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Register a new userOptical investigation of thermoelectric topological crystalline insulator Pb$_{0.77}$Sn$_{0.23}$Se
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Pb$_{0.77}$Sn$_{0.23}$Se is a novel alloy of two promising thermoelectric materials PbSe and SnSe that exhibits a temperature dependent band inversion below 300 K. Recent work has shown that this band inversion also coincides with a trivial to nontrivial topological phase transition. To understand how the properties critical to thermoelectric efficiency are affected by the band inversion, we measured the broadband optical response of Pb$_{0.77}$Sn$_{0.23}$Se as a function of temperature. We find clear optical evidence of the band inversion at $160pm15$ K, and use the extended Drude model to accurately determine a $T^{3/2}$ dependence of the bulk carrier lifetime, associated with electron-acoustic phonon scattering. Due to the high bulk carrier doping level, no discriminating signatures of the topological surface states are found, although their presence cannot be excluded from our data.
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Topological insulators are a novel class of quantum materials in which time-reversal symmetry, relativistic (spin-orbit) effects and an inverted band structure result in electronic metallic states on the surfaces of bulk crystals. These helical states exhibit a Dirac-like energy dispersion across the bulk bandgap, and they are topologically protected. Recent theoretical proposals have suggested the existence of topological crystalline insulators, a novel class of topological insulators in which crystalline symmetry replaces the role of time-reversal symmetry in topological protection [1,2]. In this study, we show that the narrow-gap semiconductor Pb(1-x)Sn(x)Se is a topological crystalline insulator for x=0.23. Temperature-dependent magnetotransport measurements and angle-resolved photoelectron spectroscopy demonstrate that the material undergoes a temperature-driven topological phase transition from a trivial insulator to a topological crystalline insulator. These experimental findings add a new class to the family of topological insulators. We expect these results to be the beginning of both a considerable body of additional research on topological crystalline insulators as well as detailed studies of topological phase transitions.
Optical and Hall-effect measurements have been performed on single crystals of Pb$_{0.77}$Sn$_{0.23}$Se, a IV-VI mixed chalcogenide. The temperature dependent (10--300 K) reflectance was measured over 40--7000 cm$^{-1}$ (5--870 meV) with an extension to 15,500 cm$^{-1}$ (1.92 eV) at room temperature. The reflectance was fit to the Drude-Lorentz model using a single Drude component and several Lorentz oscillators. The optical properties at the measured temperatures were estimated via Kramers-Kronig analysis as well as by the Drude-Lorentz fit. The carriers were p-type with the carrier density determined by Hall measurements. A signature of valence intraband transition is found in the low-energy optical spectra. It is found that the valence-conduction band transition energy as well as the free carrier effective mass reach minimum values at 100 K, suggesting temperature-driven band inversion in the material. Density function theory calculation for the electronic band structure also make similar predictions.
Since the advent of topological insulators hosting symmetry-protected Dirac surface states, efforts have been made to gap these states in a controllable way. A new route to accomplish this was opened up by the discovery of topological crystalline insulators (TCIs) where the topological states are protected by real space crystal symmetries and thus prone to gap formation by structural changes of the lattice. Here, we show for the first time a temperature-driven gap opening in Dirac surface states within the TCI phase in (Pb,Sn)Se. By using angle-resolved photoelectron spectroscopy, the gap formation and mass acquisition is studied as a function of composition and temperature. The resulting observations lead to the addition of a temperature- and composition-dependent boundary between massless and massive Dirac states in the topological phase diagram for (Pb,Sn)Se (001). Overall, our results experimentally establish the possibility to tune between a massless and massive topological state on the surface of a topological system.
Topological crystalline insulators represent a novel topological phase of matter in which the surface states are protected by discrete point group-symmetries of the underlying lattice. Rock-salt lead-tin-selenide alloy is one possible realization of this phase which undergoes a topological phase transition upon changing the lead content. We used scanning tunneling microscopy (STM) and angle resolved photoemission spectroscopy (ARPES) to probe the surface states on (001) Pb$_{1-x}$Sn$_{x}$Se in the topologically non-trivial (x=0.23) and topologically trivial (x=0) phases. We observed quasiparticle interference with STM on the surface of the topological crystalline insulator and demonstrated that the measured interference can be understood from ARPES studies and a simple band structure model. Furthermore, our findings support the fact that Pb$_{0.77}$Sn$_{0.23}$Se and PbSe have different topological nature.
In addition to novel surface states, topological insulators can also exhibit robust gapless states at crystalline defects. Step edges constitute a class of common defects on the surface of crystals. In this work we establish the topological nature of one-dimensional (1D) bound states localized at step edges of the [001] surface of a topological crystalline insulator (TCI) Pb$_{0.7}$Sn$_{0.3}$Se, both theoretically and experimentally. We show that the topological stability of the step edge states arises from an emergent particle-hole symmetry of the surface low-energy physics, and demonstrate the experimental signatures of the particle-hole symmetry breaking. We also reveal the effects of an external magnetic field on the 1D bound states. Our work suggests the possibility of similar topological step edge modes in other topological materials with a rocks-salt structure.
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