arXiv subjects

Murat Sivis

Publications and source records attributed to Murat Sivis.

15 recordsLinked to original sources

arXiv2025

Roadmap for Quantum Nanophotonics with Free Electrons

Over the past century, continuous advancements in electron microscopy have enabled the synthesis, control, and characterization of high-quality free-electron beams. These probes carry an evanescent electromagnetic field that can drive localized excitations and provide high-resolution information on material structures and their optical responses, currently reaching the sub-ångström and few-meV regime. Moreover, combining free electrons with pulsed light sources in ultrafast electron microscopy adds temporal resolution in the sub-femtosecond range while offering enhanced control of the electron wave function. Beyond their exceptional capabilities for time-resolved spectromicroscopy, free electrons are emerging as powerful tools in quantum nanophotonics, on par with photons in their ability to carry and transfer quantum information, create entanglement within and with a specimen, and reveal previously inaccessible details on nanoscale quantum phenomena. This Roadmap outlines the current state of this rapidly evolving field, highlights key challenges and opportunities, and discusses future directions through a collection of topical sections prepared by leading experts.

cond-mat.mes-hall↗

arXiv2025

Revealing domain wall stability during ultrafast demagnetization

The ultrafast control of nanoscale spin textures such as magnetic domain walls or skyrmions is essential for advancing high-speed, high-density spintronics. However, imaging their dynamics will require a technique that combines nanometer spatial and femtosecond temporal resolution. Introducing ultrafast sub-wavelength imaging in the extreme ultraviolet, we track domain wall properties during ultrafast demagnetization in ferro- and ferrimagnetic thin films. We reveal that domain walls remain invariant in position, shape, and width, down to a demonstrated sub-nanometer precision, for up to 50% demagnetization. Stronger excitation causes stochastic nanoscale domain switching. This previously unobservable robustness of laser-excited domain walls highlights the localized nature of photoinduced demagnetization and presents both challenges and opportunities for all-optical magnetic control. The presented technique can be generalized to directly probe nanoscale dynamics in spintronic materials and devices.

cond-mat.mtrl-sci↗

arXiv2025

Observation of quantum entanglement between free electrons and photons

Quantum entanglement is central to both the foundations of quantum mechanics and the development of new technologies in information processing, communication, and sensing. Entanglement has been realised in a variety of physical systems, spanning atoms, ions, photons, collective excitations, and hybrid combinations of particles. Remarkably, however, photons and free electrons -- the quanta of light and their most elementary sources -- have never been observed in an entangled state. Here, we demonstrate quantum entanglement between free electrons and photons. We show that entanglement is produced when an electron, prepared in a superposition of two beams, passes a nanostructure and generates transition radiation in a polarisation state tied to the electron path. By implementing quantum state tomography, we reconstruct the full density matrix of the electron-photon pair, and show that the Peres-Horodecki separability criterion is violated by more than 7 standard deviations. Based on this foundational element of emerging free-electron quantum optics, we anticipate manifold developments in enhanced electron imaging and spectroscopy beyond the standard quantum limit. More broadly, the ability to generate and measure entanglement opens electron microscopy to previously inaccessible quantum observables and correlations in solids and nanostructures.

quant-ph↗

arXiv2023

Attosecond electron microscopy by free-electron homodyne detection

Time-resolved electron microscopy aims at tracking nanoscale excitations and dynamic states of matter with a temporal resolution ultimately reaching the attosecond regime. Periodically time-varying fields in an illuminated specimen cause free-electron inelastic scattering, which enables the spectroscopic imaging of near-field intensities. However, access to the evolution of nanoscale fields and structures within the light cycle requires a sensitivity to the optical phase. Here, we introduce Free-Electron Homodyne Detection (FREHD) as a universally applicable approach to electron microscopy of phase-resolved optical responses at high spatiotemporal resolution. In this scheme, a phase-controlled reference interaction serves as the local oscillator to extract arbitrary sample-induced modulations of a free-electron wave function. We demonstrate this principle through the phase-resolved imaging of plasmonic fields with few-nanometer spatial and sub-cycle temporal resolutions. Due to its sensitivity to both phase- and amplitude-modulated electron beams, FREHD measurements will be able to detect and amplify weak signals stemming from a wide variety of microscopic origins, including linear and nonlinear optical polarizations, atomic and molecular resonances and attosecond-modulated structure factors.

physics.optics↗

arXiv2023

High-sensitivity extreme-ultraviolet transient absorption spectroscopy enabled by machine learning

We introduce a machine-learning-based approach to enhance the sensitivity of optical-extreme ultraviolet (XUV) transient absorption spectroscopy. A reference spectrum is used as input to a three-layer feed-forward neural network, allowing for an efficient elimination of source noise from measurement data. In pump-probe experiments using high-harmonic radiation, we show a more than tenfold improvement in noise suppression in XUV transient absorption spectra compared to conventional referencing. Utilizing strong spectral correlations in the source fluctuations, the network facilitates a pixel-wise noise reduction without the need for wavelength calibration of the reference spectrum. The presented method can be adapted to a wide range of beam lines and enables the investigation of subtle electron and lattice dynamics in the weak excitation regime, relevant for the study of photovoltaics and photoinduced phase transitions of strongly correlated materials.

