Disentangling the multiorbital contributions of excitons by photoemission exciton tomography.

Excitons are realizations of a correlated many-particle wave function, specifically consisting of electrons and holes in an entangled state. Excitons occur widely in semiconductors and are dominant excitations in semiconducting organic and low-dimensional quantum materials. To efficiently harness the strong optical response and high tuneability of excitons in optoelectronics and in energy-transformation processes, access to the full wavefunction of the entangled state is critical, but has so far not been feasible. Here, we show how time-resolved photoemission momentum microscopy can be used to gain access to the entangled wavefunction and to unravel the exciton's multiorbital electron and hole contributions. For the prototypical organic semiconductor buckminsterfullerene (C60), we exemplify the capabilities of exciton tomography and achieve unprecedented access to key properties of the entangled exciton state including localization, charge-transfer character, and ultrafast exciton formation and relaxation dynamics.

Probing electron-hole Coulomb correlations in the exciton landscape of a twisted semiconductor heterostructure.

In two-dimensional semiconductors, cooperative and correlated interactions determine the material's excitonic properties and can even lead to the creation of correlated states of matter. Here, we study the fundamental two-particle correlated exciton state formed by the Coulomb interaction between single-particle holes and electrons. We find that the ultrafast transfer of an exciton's hole across a type II band-aligned semiconductor heterostructure leads to an unexpected sub-200-femtosecond upshift of the single-particle energy of the electron being photoemitted from the two-particle exciton state. While energy relaxation usually leads to an energetic downshift of the spectroscopic signature, we show that this upshift is a clear fingerprint of the correlated interaction of the electron and hole parts of the exciton. In this way, time-resolved photoelectron spectroscopy is straightforwardly established as a powerful method to access electron-hole correlations and cooperative behavior in quantum materials. Our work highlights this capability and motivates the future study of optically inaccessible correlated excitonic and electronic states of matter.

Formation of moiré interlayer excitons in space and time.

Moiré superlattices in atomically thin van der Waals heterostructures hold great promise for extended control of electronic and valleytronic lifetimes1-7, the confinement of excitons in artificial moiré lattices8-13 and the formation of exotic quantum phases14-18. Such moiré-induced emergent phenomena are particularly strong for interlayer excitons, where the hole and the electron are localized in different layers of the heterostructure19,20. To exploit the full potential of correlated moiré and exciton physics, a thorough understanding of the ultrafast interlayer exciton formation process and the real-space wavefunction confinement is indispensable. Here we show that femtosecond photoemission momentum microscopy provides quantitative access to these key properties of the moiré interlayer excitons. First, we elucidate that interlayer excitons are dominantly formed through femtosecond exciton-phonon scattering and subsequent charge transfer at the interlayer-hybridized Σ valleys. Second, we show that interlayer excitons exhibit a momentum fingerprint that is a direct hallmark of the superlattice moiré modification. Third, we reconstruct the wavefunction distribution of the electronic part of the exciton and compare the size with the real-space moiré superlattice. Our work provides direct access to interlayer exciton formation dynamics in space and time and reveals opportunities to study correlated moiré and exciton physics for the future realization of exotic quantum phases of matter.

Far-from-Equilibrium Electron-Phonon Interactions in Optically Excited Graphene.

Comprehending far-from-equilibrium many-body interactions is one of the major goals of current ultrafast condensed matter physics research. Here, a particularly interesting but barely understood situation occurs during a strong optical excitation, where the electron and phonon systems can be significantly perturbed and the quasiparticle distributions cannot be described with equilibrium functions. In this work, we use time- and angle-resolved photoelectron spectroscopy to study such far-from-equilibrium many-body interactions for the prototypical material graphene. In accordance with theoretical simulations, we find remarkable transient renormalizations of the quasiparticle self-energy caused by the photoinduced nonequilibrium conditions. These observations can be understood by ultrafast scatterings between nonequilibrium electrons and strongly coupled optical phonons, which signify the crucial role of ultrafast nonequilibrium dynamics on many-body interactions. Our results advance the understanding of many-body physics in extreme conditions, which is important for any endeavor to optically manipulate or create non-equilibrium states of matter.

Ultrafast element-resolved magneto-optics using a fiber-laser-driven extreme ultraviolet light source.

We present a novel setup to measure the transverse magneto-optical Kerr effect in the extreme ultraviolet spectral range based on a fiber laser amplifier system with a repetition rate between 100 and 300 kHz, which we use to measure element-resolved demagnetization dynamics. The setup is equipped with a strong electromagnet and a cryostat, allowing measurements between 10 and 420 K using magnetic fields up to 0.86 T. The performance of our setup is demonstrated by a set of temperature- and time-dependent magnetization measurements with elemental resolution.

Time-resolved momentum microscopy with a 1 MHz high-harmonic extreme ultraviolet beamline.

Recent progress in laser-based high-repetition rate extreme ultraviolet (EUV) light sources and multidimensional photoelectron spectroscopy enables the build-up of a new generation of time-resolved photoemission experiments. Here, we present a setup for time-resolved momentum microscopy driven by a 1 MHz fs EUV table-top light source optimized for the generation of 26.5 eV photons. The setup provides simultaneous access to the temporal evolution of the photoelectron's kinetic energy and in-plane momentum. We discuss opportunities and limitations of our new experiment based on a series of static and time-resolved measurements on graphene.

