Controlled Switching of Bistable Nanophase Domains on a Silicon Surface.

Switching the crystalline phase of a material via electrostatic control is a proven strategy for developing memory devices such as memristors that are based on nonvolatile resistance switching phenomena. However, phase switching in atomic-scale systems is often difficult to control and poorly understood. Here, we explore nonvolatile switching of long 2.3 nm wide bistable nanophase domains in a Sn double-layer structure grown on Si(111), using a scanning tunneling microscope. We identified two mechanisms for this phase switching phenomenon. First, the electrical field across the tunnel gap continuously tunes the relative stability of the two phases and favors one over the other depending on the tunneling polarity. The second mechanism involves carrier injection into empty Sn orbitals. The coupling between these relatively long-lived hot electrons and surface phonons induces a lattice instability at sufficiently large tunneling current and provides access to a hidden metastable state of matter. This hidden state is nonvolatile but can be erased by choosing the appropriate tunneling conditions or raising the temperature. Similar mechanisms could possibly be exploited in phase-change memristor and field effect devices.

Superconductivity in a Hole-Doped Mott-Insulating Triangular Adatom Layer on a Silicon Surface.

Adsorption of one-third monolayer of Sn on an atomically clean Si(111) substrate produces a two-dimensional triangular adatom lattice with one unpaired electron per site. This dilute adatom reconstruction is an antiferromagnetic Mott insulator; however, the system can be modulation doped and metallized using heavily doped p-type Si(111) substrates. Here, we show that the hole-doped dilute adatom layer on a degenerately doped p-type Si(111) wafer is superconducting with a critical temperature of 4.7±0.3 K. While a phonon-mediated coupling scenario would be consistent with the observed T_{c}, Mott correlations in the Sn-derived dangling-bond surface state could suppress the s-wave pairing channel. The latter suggests that the superconductivity in this triangular adatom lattice may be unconventional.

Hidden phase in a two-dimensional Sn layer stabilized by modulation hole doping.

Semiconductor surfaces and ultrathin interfaces exhibit an interesting variety of two-dimensional quantum matter phases, such as charge density waves, spin density waves and superconducting condensates. Yet, the electronic properties of these broken symmetry phases are extremely difficult to control due to the inherent difficulty of doping a strictly two-dimensional material without introducing chemical disorder. Here we successfully exploit a modulation doping scheme to uncover, in conjunction with a scanning tunnelling microscope tip-assist, a hidden equilibrium phase in a hole-doped bilayer of Sn on Si(111). This new phase is intrinsically phase separated into insulating domains with polar and nonpolar symmetries. Its formation involves a spontaneous symmetry breaking process that appears to be electronically driven, notwithstanding the lack of metallicity in this system. This modulation doping approach allows access to novel phases of matter, promising new avenues for exploring competing quantum matter phases on a silicon platform.

Realization of a Hole-Doped Mott Insulator on a Triangular Silicon Lattice.

The physics of doped Mott insulators is at the heart of some of the most exotic physical phenomena in materials research including insulator-metal transitions, colossal magnetoresistance, and high-temperature superconductivity in layered perovskite compounds. Advances in this field would greatly benefit from the availability of new material systems with a similar richness of physical phenomena but with fewer chemical and structural complications in comparison to oxides. Using scanning tunneling microscopy and spectroscopy, we show that such a system can be realized on a silicon platform. The adsorption of one-third monolayer of Sn atoms on a Si(111) surface produces a triangular surface lattice with half filled dangling bond orbitals. Modulation hole doping of these dangling bonds unveils clear hallmarks of Mott physics, such as spectral weight transfer and the formation of quasiparticle states at the Fermi level, well-defined Fermi contour segments, and a sharp singularity in the density of states. These observations are remarkably similar to those made in complex oxide materials, including high-temperature superconductors, but highly extraordinary within the realm of conventional sp-bonded semiconductor materials. It suggests that exotic quantum matter phases can be realized and engineered on silicon-based materials platforms.

Stabilization and manipulation of electronically phase-separated ground states in defective indium atom wires on silicon.