physics.optics↗

arXiv2022

Electronic and structural fingerprints of charge density wave excitations in extreme ultraviolet transient absorption spectroscopy

Femtosecond core-level transient absorption spectroscopy is utilized to investigate photoinduced dynamics of the charge density wave in 1T-TiSe2 at the Ti M2,3 edge (30-50 eV). Photoexcited carriers and phonons are found to primarily induce spectral red-shifts of core-level excitations, and a carrier relaxation time and phonon heating time of approximately 360 fs and 1.0 ps are extracted, respectively. Pronounced oscillations in delay-dependent absorption spectra are assigned to coherent excitations of the optical $A_{1g}$ phonon (6.0 THz) and the $A_{1g}^*$ charge density wave amplitude mode (3.3 THz). By comparing the measured spectra with time-dependent density functional theory simulations, we determine the directions of the momentary atomic displacements of both coherent modes and estimate their amplitudes. This work presents a first look on charge density wave excitations with table-top core-level transient absorption spectroscopy, enabling simultaneous access to electronic and lattice excitation and relaxation.

cond-mat.mtrl-sci↗

arXiv2021

Chiral high-harmonic generation and spectroscopy on solid surfaces using polarization-tailored strong fields

Strong-field methods in solids enable new strategies for ultrafast nonlinear spectroscopy and provide all-optical insights into the electronic properties of condensed matter in reciprocal and real space. Additionally, solid-state media offers unprecedented possibilities to control high-harmonic generation using modified targets or tailored excitation fields. Here we merge these important points and demonstrate circularly-polarized high-harmonic generation with polarization-matched excitation fields for spectroscopy of chiral electronic properties at surfaces. The sensitivity of our approach is demonstrated for structural helicity and termination-mediated ferromagnetic order at the surface of silicon-dioxide and magnesium oxide, respectively. Circularly polarized radiation emanating from a solid sample now allows to add basic symmetry properties as chirality to the arsenal of strong-field spectroscopy in solids. Together with its inherent temporal (femtosecond) resolution and non-resonant broadband spectrum, the polarization control of high harmonics from condensed matter can illuminate ultrafast and strong field dynamics of surfaces, buried layers or thin films.

physics.optics↗

arXiv2020

Ultrafast high-harmonic nanoscopy of magnetization dynamics

Light-induced magnetization changes, such as all-optical switching, skyrmion nucleation, and intersite spin transfer, unfold on temporal and spatial scales down to femtoseconds and nanometers, respectively. Pump-probe spectroscopy and diffraction studies indicate that spatio-temporal dynamics may drastically affect the non-equilibrium magnetic evolution. Yet, direct real-space magnetic imaging on the relevant timescale has remained challenging. Here, we demonstrate ultrafast high-harmonic nanoscopy employing circularly polarized high-harmonic radiation for real-space imaging of femtosecond magnetization dynamics. We observe the reversible and irreversible evolution of nanoscale spin textures following femtosecond laser excitation. Specifically, we map quenched magnetic domains and localized spin structures in Co/Pd multilayers with a sub-wavelength spatial resolution down to 16 nm, and strobosocopically trace the local magnetization dynamics with 40 fs temporal resolution. Our approach enables the highest spatio-temporal resolution of magneto-optical imaging to date. Facilitating ultrafast imaging with an extreme sensitivity to various microscopic degrees of freedom expressed in chiral and linear dichroism, we envisage a wide range of applications spanning magnetism, phase transitions, and carrier dynamics.

physics.optics↗

arXiv2020

Clocking plasmon nanofocusing by THz near-field streaking

We apply terahertz (THz) near-field streaking in a nanofocusing geometry to investigate plasmon polariton propagation on the shaft of a conical nanotip. By evaluating the delay between a streaking spectrogram for plasmon-induced photoemission with a measurement for direct apex excitation, we obtain an average plasmon group velocity, which is in agreement with numerical simulations. Combining plasmon-induced photoemission with THz near-field streaking facilitates extensive control over localized photoelectron sources for time-resolved imaging and diffraction.

physics.optics↗

arXiv2020

Spontaneous and Stimulated Electron-Photon Interactions in Nanoscale Plasmonic Near Fields

We demonstrate spatially-resolved measurements of spontaneous and stimulated electron-photon interactions in nanoscale optical near fields using electron energy-loss spectroscopy (EELS), cathodoluminescence spectroscopy (CL), and photon-induced near-field electron microscopy (PINEM). Specifically, we study resonant surface plasmon modes that are tightly confined to the tip apexes of an Au nanostar, enabling a direct correlation of EELS, CL, and PINEM on the same physical structure at the nanometer length scale. Complemented by numerical electromagnetic boundary-element method calculations, we discuss the spontaneous and stimulated electron-photon interaction strength and spatial dependence of our EELS, CL and PINEM distributions. We demonstrate that in the limit of an isolated tip mode, spatial variations in the electron-near field coupling are fully determined by the modal electric field profile, irrespective of the spontaneous (in EELS and CL) or stimulated nature (in PINEM) of the process. Yet we show that coupling to the tip modes crucially depends on the incident electron energy with a maximum at a few keV, depending on the proximity of the interaction to the tip apex. Our results provide elementary insights into spontaneous and stimulated electron-light-matter interactions at the nanoscale that have key implications for research on (quantum) coherent optical phenomena in electron microscopy.

