arXiv subjects

Kai Rossnagel

Publications and source records attributed to Kai Rossnagel.

At least 55 records · Page 3Linked to original sources

arXiv2022

Tailoring the band structure of plexcitonic crystals by strong coupling

Transition-metal dichalcogenides with their exciton-dominated optical behavior emerge as promising materials for realizing strong light-matter interactions in the visible range and at ambient conditions. When these materials are combined with metals, the energy confining ability of plasmon polaritons in metals below the diffraction limit, allows for further enhancing and tailoring the light-matter interaction, due to the formation of plexcitons in hybrid metal-TMDC structures at the interface. Herein, we demonstrate that the coupling between quasi-propagating plasmons in plasmonic crystals and excitons in WSe2, provides a multi-oscillator playground for tailoring the band structure of plasmonic crystal structures and results in emerging flat bands. The cathodoluminescence spectroscopy and angle-resolved measurements combined with the numerically calculated photonic band structure confirm a strong exciton-plasmon coupling, leading to significant changes in the band diagram of the hybrid lattice and the ability to tailor the band diagram via strong coupling. The hybrid plexcitonic crystal structures investigated here sustain optical waves with remarkably low group velocities. These results could be used for designing tunable slow-light structures based on the strong-coupling effect and pave the way toward plexcitonic topological photonic structures.

physics.optics↗

arXiv2021

Ultrafast electronic line width broadening in the C 1s core level of graphene

Core level binding energies and absorption edges are at the heart of many experimental techniques concerned with element-specific structure, electronic structure, chemical reactivity, elementary excitations and magnetism. X-ray photoemission spectroscopy (XPS) in particular, can provide information about the electronic and vibrational many-body interactions in a solid as these are reflected in the detailed energy distribution of the photoelectrons. Ultrafast pump-probe techniques add a new dimension to such studies, introducing the ability to probe a transient state of the many-body system. Here we use a free electron laser to investigate the effect of a transiently excited electron gas on the core level spectrum of graphene, showing that it leads to a large broadening of the C 1s peak. Confirming a decade-old prediction, the broadening is found to be caused by an exchange of energy and momentum between the photoemitted core electron and the hot electron system, rather than by vibrational excitations. This interpretation is supported by a line shape analysis that accounts for the presence of the excited electrons. Fitting the spectra to this model directly yields the electronic temperature of the system, in agreement with electronic temperature values obtained from valence band data. Furthermore, making use of time- and momentum-resolved C 1s spectra, we illustrate how the momentum change of the outgoing core electrons leads to a small but detectable change in the time-resolved photoelectron diffraction pattern and to a nearly complete elimination of the core level binding energy variation associated with the narrow $σ$-band in the C 1s state. The results demonstrate that the XPS line shape can be used as an element-specific and local probe of the excited electron system and that X-ray photoelectron diffraction investigations remain feasible at very high electronic temperatures.

cond-mat.str-el↗

arXiv2021

Charting the Exciton-Polariton Landscape in WSe2 Thin Flakes by Cathodoluminescence Spectroscopy

Semiconducting transition-metal dichalcogenides (TMDCs) provide a fascinating discovery platform for strong light-matter interaction effects in the visible spectrum at ambient conditions. While most of the work has focused on hybridizing excitons with resonant photonic modes of external mirrors, cavities, or nanostructures, intriguingly, TMDC flakes of sub-wavelength thickness can themselves act as nanocavities. Here, we determine the optical response of such freestanding planar waveguides of WSe$_2$, by means of cathodoluminescence spectroscopy. We reveal strong exciton-photon interaction effects that foster long-range propagating exciton-polaritons and enable direct imaging of the energy transfer dynamics originating from cavity-like Fabry-Perot resonances. Furthermore, confinement effects due to discontinuities in the flakes are demonstrated as an efficient means to tailor the exciton-photon coupling strength, along the edges of natural flakes. Our combined experimental and theoretical results provide a deeper understanding of exciton-photon self-hybridization in semiconducting TMDCs and may pave the way to optoelectronic nanocircuits exploiting exciton-photon interaction.

