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Speckle patterns manifesting from the interaction of coherent X-rays with matter offer a glimpse into the dynamics of nanoscale domains that underpin many emergent phenomena in quantum materials. While the dynamics of the average structure can be followed with time-resolved X-ray diffraction, the ultrafast evolution of local structures in nonequilibrium conditions have thus far eluded detection due to experimental limitations, such as insufficient X-ray coherent flux. Here we demonstrate a nonequilibrium speckle visibility experiment using a split-and-delay setup at an X-ray free-electron laser. Photoinduced electronic domain fluctuations of the magnetic model material Fe$_{3}$O$_{4}$ reveal changes of the trimeron network configuration due to charge dynamics that exhibit liquid-like fluctuations, analogous to a supercooled liquid phase. This suggests that ultrafast dynamics of electronic heterogeneities under optical stimuli are fundamentally different from thermally-driven ones.

In this brief note, we prove that both forms of the Gerber statistic introduced in Gerber et al. (2022) are positive semi-definite., Comment: 5 pages, 0 figures

Quantum sensors and qubits are usually two-level systems (TLS), the quantum analogs of classical bits which assume binary values '0' or '1'. They are useful to the extent to which they can persist in quantum superpositions of '0' and '1' in real environments. However, such TLS are never alone in real materials and devices, and couplings to other degrees of freedom limit the lifetimes - called decoherence times - of the superposition states. Decoherence occurs via two major routes - excitation hopping and fluctuating electromagnetic fields. Common mitigation strategies are based on material improvements, exploitation of clock states which couple only to second rather than first order to external perturbations, and reduction of interactions via extreme dilution of pure materials made from isotopes selected to minimize noise from nuclear spins. We demonstrate that for a dense TLS network in a noisy nuclear spin bath, we can take advantage of interactions to pass from hopping to fluctuation dominance, increasing decoherence times by almost three orders of magnitude. In the dilute rare-earth insulator LiY1-xTbxF4, Tb ions realize TLS characterized by a 30GHz splitting and readily implemented clock states. Dipolar interactions lead to coherent, localized pairs of Tb ions, that decohere due to fluctuating quantum mechanical ring-exchange interaction, sensing the slow dynamics of the surrounding, nearly localized Tb spins. The hopping and fluctuation regimes are sharply distinguished by their Rabi oscillations and the invisible vs. strong effect of classic 'error correcting' microwave pulse sequences. Laying open the decoherence mechanisms at play in a dense, disordered and noisy network of interacting TLS, our work expands the search space for quantum sensors and qubits to include clusters in dense, disordered materials, that can be explored for localization effects., Comment: 39 pages

We present the commissioning of the Fast Annihilation Cryogenic Tracker detector (FACT), installed around the antihydrogen production trap inside the 1 T superconducting magnet of the AE\=gIS experiment. FACT is designed to detect pions originating from the annihilation of antiprotons. Its 794 scintillating fibers operate at 4 K and are read out by silicon photomultipliers (MPPCs) at near room temperature. FACT provides the antiproton/antihydrogen annihilation position information with a few ns timing resolution. We present the hardware and software developments which led to the successful operation of the detector for antihydrogen detection and the results of an antiproton-loss based efficiency assessment. The main background to the antihydrogen signal is that of the positrons impinging onto the positronium conversion target and creating a large amount of gamma rays which produce a sizeable signal in the MPPCs shortly before the antihydrogen signal is expected. We detail the characterization of this background signal and its impact on the antihydrogen detection efficiency.

We review recent progress in utilizing ultrafast light-matter interaction to control the macroscopic properties of quantum materials. Particular emphasis is placed on photoinduced phenomena that do not result from ultrafast heating effects but rather emerge from microscopic processes that are inherently nonthermal in nature. Many of these processes can be described as transient modifications to the free-energy landscape resulting from the redistribution of quasiparticle populations, the dynamical modification of coupling strengths and the resonant driving of the crystal lattice. Other pathways result from the coherent dressing of a material's quantum states by the light field. We discuss a selection of recently discovered effects leveraging these mechanisms, as well as the technological advances that led to their discovery. A road map for how the field can harness these nonthermal pathways to create new functionalities is presented., Comment: 36 pages, 12 figures; all authors contributed equally to this work

