arXiv subjects

Steven C. Erwin

Publications and source records attributed to Steven C. Erwin.

At least 19 recordsLinked to original sources

arXiv2024

Topological boundary states in engineered quantum-dot molecules on the InAs(111)A surface

Atom manipulation by scanning tunneling microscopy was used to construct quantum dots on the InAs(111)A surface. Each dot comprised six ionized indium adatoms. The positively charged adatoms create a confining potential acting on surface-state electrons, leading to the emergence of a bound state associated with the dot. By lining up the dots into N-dot chains with alternating tunnel coupling between them, quantum-dot molecules were constructed that revealed electronic boundary states as predicted by the Su-Schrieffer-Heeger (SSH) model of one-dimensional topological phases. Dot chains with odd N were constructed such that they host a single end or domain-wall state, allowing one to probe the localization of the boundary state on a given sublattice by scanning tunneling spectroscopy. We found probability density also on the forbidden sublattice together with an asymmetric energy spectrum of the chain-confined states. This deviation from the SSH model arises because the dots are charged and create a variation in onsite potential along the chain - which does not remove the boundary states but shifts their energy away from the midgap position. Our results demonstrate that topological boundary states can be created in quantum-dot arrays engineered with atomic-scale precision.

cond-mat.mes-hall↗

arXiv2023

Quantum dots on the InAs(110) cleavage surface created by atom manipulation

Cryogenic scanning tunneling microscopy was employed in combination with density-functional theory calculations to explore quantum dots made of In adatoms on the InAs(110) surface. Each adatom adsorbs at a surface site coordinated by one cation and two anions, and transfers one electron to the substrate, creating an attractive quantum well for electrons in surface states. We used the scanning-probe tip to assemble the positively charged adatoms into precisely defined quantum dots exhibiting a bound state roughly 0.1 eV below the Fermi level at an intrinsic linewidth of only ~4 meV, as revealed by scanning tunneling spectroscopy. For quantum-dot dimers, we observed the emergence of a bonding and an antibonding state with even and odd wave-function character, respectively, demonstrating the capability to engineer quasi-molecular electronic states. InAs(110) constitutes a promising platform in this respect because highly perfect surfaces can be readily prepared by cleavage and charged adatoms can be generated in-situ by the scanning-probe tip.

cond-mat.mes-hall↗

arXiv2021

Topological States in Dimerized Quantum-Dot Chains Created by Atom Manipulation

Topological electronic phases exist in a variety of naturally occurring materials but can also be created artificially. We used a cryogenic scanning tunneling microscope to create dimerized chains of identical quantum dots on a semiconductor surface and to demonstrate that these chains give rise to one-dimensional topological phases. The dots were assembled from charged adatoms, creating a confining potential with single-atom precision acting on electrons in surface states of the semiconductor. Quantum coupling between the dots leads to electronic states localized at the ends of the chains, as well as at deliberately created internal domain walls, in agreement with the predictions of the Su-Schrieffer-Heeger model. Scanning tunneling spectroscopy also reveals deviations from this well-established model manifested in an asymmetric level spectrum and energy shifts of the boundary states. The deviations arise because the dots are charged and hence lead to an onsite potential that varies along the chain. We show that this variation can be mitigated by electrostatic gating using auxiliary charged adatoms, enabling fine-tuning of the boundary states and control of their quantum superposition. The experimental data, which are complemented by theoretical modeling of the potential and the resulting eigenstates, reveal the important role of electrostatics in these engineered quantum structures.

cond-mat.mes-hall↗

arXiv2016

How semiconductor nanoplatelets form

Colloidal nanoplatelets - quasi-two-dimensional sheets of semiconductor exhibiting efficient, spectrally pure fluorescence - form when liquid-phase syntheses of spherical quantum dots are modified. Despite intense interest in their properties, the mechanism behind their anisotropic shape and precise atomic-scale thickness remains unclear, and even counterintuitive when their crystal structure is isotropic. One commonly accepted explanation is that nanoclusters nucleate within molecular templates and then fuse. Here, we test this mechanism for zincblende nanoplatelets and show that they form instead due to an intrinsic instability in growth kinetics. We synthesize CdSe and CdS1-xSex nanoplatelets in template- and solvent-free isotropic melts containing only cadmium carboxylate and chalcogen, a finding incompatible with previous explanations. Our model, based on theoretical results showing enhanced growth on narrow surface facets, rationalizes nanoplatelet formation and experimental dependencies on temperature, time, and carboxylate length. Such understanding should lead to improved syntheses, controlled growth on surfaces, and broader libraries of nanoplatelet materials.