physics.app-ph↗

arXiv2021

Strong Interaction of Cherenkov Radiation with Excitons in WSe2 Crystals

The optical responses of semiconducting transition metal dichalcogenides are dominated by excitons. Being able to strongly interact with light and other materials excitations, excitons in semiconductors are prototypes for investigating many-particle and strong-field physics, including exciton-exciton, exciton-photon, and exciton-phonon interactions. Strong exciton-photon interactions, in particular, can lead to the emergence of exciton-polariton hybrid quasiparticles with peculiar characteristics, and a tendency toward macroscopic and spontaneous coherence. Normally, far-field and near-field optical spectroscopy techniques are used to investigate exciton-photon interactions. Here, we demonstrate that the radiation generated by moving electrons in transition metal dichalcogenides, namely Cherenkov radiation, can strongly interact with excitons. We investigate the coherence properties and spectral signatures of exciton-photon interactions in TMDC bulk crystals, using cathodoluminescence spectroscopy. Our findings lay the ground for cathodoluminescence spectroscopy and in particular electron-beam techniques as probes of exciton-polariton spontaneous coherence in semiconductors, beyond the well-known plasmonic investigations.

cond-mat.mes-hall↗

arXiv2020

Creation of a novel inverted charge density wave state

Charge density wave (CDW) order is an emergent quantum phase that is characterized by a periodic lattice distortion and charge density modulation, often present near superconducting transitions. Here we uncover a novel inverted CDW state by using a femtosecond laser to coherently over-drive the unique star-of-David lattice distortion in 1T-TaSe$_2$. We track the signature of this novel CDW state using time- and angle-resolved photoemission spectroscopy and time-dependent density functional theory, and validate that it is associated with a unique lattice and charge arrangement never before realized. The dynamic electronic structure further reveals its novel properties, that are characterized by an increased density of states near the Fermi level, high metallicity, and altered electron-phonon couplings. Our results demonstrate how ultrafast lasers can be used to create unique states in materials, by manipulating charge-lattice orders and couplings.

cond-mat.mtrl-sci↗

arXiv2020

Surface structure and stacking of the commensurate $\left(\sqrt{13}\times\sqrt{13}\right)$R13.9° charge density wave phase of 1T-TaS$_2$(0001)

By quantitative low-energy electron diffraction (LEED) we investigate the extensively studied commensurate charge density wave (CDW) phase of trigonal tantalum disulphide (1T-TaS$_2$), which develops at low temperatures with a $\left(\sqrt{13}\times\sqrt{13}\right)$R13.9° periodicity. A full-dynamical analysis of the energy dependence of diffraction spot intensities reveals the entire crystallographic surface structure, i.e. the detailed atomic positions within the outermost two trilayers consisting of 78 atoms as well as the CDW stacking. The analysis is based on an unusually large data set consisting of spectra for 128 inequivalent beams taken in the energy range 20-250 eV and an excellent fit quality expressed by a bestfit Pendry R-factor of R=0.110. The LEED intensity analysis reveals that the well-accepted model of star-of-David-shaped clusters of Ta atoms for the bulk structure also holds for the outermost two TaS$_2$ trilayers. Specifically, in both layers the clusters of Ta atoms contract laterally by up to 0.25 $Å$ and also slightly rotate within the superstructure cell, causing respective distortions as well as heavy bucklings (up to 0.23 $Å$) in the adjacent sulphur layers. Most importantly, our analysis finds that the CDWs of the 1$^{\text{st}}$ and 2$^{\text{nd}}$ trilayer are vertically aligned, while there is a lateral shift of two units of the basic hexagonal lattice (6.71 $Å$) between the 2$^{\text{nd}}$ and 3$^{\text{rd}}$ trilayer. The results may contribute to a better understanding of the intricate electronic structure of the reference compound 1T-TaS$_2$ and guide the way to the analysis of complex structures in similar quantum materials.

