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The bulk-boundary correspondence is a key concept in topological quantum materials. For instance, a quantum spin Hall insulator features a bulk insulating gap with gapless helical boundary states protected by the underlying Z2 topology. However, the bulk-boundary dichotomy and distinction are rarely explored in optical experiments, which can provide unique information about topological charge carriers beyond transport and electronic spectroscopy techniques. Here, we utilize mid-infrared absorption micro-spectroscopy and pump-probe micro-spectroscopy to elucidate the bulk-boundary optical responses of Bi4Br4, a recently discovered room-temperature quantum spin Hall insulator. Benefiting from the low energy of infrared photons and the high spatial resolution, we unambiguously resolve a strong absorption from the boundary states while the bulk absorption is suppressed by its insulating gap. Moreover, the boundary absorption exhibits a strong polarization anisotropy, consistent with the one-dimensional nature of the topological boundary states. Our infrared pump-probe microscopy further measures a substantially increased carrier lifetime for the boundary states, which reaches one nanosecond scale. The nanosecond lifetime is about one to two orders longer than that of most topological materials and can be attributed to the linear dispersion nature of the helical boundary states. Our findings demonstrate the optical bulk-boundary dichotomy in a topological material and provide a proof-of-principal methodology for studying topological optoelectronics., Comment: 26 pages, 4 figures

The quasi-one-dimensional van der Waals compound Bi$_4$Br$_4$ was recently found to be a promising high-order topological insulator with exotic electronic states. In this paper, we study the electrical transport properties of Bi$_4$Br$_4$ bulk crystals. Two electron-type samples with different electron concentrations are investigated. Both samples have saturation resistivity behavior in low temperature. In the low-concentration sample, two-dimensional quantum oscillations are clearly observed in the magnetoresistance measurements, which are attributed to the band-bending-induced surface state on the (001) facet. In the high-concentration sample, the angular magnetoresistance exhibits two pairs of symmetrical sharp valleys with an angular difference close to the angle between the crystal planes (001) and (100). The additional valley can be explained by the contribution of the boundary states on the (100) facet. Besides, Hall measurements at low temperatures reveal an anomalous decrease of electron concentration with increasing temperature, which can be explained by the temperature-induced Lifshitz transition. These results shed light on the abundant surface and boundary state transport signals and the temperature-induced Lifshitz transition in Bi$_4$Br$_4$.

The inferior electrical contact to two-dimensional (2D) materials is a critical challenge for their application in post-silicon very large-scale integrated circuits. Electrical contacts were generally related to their resistive effect, quantified as contact resistance. With a systematic investigation, this work demonstrates a capacitive metal-insulator-semiconductor (MIS) field-effect at the electrical contacts to 2D materials: the field-effect depletes or accumulates charge carriers, redistributes the voltage potential, and give rise to abnormal current saturation and nonlinearity. On the one hand, the current saturation hinders the devices' driving ability, which can be eliminated with carefully engineered contact configurations. On the other hand, by introducing the nonlinearity to monolithic analog artificial neural network circuits, the circuits' perception ability can be significantly enhanced, as evidenced using a COVID-19 critical illness prediction model. This work provides a comprehension of the field-effect at the electrical contacts to 2D materials, which is fundamental to the design, simulation, and fabrication of electronics based on 2D material.

The rising of quantum spin Hall insulators (QSHI) in two-dimensional (2D) systems has been attracting significant interest in current research, for which the 1D helical edge states, a hallmark of QSHI, are widely expected to be a promising platform for next-generation optoelectronics. However, the dynamics of the 1D edge states has not yet been experimentally addressed. Here, we report the observation of optical response of the topological helical edge states in a-Bi4Br4, using the infrared-pump infrared-probe microscopic spectroscopy. Remarkably, we observe that the carrier lifetime of the helical edge states reaches nanosecond-scale at room temperature, which is about 2 - 3 orders longer than that of most 2D topological surface states and is even comparable with that of the well developed optoelectronics semiconductors used in modern industry. The ultralong carrier lifetime of the topological edge states may be attributed to their helical and 1D nature. Our findings not only provide an ideal material for further investigations of the carrier dynamics of 1D helical edge states but also pave the way for its application in optoelectronics., Comment: 18 pages, 4 figures, 57 references