cond-mat.mtrl-sci↗

arXiv2016

Diffraction at GaAs/Fe$_{3}$Si core/shell nanowires: the formation of nanofacets

GaAs/Fe$_{3}$Si core/shell nanowire structures were fabricated by molecular-beam epitaxy on oxidized Si(111) substrates and investigated by synchrotron x-ray diffraction. The surfaces of the Fe$_3$Si shells exhibit nanofacets. These facets consist of well pronounced Fe$_3$Si{111} planes. Density functional theory reveals that the Si-terminated Fe$_3$Si{111} surface has the lowest energy in agreement with the experimental findings. We can analyze the x-ray diffuse scattering and diffraction of the ensemble of nanowires avoiding the signal of the substrate and poly-crystalline films located between the wires. Fe$_3$Si nanofacets cause streaks in the x-ray reciprocal space map rotated by an azimuthal angle of 30° compared with those of bare GaAs nanowires. In the corresponding TEM micrograph the facets are revealed only if the incident electron beam is oriented along [1$\overline{1}$0] in accordance with the x-ray results. Additional maxima in the x-ray scans indicate the onset of chemical reactions between Fe$_{3}$Si shells and GaAs cores occurring at increased growth temperatures.

cond-mat.mtrl-sci↗

arXiv2016

Spin Chains and Electron Transfer at Stepped Silicon Surfaces

High-index surfaces of silicon with adsorbed gold can reconstruct to form highly ordered linear step arrays. These steps take the form of a narrow strip of graphitic silicon. In some cases - specifically, for Si(553)-Au and Si(557)-Au - a large fraction of the silicon atoms at the exposed edge of this strip are known to be spin-polarized and charge-ordered along the edge. The periodicity of this charge ordering is always commensurate with the structural periodicity along the step edge and hence leads to highly ordered arrays of local magnetic moments that can be regarded as "spin chains". Here, we demonstrate theoretically as well as experimentally that the closely related Si(775)-Au surface has - despite its very similar overall structure - zero spin polarization at its step edge. Using a combination of density-functional theory and scanning tunneling microscopy, we propose an electron-counting model that accounts for these differences. The model also predicts that unintentional defects and intentional dopants can create local spin moments at Si(hhk)-Au step edges. We analyze in detail one of these predictions and verify it experimentally. This finding opens the door to using techniques of surface chemistry and atom manipulation to create and control silicon spin chains.

cond-mat.str-el↗

arXiv2016

Gating a single-molecule transistor with individual atoms

Transistors, regardless of their size, rely on electrical gates to control the conductance between source and drain contacts. In atomic-scale transistors, this conductance is exquisitely sensitive to single electrons hopping via individual orbitals. Single-electron transport in molecular transistors has been previously studied using top-down approaches to gating, such as lithography and break junctions. But atomically precise control of the gate - which is crucial to transistor action at the smallest size scales - is not possible with these approaches. Here, we used individual charged atoms, manipulated by a scanning tunnelling microscope, to create the electrical gates for a single-molecule transistor. This degree of control allowed us to tune the molecule into the regime of sequential single-electron tunnelling, albeit with a conductance gap more than one order of magnitude larger than observed previously. This unexpected behaviour arises from the existence of two different orientational conformations of the molecule, depending on its charge state. Our results show that strong coupling between these charge and conformational degrees of freedom leads to new behaviour beyond the established picture of single-electron transport in atomic-scale transistors.

cond-mat.mes-hall↗

arXiv2014

Microscopic Theory of Cation Exchange in CdSe Nanocrystals

Although poorly understood, cation-exchange reactions are increasingly used to dope or transform colloidal semiconductor nanocrystals (quantum dots). We used density-functional theory and kinetic Monte Carlo simulations to develop a microscopic theory that explains structural, optical, and electronic changes observed experimentally in Ag-cation-exchanged CdSe nanocrystals. We find that Coulomb interactions, both between ionized impurities and with the polarized nanocrystal surface, play a key role in cation exchange. Our theory also resolves several experimental puzzles related to photoluminescence and electrical behavior in CdSe nanocrystals doped with Ag.