cond-mat.str-el↗

arXiv2020

Structurally assisted melting of excitonic correlations in 1T-TiSe2

The simultaneous condensation of electronic and structural degrees of freedom gives rise to new states of matter, including superconductivity and charge-density-wave formation. When exciting such a condensed system, it is commonly assumed that the ultrafast laser pulse disturbs primarily the electronic order, which in turn destabilizes the atomic structure. Contrary to this conception, we show here that structural destabilization of few atoms causes melting of the macroscopic ordered charge-density wave in 1T-TiSe2. Using ultrafast pump-probe non-resonant and resonant X-ray diffraction, we observe full suppression of the Se 4p orbital order and the atomic structure at excitation energies more than one order of magnitude below the suggested excitonic binding energy. Complete melting of the charge-density wave occurs 4-5 times faster than expected from a purely electronic charge-screening process, strongly suggesting a structurally assisted breakup of excitonic correlations. Our experimental data clarifies several questions on the intricate coupling between structural and electronic order in stabilizing the charge-density-wave in 1T-TiSe2. The results further show that electron-phonon-coupling can lead to different, energy dependent phase-transition pathways in condensed matter systems, opening new possibilities in the conception of non-equilibrium phenomena at the ultrafast scale.

cond-mat.str-el↗

arXiv2020

Correlation between electronic and structural orders in 1T-TiSe2

The correlation between electronic and crystal structures of 1T-TiSe2 in the charge density wave (CDW) state is studied by x-ray diffraction. Three families of reflections are used to probe atomic displacements and the orbital asymmetry in Se. Two distinct onset temperatures are found, TCDW and a lower T* indicative for an onset of Se out-of-plane atomic displacements. T* coincides with a DC resistivity maximum and the onset of the proposed gyrotropic electronic structure. However, no indication for chirality is found. The relation between the atomic displacements and the transport properties is discussed in terms of Ti 3d and Se 4p states that only weakly couple to the CDW order.

cond-mat.str-el↗

arXiv2020

Structural Dynamics of incommensurate Charge-Density Waves tracked by Ultrafast Low-Energy Electron Diffraction

We study the non-equilibrium structural dynamics of the incommensurate and nearly-commensurate charge-density wave phases in 1T-TaS$_2$. Employing ultrafast low-energy electron diffraction (ULEED) with 1 ps temporal resolution, we investigate the ultrafast quench and recovery of the CDW-coupled periodic lattice distortion. Sequential structural relaxation processes are observed by tracking the intensities of main lattice as well as satellite diffraction peaks as well as the diffuse scattering background. Comparing distinct groups of diffraction peaks, we disentangle the ultrafast quench of the PLD amplitude from phonon-related reductions of the diffraction intensity. Fluence-dependent relaxation cycles reveal a long-lived partial suppression of the order parameter for up to 60 picoseconds, far outlasting the initial amplitude recovery and electron-phonon scattering times. This delayed return to a quasi-thermal level is controlled by lattice thermalization and coincides with the population of zone-center acoustic modes, as evidenced by a structured diffuse background. The long-lived non-equilibrium order parameter suppression suggests hot populations of CDW-coupled lattice modes. Finally, a broadening of the superlattice peaks is observed at high fluences, pointing to a nonlinear generation of phase fluctuations.

cond-mat.str-el↗

arXiv2020

Collapse of layer dimerization in the photo-induced hidden state of 1T-TaS2

Photo-induced switching between collective quantum states of matter is a fascinating rising field with exciting opportunities for novel technologies. Presently very intensively studied examples in this regard are nanometer-thick single crystals of the layered material 1T-TaS2 , where picosecond laser pulses can trigger a fully reversible insulator-to-metal transition (IMT). This IMT is believed to be connected to the switching between metastable collective quantum states, but the microscopic nature of this so-called hidden quantum state remained largely elusive up to now. Here we determine the latter by means of state-of-the-art x-ray diffraction and show that the laser-driven IMT involves a marked rearrangement of the charge and orbital order in the direction perpendicular to the TaS2-layers. More specifically, we identify the collapse of inter-layer molecular orbital dimers, which are a characteristic feature of the insulating phase, as a key mechanism for the non-thermal IMT in 1T-TaS2, which indeed involves a collective transition between two truly long-range ordered electronic crystals.