physics.optics↗

arXiv2019

Controlling free electrons with optical whispering-gallery modes

Free-electron beams serve as uniquely versatile probes of microscopic structure and composition, and have repeatedly revolutionized atomic-scale imaging, from solid-state physics to structural biology. Over the past decade, the manipulation and interaction of electrons with optical fields has seen significant progress, enabling novel imaging methods, schemes of near-field electron acceleration, and culminating in 4D microscopy techniques with both high temporal and spatial resolution. However, weak coupling strengths of electron beams to optical excitations are a standing issue for existing and emerging applications of optical free-electron control. Here, we demonstrate phase matched near-field coupling of a free-electron beam to optical whispering gallery modes of dielectric microresonators. The cavity-enhanced interaction with these optically excited modes imprints a strong phase modulation on co-propagating electrons, which leads to electron-energy sidebands up to hundreds of photon orders and a spectral broadening of 700 eV. Mapping the near-field interaction with ultrashort electron pulses in space and time, we trace the temporal ring-down of the microresonator following a femtosecond excitation and observe the cavity's resonant spectral response. Resonantly enhancing the coupling of electrons and light via optical cavities, with efficient injection and extraction, can open up novel applications such as continuous-wave acceleration, attosecond structuring, and real-time all-optical electron detection.

physics.optics↗

arXiv2017

Continuous-Wave Multiphoton Photoemission from Plasmonic Nanostars

Highly nonlinear optical processes, such as multiphoton photoemission, require high intensities, typically achieved with ultrashort laser pulses and, hence, were first observed with the advent of picosecond laser technology. An alternative approach for reaching the required field intensities is offered by localized optical resonances such as plasmons. Here, we demonstrate localized multiphoton photoemission from plasmonic nanostructures under continuous-wave illumination. We use synthesized plasmonic gold nanostars, which exhibit sharp tips with structural features smaller than 5 nm, leading to near-field-intensity enhancements exceeding 1000. This large enhancement facilitates 3-photon photoemission driven by a simple continuous-wave laser diode. We characterize the intensity and polarization dependencies of the photoemission yield from both individual nanostars and ensembles. Numerical simulations of the plasmonic enhancement, the near-field distributions, and the photoemission intensities are in good agreement with experiment. Our results open a new avenue for the design of nanoscale electron sources.

physics.optics↗

arXiv2017

Nanoscale Magnetic Imaging using Circularly Polarized High-Harmonic Radiation

This work demonstrates nanoscale magnetic imaging using bright circularly polarized high-harmonic radiation. We utilize the magneto-optical contrast of worm-like magnetic domains in a Co/Pd multilayer structure, obtaining quantitative amplitude and phase maps by lensless imaging. A diffraction-limited spatial resolution of 49 nm is achieved with iterative phase reconstruction enhanced by a holographic mask. Harnessing the unique coherence of high harmonics, this approach will facilitate quantitative, element-specific and spatially-resolved studies of ultrafast magnetization dynamics, advancing both fundamental and applied aspects of nanoscale magnetism.

physics.optics↗

arXiv2016

Ultrafast transmission electron microscopy using a laser-driven field emitter: femtosecond resolution with a high coherence electron beam

We present the development of the first ultrafast transmission electron microscope (UTEM) driven by localized photoemission from a field emitter cathode. We describe the implementation of the instrument, the photoemitter concept and the quantitative electron beam parameters achieved. Establishing a new source for ultrafast TEM, the Göttingen UTEM employs nano-localized linear photoemission from a Schottky emitter, which enables operation with freely tunable temporal structure, from continuous wave to femtosecond pulsed mode. Using this emission mechanism, we achieve record pulse properties in ultrafast electron microscopy of 9 Å focused beam diameter, 200 fs pulse duration and 0.6 eV energy width. We illustrate the possibility to conduct ultrafast imaging, diffraction, holography and spectroscopy with this instrument and also discuss opportunities to harness quantum coherent interactions between intense laser fields and free electron beams.

cond-mat.mes-hall↗

arXiv2013

Generation and Bistability of a Waveguide Nanoplasma Observed by Enhanced Extreme-Ultraviolet Fluorescence

We present a study of the highly nonlinear optical excitation of noble gases in tapered hollow waveguides using few-femtosecond laser pulses. The local plasmonic field enhancement induces the generation of a nanometric plasma, resulting in incoherent extreme-ultraviolet fluorescence from optical transitions of neutral and ionized xenon, argon, and neon. Despite sufficient intensity in the waveguide, high-order harmonic generation is not observed. The fluorescent emission exhibits a strong bistability manifest as an intensity hysteresis, giving strong indications for multistep collisional excitations.

physics.optics↗