ACS Photonics · 2020 · 26 citations · 36 references
Natural SciencesMaterials SciencePhysicsCondensed Matter PhysicsSemiconductor MaterialsSolid State PhysicsOptical Properties Of SolidsSemiconducting MaterialsSemiconductor PhysicsSurface PhysicsTerahertz SpectroscopyTopological MaterialsDirac Surface StatesPhase Transition DynamicsPulse Excitation ResponseTopological InsulatorsUltrafast Carrier DynamicsUltrafast Electron DynamicsUltrafast Optical ResponseUltrafast Spectroscopy
Resolving the complex interplay between surface and bulk response is a long-standing issue in the topological insulators (TIs). Some studies have reported surface-dominated metallic responses, yet others show semiconducting-like bulk photoconductance. Using ultrafast terahertz spectroscopy with the advent of Fermi-level engineered TIs, we discovered that such difference arises from the time-dependent competing process of two parameters, namely, the Dirac-carrier surface scattering rate and the bulk Drude weight. After infrared femtosecond pulse excitation, we observed a metal-like photoconductance reduction for the prototypical n-type Bi2Se3 and a semiconductor-like increased photoconductance for the p-type Bi2Se3. Surprisingly, the bulk-insulating Bi2Se3, which is presumably similar to graphene, exhibits a semiconducting-to-metallic phase apparent transition at 10 ps. The sign-reversed, yet long-lasting (≥500 ps) metallic photoconductance was observed only in the bulk-insulating Bi2Se3, indicating that such dynamic phase transition is governed by the time-dependent competing interplay between the surface scattering rate and the bulk Drude weight. Our observations illustrate new photophysical phenomena of the photoexcited-phase transition in TIs and demonstrate entirely distinct dynamics compared to graphene and conventional gapped semiconductors.
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