Bi2Se3 is a prototypical topological insulator, which has a small bandgap (∼0.3 eV) and topologically protected conducting surface states. This material exhibits quite strong thermoelectric effects. Here, we show in a mechanically exfoliated thick (∼100 nm) nanoflake device that we can measure the energy dependent optical absorption through the photothermoelectric effect. Spectral signatures are seen for a number of optical transitions between the valence and conduction bands, including a broad peak at 1.5 eV, which is likely dominated by bulk band-to-band optical transitions but is at the same energy as the well-known optical transition between the two topologically protected conducting surface states. We also observe a surprising linear polarization dependence in the response of the device that reflects the influence of the metal contacts.
There is tremendous interest in measuring the strong electron-phonon interactions seen in topological Weyl semimetals. The semimetal NbIrTe4 has been proposed to be a Type-II Weyl semimetal with 8 pairs of opposite Chirality Weyl nodes which are very close to the Fermi energy. We show using polarized angular-resolved micro-Raman scattering at two excitation energies that we can extract the phonon mode dependence of the Raman tensor elements from the shape of the scattering efficiency versus angle. This van der Waals semimetal with broken inversion symmetry and 24 atoms per unit cell has 69 possible phonon modes of which we measure 19 modes with frequencies and symmetries consistent with Density Functional Theory calculations. We show that these tensor elements vary substantially in a small energy range which reflects a strong variation of the electron-phonon coupling for these modes.
We show that two major carrier excitation mechanisms are present in II-VI self-assembled quantum dots. The first one is related to direct excited state - ground state transition. It manifests itself by the presence of sharp and intense lines in the excitation spectrum measured from single quantum dots. Apart from these lines, we also observe up to four much broader excitation lines. The energy spacing between these lines indicates that they are associated with absorption related to longitudinal optical phonons. By analyzing resonantly excited photoluminescence spectra, we are able to separate the contributions from these two mechanisms. In the case of CdTe dots, the excited state - ground state relaxation is important for all dots in ensemble, while phonon - assisted processes are dominant for the dots with smaller lateral size.
The ternary van der Waals material NbIrTe_4 is a Type-II Weyl semimetal. We use a tunable circularly polarized mid-infrared laser to investigate the existence of band-to-band excitations using transient reflectivity in an exfoliated nanoflake and photothermoelectric and photogalvanic signals in a device. Unpolarized photothermoelectric spectroscopy shows that the absorption in the Weyl semimetal increases rapidly above 0.3 eV as expected from the increase in the density of states from DFT calculations. However, the reflectivity shows a sign change in the circular dichroism of the reflected light which is dominated by σ^- light for energies below 0.5 eV and σ^+ light for energies above that energy. Using an intense pulse to perturb the electrons near the Fermi level, we show that this 0.5 eV energy is associated with a band-to-band transition from a band slightly below the Fermi energy to a higher lying empty band. We use spectroscopy of the circular photogalvanic effect (CPGE) from 0.3 to 1 eV to show a strong peak near 0.5 eV which lies on top of a two orders-of-magnitude increase at the lowest energies as the Weyl points are approached. We conclude that this band-to-band optical transition enhances the Berry Curvature responsible for the CPGE, and may involve the Weyl points just below the Fermi energy.
Trigonal tellurium (Te) is a chiral semiconductor that lacks both mirror and inversion symmetries, resulting in complex band structures with Weyl crossings and unique spin textures. Detailed time-resolved polarized reflectance spectroscopy is used to investigate its band structure and carrier dynamics. The polarized transient spectra reveal optical transitions between the uppermost spin-split H 4 and H 5 and the degenerate H 6 valence bands (VB) and the lowest degenerate H 6 conduction band (CB) as well as a higher energy transition at the L-point. Surprisingly, the degeneracy of the H 6 CB (a proposed Weyl node) is lifted and the spin-split VB gap is reduced upon photoexcitation before relaxing to equilibrium as the carriers decay. Using ab initio density functional theory (DFT) calculations, we conclude that the dynamic band structure is caused by a photoinduced shear strain in the Te film that breaks the screw symmetry of the crystal. The band-edge anisotropy is also reflected in the hot carrier decay rate, which is a factor of two slower along the c -axis than perpendicular to it. The majority of photoexcited carriers near the band-edge are seen to recombine within 30 ps while higher lying transitions observed near 1.2 eV appear to have substantially longer lifetimes, potentially due to contributions of intervalley processes in the recombination rate. These new findings shed light on the strong correlation between photoinduced carriers and electronic structure in anisotropic crystals, which opens a potential pathway for designing novel Te-based devices that take advantage of the topological structures as well as strong spin-related properties.
We use polarized photocurrent spectroscopy in a nanowire device to investigate the band structure of hexagonal Wurtzite InAs. Signatures of optical transitions between four valence bands and two conduction bands are observed which are consistent with the symmetries expected from group theory. The ground state transition energy identified from photocurrent spectra is seen to be consistent with photoluminescence emitted from a cluster of nanowires from the same growth substrate. From the energies of the observed bands we determine the spin orbit and crystal field energies in Wurtzite InAs. This information is vital to the development of crystal phase engineering of this important III-V semiconductor.
The semimetal NbIrTe4 has been proposed to be a Type-II Weyl semimetal with 8 pairs of opposite Chirality Weyl nodes which are very close to the Fermi energy. This topological electronic structure is made possible because of the broken inversion symmetry of NbIrTe4 which is an orthorhombic crystal with Td symmetry. Using micro-Raman scattering as a probe, we observe the frequencies and symmetries of 19 phonon modes (ranging from 40 to 260 cm-1) in this material and compare to Density Functional Theory calculations. Using angular and polarization resolved Raman scattering for green (514 nm) and red (633 nm) laser excitation, we show that it is possible to extract the excitation energy dependence of the Raman tensor elements associated with each measurable phonon mode. We show that these tensor elements vary substantially in a small energy range which reflects a strong variation of the electron-phonon coupling for these modes.
We use transient Rayleigh scattering to study the thermalization of hot photoexcited carriers in single GaAs0.7Sb0.3/InP nanowire heterostructures. By comparing the energy loss rate in single core-only GaAs0.7Sb0.3 nanowires which do not show substantial hot carrier effects with the core-shell nanowires, we show that the presence of an InP shell substantially suppresses the longitudinal optical phonon emission rate at low temperatures which then leads to strong hot carrier effects.
Bismuth selenide (Bi2Se3) is a prototypical 3D topological insulator whose Dirac surface states have been extensively studied theoretically and experimentally. Surprisingly little, however, is known about the energetics and dynamics of electrons and holes within the bulk band structure of the semiconductor. We use mid-infrared femtosecond transient reflectance measurements on a single nanoflake to study the ultrafast thermalization and recombination dynamics of photoexcited electrons and holes within the extended bulk band structure over a wide energy range (0.3 to 1.2 eV). Theoretical modeling of the reflectivity spectral line shapes at 10 K demonstrates that the electrons and holes are photoexcited within a dense and cold electron gas with a Fermi level positioned well above the bottom of the lowest conduction band. Direct optical transitions from the first and the second spin-orbit split valence bands to the Fermi level above the lowest conduction band minimum are identified. The photoexcited carriers thermalize rapidly to the lattice temperature within a couple of picoseconds due to optical phonon emission and scattering with the cold electron gas. The minority carrier holes recombine with the dense electron gas within 150 ps at 10 K and 50 ps at 300 K. Such knowledge of interaction of electrons and holes within the bulk band structure provides a foundation for understanding how such states interact dynamically with the topologically protected Dirac surface states.