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- ItemProbing multiphoton light-induced molecular potentials([London] : Nature Publishing Group UK, 2020) Kübel, M.; Spanner, M.; Dube, Z.; Naumov, A.Yu.; Chelkowski, S.; Bandrauk, A.D.; Vrakking, M.J.J.; Corkum, P.B.; Villeneuve, D.M.; Staudte, A.The strong coupling between intense laser fields and valence electrons in molecules causes distortions of the potential energy hypersurfaces which determine the motion of the nuclei and influence possible reaction pathways. The coupling strength varies with the angle between the light electric field and valence orbital, and thereby adds another dimension to the effective molecular potential energy surface, leading to the emergence of light-induced conical intersections. Here, we demonstrate that multiphoton couplings can give rise to complex light-induced potential energy surfaces that govern molecular behavior. In the laser-induced dissociation of H2+, the simplest of molecules, we measure a strongly modulated angular distribution of protons which has escaped prior observation. Using two-color Floquet theory, we show that the modulations result from ultrafast dynamics on light-induced molecular potentials. These potentials are shaped by the amplitude, duration and phase of the dressing fields, allowing for manipulating the dissociation dynamics of small molecules.
- ItemDirected exciton transport highways in organic semiconductors([London] : Nature Publishing Group UK, 2023) Müller, Kai; Schellhammer, Karl S.; Gräßler, Nico; Debnath, Bipasha; Liu, Fupin; Krupskaya, Yulia; Leo, Karl; Knupfer, Martin; Ortmann, FrankExciton bandwidths and exciton transport are difficult to control by material design. We showcase the intriguing excitonic properties in an organic semiconductor material with specifically tailored functional groups, in which extremely broad exciton bands in the near-infrared-visible part of the electromagnetic spectrum are observed by electron energy loss spectroscopy and theoretically explained by a close contact between tightly packing molecules and by their strong interactions. This is induced by the donor–acceptor type molecular structure and its resulting crystal packing, which induces a remarkable anisotropy that should lead to a strongly directed transport of excitons. The observations and detailed understanding of the results yield blueprints for the design of molecular structures in which similar molecular features might be used to further explore the tunability of excitonic bands and pave a way for organic materials with strongly enhanced transport and built-in control of the propagation direction.
- ItemAnharmonic strong-coupling effects at the origin of the charge density wave in CsV3Sb5([London] : Nature Publishing Group UK, 2024) He, Ge; Peis, Leander; Cuddy, Emma Frances; Zhao, Zhen; Li, Dong; Zhang, Yuhang; Stumberger, Romona; Moritz, Brian; Yang, Haitao; Gao, Hongjun; Devereaux, Thomas Peter; Hackl, RudiThe formation of charge density waves is a long-standing open problem, particularly in dimensions higher than one. Various observations in the vanadium antimonides discovered recently further underpin this notion. Here, we study the Kagome metal CsV3Sb5 using polarized inelastic light scattering and density functional theory calculations. We observe a significant gap anisotropy with 2Δmax/kBTCDW≈20, far beyond the prediction of mean-field theory. The analysis of the A1g and E2g phonons, including those emerging below TCDW, indicates strong phonon-phonon coupling, presumably mediated by a strong electron-phonon interaction. Similarly, the asymmetric Fano-type lineshape of the A1g amplitude mode suggests strong electron-phonon coupling below TCDW. The large electronic gap, the enhanced anharmonic phonon-phonon coupling, and the Fano shape of the amplitude mode combined are more supportive of a strong-coupling phonon-driven charge density wave transition than of a Fermi surface instability or an exotic mechanism in CsV3Sb5.
- ItemSignatures of a magnetic-field-induced Lifshitz transition in the ultra-quantum limit of the topological semimetal ZrTe5([London] : Nature Publishing Group UK, 2022) Galeski, S.; Legg, H.F.; Wawrzyńczak, R.; Förster, T.; Zherlitsyn, S.; Gorbunov, D.; Uhlarz, M.; Lozano, P.M.; Li, Q.; Gu, G.D.; Felser, C.; Wosnitza, J.; Meng, T.; Gooth, J.The quantum limit (QL) of an electron liquid, realised at strong magnetic fields, has long been proposed to host a wealth of strongly correlated states of matter. Electronic states in the QL are, for example, quasi-one dimensional (1D), which implies perfectly nested Fermi surfaces prone to instabilities. Whereas the QL typically requires unreachably strong magnetic fields, the topological semimetal ZrTe5 has been shown to reach the QL at fields of only a few Tesla. Here, we characterize the QL of ZrTe5 at fields up to 64 T by a combination of electrical-transport and ultrasound measurements. We find that the Zeeman effect in ZrTe5 enables an efficient tuning of the 1D Landau band structure with magnetic field. This results in a Lifshitz transition to a 1D Weyl regime in which perfect charge neutrality can be achieved. Since no instability-driven phase transitions destabilise the 1D electron liquid for the investigated field strengths and temperatures, our analysis establishes ZrTe5 as a thoroughly understood platform for potentially inducing more exotic interaction-driven phases at lower temperatures.
