Hamburg Centre for Ultrafast Imaging

Topological properties lie at the heart of many fascinating phenomena in solid-state systems such as quantum Hall systems or Chern insulators. The topology of the bands can be captured by the distribution of Berry curvature, which describes the geometry of the eigenstates across the Brillouin zone. Using fermionic ultracold atoms in a hexagonal optical lattice, we engineered the Berry curvature of the Bloch bands using resonant driving and show a full momentum-resolved measurement of the ensuing Berry curvature. Our results pave the way to explore intriguing phases of matter with interactions in topological band structures.

Driving strontium titanate ferroelectric Hidden phases are metastable collective states of matter that are typically not accessible on equilibrium phase diagrams. Nova et al. used infrared pulses to excite higher-frequency lattice modes that drive the crystal into a metastable ferroelectric phase, a phase that can persist for many hours. X. Li et al. used terahertz fields to drive the soft mode that moves the ions in the crystal into the positions they occupy in the new phase. The ferroelectric phase in this case was transient, lasting on the order of 10 picoseconds. Because these hidden phases can host exotic properties in otherwise conventional materials, the accessibility to and control of such hidden phases may broaden potential functionality and applications. Science , this issue p. 1075 , p. 1079

With the recent advances in ultrabright electron and x-ray sources, it is now possible to extend crystallography to the femtosecond time domain to literally light up atomic motions involved in the primary processes governing structural transitions. This review chronicles the development of brighter and brighter electron and x-ray sources that have enabled atomic resolution to structural dynamics for increasingly complex systems. The primary focus is on achieving sufficient brightness using pump-probe protocols to resolve the far-from-equilibrium motions directing chemical processes that in general lead to irreversible changes in samples. Given the central importance of structural transitions to conceptualizing chemistry, this emerging field has the potential to significantly improve our understanding of chemistry and its connection to driving biological processes.

The “hole” story of water ionization The direct observation of the cationic hole H 2 O + that is formed in liquid water after ionization has been a long-standing experimental challenge. Previous attempts using optical and ultraviolet techniques have failed to reveal its key spectroscopic signature during ultrafast transformation into a OH radical. Loh et al. address this gap by using intense, ultrafast x-ray pulses from an x-ray free electron laser at ∼530 electron volts. They found compelling evidence for the formation H 2 O + and its decay to an OH radical by a proton transfer mechanism and elucidated the other fastest–time scale steps in the early-time dynamics of ionized liquid water. Science , this issue p. 179

Atomic models based on high-resolution density maps are the ultimate result of the cryo-EM structure determination process. Here, we introduce a general procedure for local sharpening of cryo-EM density maps based on prior knowledge of an atomic reference structure. The procedure optimizes contrast of cryo-EM densities by amplitude scaling against the radially averaged local falloff estimated from a windowed reference model. By testing the procedure using six cryo-EM structures of TRPV1, β-galactosidase, γ-secretase, ribosome-EF-Tu complex, 20S proteasome and RNA polymerase III, we illustrate how local sharpening can increase interpretability of density maps in particular in cases of resolution variation and facilitates model building and atomic model refinement.

hole intercepts the classic oxidation event and leads to the formation of the catalytically active gold clusters on subnanometer scale.

The emergent field of cavity quantum materials bridges collective many-body phenomena in solid state platforms with strong light–matter coupling in cavity quantum electrodynamics. This brief review provides an overview of the state of the art of cavity platforms and highlights recent theoretical proposals and first experimental demonstrations of cavity control of collective phenomena in quantum materials. This encompasses light–matter coupling between electrons and cavity modes, cavity superconductivity, cavity phononics and ferroelectricity, correlated systems in a cavity, light–magnon coupling, cavity topology and the quantum Hall effect, as well as super-radiance. An outlook of potential future developments is given.

Long-distance quantum communication and networking require quantum memory nodes with efficient optical interfaces and long memory times. We report the realization of an integrated two-qubit network node based on silicon-vacancy centers (SiVs) in diamond nanophotonic cavities. Our qubit register consists of the SiV electron spin acting as a communication qubit and the strongly coupled silicon-29 nuclear spin acting as a memory qubit with a quantum memory time exceeding 2 seconds. By using a highly strained SiV, we realize electron-photon entangling gates at temperatures up to 1.5 kelvin and nucleus-photon entangling gates up to 4.3 kelvin. We also demonstrate efficient error detection in nuclear spin-photon gates by using the electron spin as a flag qubit, making this platform a promising candidate for scalable quantum repeaters.