Phase retrieval algorithms for lensless imaging using diffractive shearing interferometry.

Diffractive shearing interferometry (DSI) is a method that has recently been developed to perform lensless imaging using extreme ultraviolet radiation generated by high-harmonic generation. In this paper, we investigate the uniqueness of the DSI solution and the requirements for the support constraint size. We find that there can be multiple solutions to the DSI problem that consist of displaced copies of the actual object. These alternative solutions can be eliminated by enforcing a sufficiently tight support constraint, or by introducing additional synthetic constraints. We furthermore propose a new DSI algorithm inspired by the analogy with coherent diffractive imaging (CDI) algorithms: the original DSI algorithm is in a way analogous to the hybrid input-output algorithm as used in CDI, and we propose a new algorithm that is more analogous to the error reduction algorithm as used in CDI. We find that the newly proposed algorithm is suitable for final refinement of the reconstruction.

Extreme ultraviolet lensless imaging without object support through rotational diversity in diffractive shearing interferometry.

We report on a method that allows microscopic image reconstruction from extreme-ultraviolet diffraction patterns without the need for object support constraints or other prior knowledge about the object structure. This is achieved by introducing additional diversity through rotation of an object in a rotationally asymmetric probe beam, produced by the spatial interference between two phase-coherent high-harmonic beams. With this rotational diffractive shearing interferometry method, we demonstrate robust image reconstruction of microscopic objects at wavelengths around 30 nm, using images recorded at only three to five different object rotations.

Broadband extreme ultraviolet dispersion measurements using a high-harmonic source.

We demonstrate direct dispersion measurements of various thin films at extreme ultraviolet (EUV) wavelengths, using a table-top laser-driven high-harmonic generation (HHG) source. In this method, spatially separated identical EUV pulses are generated through HHG with a pair of phase-locked infrared pulses. The EUV pulses are re-imaged to a sample plane using a single toroidal mirror, such that one pulse illuminates the target thin film, while the other pulse passes through a reference aperture. By comparing the EUV interference with and without a sample, we are able to extract the dispersion properties of the sample, integrated over the full film thickness. We have measured thin films of titanium, nickel, copper, and silicon nitride, demonstrating that this technique can be applied to a wide range of materials, only requiring a film thin, enough for sufficient EUV transmission.

Diffractive shear interferometry for extreme ultraviolet high-resolution lensless imaging.

We demonstrate a novel imaging approach and associated reconstruction algorithm for far-field coherent diffractive imaging, based on the measurement of a pair of laterally sheared diffraction patterns. The differential phase profile retrieved from such a measurement leads to improved reconstruction accuracy, increased robustness against noise, and faster convergence compared to traditional coherent diffractive imaging methods. We measure laterally sheared diffraction patterns using Fourier-transform spectroscopy with two phase-locked pulse pairs from a high-harmonic source. Using this approach, we demonstrate spectrally resolved imaging at extreme ultraviolet wavelengths between 28 and 35 nm.

Spectrally resolved single-shot wavefront sensing of broadband high-harmonic sources.

Wavefront sensors are an important tool to characterize coherent beams of extreme ultraviolet radiation. However, conventional Hartmann-type sensors do not allow for independent wavefront characterization of different spectral components that may be present in a beam, which limits their applicability for intrinsically broadband high-harmonic generation (HHG) sources. Here we introduce a wavefront sensor that measures the wavefronts of all the harmonics in a HHG beam in a single camera exposure. By replacing the mask apertures with transmission gratings at different orientations, we simultaneously detect harmonic wavefronts and spectra, and obtain sensitivity to spatiotemporal structure such as pulse front tilt as well. We demonstrate the capabilities of the sensor through a parallel measurement of the wavefronts of 9 harmonics in a wavelength range between 25 and 49 nm, with up to λ/32 precision.

Effect of soil temperature on optical frequency transfer through unidirectional dense-wavelength-division-multiplexing fiber-optic links.

Results of optical frequency transfer over a carrier-grade dense-wavelength-division-multiplexing (DWDM) optical fiber network are presented. The relation between soil temperature changes on a buried optical fiber and frequency changes of an optical carrier through the fiber is modeled. Soil temperatures, measured at various depths by the Royal Netherlands Meteorology Institute (KNMI) are compared with observed frequency variations through this model. A comparison of a nine-day record of optical frequency measurements through the 2×298 km fiber link with soil temperature data shows qualitative agreement. A soil temperature model is used to predict the link stability over longer periods (days-months-years). We show that optical frequency dissemination is sufficiently stable to distribute and compare, e.g., rubidium frequency standards over standard DWDM optical fiber networks using unidirectional fibers.

Measuring plasma levels of carbamazepine. A pharmacokinetic study in patients with affective disorders.

Twenty-four patients suffering from affective disorders, who were being regularly treated with carbamazepine, were studied to determine the course of plasma levels of carbamazepine before (trough levels) and two and four hours after morning intake (peak levels). A large interindividual variation was found between highest peak level and trough level. Despite the lack of systematic studies it is concluded that measuring plasma levels to determine the therapeutic range of carbamazepine should use trough levels, which should provisionally be aimed at between six and eight mg/l. In order to avoid adverse effects, peak levels should not exceed 12 (or even 10) mg/l.