Exploration and manipulation of electronic states in low-dimensional systems are of great importance in the fundamental and practical aspects of nanomaterial and nanotechnology. Here, we demonstrate that the incorporation of vacancy defects into monatomic indium wires on n-type Si(111) can stabilize electronically phase-separated ground states where the insulating 8×2 and metallic 4×1 phases coexist. Furthermore, the areal ratio of the two phases in the phase-separated states can be tuned reversibly by electric field or charge doping, and such tunabilities can be quantitatively captured by first principles-based modeling and simulations. The present results extend the realm of electronic phase separation from strongly correlated d-electron materials typically in bulk form to weakly interacting sp-electron systems in reduced dimensionality.

Polaronic transport and current blockades in epitaxial silicide nanowires and nanowire arrays.

Crystalline micrometer-long YSi2 nanowires with cross sections as small as 1 × 0.5 nm(2) can be grown on the Si(001) surface. Their extreme aspect ratios make electron conduction within these nanowires almost ideally one-dimensional, while their compatibility with the silicon platform suggests application as metallic interconnect in Si-based nanoelectronic devices. Here we combine bottom-up epitaxial wire synthesis in ultrahigh vacuum with top-down miniaturization of the electrical measurement probes to elucidate the electronic conduction mechanism of both individual wires and arrays of nanowires. Temperature-dependent transport through individual nanowires is indicative of thermally assisted tunneling of small polarons between atomic-scale defect centers. In-depth analysis of complex wire networks emphasize significant electronic crosstalk between the nanowires due to the long-range Coulomb fields associated with polaronic charge fluctuations. This work establishes a semiquantitative correlation between the density and distributions of atomic-scale defects and resulting current-voltage characteristics of nanoscale network devices.

Correlating electronic transport to atomic structures in self-assembled quantum wires.

Quantum wires, as a smallest electronic conductor, are expected to be a fundamental component in all quantum architectures. The electronic conductance in quantum wires, however, is often dictated by structural instabilities and electron localization at the atomic scale. Here we report on the evolutions of electronic transport as a function of temperature and interwire coupling as the quantum wires of GdSi(2) are self-assembled on Si(100) wire-by-wire. The correlation between structure, electronic properties, and electronic transport are examined by combining nanotransport measurements, scanning tunneling microscopy, and density functional theory calculations. A metal-insulator transition is revealed in isolated nanowires, while a robust metallic state is obtained in wire bundles at low temperature. The atomic defects lead to electron localizations in isolated nanowire, and interwire coupling stabilizes the structure and promotes the metallic states in wire bundles. This illustrates how the conductance nature of a one-dimensional system can be dramatically modified by the environmental change on the atomic scale.

Plasmon response of a quantum-confined electron gas probed by core-level photoemission.

We demonstrate the existence of quantized "bulk" plasmons in ultrathin magnesium films on Si(111) by analyzing plasmon-loss satellites in core-level photoemission spectra, recorded as a function of the film thickness d. Remarkably, the plasmon energy is shown to vary as 1/d2 all the way down to three atomic layers. The loss spectra are dominated by the n=1 and n=2 normal modes, consistent with the excitation of plasmons involving quantized electronic subbands. With decreasing film thickness, spectral weight is gradually transferred from the plasmon modes to the low-energy single-particle excitations. These results represent striking manifestations of the role of quantum confinement on plasmon resonances in precisely controlled nanostructures.

Band gap narrowing of titanium oxide semiconductors by noncompensated anion-cation codoping for enhanced visible-light photoactivity.

"Noncompensated n-p codoping" is established as an enabling concept for enhancing the visible-light photoactivity of TiO2 by narrowing its band gap. The concept embodies two crucial ingredients: the electrostatic attraction within the n-p dopant pair enhances both the thermodynamic and kinetic solubilities, and the noncompensated nature ensures the creation of tunable intermediate bands that effectively narrow the band gap. The concept is demonstrated using first-principles calculations, and is validated by direct measurements of band gap narrowing using scanning tunneling spectroscopy, dramatically redshifted optical absorbance, and enhanced photoactivity manifested by efficient electron-hole separation in the visible-light region. This concept is broadly applicable to the synthesis of other advanced functional materials that demand optimal dopant control.

Charge-order fluctuations in one-dimensional silicides.