= 125 K. XPCS probes the dynamics in momentum space, which in the SAXS geometry reflects structural relaxation on the nanometer length scale. The dynamics of HDA are characterized by a slow component with a large time constant, arising from viscoelastic relaxation and stress release from nanometer-sized heterogeneities. Above 110 K a faster, strongly temperature-dependent component appears, with momentum transfer dependence pointing toward nanoscale diffusion. This dynamical component slows down after transition into the low-density form at 130 K, but remains diffusive. The diffusive character of both the high- and low-density forms is discussed among different interpretations and the results are most consistent with the hypothesis of a liquid-liquid transition in the ultraviscous regime.

Alzheimer's disease is a common neurodegenerative, progressive, and fatal disorder. Generation and deposition of amyloid beta (Aβ) peptides associate with its pathogenesis and small soluble Aβ oligomers show the most pronounced neurotoxic effects and correlate with disease initiation and progression. Recent findings showed that Aβ oligomers bind to the cellular prion protein (PrP(C) ) eliciting neurotoxic effects. The role of exosomes, small extracellular vesicles of endosomal origin, in Alzheimer's disease is only poorly understood. Besides serving as disease biomarkers they may promote Aβ plaque formation, decrease Aβ-mediated synaptotoxicity, and enhance Aβ clearance. Here, we explore how exosomal PrP(C) connects to protective functions attributed to exosomes in Alzheimer's disease. To achieve this, we generated a mouse neuroblastoma PrP(C) knockout cell line using transcription activator-like effector nucleases. Using these, as well as SH-SY5Y human neuroblastoma cells, we show that PrP(C) is highly enriched on exosomes and that exosomes bind amyloid beta via PrP(C) . Exosomes showed highest binding affinity for dimeric, pentameric, and oligomeric Aβ species. Thioflavin T assays revealed that exosomal PrP(C) accelerates fibrillization of amyloid beta, thereby reducing neurotoxic effects imparted by oligomeric Aβ. Our study provides further evidence for a protective role of exosomes in Aβ-mediated neurodegeneration and highlights the importance of exosomal PrP(C) in molecular mechanisms of Alzheimer's disease. We show that the prion protein (PrP(C) ) on exosomes captures neurotoxic species of amyloid beta (Aβ) promoting its fibrillization. Our study provides evidence for a protective role of exosomes in Alzheimer`s disease and suggests that, depending on its membrane topology, PrP(C) holds a dual function: when expressed at the neuronal surface it acts as receptor for Aβ leading to neurotoxic signaling, whereas it detoxifies Aβ when present on exosomes. This provides further support for key roles of PrP(C) in Alzheimer's disease.

Integer-valued topological indices, characterizing nonlocal properties of quantum states of matter, are known to directly predict robust physical properties of equilibrium systems. The Chern number, e.g., determines the quantized Hall conductivity of an insulator. Using non-interacting fermionic atoms in a periodically driven optical lattice, here we demonstrate experimentally that the Chern number determines also the far-from-equilibrium dynamics of a quantum system. Extending a respective proposal to Floquet systems, we measure the linking number that characterizes the trajectories of momentum-space vortices emerging after a strong quench. We observe that it directly corresponds to the ground-state Chern number. This one-to-one relation between a dynamical and a static topological index allows us to experimentally map out the phase diagram of our system. Furthermore, we measure the instantaneous Chern number and show that it remains zero under the unitary dynamics.

Abstract Integer-valued topological indices, characterizing nonlocal properties of quantum states of matter, are known to directly predict robust physical properties of equilibrium systems. The Chern number, e.g., determines the quantized Hall conductivity of an insulator. Using non-interacting fermionic atoms in a periodically driven optical lattice, here we demonstrate experimentally that the Chern number determines also the far-from-equilibrium dynamics of a quantum system. Extending a respective proposal to Floquet systems, we measure the linking number that characterizes the trajectories of momentum-space vortices emerging after a strong quench. We observe that it directly corresponds to the ground-state Chern number. This one-to-one relation between a dynamical and a static topological index allows us to experimentally map out the phase diagram of our system. Furthermore, we measure the instantaneous Chern number and show that it remains zero under the unitary dynamics.

