Long-lifetime spin excitations near domain walls in 1T-TaS2.

SignificanceThere is an intense ongoing search for two-level quantum systems with long lifetimes for applications in quantum communication and computation. Much research has been focused on studying isolated spins in semiconductors or band insulators. Mott insulators provide an interesting alternative platform but have been far less explored. In this work we use a technique capable of resolving individual spins at atomic length scales, to measure the two-level switching of spin states in 1T-TaS2. We find quasi-1D chains of spin-1/2 electrons embedded in 1T-TaS2 which have exceptionally long lifetimes. The discovery of long-lived spin states in a tractable van der Waal material opens doors to using Mott systems in future quantum information applications.

Charge Density Wave Vortex Lattice Observed in Graphene-Passivated 1T-TaS2 by Ambient Scanning Tunneling Microscopy.

The nearly commensurate charge density wave (CDW) excitations native to the transition-metal dichalcogenide crystal, 1T-TaS2, under ambient conditions are revealed by scanning tunneling microscopy (STM) and spectroscopy (STS) measurements of a graphene/TaS2 heterostructure. Surface potential measurements show that the graphene passivation layer prevents oxidation of the air-sensitive 1T-TaS2 surface. The graphene protective layer does not however interfere with probing the native electronic properties of 1T-TaS2 by STM/STS, which revealed that nearly commensurate CDW hosts an array of vortex-like topological defects. We find that these topological defects organize themselves to form a lattice with quasi-long-range order, analogous to the vortex Bragg glass in type-II superconductors but accessible in ambient conditions.

Excitations of Intercalated Metal Monolayers in Transition Metal Dichalcogenides.

We combine Raman scattering spectroscopy and lattice dynamics calculations to reveal the fundamental excitations of the intercalated metal monolayers in the FexTaS2 (x = 1/4, 1/3) family of materials. Both in- and out-of-plane modes are identified, each of which has trends that depend upon the metal-metal distance, the size of the van der Waals gap, and the metal-to-chalcogenide slab mass ratio. We test these trends against the response of similar systems, including Cr-intercalated NbS2 and RbFe(SO4)2, and demonstrate that the metal monolayer excitations are both coherent and tunable. We discuss the consequences of intercalated metal monolayer excitations for material properties and developing applications.

Ultrafast Modulations and Detection of a Ferro-Rotational Charge Density Wave Using Time-Resolved Electric Quadrupole Second Harmonic Generation.

We show the ferro-rotational nature of the commensurate charge density wave (CCDW) in 1T-TaS_{2} and track its dynamic modulations by temperature-dependent and time-resolved electric quadrupole rotation anisotropy-second harmonic generation (EQ RA-SHG), respectively. The ultrafast modulations manifest as the breathing and the rotation of the EQ RA-SHG patterns at three frequencies around the reported single CCDW amplitude mode frequency. A sudden shift of the triplet frequencies and a dramatic increase in the breathing and rotation magnitude further reveal a photoinduced transient CDW phase across a critical pump fluence of ∼0.5 mJ/cm^{2}.

Atomic-Scale Observation of Topological Vortices in the Incommensurate Charge Density Wave of 2H-TaSe2.

It has been only recently realized that topological vortices associated with structural distortions or ordered spins are rather common in numerous materials where long-range interactions are not dominant. Incommensurate modulations that frequently occur in charge density wave (CDW) materials are often understood in terms of discommensurations with a periodic phase shift. The accumulation of a one-dimensional (1D) phase shift can result in, for example, CDW dislocations in 2H-TaSe2 with incommensurate CDW (I-CDW). Since any atomic-scale experimental investigation of CDW dislocations in 2H-TaSe2 has been lacking, we have performed the atomic-scale observation of 2H-TaSe2 with I-CDW, stabilized with Pd intercalation or strain, with scanning probe microscopy, and unveiled the existence of topological Z6 or Z4 vortices with topologically protected 2D winding movements of atomic displacement vectors. The discovery opens the ubiquitous nature of topological vortex domains and a new avenue to explore new facets of various incommensurate modulations or discommensurations.

Honeycomb-Lattice Mott Insulator on Tantalum Disulphide.

Effects of electron many-body interactions amplify in an electronic system with a narrow bandwidth opening a way to exotic physics. A narrow band in a two-dimensional (2D) honeycomb lattice is particularly intriguing as combined with Dirac bands and topological properties but the material realization of a strongly interacting honeycomb lattice described by the Kane-Mele-Hubbard model has not been identified. Here we report a novel approach to realize a 2D honeycomb-lattice narrow-band system with strongly interacting 5d electrons. We engineer a well-known triangular lattice 2D Mott insulator 1T-TaS_{2} into a honeycomb lattice utilizing an adsorbate superstructure. Potassium (K) adatoms at an optimum coverage deplete one-third of the unpaired d electrons and the remaining electrons form a honeycomb lattice with a very small hopping. Ab initio calculations show extremely narrow Z_{2} topological bands mimicking the Kane-Mele model. Electron spectroscopy detects an order of magnitude bigger charge gap confirming the substantial electron correlation as confirmed by dynamical mean field theory. It could be the first artificial Mott insulator with a finite spin Chern number.

