No Arabic abstract
Topological insulator films are promising materials for optoelectronics due to a strong optical absorption and a thickness dependent band gap of the topological surface states. They are superior candidates for photodetector applications in the THz-infrared spectrum, with a potential performance higher than graphene. Using a first-principles $kcdot p$ Hamiltonian, incorporating all symmetry-allowed terms to second order in the wave vector $k$, first order in the strain $epsilon$ and of order $epsilon k$, we demonstrate significantly improved optoelectronic performance due to strain. For Bi$_2$Se$_3$ films of variable thickness, the surface state band gap, and thereby the optical absorption, can be effectively tuned by application of uniaxial strain, $epsilon_{zz}$, leading to a divergent band edge absorbance for $epsilon_{zz}gtrsim 6%$. Shear strain breaks the crystal symmetry and leads to an absorbance varying significantly with polarization direction. Remarkably, the directional average of the absorbance always increases with strain, independent of material parameters.
The design of novel functional materials in silico is severely hampered by the lack of robust and computationally efficient methods for describing both molecular absorbance and screening on substrates. Here we employ our hybrid $G_0[W_0+Delta W]$-BSE implementation, which incorporates the substrate via its screening $Delta W$ at both the quasiparticle $G_0W_0$ level and when solving the Bethe-Salpeter equation (BSE). We show this method can be used to both efficiently and accurately describe the absorption spectra of physisorbed molecules on metal substrates and thereby tailor the molecules absorbance by altering the surface plasmons energy. Specifically, we investigate how the optical absorption spectra of three prototypical $pi$-conjugated molecules: benzene (C$_6$H$_6$), terrylene (C$_{30}$H$_{16}$) and fullerene (C$_{60}$), depends on the Wigner-Seitz radius $r_s$ of the metallic substrate. To gain further understanding of the light--molecule/substrate interaction, we also study the bright excitons electron and hole densities and their interactions with infrared active vibrational modes. Our results show that (1) benzenes bright $E_{1u}^1$ exciton at 7.0 eV, whose energy is insensitive to changes in $r_s$, could be relevant for photocatalytic dehydrogenation and polymerization reactions, (2) terrylenes bright $B_{3u}$ exciton at 2.3 eV hybridizes with the surface plasmon, allowing the tailoring of the excitonic energy and optical activation of a surface plasmon-like exciton, and (3) fullerenes $pi-pi^*$ bright and dark excitons at 6.4 and 6.8 eV hybridize with the surface plasmon, resulting in the tailoring of their excitonic energy and the activation of both a surface plasmon-like exciton and a dark quadrupolar mode via symmetry breaking by the substrate.
Topological insulators (TIs) have attracted much attention due to their spin-polarized surface and edge states, whose origin in symmetry gives them intriguing quantum-mechanical properties. Robust control over the chemical potential of TI materials is important if these states are to become useful in new technologies, or as a venue for exotic physics. Unfortunately, chemical potential tuning is challenging in TIs in part because the fabrication of electrostatic top-gates tends to degrade material properties and the addition of chemical dopants or adsorbates can cause unwanted disorder. Here, we present an all-optical technique which allows persistent, bidirectional gating of a (Bi,Sb)2Te3 channel by optically manipulating the distribution of electric charge below its interface with an insulating SrTiO3 substrate. In this fashion we optically pattern p-n junctions in a TI material, which we subsequently image using scanning photocurrent microscopy. The ability to dynamically write and re-write mesoscopic electronic structures in a TI may aid in the investigation of the unique properties of the topological insulating phase. The optical gating effect may be adaptable to other material systems, providing a more general mechanism for reconfigurable electronics.
Dynamic manipulation of magnetism in topological materials is demonstrated here via a Floquet engineering approach using circularly polarized light. Increasing the strength of the laser field, besides the expected topological phase transition, the magnetically doped topological insulator thin film also undergoes a magnetic phase transition from ferromagnetism to paramagnetism, whose critical behavior strongly depends on the quantum quenching. In sharp contrast to the equilibrium case, the non-equilibrium Curie temperatures vary for different time scale and experimental setup, not all relying on change of topology. Our discoveries deepen the understanding of the relationship between topology and magnetism in the non-equilibrium regime and extend optoelectronic device applications to topological materials.
Electrical field control of the carrier density of topological insulators (TI) has greatly expanded the possible practical use of these materials. However, the combination of low temperature local probe studies and a gate tunable TI device remains challenging. We have overcome this limitation by scanning tunneling microscopy and spectroscopy measurements on in-situ molecular beam epitaxy growth of Bi2Se3 films on SrTiO3 substrates with pre-patterned electrodes. Using this gating method, we are able to shift the Fermi level of the top surface states by 250 meV on a 3 nm thick Bi2Se3 device. We report field effect studies of the surface state dispersion, band gap, and electronic structure at the Fermi level.
We investigate the optical properties of an ultrathin film of a topological insulator in the presence of an in-plane magnetic field. We show that due to the combination of the overlap between the surface states of the two layers and the magnetic field, the optical conductivity can show strong anisotropy. This leads to the effective optical activity of the ultrathin film by influencing the circularly polarized incident light. Intriguingly, for a range of magnetic fields, the reflected and transmitted lights exhibit elliptic character. Even for certain values almost linear polarizations are obtained, indicating that the thin film can act as a polaroid in reflection. All these features are discussed in the context of the time reversal symmetry breaking as one of key ingredients for the optical activity.