We use complementary optical spectroscopy methods to directly measure the lowest crystal-field energies of the rare-earth quantum magnet LiY$_{1-x}$Ho$_{x}$F$_{4}$, including their hyperfine splittings, with more than 10 times higher resolution than previous work. We are able to observe energy level splittings due to the $^6\mathrm{Li}$ and $^7\mathrm{Li}$ isotopes, as well as non-equidistantly spaced hyperfine transitions originating from dipolar and quadrupolar hyperfine interactions. We provide refined crystal field parameters and extract the dipolar and quadrupolar hyperfine constants ${A_J=0.02703\pm0.00003}$ $\textrm{cm}^{-1}$ and ${B= 0.04 \pm0.01}$ $\textrm{cm}^{-1}$, respectively. Thereupon we determine all crystal-field energy levels and magnetic moments of the $^5I_8$ ground state manifold, including the (non-linear) hyperfine corrections. The latter match the measurement-based estimates. The scale of the non-linear hyperfine corrections sets an upper bound for the inhomogeneous line widths that would still allow for unique addressing of a selected hyperfine transition. e.g. for quantum information applications. Additionally, we establish the far-infrared, low-temperature refractive index of LiY$_{1-x}$Ho$_{x}$F$_{4}$., Comment: 9 pages, 6 Figures, 3 Tables

X-ray free-electron lasers (FEL) deliver ultrabright X-ray pulses, but not the sequences of phase-coherent pulses required for time-domain interferometry and control of quantum states. For conventional split-and-delay schemes to produce such sequences the challenge stems from extreme stability requirements when splitting Angstrom wavelength beams where tiniest path length differences introduce phase jitter. We describe an FEL mode based on selective electron bunch degradation and transverse beam shaping in the accelerator, combined with a self-seeded photon emission scheme. Instead of splitting the photon pulses after their generation by the FEL, we split the electron bunch in the accelerator, prior to photon generation, to obtain phase-locked X-ray pulses with sub-femtosecond duration. Time-domain interferometry becomes possible, enabling the concomitant program of classical and quantum optics experiments with X-rays. The scheme leads to new scientific benefits of cutting-edge FELs with attosecond and/or high-repetition rate capabilities, ranging from the X-ray analog of Fourier transform infrared spectroscopy to damage-free measurements.

We characterized the pulsed Rydberg-positronium production inside the AEgIS (Antimatter Experiment: Gravity, Interferometry, Spectroscopy) apparatus in view of antihydrogen formation by means of a charge exchange reaction between cold antiprotons and slow Rydberg-positronium atoms. Velocity measurements on positronium along two axes in a cryogenic environment (10K) and in 1T magnetic field were performed. The velocimetry was done by MCP-imaging of photoionized positronium previously excited to the $n=3$ state. One direction of velocity was measured via Doppler-scan of this $n=3$-line, another direction perpendicular to the former by delaying the exciting laser pulses in a time-of-flight measurement. Self-ionization in the magnetic field due to motional Stark effect was also quantified by using the same MCP-imaging technique for Rydberg positronium with an effective principal quantum number $n_{eff}$ ranging between 14 and 22. We conclude with a discussion about the optimization of our experimental parameters for creating Rydberg-positronium in preparation for an efficient pulsed production of antihydrogen.

The charge density wave in the high-temperature superconductor YBa$_2$Cu$_3$O$_{7-x}$ (YBCO) is now known to have two different ordering tendencies differentiated by their $c$-axis correlations. These correspond to ferro- (F-CDW) and antiferro- (AF-CDW) couplings between CDW in neighbouring CuO$_2$ bilayers. This discovery has prompted a number of fundamental questions. For example, how does superconductivity adjust to two competing orders and are either of these orders responsible for the electronic reconstruction? Here we use high-energy x-ray diffraction to study YBa$_2$Cu$_3$O$_{6.67}$ as a function of magnetic field and temperature. We show that regions of the sample with F-CDW correlations suppress superconductivity more strongly than those with AF-CDW correlations. This implies that an inhomogeneous superconducting state exists, in which some regions show a weak or fragile form of superconductivity. By comparison of F-CDW and AF-CDW correlation lengths, it is furthermore concluded that F-CDW ordering is sufficiently long-range to modify the electronic structure. Our study thus suggests that F-CDW correlations have an important impact on superconducting and normal state properties of underdoped YBCO., Comment: 9 pages, 5 figures, and supplementary information

