled insulator. Characterization of the superconducting state in this heavy metal spinel through determination of ΔC/γTc, indicates that it is BCS-like. The relatively high upper critical field at the optimal superconducting composition (Hc2(0) = 3.2 T) is much larger than that reported for analogous rhodium spinels and is comparable to or exceeds the Pauli field (mu0Hp), suggesting that strong spin orbit coupling may influence the superconducting state. Further, comparison to doped CuIr2S4 suggests that superconductivity in iridium spinels is not necessarily associated with the destabilization of a charge-ordered spin-paired state through doping.

cond-mat.supr-con↗