- ItemGate controlled valley polarizer in bilayer graphene([London] : Nature Publishing Group UK, 2020) Chen, Hao; Zhou, Pinjia; Liu, Jiawei; Qiao, Jiabin; Oezyilmaz, Barbaros; Martin, JensSign reversal of Berry curvature across two oppositely gated regions in bilayer graphene can give rise to counter-propagating 1D channels with opposite valley indices. Considering spin and sub-lattice degeneracy, there are four quantized conduction channels in each direction. Previous experimental work on gate-controlled valley polarizer achieved good contrast only in the presence of an external magnetic field. Yet, with increasing magnetic field the ungated regions of bilayer graphene will transit into the quantum Hall regime, limiting the applications of valley-polarized electrons. Here we present improved performance of a gate-controlled valley polarizer through optimized device geometry and stacking method. Electrical measurements show up to two orders of magnitude difference in conductance between the valley-polarized state and gapped states. The valley-polarized state displays conductance of nearly 4e2/h and produces contrast in a subsequent valley analyzer configuration. These results pave the way to further experiments on valley-polarized electrons in zero magnetic field.
- ItemUnconventional Hall response in the quantum limit of HfTe5([London] : Nature Publishing Group UK, 2020) Galeski, S.; Zhao, X.; Wawrzyńczak, R.; Meng, T.; Förster, T.; Lozano, P.M.; Honnali, S.; Lamba, N.; Ehmcke, T.; Markou, A.; Li., Q.; Gu, G.; Zhu, W.; Wosnitza, J.; Felser, C.; Chen, G.F.; Gooth, J.Interacting electrons confined to their lowest Landau level in a high magnetic field can form a variety of correlated states, some of which manifest themselves in a Hall effect. Although such states have been predicted to occur in three-dimensional semimetals, a corresponding Hall response has not yet been experimentally observed. Here, we report the observation of an unconventional Hall response in the quantum limit of the bulk semimetal HfTe5, adjacent to the three-dimensional quantum Hall effect of a single electron band at low magnetic fields. The additional plateau-like feature in the Hall conductivity of the lowest Landau level is accompanied by a Shubnikov-de Haas minimum in the longitudinal electrical resistivity and its magnitude relates as 3/5 to the height of the last plateau of the three-dimensional quantum Hall effect. Our findings are consistent with strong electron-electron interactions, stabilizing an unconventional variant of the Hall effect in a three-dimensional material in the quantum limit.
- ItemTunable positions of Weyl nodes via magnetism and pressure in the ferromagnetic Weyl semimetal CeAlSi([London] : Nature Publishing Group UK, 2024) Cheng, Erjian; Yan, Limin; Shi, Xianbiao; Lou, Rui; Fedorov, Alexander; Behnami, Mahdi; Yuan, Jian; Yang, Pengtao; Wang, Bosen; Cheng, Jin-Guang; Xu, Yuanji; Xu, Yang; Xia, Wei; Pavlovskii, Nikolai; Peets, Darren C.; Zhao, Weiwei; Wan, Yimin; Burkhardt, Ulrich; Guo, Yanfeng; Li, Shiyan; Felser, Claudia; Yang, Wenge; Büchner, BerndThe noncentrosymmetric ferromagnetic Weyl semimetal CeAlSi with simultaneous space-inversion and time-reversal symmetry breaking provides a unique platform for exploring novel topological states. Here, by employing multiple experimental techniques, we demonstrate that ferromagnetism and pressure can serve as efficient parameters to tune the positions of Weyl nodes in CeAlSi. At ambient pressure, a magnetism-facilitated anomalous Hall/Nernst effect (AHE/ANE) is uncovered. Angle-resolved photoemission spectroscopy (ARPES) measurements demonstrated that the Weyl nodes with opposite chirality are moving away from each other upon entering the ferromagnetic phase. Under pressure, by tracing the pressure evolution of AHE and band structure, we demonstrate that pressure could also serve as a pivotal knob to tune the positions of Weyl nodes. Moreover, multiple pressure-induced phase transitions are also revealed. These findings indicate that CeAlSi provides a unique and tunable platform for exploring exotic topological physics and electron correlations, as well as catering to potential applications, such as spintronics.
- ItemCavity electromechanics with parametric mechanical driving([London] : Nature Publishing Group UK, 2020) Bothner, D.; Yanai, S.; Iniguez-Rabago, A.; Yuan, M.; Blanter, Ya. M.; Steele, G. A.Microwave optomechanical circuits have been demonstrated to be powerful tools for both exploring fundamental physics of macroscopic mechanical oscillators, as well as being promising candidates for on-chip quantum-limited microwave devices. In most experiments so far, the mechanical oscillator is either used as a passive element and its displacement is detected using the superconducting cavity, or manipulated by intracavity fields. Here, we explore the possibility to directly and parametrically manipulate the mechanical nanobeam resonator of a cavity electromechanical system, which provides additional functionality to the toolbox of microwave optomechanics. In addition to using the cavity as an interferometer to detect parametrically modulated mechanical displacement and squeezed thermomechanical motion, we demonstrate that this approach can realize a phase-sensitive parametric amplifier for intracavity microwave photons. Future perspectives of optomechanical systems with a parametrically driven mechanical oscillator include exotic bath engineering with negative effective photon temperatures, or systems with enhanced optomechanical nonlinearities.