Kinkless Electronic Junction along 1D Electronic Channel Embedded in a Van Der Waals Layer.

Here, the formation of type-I and type-II electronic junctions with or without any structural discontinuity along a well-defined 1 nm-wide 1D electronic channel within a van der Waals layer is reported. Scanning tunneling microscopy and spectroscopy techniques are employed to investigate the atomic and electronic structure along peculiar domain walls formed on the charge-density-wave phase of 1T-TaS2 . Distinct kinds of abrupt electronic junctions with discontinuities of the band gap along the domain walls are found, some of which even do not have any structural kinks and defects. Density-functional calculations reveal a novel mechanism of the electronic junction formation; they are formed by a kinked domain wall in the layer underneath through substantial electronic interlayer coupling. This work demonstrates that the interlayer electronic coupling can be an effective control knob over nanometer-scale electronic property of 2D atomic monolayers.

Dual Higgs modes entangled into a soliton lattice in CuTe.

Recently discovered Higgs particle is a key element in the standard model of elementary particles and its analogue in materials, massive Higgs mode, has elucidated intriguing collective phenomena in a wide range of materials with spontaneous symmetry breaking such as antiferromagnets, cold atoms, superconductors, superfluids, and charge density waves (CDW). As a straightforward extension beyond the standard model, multiple Higgs particles have been considered theoretically but not yet for Higgs modes. Here, we report the real-space observations, which suggest two Higgs modes coupled together with a soliton lattice in a solid. Our scanning tunneling microscopy reveals the 1D CDW state of an anisotropic transition metal monochalcogenide crystal CuTe is composed of two distinct but degenerate CDW structures by the layer inversion symmetry broken. More importantly, the amplitudes of each CDW structure oscillate in an out-of-phase fashion to result in a regular array of alternating domains with repeating phase-shift domain walls. This unusual finding is explained by the extra degeneracy in CDWs within the standard Landau theory of the free energy. The multiple and entangled Higgs modes demonstrate how novel collective modes can emerge in systems with distinct symmetries broken simultaneously.

Real-space observation of fluctuating antiferromagnetic domains.

Magnetic domains play a fundamental role in physics of magnetism and its technological applications. Dynamics of antiferromagnetic domains is poorly understood, although antiferromagnets are expected to be extensively used in future electronic devices wherein it determines the stability and operational speed. Dynamics of antiferromagnets also features prominently in the studies of topological quantum matter. Real-space imaging of fluctuating antiferromagnetic domains is therefore highly desired but has never been demonstrated. We use coherent x-ray diffraction to obtain videos of fluctuating micrometer-scale antiferromagnetic domains in Ni2MnTeO6 on time scales from 10-1 to 103 s. In the collinear phase, thermally activated domain wall motion is observed in the vicinity of the Néel temperature. Unexpectedly, the fluctuations persist through the full range of the higher-temperature helical phase. These observations illustrate the high potential significance of the dynamic domain imaging in phase transition studies and in magnetic device research.

Crystal and Magnetic Structures of La2CoPtO6 Double Perovskite.

We investigated the crystal structure and magnetic structure in cobaltite-platinate double perovskite of La2CoPtO6, employing various techniques of X-ray diffraction, neutron diffraction, and the extended X-ray absorption fine structure analysis. It is shown that the crystal symmetry is maintained as P21/n in the temperature range of <500 °C, whereas the lattice constants and the Co-Co distances undergo a continuous structural evolution toward the high-symmetry phases with increasing temperature. The Co-O bonds were overall longer and had a larger degree of structural and thermal disorders than the Pt-O bonds. As for the magnetism, an antiferromagnetic order is stabilized in the Co2+ sublattice at temperatures below 28 K. It is demonstrated that owing to the substantial distortions (quantified by a distortion parameter Σ > 0.03 Å) of the Co-Co networks, the system is not subject to spin frustration effect. Details in the magnetic structure are determined; at 12 K, the Co magnetic moment was (0.8, 0, 2.7) Bohr magneton, the magnetic propagation vector was (-0.5, 0, 0.5), and the magnetic symmetry was preferably Γ1(Ag).

Antiferromagnetic ordering in Li2MnO3 single crystals with a two-dimensional honeycomb lattice.

Li(2)MnO(3) consists of a layered Mn honeycomb lattice separated by a single layer of LiO(6) octahedra along the c-axis. By using single crystal Li(2)MnO(3) samples, we have examined the physical properties and carried out both powder and single crystal neutron diffraction studies to determine that Mn moments order antiferromagnetically at T(N) = 36 K with an ordered magnetic moment of 2.3 µ(B) perpendicular to the ab plane. We have also discovered that about 35% of the full magnetic entropy is released in the supposedly simple paramagnetic phase, indicative of unusual spin dynamics at higher temperature.