Two-dimensional topological insulator features time-reversal-invariant spin-momentum-locked one-dimensional (1D) edge states with a linear energy dispersion. However, experimental access to 1D edge states is still of great challenge and only limited to few techniques to date. Here, by using infrared absorption spectroscopy, we observed robust topologically originated edge states in a-Bi4Br4 belts with definitive signature of strong infrared absorption at belt sides and distinct anisotropy with respect to light polarizations, which is further supported by first-principles calculations. Our work demonstrates for the first time that the infrared spectroscopy can offer a power-efficient approach in experimentally probing 1D edge states of topological materials., Comment: 15 pages, 5 figures, 29 references

Photo sensing and energy harvesting based on exotic properties of quantum materials and new operation principles have great potentials to break the fundamental performance limit of conventional photodetectors and solar cells. As topological nontrivial materials, Weyl semimetals have demonstrated novel optoelectronic properties that promise potential applications in photo detection and energy harvesting arising from their gapless linear dispersion near Weyl nodes and Berry field enhanced nonlinear optical effect at the vicinity of Weyl nodes. In this work, we demonstrate robust photocurrent generation from charge separation of photoexctied electron-hole pairs at the edge of Td-WTe2, a type-II Weyl semimetal, due to crystalline-symmetry breaking along certain crystal fracture directions and possibly enhanced by robust fermi-arc type surface states. Using scanning photocurrent microscopy (SPCM) measurements, we further demonstrate that the edge current response is robust over a wide excitation photon energy. We find that this robust feature is highly generic, and shall arise universally in a wide class of quantum materials with similar crystal symmetries. In addition, possible connections between these edge photocurrents and topological properties of Weyl semimetals are explored. The robust and generic edge current response demonstrated in this work provides a new type of charge separation mechanism for photosensing and energy harvesting over broad wavelength range.

Weyl semimetals have been classified into type-I and type-II with respect to the geometry of their Fermi surfaces at the Weyl points. Here, we propose a new class of Weyl semimetal, whose unique Fermi surface contains two electron or two hole pockets touching at a multi-Weyl point, dubbed as type-III Weyl semimetal. Based on first-principles calculations, we first show that quasi-one-dimensional compound (TaSe4)2I is a type-III Weyl semimetal with larger chiral charges. (TaSe4)2I can support four-fold helicoidal surface states with remarkably long Fermi arcs on the (001) surface. Angle-resolved photoemission spectroscopy measurements are in agreement with the gapless nature of (TaSe4)2I at room temperature and reveal its characteristic dispersion. In addition, our calculations show that external strain could induce topological phase transitions in (TaSe4)2I among the type-III, type-II, and type-I Weyl semimetals, accompanied with the Lifshitz transitions of the Fermi surfaces. Therefore, our work first experimentally indicates (TaSe4)2I as a type-III Weyl semimetal and provides a promising platform to further investigate the novel physics of type-III Weyl fermions., Comment: 5 figures

We report the magnetization, electrical resistivity, specific heat measurements and band structure calculations of layered superconductor SnTaS$_2$. The experiments are performed on single crystals grown by chemical vapor transport method. The resistivity and magnetic susceptibility indicate that SnTaS$_2$ is a type-II superconductor with transition temperature $T_c = 3$ K. The upper critical field ($H_{c2}$) shows large anisotropy for magnetic field parallel to $ab$ plane ($H//ab$) and $c$ axis ($H//c$), and the temperature dependence of $H_{c2}$ for $H//ab$ shows obvious unconventional upward feature at low temperature. Band structure of SnTaS$_2$ shows several band crossings near the Fermi level, which form three nodal lines in the k$_z$ = 0 plane resulting in drumhead-like surface states when spin-orbit coupling is not considered. These results indicate that SnTaS$_2$ is a superconductor with possible topological nodal line semimetal character.

A new two-dimensional material, the C$_2$N holey 2D (C$_2$N-$h$2D) crystal, has recently been synthesized. Here we investigate the strain effects on the properties of this new material by first-principles calculations. We show that the material is quite soft with a small stiffness constant and can sustain large strains $\geq 12\%$. It remains a direct gap semiconductor under strain and the bandgap size can be tuned in a wide range as large as 1 eV. Interestingly, for biaxial strain, a band crossing effect occurs at the valence band maximum close to a 8\% strain, leading to a dramatic increase of the hole effective mass. Strong optical absorption can be achieved by strain tuning with absorption coefficient $\sim10^6$ cm$^{-1}$ covering a wide spectrum. Our findings suggest the great potential of strain-engineered C$_2$N-$h$2D in electronic and optoelectronic device applications., Comment: 5 pages, 6 figures