Metallic nanowires are of great interest as interconnects in nanoelectronic devices. They also represent important systems for understanding the complexity of electronic interactions and conductivity in one dimension. We have fabricated exceptionally long and uniform YSi(2) nanowires through self-assembly of yttrium atoms on Si(001). The wire widths are quantized in odd multiples of the Si substrate lattice constant. The thinnest wires represent one of the closest realizations of the isolated Peierls chain, exhibiting van Hove type singularities in the one-dimensional density of states and charge-order fluctuations below 150 K. The structure of the wire was determined through a detailed comparison of scanning tunnelling microscopy data and first-principles calculations. Quantized width variations along the thinnest wires produce built-in Schottky junctions, the electronic properties of which are governed by the finite size and temperature scaling of the charge-ordering correlation. This illustrates how a collective phenomenon such as charge ordering might be exploited in nanoelectronic devices.

Optimal doping control of magnetic semiconductors via subsurfactant epitaxy.

"Subsurfactant epitaxy" is established as a conceptually new approach for introducing manganese as a magnetic dopant into germanium. A kinetic pathway is devised in which the subsurface interstitial sites on Ge(100) are first selectively populated with Mn, while lateral diffusion and clustering on or underneath the surface are effectively suppressed. Subsequent Ge deposition as a capping layer produces a novel surfactantlike phenomenon as the interstitial Mn atoms float towards newly defined subsurface sites at the growth front. Furthermore, the Mn atoms that failed to float upwards are uniformly distributed within the Ge capping layer. The resulting doping levels of order 0.25 at. % would normally be considered too low for ferromagnetic ordering, but the Curie temperature exceeds room temperature by a comfortable margin. Subsurfactant epitaxy thus enables superior dopant control in magnetic semiconductors.

Tuning the quantum stability and superconductivity of ultrathin metal alloys.

Quantum confinement of itinerant electrons in atomically smooth ultrathin lead films produces strong oscillations in the thickness-dependent film energy. By adding extra electrons via bismuth alloying, we showed that both the structural stability and the superconducting properties of such films can be tuned. The phase boundary (upper critical field) between the superconducting vortex state and the normal state indicates an anomalous suppression of superconducting order just below the critical temperature, Tc. This suppression varies systematically with the film thickness and the bismuth content and can be parametrized in terms of a characteristic temperature, Tc* (less than Tc), that is inversely proportional to the scattering mean free path. The results indicate that the isotropic nature of the superconductive pairing in bulk lead-bismuth alloys is altered in the quantum regime.

A cryogenic Quadraprobe scanning tunneling microscope system with fabrication capability for nanotransport research.

We describe the development and the capabilities of an advanced system for nanoscale electrical transport studies. This system consists of a low temperature four-probe scanning tunneling microscope (STM) and a high-resolution scanning electron microscope coupled to a molecular-beam epitaxy sample preparation chamber. The four STM probes can be manipulated independently with subnanometer precision, enabling atomic resolution STM imaging and four-point electrical transport study of surface electronic systems and nanostructured materials at temperatures down to 10 K. Additionally, an integrated energy analyzer allows for scanning Auger microscopy to probe chemical species of nanostructures. Some testing results are presented.

Epitaxial stabilization of ferromagnetism in the nanophase of FeGe.

Epitaxial nanocrystals of FeGe have been stabilized on Ge(111). The nanocrystals assume a quasi-one-dimensional shape as they grow exclusively along the <110> direction of the Ge(111) substrate, culminating in a compressed monoclinic modification of FeGe. Whereas monoclinic FeGe is antiferromagnetic in the bulk, the nanowires are surprisingly strong ferromagnets below approximately 200 K with an average magnetic moment of 0.8 microB per Fe atom. Density functional calculations indicate an unusual stabilization mechanism for the observed ferromagnetism: lattice compression destabilizes the antiferromagnetic Peierls-like ground state observed in the bulk while increased p-d hybridization suppresses the magnetic moments and stabilizes ferromagnetism.

Linear magnetization dependence of the intrinsic anomalous Hall effect.

The anomalous Hall effect is investigated experimentally and theoretically for ferromagnetic thin films of Mn5Ge3. We have separated the intrinsic and extrinsic contributions to the experimental anomalous Hall effect and calculated the intrinsic anomalous Hall conductivity from the Berry curvature of the Bloch states using first-principles methods. The intrinsic anomalous Hall conductivity depends linearly on the magnetization, which can be understood from the long-wavelength fluctuations of the spin orientation at finite temperatures. The quantitative agreement between theory and experiment is remarkably good, not only near 0 K but also at finite temperatures, up to about approximately 240 K (0.8TC).