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Register a new userBloch Wavefunction Reconstruction using Multidimensional Photoemission Spectroscopy
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Added by
Michael Sch\\\"uler
Publication date
2021
fields
Physics
and research's language is
English
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Angle-resolved spectroscopy is the most powerful technique to investigate the electronic band structure of crystalline solids. To completely characterize the electronic structure of topological materials, one needs to go beyond band structure mapping and probe the texture of the Bloch wavefunction in momentum-space, associated with Berry curvature and topological invariants. Because phase information is lost in the process of measuring photoemission intensities, retrieving the complex-valued Bloch wavefunction from photoemission data has yet remained elusive. In this Article, we introduce a novel measurement methodology and observable in extreme ultraviolet angle-resolved photoemission spectroscopy, based on continuous modulation of the ionizing radiation polarization axis. By tracking the energy- and momentum-resolved amplitude and phase of the photoemission modulation upon polarization variation, we reconstruct the Bloch wavefunction of prototypical semiconducting transition metal dichalcogenide 2H-WSe$_2$ with minimal theory input. This novel experimental scheme, which is articulated around the manipulation of the photoionization transition dipole matrix element, in combination with a simple tight-binding theory, is general and can be extended to provide insights into the Bloch wavefunction of many relevant crystalline solids.
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The heterostructure consisting of the Mott insulator LaVO$_3$ and the band insulator SrTiO$_3$ is considered a promising candidate for future photovoltaic applications. Not only does the (direct) excitation gap of LaVO$_3$ match well the solar spectrum, but its correlated nature and predicted built-in potential, owing to the non-polar/polar interface when integrated with SrTiO$_3$, also offer remarkable advantages over conventional solar cells. However, experimental data beyond the observation of a thickness-dependent metal-insulator transition is scarce and a profound, microscopic understanding of the electronic properties is still lacking. By means of soft and hard X-ray photoemission spectroscopy as well as resistivity and Hall effect measurements we study the electrical properties, band bending, and band alignment of LaVO$_3$/SrTiO$_3$ heterostructures. We find a critical LaVO$_3$ thickness of five unit cells, confinement of the conducting electrons to exclusively Ti 3$d$ states at the interface, and a potential gradient in the film. From these findings we conclude on electronic reconstruction as the driving mechanism for the formation of the metallic interface in LaVO$_3$/SrTiO$_3$.
The momentum-dependent orbital character in crystalline solids, referred to as orbital texture, is of capital importance in the emergence of symmetry-broken collective phases such as charge density waves as well as superconducting and topological states of matter. By performing extreme ultraviolet multidimensional angle-resolved photoemission spectroscopy for two different crystal orientations linked to each other by mirror symmetry, we isolate and identify the role of orbital texture in photoemission from the transition metal dichalcogenide 1T-TiTe$_2$. By comparing our experimental results with theoretical calculations based on both a quantitative one-step model of photoemission and an intuitive tight-binding model, we unambiguously demonstrate the link between the momentum-dependent orbital orientation and the emergence of strong intrinsic linear dichroism in the photoelectron angular distributions. Our results represent an important step towards going beyond band structure (eigenvalues) mapping and learn about electronic wavefunction and orbital texture of solids by exploiting matrix element effects in photoemission spectroscopy.
Anticipated breakthroughs in solid-state quantum computing will rely on achieving unprecedented control over the wave-like states of electrons in crystalline materials. For example, an international effort to build a quantum computer that is topologically protected from decoherence is focusing on carefully engineering the wave-like states of electrons in hybrid devices that proximatize an elemental superconductor and a semiconductor nanostructure[1-6]. However, more than 90 years after Bloch derived the functional forms of electronic waves in crystals[7](now known as Bloch wavefunction) rapid scattering processes have so far prevented their direct experimental reconstruction, even in bulk materials. In high-order sideband generation (HSG)[8-15], electrons and holes generated in semiconductors by a near-infrared (NIR) laser are accelerated to high kinetic energy by a strong terahertz field, and recollide to emit NIR sidebands before they are scattered. Here we reconstruct the Bloch wavefunctions of two types of holes in gallium arsenide by experimentally measuring sideband polarizations and introducing an elegant theory that ties those polarizations to quantum interference between different recollision pathways. Because HSG can, in principle, be observed from any direct-gap semiconductor or insulator, we expect the method introduced in this Article can be used to reconstruct Bloch wavefunctions in a large class of bulk and nanostructured materials, accelerating the development of topologically-protected quantum computers as well as other important electronic and optical technologies.
We characterize the topological insulator Bi$_2$Se$_3$ using time- and angle- resolved photoemission spectroscopy. By employing two-photon photoemission, a complete picture of the unoccupied electronic structure from the Fermi level up to the vacuum level is obtained. We demonstrate that the unoccupied states host a second, Dirac surface state which can be resonantly excited by 1.5 eV photons. We then study the ultrafast relaxation processes following optical excitation. We find that they culminate in a persistent non-equilibrium population of the first Dirac surface state, which is maintained by a meta-stable population of the bulk conduction band. Finally, we perform a temperature-dependent study of the electron-phonon scattering processes in the conduction band, and find the unexpected result that their rates decrease with increasing sample temperature. We develop a model of phonon emission and absorption from a population of electrons, and show that this counter-intuitive trend is the natural consequence of fundamental electron-phonon scattering processes. This analysis serves as an important reminder that the decay rates extracted by time-resolved photoemission are not in general equal to single electron scattering rates, but include contributions from filling and emptying processes from a continuum of states.
We have performed a systematic high-momentum-resolution photoemission study on ZrTe$_5$ using $6$ eV photon energy. We have measured the band structure near the $Gamma$ point, and quantified the gap between the conduction and valence band as $18 leq Delta leq 29$ meV. We have also observed photon-energy-dependent behavior attributed to final-state effects and the 3D nature of the materials band structure. Our interpretation indicates the gap is intrinsic and reconciles discrepancies on the existence of a topological surface state reported by different studies. The existence of a gap suggests that ZrTe$_5$ is not a 3D strong topological insulator nor a 3D Dirac semimetal. Therefore, our experiment is consistent with ZrTe$_5$ being a 3D weak topological insulator.
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