Recent advances in high-order harmonic generation have made it possible to use a tabletop-scale setup to produce spatially and temporally coherent beams of light with bandwidth spanning 12 octaves, from the ultraviolet up to x-ray photon energies >1.6 keV. Here we demonstrate the use of this light for x-ray-absorption spectroscopy at the K- and L-absorption edges of solids at photon energies near 1 keV. We also report x-ray-absorption spectroscopy in the water window spectral region (284-543 eV) using a high flux high-order harmonic generation x-ray supercontinuum with 10^{9} photons/s in 1% bandwidth, 3 orders of magnitude larger than has previously been possible using tabletop sources. Since this x-ray radiation emerges as a single attosecond-to-femtosecond pulse with peak brightness exceeding 10^{26} photons/s/mrad^{2}/mm^{2}/1% bandwidth, these novel coherent x-ray sources are ideal for probing the fastest molecular and materials processes on femtosecond-to-attosecond time scales and picometer length scales.

Abstract Sunlight-driven H 2 generation is a central technology to tackle our impending carbon-based energy collapse. Colloidal photocatalysts consisting of plasmonic and catalytic nanoparticles are promising for H 2 production at solar irradiances, but their performance is hindered by absorption and multiscattering events. Here we present a two-dimensional bimetallic catalyst by incorporating platinum nanoparticles into a well-defined supercrystal of gold nanoparticles. The bimetallic supercrystal exhibited an H 2 generation rate of $$139\,{\mathrm{mmol}}\,{\mathrm{g}}_{\mathrm{cat}}^{-1}\,{\mathrm{h}}^{-1}$$ <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:mn>139</mml:mn> <mml:mspace/> <mml:mi>mmol</mml:mi> <mml:mspace/> <mml:msubsup> <mml:mrow> <mml:mi>g</mml:mi> </mml:mrow> <mml:mrow> <mml:mi>cat</mml:mi> </mml:mrow> <mml:mrow> <mml:mo>−</mml:mo> <mml:mn>1</mml:mn> </mml:mrow> </mml:msubsup> <mml:mspace/> <mml:msup> <mml:mrow> <mml:mi>h</mml:mi> </mml:mrow> <mml:mrow> <mml:mo>−</mml:mo> <mml:mn>1</mml:mn> </mml:mrow> </mml:msup> </mml:mrow> </mml:math> via formic acid dehydrogenation under visible light illumination and solar irradiance. This configuration makes it possible to study the interaction between the two metallic materials and the influence of this in catalysis. We observe a correlation between the intensity of the electric field in the hotspots and the boosted catalytic activity of platinum nanoparticles, while identifying a minor role of heat and gold-to-platinum charge transfer in the enhancement. Our results demonstrate the benefits of two-dimensional configurations with optimized architecture for liquid-phase photocatalysis.

We develop the multi-layer multi-configuration time-dependent Hartree method for bosons (ML-MCTDHB), a variational numerically exact ab initio method for studying the quantum dynamics and stationary properties of general bosonic systems. ML-MCTDHB takes advantage of the permutation symmetry of identical bosons, which allows for investigations of the quantum dynamics from few to many-body systems. Moreover, the multi-layer feature enables ML-MCTDHB to describe mixed bosonic systems consisting of arbitrary many species. Multi-dimensional as well as mixed-dimensional systems can be accurately and efficiently simulated via the multi-layer expansion scheme. We provide a detailed account of the underlying theory and the corresponding implementation. We also demonstrate the superior performance by applying the method to the tunneling dynamics of bosonic ensembles in a one-dimensional double well potential, where a single-species bosonic ensemble of various correlation strengths and a weakly interacting two-species bosonic ensemble are considered.

