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Photocurrents in Bi2Se3: bulk versus surface, and injection versus shift currents

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 Publication date 2016
  fields Physics
and research's language is English




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Optical injection and detection of charge currents can complement conventional transport and photoemission measurements without the necessity of invasive contact that may disturb the system being examined. This is a particular concern for the surface states of a topological insulator. In this work one- and two-color sources of photocurrents are examined in epitaxial, thin films of Bi2Se3. We demonstrate that optical excitation and terahertz detection simultaneously captures one- and two- color photocurrent contributions, as previously not required in other material systems. A method is devised to isolate the two components, and in doing so each can be related to surface or bulk excitations through symmetry. This strategy allows surface states to be examined in a model system, where they have independently been verified with angle-resolved photoemission spectroscopy.

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Films of the topological insulator Bi2Se3 are grown by molecular beam epitaxy with in-situ reflection high-energy electron diffraction. The films are shown to be high-quality by X-ray reflectivity and diffraction and atomic-force microscopy. Quantum interference control of photocurrents is observed by excitation with harmonically related pulses and detected by terahertz radiation. The injection current obeys the expected excitation irradiance dependence, showing linear dependence on the fundamental pulse irradiance and square-root irradiance dependence of the frequency-doubled optical pulses. The injection current also follows a sinusoidal relative-phase dependence between the two excitation pulses. These results confirm the third-order nonlinear optical origins of the coherently controlled injection current. Experiments are compared to a tight-binding band structure to illustrate the possible optical transitions that occur in creating the injection current.
Topological insulators (TIs) are predicted to be composed of an insulating bulk state along with conducting channels on the boundary of the material. In Bi2Se3, however, the Fermi level naturally resides in the conduction band due to intrinsic doping by selenium vacancies, leading to metallic bulk states. In such non-ideal TIs it is not well understood how the surface and bulk states behave under environmental disorder. In this letter, based on transport measurements of Bi2Se3 thin films, we show that the bulk states are sensitive to environmental disorder but the surface states remain robust.
In ideal topological insulator (TI) films the bulk state, which is supposed to be insulating, should not provide any electric coupling between the two metallic surfaces. However, transport studies on existing TI films show that the topological states on opposite surfaces are electrically tied to each other at thicknesses far greater than the direct coupling limit where the surface wavefunctions overlap. Here, we show that as the conducting bulk channels are suppressed, the parasitic coupling effect diminishes and the decoupled surface channels emerge as expected for ideal TIs. In Bi2Se3 thin films with fully suppressed bulk states, the two surfaces, which are directly coupled below ~10 QL, become gradually isolated with increasing thickness and are completely decoupled beyond ~20 QL. On such a platform, it is now feasible to implement transport devices whose functionality relies on accessing the individual surface layers without any deleterious coupling effects.
By studying Fe-doped ZnO pellets and thin films with various x-ray spectroscopic techniques, and complementing this with density functional theory calculations, we find that Fe-doping in bulk ZnO induces isovalent (and isostructural) cation substitution (Fe2+ -> Zn2+). In contrast to this, Fe-doping near the surface produces both isovalent and heterovalent substitution (Fe3+ -> Zn2+). The calculations performed herein suggest that the most likely defect structure is the single or double substitution of Zn with Fe, although, if additional oxygen is available, then Fe substitution with interstitial oxygen is even more energetically favourable. Furthermore, it is found that ferromagnetic states are energetically unfavourable, and ferromagnetic ordering is likely to be realized only through the formation of a secondary phase (i.e. ZnFe2O4), or codoping with Cu.
We theoretically investigate the one-color injection currents and shift currents in zigzag graphene nanoribbons with applying a static electric field across the ribbon, which breaks the inversion symmetry to generate nonzero second order optical responses by dipole interaction. These two types of currents can be separately excited by specific light polarization, circularly polarized lights for injection currents and linearly polarized lights for shift currents. Based on a tight binding model formed by carbon 2p$_z$ orbitals, we numerically calculate the spectra of injection coefficients and shift conductivities, as well as their dependence on the static field strength and ribbon width. The spectra show many peaks associated with the optical transition between different subbands, and the positions and amplitudes of these peaks can be effectively controlled by the static electric field. By constructing a simple two band model, the static electric fields are found to modify the edge states in a nonperturbative way, and their associated optical transitions dominate the current generation at low photon energies. For typical parameters, such as a static field 10$^6$ V/m and light intensity 0.1 GW/cm$^2$, the magnitude of the injection and shift currents for a ribbon with width 5 nm can be as large as the order of 1 $mu$A. Our results provide a physical basis for realizing passive optoelectronic devices based on graphene nanoribbons.
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