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The downscaling of nonlinear optical devices is significantly hindered by the inherently weak nonlinearity in regular materials. Here, we report a giant third-harmonic generation discovered in epitaxial thin films of V-VI chalcogenide topological insulators. Using a tailored substrate and capping layer, a single reflection from a 13 nm film can produce a nonlinear conversion efficiency of nearly 0.01%, a performance that rivals micron-scale waveguides made from conventional materials or metasurfaces with far more complex structures. Such strong nonlinear optical emission, absent from the topologically trivial member in the same compound family, is found to be generated by the same bulk band characteristics that are responsible for producing the band inversion and the nontrivial topological ordering. This finding reveals the possibility of obtaining superior optical nonlinearity by examining the large pool of newly discovered topological materials with similar band characteristics.

The de Gennes extrapolation length is a direction dependent measure of the spatial evolution of the pairing gap near the boundary of a superconductor, and thus provides a viable means to probe its symmetry. It is expected to be infinite and isotropic for plain s-wave pairing, and finite and anisotropic for d-wave. Here, we synthesize single layer FeSe films on SrTiO3(001) (STO) substrates by molecular beam epitaxy, and measure the de Gennes extrapolation length by scanning tunneling microscopy/spectroscopy. We find a 40% reduction of the superconducting gap near specular [110]Fe edges, yielding an extrapolation length of 8.0 nm. However, near specular [010]Fe edges the extrapolation length is nearly infinite. These findings are consistent with a phase changing pairing with 2-fold symmetry, indicating d-wave superconductivity. This is further supported by the presence of in-gap states near the specular [110]Fe edges, but not the [010]Fe edges. This work provides direct experimental evidence for d-wave superconductivity in single layer FeSe/STO, and demonstrates quasiparticle scattering at boundaries to be a viable phase sensitive probe of pairing symmetry in Fe-based superconductors., Comment: 18 pages, 4 figures

Despite the rapid progress in understanding the first intrinsic magnetic topological insulator MnBi$_2$Te$_4$, its electronic structure remains a topic under debates. Here we perform a thorough spectroscopic investigation into the electronic structure of MnBi$_2$Te$_4$ via laser-based angle-resolved photoemission spectroscopy. Through quantitative analysis, we estimate an upper bound of 3 meV for the gap size of the topological surface state. Furthermore, our circular dichroism measurements reveal band chiralities for both the topological surface state and quasi-2D bands, which can be well reproduced in a band hybridization model. A numerical simulation of energy-momentum dispersions based on a four-band model with an additional step potential near the surface provides a promising explanation for the origin of the quasi-2D bands. Our study represents a solid step forward in reconciling the existing controversies in the electronic structure of MnBi$_2$Te$_4$, and provides an important framework to understand the electronic structures of other relevant topological materials MnBi$_{2n}$Te$_{3n+1}$., 4 figures

Tailoring magnetic orders in topological insulators is critical to the realization of topological quantum phenomena. An outstanding challenge is to find a material where atomic defects lead to tunable magnetic orders while maintaining a nontrivial topology. Here, by combining magnetization measurements, angle-resolved photoemission spectroscopy, and transmission electron microscopy, we reveal disorder-enabled, tunable magnetic ground states in MnBi$_6$Te$_{10}$. In the ferromagnetic phase, an energy gap of 15 meV is resolved at the Dirac point on the MnBi$_2$Te$_4$ termination. In contrast, antiferromagnetic MnBi$_6$Te$_{10}$ exhibits gapless topological surface states on all terminations. Transmission electron microscopy and magnetization measurements reveal substantial Mn vacancies and Mn migration in ferromagnetic MnBi$_6$Te$_{10}$. We provide a conceptual framework where a cooperative interplay of these defects drives a delicate change of overall magnetic ground state energies, and leads to tunable magnetic topological orders. Our work provides a clear pathway for nanoscale defect-engineering towards the realization of topological quantum phases., Comment: 22 pages, 3 figures

How superconductivity emerges from antiferromagnetic ordering is an essential question for Fe-based superconductors. Here, we explore the effect of dimensionality on the interplay between antiferromagnetic ordering and superconductivity by investigating nanoribbons of single-layer FeTe1-xSex films grown on SrTiO3(001) substrates by molecular beam epitaxy. Using scanning tunneling microscopy/spectroscopy, we find a one-dimensional (1D) superconducting channel 2 nm wide with a TC of 42 ± 4 K on the edge of FeTe1-xSex (x < 0.1) ribbons, coexisting with a non-superconducting ribbon interior that remains bicollinear antiferromagnetically ordered. Density functional theory calculations indicate that both Se and the presence of the edge destabilize the bicollinear antiferromagnetic magnetic order, resulting in a paramagnetic region near the edge with strong local checkerboard fluctuations that is conducive to superconductivity. Our results represent the highest TC achieved in 1D superconductors and demonstrate an effective route toward stabilizing superconductivity in Fe-based superconductors at reduced dimensions.

Using migration enhanced molecular beam epitaxy, we synthesize single- and bilayer ${\mathrm{WSe}}_{2}$ on epitaxial graphene/SiC(0001) and investigate the electronic properties of their edges with different terminations using scanning tunneling microscopy/spectroscopy (STM/S). Density functional theory calculations predict edge states at both Se and W edges, whose position and spatial distribution depend on how the edges are terminated. STS reveals that whether edge states at the nominal W edge are detectable depends on the number and spatial distribution of additional Se, whereas edge states on the Se edge are always detectable. Our findings indicate that edge termination plays an important role on edge states, and modification of the edge is a viable means to tailor the electronic properties of ${\mathrm{WSe}}_{2}$ nanostructures.