cond-mat.str-el↗

arXiv2020

Yu-Shiba-Rusinov states in the charge-density modulated superconductor NbSe2

NbSe$_2$ is a remarkable superconductor in which charge-density order coexists with pairing correlations at low temperatures. Here, we study the interplay of magnetic adatoms and their Yu-Shiba-Rusinov (YSR) bound states with the charge density order. Exploiting the incommensurate nature of the charge-density wave (CDW), our measurements provide a thorough picture of how the CDW affects both the energies and the wavefunctions of the YSR states. Key features of the dependence of the YSR states on adsorption site relative to the CDW are explained by model calculations. Several properties make NbSe$_2$ a promising substrate for realizing topological nanostructures. Our results will be important in designing such systems.

cond-mat.mes-hall↗

arXiv2020

Ubiquitous impact of localised impurity states on the exchange coupling mechanism in magnetic topological insulators

Since the discovery of the quantum anomalous Hall effect in the magnetically doped topological insulators (MTI) Cr:(Bi,Sb)$_2$Te$_3$ and V:(Bi,Sb)$_2$Te$_3$, the search for the exchange coupling mechanisms underlying the onset of ferromagnetism has been a central issue, and a variety of different scenarios have been put forward. By combining resonant photoemission, X-ray magnetic dichroism and multiplet ligand field theory, we determine the local electronic and magnetic configurations of V and Cr impurities in (Bi,Sb)$_2$Te$_3$. While strong pd hybridisation is found for both dopant types, their 3d densities of states show pronounced differences. State-of-the-art first-principles calculations show how these impurity states mediate characteristic short-range pd exchange interactions, whose strength sensitively varies with the position of the 3d states relative to the Fermi level. Measurements on films with varying host stoichiometry support this trend. Our results establish the essential role of impurity-state mediated exchange interactions in the magnetism of MTI.

cond-mat.str-el↗

arXiv2019

Time- and momentum-resolved photoemission studies using time-of-flight momentum microscopy at a free-electron laser

Time-resolved photoemission with ultrafast pump and probe pulses is an emerging technique with wide application potential. Real-time recording of non-equilibrium electronic processes, transient states in chemical reactions or the interplay of electronic and structural dynamics offers fascinating opportunities for future research. Combining valence-band and core-level spectroscopy with photoelectron diffraction for electronic, chemical and structural analysis requires few 10 fs soft X-ray pulses with some 10 meV spectral resolution, which are currently available at high repetition rate free-electron lasers. The PG2 beamline at FLASH (DESY, Hamburg) provides a high pulse rate of 5000 pulses/s, 60 fs pulse duration and 40 meV bandwidth in an energy range of 25-830 eV with a photon beam size down to 50 microns in diameter. We have constructed and optimized a versatile setup commissioned at FLASH/PG2 that combines FEL capabilities together with a multidimensional recording scheme for photoemission studies. We use a full-field imaging momentum microscope with time-of-flight energy recording as the detector for mapping of 3D band structures in ($k_x$, $k_y$, $E$) parameter space with unprecedented efficiency. Our instrument can image full surface Brillouin zones with up to 7 Å $^{-1}$ diameter in a binding-energy range of several eV, resolving about $2.5\times10^5$ data voxels. As an example, we present results for the ultrafast excited state dynamics in the model van der Waals semiconductor WSe$_2$.

cond-mat.mtrl-sci↗

arXiv2019

Doublon bottleneck in the ultrafast relaxation dynamics of hot electrons in 1T-TaS_2

Employing time-resolved photoelectron spectroscopy we analyze the relaxation dynamics of hot electrons in the charge density wave / Mott material 1T-TaS_2. At 1.2 eV above the Fermi level we observe a hot electron lifetime of 12 +- 5 fs in the metallic state and of 60 +- 10 fs in the broken symmetry ground state - a direct consequence of the reduced phase space for electron-electron scattering determined by the Mott gap. Boltzmann equation calculations which account for the interaction of hot electrons in a Bloch band with a doublon-holon excitation in the Mott state provide insight into the unoccupied electronic structure in the correlated state.