cond-mat.mes-hall↗

arXiv2013

Theory of magnetic enhancement in strontium hexaferrite through Zn-Sn pair substitution

We study the site occupancy and magnetic properties of Zn-Sn substituted M-type Sr-hexaferrite SrFe$_{12-x}$(Zn$_{0.5}$Sn$_{0.5}$)$_x$O$_{19}$ with x = 1 using first-principles total-energy calculations. We find that in a ground-state configuration Zn-Sn ions preferentially occupy $4f_1$ and $4f_2$ sites unlike the model previously suggested by Ghasemi et al. [J. Appl. Phys, \textbf{107}, 09A734 (2010)], where Zn$^{2+}$ and Sn$^{4+}$ ions occupy the $2b$ and $4f_2$ sites. Density-functional theory calculations show that our model has a lower total energy by more than 0.2 eV per unit cell compared to Ghasemi's model. More importantly, the latter does not show an increase in saturation magnetization ($M_s$) compared to the pure $M$-type Sr-hexaferrite, in disagreement with the experiment. On the other hand, our model correctly predicts a rapid increase in $M_s$ as well as a decrease in magnetic anisotropy compared to the pure $M$-type Sr-hexaferrite, consistent with experimental measurements.

cond-mat.mtrl-sci↗

arXiv2013

Silicon spin chains at finite temperature: dynamics of Si(553)-Au

When gold is deposited on Si(553), the surface self-assembles to form a periodic array of steps with nearly perfect structural order. In scanning tunneling microscopy these steps resemble quasi-one-dimensional atomic chains. At temperatures below ~50 K the chains develop tripled periodicity. We recently predicted, on the basis of density-functional theory calculations at T=0, that this tripled periodicity arises from the complete polarization of the electron spin on every third silicon atom along the step; in the ground state these linear chains of silicon spins are antiferromagnetically ordered. Here we explore, using ab-initio molecular dynamics and kinetic Monte Carlo simulations, the behavior of silicon spin chains on Si(553)-Au at finite temperature. Thermodynamic phase transitions at T>0 in one-dimensional systems are prohibited by the Mermin-Wagner theorem. Nevertheless we find that a surprisingly sharp onset occurs upon cooling---at about 30 K for perfect surfaces and at higher temperature for surfaces with defects---to a well-ordered phase with tripled periodicity, in good agreement with experiment.

cond-mat.mtrl-sci↗

arXiv2011

Epitaxial interfaces between crystallographically mismatched materials

We report an unexpected mechanism by which an epitaxial interface can form between materials having strongly mismatched lattice constants. A simple model is proposed in which one material tilts out of the interface plane to create a coincidence-site lattice that balances two competing geometrical criteria---low residual strain and short coincidence-lattice period. We apply this model, along with complementary first-principles total-energy calculations, to the interface formed by molecular-beam epitaxy of cubic Fe on hexagonal GaN and find excellent agreement between theory and experiment.

cond-mat.mtrl-sci↗

arXiv2010

Intrinsic magnetism at silicon surfaces

It has been a long-standing goal to create magnetism in a nonmagnetic material by manipulating its structure at the nanometer scale. This idea may be realized in graphitic carbon: evidence suggests magnetic states at the edges of graphene ribbons and at grain boundaries in graphite. Such phenomena have long been regarded as unlikely in silicon because there is no graphitic bulk phase. Here we show theoretically that intrinsic magnetism indeed exists in a class of silicon surfaces whose step edges have a nanoscale graphitic structure. This magnetism is intimately connected to recent observations, including the coexistence of double- and triple-period distortions and the absence of edge states in photoemission. Magnetism in silicon may ultimately provide a path toward spin-based logic and storage at the atomic level.

