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Multidimensional high harmonic spectroscopy of polyatomic molecules: detecting sub-cycle laser-driven hole dynamics upon ionization in strong mid-IR laser fields
High harmonic generation (HHG) spectroscopy has opened up a new frontier in ultrafast science, where electronic dynamics can be measured on an attosecond time scale. The strong laser field that triggers the high harmonic response also opens multiple quantum pathways for multielectron dynamics in molecules, resulting in a complex process of multielectron rearrangement during ionization. Using combined experimental and theoretical approaches, we show how multi-dimensional HHG spectroscopy can be used to detect and follow electronic dynamics of core rearrangement on sub-laser cycle time scales. We detect the signatures of laser-driven hole dynamics upon ionization and reconstruct the relative phases and amplitudes for relevant ionization channels in a CO2 molecule on a sub-cycle time scale. Reconstruction of channel-resolved complex ionization amplitudes on attosecond time scales has been a long-standing goal of high harmonic spectroscopy. Our study brings us one step closer to fulfilling this initial promise and developing robust schemes for sub-femtosecond imaging of multielectron rearrangement in complex molecular systems.
Contrast Reversal in Scanning Tunneling Microscopy and Its Implications for the Topological Classification of SmB6
SmB6 has recently attracted considerable interest as a candidate for the first strongly correlated topological insulator. Such materials promise entirely new properties such as correlation-enhanced bulk bandgaps or a Fermi surface from spin excitations. Whether SmB6 and its surface states are topological or trivial is still heavily disputed however, and a solution is hindered by major disagreement between angle-resolved photoemission (ARPES) and scanning tunneling microscopy (STM) results. Here, a combined ARPES and STM experiment is conducted. It is discovered that the STM contrast strongly depends on the bias voltage and reverses its sign beyond 1 V. It is shown that the understanding of this contrast reversal is the clue to resolving the discrepancy between ARPES and STM results. In particular, the scanning tunneling spectra reflect a low-energy electronic structure at the surface, which supports a trivial origin of the surface states and the surface metallicity of SmB6. © 2020 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
Strong surface termination dependence of the electronic structure of polar superconductor LaFeAsO revealed by nano-ARPES
The electronic structures of the iron-based superconductors have been intensively studied by using angle-resolved photoemission spectroscopy (ARPES). A considerable amount of research has been focused on the LaFeAsO family, showing the highest transition temperatures, where previous ARPES studies have found much larger Fermi surfaces than bulk theoretical calculations would predict. The discrepancy has been attributed to the presence of termination-dependent surface states. Here, using photoemission spectroscopy with a sub-micron focused beam spot (nano-ARPES) we have successfully measured the electronic structures of both the LaO and FeAs terminations in LaFeAsO. Our data reveal very different band dispersions and core-level spectra for different surface terminations, showing that previous macro-focus ARPES measurements were incomplete. Our results give direct evidence for the surface-driven electronic structure reconstruction in LaFeAsO, including formation of the termination-dependent surface states at the Fermi level. This experimental technique, which we have shown to be very powerful when applied to this prototypical compound, can now be used to study various materials with different surface terminations.