cond-mat.str-el↗

arXiv2019

Coherent modulation of the electron temperature and electron-phonon couplings in a 2D material

Ultrashort light pulses can selectively excite charges, spins and phonons in materials, providing a powerful approach for manipulating their properties. Here we use femtosecond laser pulses to coherently manipulate the electron and phonon distributions, and their couplings, in the charge density wave (CDW) material 1T-TaSe$_2$. After exciting the material with a short light pulse, spatial smearing of the electrons launches a coherent lattice breathing mode, which in turn modulates the electron temperature. This indicates a bi-directional energy exchange between the electrons and the strongly-coupled phonons. By tuning the laser excitation fluence, we can control the magnitude of the electron temperature modulation, from ~ 200 K in the case of weak excitation, to ~ 1000 K for strong laser excitation. This is accompanied by a switching of the dominant mechanism from anharmonic phonon-phonon coupling to coherent electron-phonon coupling, as manifested by a phase change of $π$ in the electron temperature modulation. Our approach thus opens up possibilities for coherently manipulating the interactions and properties of quasi-2D and other quantum materials using light.

cond-mat.mtrl-sci↗

arXiv2019

Orbital- and $k_z$-selective hybridisation of Se 4p and Ti 3d states in the charge density wave phase of TiSe$_2$

We revisit the enduring problem of the $2\times{}2\times{}2$ charge density wave (CDW) order in TiSe$_2$, utilising photon energy-dependent angle-resolved photoemission spectroscopy to probe the full three-dimensional high- and low-temperature electronic structure. Our measurements demonstrate how a mismatch of dimensionality between the 3D conduction bands and the quasi-2D valence bands in this system leads to a hybridisation that is strongly $k_z$-dependent. While such a momentum-selective coupling can provide the energy gain required to form the CDW, we show how additional "passenger" states remain, which couple only weakly to the CDW and thus dominate the low-energy physics in the ordered phase of TiSe$_2$.

cond-mat.str-el↗

arXiv2019

Ultrafast electron calorimetry uncovers a new long-lived metastable state in 1T-TaSe$_2$ mediated by mode-selective electron-phonon coupling

Quantum materials represent one of the most promising frontiers in the quest for faster, lightweight, energy efficient technologies. However, their inherent complexity and rich phase landscape make them challenging to understand or manipulate in useful ways. Here we present a new ultrafast electron calorimetry technique that can systematically uncover new phases of quantum matter. Using time- and angle-resolved photoemission spectroscopy, we measure the dynamic electron temperature, band structure and heat capacity. We then show that this is a very sensitive probe of phase changes in materials, because electrons react very quickly, and moreover generally are the smallest component of the total heat capacity. This allows us to uncover a new long-lived metastable state in the charge density wave material 1T-TaSe$_2$, that is distinct from all of the known equilibrium phases: it is characterized by a significantly reduced effective heat capacity that is only 30% of the normal value, due to selective electron-phonon coupling to a subset of phonon modes. As a result, significantly less energy is required to melt the charge order and transform the state of the material than under thermal equilibrium conditions.

cond-mat.mtrl-sci↗

arXiv2018

Decoding the ultrafast formation of a Fermi-Dirac distributed electron gas

Time- and angle-resolved photoelectron spectroscopy with 13 fs temporal resolution is used to follow the different stages in the formation of a Fermi-Dirac distributed electron gas in graphite after absorption of an intense 7 fs laser pulse. Within the first 50 fs after excitation a sequence of time frames is resolved which are characterized by different energy and momentum exchange processes among the involved photonic, electronic, and phononic degrees of freedom. The results reveal experimentally the complexity of the transition from a nascent non-thermal towards a thermal electron distribution due to the different timescales associated with the involved interaction processes.

cond-mat.mtrl-sci↗