One of the most striking properties of three-dimensional topological insulators (TIs) is spin-momentum locking, where the spin is locked at right angles to momentum and hence an unpolarized charge current creates a net spin polarization. Alternatively, if a net spin is injected into the TI surface state system, it is distinctively associated with a unique carrier momentum and hence should generate a charge accumulation, as in the so-called inverse Edelstein effect. Here using a Fe/Al2O3/BN tunnel barrier, we demonstrate both effects in a single device in Bi2Te3: the electrical detection of the spin accumulation generated by an unpolarized current flowing through the surface states, and that of the charge accumulation generated by spins injected into the surface state system. This work is the first to utilize BN as part of a hybrid tunnel barrier on TI, where we observed a high spin polarization of 93% for the TI surfaces states. The reverse spin-to-charge measurement is an independent confirmation that spin and momentum are locked in the surface states of TI, and offers additional avenues for spin manipulation. It further demonstrates the robustness and versatility of electrical access to the spin system within TI surface states, an important step towards its utilization in TI-based spintronics devices.

Three-dimensional (3D) Dirac cones are predicted to reside in semimetals A3Bi (A = Na, K). By using molecular beam epitaxy (MBE) and scanning tunneling microscopy (STM), we have successfully established the growth conditions for Na3Bi thin films on Si(1 1 1)-7 × 7, and determined that the lattice of Na3Bi is rotated by 30 degree with respect to that of Si(1 1 1)-7 × 7. The Na3Bi/Si(1 1 1)-7 × 7 thin film was further used as the substrate for the growth of K3Bi. The 3D Dirac-cone-like electronic band structures of Na3Bi and K3Bi have been clearly revealed by angle resolved photoelectron spectroscopy (ARPES).

We present the growth of atomically flat topological crystalline insulator (TCI) SnTe films on Si(111) substrate by molecular beam epitaxy (MBE). The growth condition for achieving high quality SnTe film was established by a combination of reflection high energy electron diffraction (RI-TEED) and scanning tunneling microscopy (STM) studies. In-situ angle resolved photoemission spectroscopy (ARPES) measurements elucidate the topological nature of the SnTe films. The electronic structure of SnTe films can be tuned by film thickness and Pb doping. The success in growing high quality SnTe thin films with tunable electronic structure is crucial for potential device applications. (C) 2013 Elsevier B.V. All rights reserved.

Grain boundaries (GBs) are inherent extended defects in chemical vapor deposited (CVD) transition metal dichalcogenide (TMD) films. Characterization of the atomic structure and electronic properties of these GBs is crucial for understanding and controlling the properties of TMDs via defect engineering. Here, we report the atomic and electronic structure of GBs in CVD grown MoS2 on epitaxial graphene/SiC(0001). Using scanning tunneling microscopy/spectroscopy, we find that GBs mostly consist of arrays of dislocation cores, where the presence of mid-gap states shifts both conduction and valence band edges by up to 1 eV. Our findings demonstrate the first charging effect near GBs in CVD grown MoS2, providing insights into the significant impact GBs can have on materials properties.

The surface of a topological crystalline insulator (TCI) carries an even number of Dirac cones protected by crystalline symmetry. We epitaxially grew high-quality Pb(1-x)Sn(x)Te(111) films and investigated the TCI phase by in situ angle-resolved photoemission spectroscopy. Pb(1-x)Sn(x)Te(111) films undergo a topological phase transition from a trivial insulator to TCI via increasing the Sn/Pb ratio, accompanied by a crossover from n-type to p-type doping. In addition, a hybridization gap is opened in the surface states when the thickness of the film is reduced to the two-dimensional limit. The work demonstrates an approach to manipulating the topological properties of TCI, which is of importance for future fundamental research and applications based on TCI.

Atomically flat thin films of topological semimetal Na3Bi are grown on double-layer graphene formed on 6H-SiC(0001) substrates by molecular beam epitaxy. By combined techniques of molecular beam epitaxy, scanning tunneling microscopy and angle resolved photoelectron spectroscopy, the growth conditions for Na3Bi thin films on double-layer graphene are successfully established. The band structure of Na3Bi grown on graphene is mapped along (Gamma) over bar-(M) over bar and (Gamma) over bar-(K) over bar directions. Furthermore, the energy band of Na3Bi at higher energy is uncovered by doping Cs atoms on the surface.

In this letter, we report a systematic study of topological crystalline insulator PbxSn1-xTe (0 < x < 1) thin films grown by molecular beam epitaxy on SrTiO3(001). Two domains of PbxSn1-xTe thin films with intersecting angle of α ≈ 45° were confirmed by reflection high energy diffraction, scanning tunneling microscopy, and angle-resolved photoemission spectroscopy (ARPES). ARPES study of PbxSn1-xTe thin films demonstrated that the Fermi level of PbTe could be tuned by altering the temperature of substrate whereas SnTe cannot. An M-shaped valance band structure was observed only in SnTe but PbTe is in a topological trivial state with a large gap. In addition, co-evaporation of SnTe and PbTe results in an equivalent variation of Pb concentration as well as the Fermi level of PbxSn1-xTe thin films.