Photoionization using attosecond pulses can lead to the formation of coherent superpositions of the electronic states of the parent ion. However, ultrafast electron ejection triggers not only electronic but also nuclear dynamics---leading to electronic decoherence, which is typically neglected on time scales up to tens of femtoseconds. We propose a full quantum-dynamical treatment of nuclear motion in an adiabatic framework, where nuclear wave packets move on adiabatic potential energy surfaces expanded up to second order at the Franck-Condon point. We show that electronic decoherence is caused by the interplay of a large number of nuclear degrees of freedom and by the relative topology of the potential energy surfaces. Application to ${\mathrm{H}}_{2}\mathrm{O}$, paraxylene, and phenylalanine shows that an initially coherent state evolves to an electronically mixed state within just a few femtoseconds. In these examples the fast vibrations involving hydrogen atoms do not affect electronic coherence at short times. Conversely, vibrational modes involving the whole molecular skeleton, which are slow in the ground electronic state, quickly destroy it upon photoionization.

The assembly of plasmonic nanoparticles into ordered 2D- and 3D-superlattices could pave the way towards new tailored materials for plasmonic sensing, photocatalysis and manipulation of light on the nanoscale. The properties of such materials strongly depend on their geometry, and accordingly straightforward protocols to obtain precise plasmonic superlattices are highly desirable. Here, we synthesize large areas of crystalline mono-, bi- and multilayers of gold nanoparticles >20 nm with a small number of defects. The superlattices can be described as hexagonal crystals with standard deviations of the lattice parameter below 1%. The periodic arrangement within the superlattices leads to new well-defined collective plasmon-polariton modes. The general level of achieved superlattice quality will be of benefit for a broad range of applications, ranging from fundamental studies of light-matter interaction to optical metamaterials and substrates for surface-enhanced spectroscopies.

We explore an analogue of optical frequency combs in driven nonlinear phononic systems, and present a mechanism for generating phononic frequency combs through nonlinear resonances. In the underlying process, a set of phonon modes is simultaneously excited by the external driving which yields frequency combs with an array of discrete and equidistant spectral lines of each nonlinearly excited phonon mode. Frequency combs through nonlinear resonance of different orders are investigated, and in particular the possibility of correlation tailoring in higher-order cases is revealed. We suggest that our results can be applied in various nonlinear acoustic processes, such as phonon harvesting, and can also be generalized to other nonlinear systems.

p62/SQSTM1 is an autophagy receptor and signaling adaptor with an N-terminal PB1 domain that forms the scaffold of phase-separated p62 bodies in the cell. The molecular determinants that govern PB1 domain filament formation in vitro remain to be determined and the role of p62 filaments inside the cell is currently unclear. We here determine four high-resolution cryo-EM structures of different human and Arabidopsis PB1 domain assemblies and observed a filamentous ultrastructure of p62/SQSTM1 bodies using correlative cellular EM. We show that oligomerization or polymerization, driven by a double arginine finger in the PB1 domain, is a general requirement for lysosomal targeting of p62. Furthermore, the filamentous assembly state of p62 is required for autophagosomal processing of the p62-specific cargo KEAP1. Our results show that using such mechanisms, p62 filaments can be critical for cargo uptake in autophagy and are an integral part of phase-separated p62 bodies.

Abstract Following structural dynamics in real time is a fundamental goal towards a better understanding of chemical reactions. Recording snapshots of individual molecules with ultrashort exposure times is a key ingredient towards this goal, as atoms move on femtosecond (10 −15 s) timescales. For condensed-phase samples, ultrafast, atomically resolved structure determination has been demonstrated using X-ray and electron diffraction. Pioneering experiments have also started addressing gaseous samples. However, they face the problem of low target densities, low scattering cross sections and random spatial orientation of the molecules. Therefore, obtaining images of entire, isolated molecules capturing all constituents, including hydrogen atoms, remains challenging. Here we demonstrate that intense femtosecond pulses from an X-ray free-electron laser trigger rapid and complete Coulomb explosions of 2-iodopyridine and 2-iodopyrazine molecules. We obtain intriguingly clear momentum images depicting ten or eleven atoms, including all the hydrogens, and thus overcome a so-far impregnable barrier for complete Coulomb explosion imaging—its limitation on molecules consisting of three to five atoms. In combination with state-of-the-art multi-coincidence techniques and elaborate theoretical modelling, this allows tracing ultrafast hydrogen emission and obtaining information on the result of intramolecular electron rearrangement. Our work represents an important step towards imaging femtosecond chemistry via Coulomb explosion.