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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
2016, Bruner, Barry D., MaÅ¡Ãn, ZdenÄ›k, Negro, Matteo, Morales, Felipe, Brambila, Danilo, Devetta, Michele, Faccialà , Davide, Harvey, Alex G., Ivanov, Misha, Mairesse, Yann, Patchkovskii, Serguei, Serbinenko, Valeria, Soifer, Hadas, Stagira, Salvatore, Vozzi, Caterina, Dudovich, Nirit, Smirnova, Olga
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.
Attosecond time-resolved photoelectron holography
2018, Porat, G., Alon, G., Rozen, S., Pedatzur, O., Krüger, M., Azoury, D., Natan, A., Orenstein, G., Bruner, B.D., Vrakking, M. J.J., Dudovich, N.
Ultrafast strong-field physics provides insight into quantum phenomena that evolve on an attosecond time scale, the most fundamental of which is quantum tunneling. The tunneling process initiates a range of strong field phenomena such as high harmonic generation (HHG), laser-induced electron diffraction, double ionization and photoelectron holography - all evolving during a fraction of the optical cycle. Here we apply attosecond photoelectron holography as a method to resolve the temporal properties of the tunneling process. Adding a weak second harmonic (SH) field to a strong fundamental laser field enables us to reconstruct the ionization times of photoelectrons that play a role in the formation of a photoelectron hologram with attosecond precision. We decouple the contributions of the two arms of the hologram and resolve the subtle differences in their ionization times, separated by only a few tens of attoseconds.
Time-reversal symmetry breaking type-II Weyl state in YbMnBi2
2019, Borisenko, S., Evtushinsky, D., Gibson, Q., Yaresko, A., Koepernik, K., Kim, T., Ali, M., van den Brink, J., Hoesch, M., Fedorov, A., Haubold, E., Kushnirenko, Y., Soldatov, I., Schäfer, R., Cava, R.J.
Spectroscopic detection of Dirac and Weyl fermions in real materials is vital for both, promising applications and fundamental bridge between high-energy and condensed-matter physics. While the presence of Dirac and noncentrosymmetric Weyl fermions is well established in many materials, the magnetic Weyl semimetals still escape direct experimental detection. In order to find a time-reversal symmetry breaking Weyl state we design two materials and present here experimental and theoretical evidence of realization of such a state in one of them, YbMnBi2. We model the time-reversal symmetry breaking observed by magnetization and magneto-optical microscopy measurements by canted antiferromagnetism and find a number of Weyl points. Using angle-resolved photoemission, we directly observe two pairs of Weyl points connected by the Fermi arcs. Our results not only provide a fundamental link between the two areas of physics, but also demonstrate the practical way to design novel materials with exotic properties.
Correlation induced electron-hole asymmetry in quasi- two-dimensional iridates
2017, Pärschke, E.M., Wohlfeld, K., Foyevtsova, K., Van Den Brink, J.
The resemblance of crystallographic and magnetic structures of the quasi-two-dimensional iridates Ba2IrO4 and Sr2IrO4 to La2CuO4 points at an analogy to cuprate high-Tc superconductors, even if spin-orbit coupling is very strong in iridates. Here we examine this analogy for the motion of a charge (hole or electron) added to the antiferromagnetic ground state. We show that correlation effects render the hole and electron case in iridates very different. An added electron forms a spin polaron, similar to the cuprates, but the situation of a removed electron is far more complex. Many-body 5d 4 configurations form which can be singlet and triplet states of total angular momentum that strongly affect the hole motion. This not only has ramifications for the interpretation of (inverse-)photoemission experiments but also demonstrates that correlation physics renders electron- and hole-doped iridates fundamentally different.
Physics inspired compact modelling of BiFeO3 based memristors
2022, Yarragolla, Sahitya, Du, Nan, Hemke, Torben, Zhao, Xianyue, Chen, Ziang, Polian, Ilia, Mussenbrock, Thomas
With the advent of the Internet of Things, nanoelectronic devices or memristors have been the subject of significant interest for use as new hardware security primitives. Among the several available memristors, BiFeO3 (BFO)-based electroforming-free memristors have attracted considerable attention due to their excellent properties, such as long retention time, self-rectification, intrinsic stochasticity, and fast switching. They have been actively investigated for use in physical unclonable function (PUF) key storage modules, artificial synapses in neural networks, nonvolatile resistive switches, and reconfigurable logic applications. In this work, we present a physics-inspired 1D compact model of a BFO memristor to understand its implementation for such applications (mainly PUFs) and perform circuit simulations. The resistive switching based on electric field-driven vacancy migration and intrinsic stochastic behaviour of the BFO memristor are modelled using the cloud-in-a-cell scheme. The experimental current–voltage characteristics of the BFO memristor are successfully reproduced. The response of the BFO memristor to changes in electrical properties, environmental properties (such as temperature) and stress are analyzed and consistant with experimental results.