Dominant role of two-photon vertex in nonlinear response in two-dimensional Dirac systems

We show that the standard concepts of nonlinear response to electromagnetic fields break down in two-dimensional Dirac systems, like graphene, in the quantum regime close to the Dirac point. We present a compelling many-body theory for nonlinear transport focusing on disorder scattering as a benchmark example. We show that, although the diamagnetic two-photon vertex is absent at the non-interacting level, disorder effects give rise to a self-generation of such two-photon vertex surviving even in the clean limit. We predict that the two-photon vertex self-generation is present only in two dimensions. The impact of such a striking scenario on the nonlinear quantum transport is discussed, predicting a huge enhancement of third-order dc conductivity comparing to the common models.

Theory of optical responses in clean multi-band superconductors

Electromagnetic responses in superconductors provide valuable information on the pairing symmetry as well as physical quantities such as the superfluid density. However, at the superconducting gap energy scale, optical excitations of the Bogoliugov quasiparticles are forbidden in conventional Bardeen-Cooper-Schrieffer superconductors when momentum is conserved. Accordingly, far-infrared optical responses have been understood in the framework of a dirty-limit theory by Mattis and Bardeen for over 60 years. Here we show, by investigating the selection rules imposed by particle-hole symmetry and unitary symmetries, that intrinsic momentum-conserving optical excitations can occur in clean multi-band superconductors when one of the following three conditions is satisfied: (i) inversion symmetry breaking, (ii) symmetry protection of the Bogoliubov Fermi surfaces, or (iii) simply finite spin-orbit coupling with unbroken time reversal and inversion symmetries. This result indicates that clean-limit optical responses are common beyond the straightforward case of broken inversion symmetry. We apply our theory to optical responses in FeSe, a clean multi-band superconductor with inversion symmetry and significant spin-orbit coupling. This result paves the way for studying clean-limit superconductors through optical measurements.

Two-dimensional charge order stabilized in clean polytype heterostructures

Strong evidence suggests that transformative correlated electron behavior may exist only in unrealized clean-limit 2D materials such as 1T-TaS2. Unfortunately, experiment and theory suggest that extrinsic disorder in free standing 2D layers impedes correlation-driven quantum behavior. Here we demonstrate a new route to realizing fragile 2D quantum states through epitaxial polytype engineering of van der Waals materials. The isolation of truly 2D charge density waves (CDWs) between metallic layers stabilizes commensurate long-range order and lifts the coupling between neighboring CDW layers to restore mirror symmetries via interlayer CDW twinning. The twinned-commensurate charge density wave (tC-CDW) reported herein has a single metal–insulator phase transition at ∼350 K as measured structurally and electronically. Fast in-situ transmission electron microscopy and scanned nanobeam diffraction map the formation of tC-CDWs. This work introduces epitaxial polytype engineering of van der Waals materials to access latent 2D ground states distinct from conventional 2D fabrication.

Quantum frequency doubling in the topological insulator Bi2Se3

The nonlinear Hall effect due to Berry curvature dipole (BCD) induces frequency doubling, which was recently observed in time-reversal-invariant materials. Here we report novel electric frequency doubling in the absence of BCD on a surface of the topological insulator Bi2Se3 under zero magnetic field. We observe that the frequency-doubling voltage transverse to the applied ac current shows a threefold rotational symmetry, whereas it forbids BCD. One of the mechanisms compatible with the symmetry is skew scattering, arising from the inherent chirality of the topological surface state. We introduce the Berry curvature triple, a high-order moment of the Berry curvature, to explain skew scattering under the threefold rotational symmetry. Our work paves the way to obtain a giant second-order nonlinear electric effect in high mobility quantum materials, as the skew scattering surpasses other mechanisms in the clean limit.

Clean 2D superconductivity in a bulk van der Waals superlattice

Advances in low-dimensional superconductivity are often realized through improvements in material quality. Apart from a small group of organic materials, there is a near absence of clean-limit two-dimensional (2D) superconductors, which presents an impediment to the pursuit of numerous long-standing predictions for exotic superconductivity with fragile pairing symmetries. We developed a bulk superlattice consisting of the transition metal dichalcogenide (TMD) superconductor 2H-niobium disulfide (2H-NbS2) and a commensurate block layer that yields enhanced two-dimensionality, high electronic quality, and clean-limit inorganic 2D superconductivity. The structure of this material may naturally be extended to generate a distinct family of 2D superconductors, topological insulators, and excitonic systems based on TMDs with improved material properties.

Variation of the giant intrinsic spin Hall conductivity of Pt with carrier lifetime

More than a decade after the first theoretical and experimental studies of the spin Hall conductivity (SHC) of Pt, both its dominant origin and amplitude remain in dispute. We report the experimental determination of the rapid variation of the intrinsic SHC of Pt with the carrier lifetime (τ) in the dirty-metal regime by incorporating finely dispersed MgO intersite impurities into the Pt, while maintaining its essential band structure. This conclusively validates the theoretical prediction that the SHC in Pt in the dirty-metal regime should be dominated by the intrinsic contribution, and should decrease rapidly with shortening τ. When interfacial spin backflow is taken into account, the intrinsic SHC of Pt in the clean limit is at least 1.6 × 106 (ℏ/2e) ohm−1 m−1, more than 3.5 times greater than the available theoretical predictions. Our work also establishes a compelling spin Hall metal Pt0.6(MgO)0.4 with an internal giant spin Hall ratio of 0.73.

Temperature-Dependent s± ↔ s++ Transitions in the Multiband Model for Fe-Based Superconductors with Impurities

We study the dependence of the superconducting gaps on both the disorder and the temperature within the two-band model for iron-based materials. In the clean limit, the system is in the s± state with sign-changing gaps. Scattering by nonmagnetic impurities leads to the change of the sign of the smaller gap, resulting in a transition from the s± to the s++ state with the sign-preserving gaps. We show here that the transition is temperature-dependent. Thus, there is a line of s±→s++ transition in the temperature–disorder phase diagram. There is a narrow range of impurity scattering rates, where the disorder-induced s±→s++ transition occurs at low temperatures, but then the low-temperature s++ state transforms back to the s± state at higher temperatures. With increasing impurity scattering rate, the temperature of such s++→s± transition shifts to the critical temperature Tc, and only the s++ state is left for higher amounts of disorder.

Spin jam induced by quantum fluctuations in a frustrated magnet

Since the discovery of spin glasses in dilute magnetic systems, their study has been largely focused on understanding randomness and defects as the driving mechanism. The same paradigm has also been applied to explain glassy states found in dense frustrated systems. Recently, however, it has been theoretically suggested that different mechanisms, such as quantum fluctuations and topological features, may induce glassy states in defect-free spin systems, far from the conventional dilute limit. Here we report experimental evidence for existence of a glassy state, which we call a spin jam, in the vicinity of the clean limit of a frustrated magnet, which is insensitive to a low concentration of defects. We have studied the effect of impurities on SrCr9pGa12-9pO19 [SCGO(p)], a highly frustrated magnet, in which the magnetic Cr3+ (s = 3/2) ions form a quasi-2D triangular system of bipyramids. Our experimental data show that as the nonmagnetic Ga3+ impurity concentration is changed, there are two distinct phases of glassiness: an exotic glassy state, which we call a spin jam, for the high magnetic concentration region (p>0.8) and a cluster spin glass for lower magnetic concentration (p<0.8). This observation indicates that a spin jam is a unique vantage point from which the class of glassy states of dense frustrated magnets can be understood.