cond-mat.mtrl-sci↗

arXiv2009

Structure and energetics of Si(111)-(5x2)-Au

We propose a new structural model for the Si(111)-(5x2)-Au reconstruction. The model incorporates a new experimental value of 0.6 monolayer for the coverage of gold atoms, equivalent to six gold atoms per 5x2 cell. Five main theoretical results, obtained from first-principles total-energy calculations, support the model. (1) In the presence of silicon adatoms the periodicity of the gold rows spontaneously doubles, in agreement with experiment. (2) The dependence of the surface energy on the adatom coverage indicates that a uniformly covered phase is unstable and will phase-separate into empty and covered regions, as observed experimentally. (3) Theoretical scanning tunneling microscopy images are in excellent agreement with experiment. (4) The calculated band structure is consistent with angle-resolved photoemission spectra; analysis of their correspondence allows the straightforward assignment of observed surface states to specific atoms. (5) The calculated activation barrier for diffusion of silicon adatoms along the row direction is in excellent agreement with the experimentally measured barrier.

cond-mat.mtrl-sci↗

arXiv2008

Stability and structure of atomic chains on Si(111)

We study the stability and structure of self-assembled atomic chains on Si(111) induced by monovalent, divalent and trivalent adsorbates, using first-principles total-energy calculations and scanning tunneling microscopy. We find that only structures containing exclusively silicon honeycomb or silicon Seiwatz chains are thermodynamically stable, while mixed configurations, with both honeycomb and Seiwatz chains, may be kinetically stable. The stability and structure of these atomic chains can be understood using a surprisingly simple electron-counting rule.

cond-mat.other↗

arXiv2007

Bipolar spintronics: From spin injection to spin-controlled logic

An impressive success of spintronic applications has been typically realized in metal-based structures which utilize magnetoresistive effects for substantial improvements in the performance of computer hard drives and magnetic random access memories. Correspondingly, the theoretical understanding of spin-polarized transport is usually limited to a metallic regime in a linear response, which, while providing a good description for data storage and magnetic memory devices, is not sufficient for signal processing and digital logic. In contrast, much less is known about possible applications of semiconductor-based spintronics and spin-polarized transport in related structures which could utilize strong intrinsic nonlinearities in current-voltage characteristics to implement spin-based logic. Here we discuss the challenges for realizing a particular class of structures in semiconductor spintronics: our proposal for bipolar spintronic devices in which carriers of both polarities (electrons and holes) contribute to spin-charge coupling. We formulate the theoretical framework for bipolar spin-polarized transport, and describe several novel effects in two- and three-terminal structures which arise from the interplay between nonequilibrium spin and equilibrium magnetization.

cond-mat.other↗

arXiv2007

Thermodynamics of carrier-mediated magnetism in semiconductors

We propose a model of carrier-mediated ferromagnetism in semiconductors that accounts for the temperature dependence of the carriers. The model permits analysis of the thermodynamic stability of competing magnetic states, opening the door to the construction of magnetic phase diagrams. As an example we analyze the stability of a possible reentrant ferromagnetic semiconductor, in which increasing temperature leads to an increased carrier density, such that the enhanced exchange coupling between magnetic impurities results in the onset of ferromagnetism as temperature is raised.

cond-mat.mtrl-sci↗

arXiv2006

Determination of Interface Atomic Structure and Its Impact on Spin Transport Using Z-Contrast Microscopy and Density-Functional Theory

We combine Z-contrast scanning transmission electron microscopy with density-functional-theory calculations to determine the atomic structure of the Fe/AlGaAs interface in spin-polarized light-emitting diodes. A 44% increase in spin-injection efficiency occurs after a low-temperature anneal, which produces an ordered, coherent interface consisting of a single atomic plane of alternating Fe and As atoms. First-principles transport calculations indicate that the increase in spin-injection efficiency is due to the abruptness and coherency of the annealed interface.

cond-mat.mtrl-sci↗

arXiv2005

Phase transition at finite temperature in one dimension: Adsorbate ordering in Ba/Si(111)3x2

We demonstrate that the Ba-induced Si(111)3x2 reconstruction is a physical realization of a one-dimensional antiferromagnetic Ising model with long-range Coulomb interactions. Monte Carlo simulations performed on a corresponding Coulomb-gas model, which we construct based on density-functional calculations, reveal an adsorbate-ordering phase transition at finite temperature. We show numerically that this unusual one-dimensional phase transition should be detectable by low-energy electron diffraction.

cond-mat.mtrl-sci↗