We investigate experimentally the possibility of enhancing the production of $2^3S$ positronium atoms by driving the $1^3S$-$3^3P$ and $3^3P$-$2^3S$ transitions, overcoming the natural branching ratio limitation of spontaneous decay from $3^3P$ to $2^3S$. The decay of $3^3P$ positronium atoms towards the $2^3S$ level has been effciently stimulated by a 1312.2nm broadband IR laser pulse. The dependence of the stimulating transition efficiency on the intensity of the IR pulse has been measured to find the optimal enhancement conditions. A maximum relative increase of $ \times (3.1 \pm 1.0) $ in the $2^3S$ production efficiency, with respect to the case where only spontaneous decay is present, was obtained., Comment: 6 pages, 4 figures

Phase transitions and symmetry are intimately linked. Melting of ice, for example, restores translation invariance. The mysterious hidden order (HO) phase of URu$_2$Si$_2$ has, despite relentless research efforts, kept its symmetry breaking element intangible. Here we present a high-resolution x-ray diffraction study of the URu$_2$Si$_2$ crystal structure as a function of hydrostatic pressure. Below a critical pressure threshold $p_c\approx3$ kbar, no tetragonal lattice symmetry breaking is observed even below the HO transition $T_{HO}=17.5$ K. For $p>p_c$, however, a pressure-induced rotational symmetry breaking is identified with an onset temperatures $T_{OR}\sim 100$ K. The emergence of an orthorhombic phase is found and discussed in terms of an electronic nematic order that appears unrelated to the HO, but with possible relevance for the pressure-induced antiferromagnetic (AF) phase. Existing theories describe the HO and AF phases through an adiabatic continuity of a complex order parameter. Since none of these theories predicts a pressure-induced nematic order, our finding adds an additional symmetry breaking element to this long-standing problem., Comment: 6 pages, 4 figures and supplemental materials

Positronium in the $2^3S$ metastable state exhibits a low electrical polarizability and a long lifetime (1140 ns) making it a promising candidate for interferometry experiments with a neutral matter-antimatter system. In the present work, $2^3S$ positronium is produced - in absence of electric field - via spontaneous radiative decay from the $3^3P$ level populated with a 205nm UV laser pulse. Thanks to the short temporal length of the pulse, 1.5 ns full-width at half maximum, different velocity populations of a positronium cloud emitted from a nanochannelled positron/positronium converter were selected by delaying the excitation pulse with respect to the production instant. $ 2^3S $ positronium atoms with velocity tuned between $ 7 \cdot 10^4 $ m/s and $ 10 \cdot 10^4 $ m/s were thus produced. Depending on the selected velocity, a $2^3S$ production effciency ranging from $\sim 0.8 \%$ to $\sim 1.7%$, with respect to the total amount of emitted positronium, was obtained. The observed results give a branching ratio for the $3^3P$-$2^3S$ spontaneous decay of $(9.7 \pm 2.7) \% $. The present velocity selection technique could allow to produce an almost monochromatic beam of $\sim 1 \cdot 10^3 $ $2^3S$ atoms with a velocity spread $ < 10^4 $ m/s and an angular divergence of $\sim$ 50 mrad., Comment: 6 pages, 3 figures, 1 table

We investigated the doping dependence of magnetic excitations in the lightly doped cuprate La2-xSrxCuO4 via combined studies of resonant inelastic x-ray scattering (RIXS) at the Cu L3-edge and theoretical calculations. With increasing doping, the magnon dispersion is found to be essentially unchanged, but the spectral width broadens and the spectral weight varies differently at different momenta. Near the Brillouin zone center, we directly observe bimagnon excitations which possess the same energy scale and doping dependence as previously observed by Raman spectroscopy. They disperse weakly in energy-momentum space, and are consistent with a bimagnon dispersion that is renormalized by the magnon-magnon interaction at the zone center., Comment: 8 pages, 6 figures

Producing positronium (Ps) in the metastable $2^3\text{S}$ state is of interest for various applications in fundamental physics. We report here about an experiment in which Ps atoms are produced in this long-lived state by spontaneous radiative decay of Ps excited to the $3^3\text{P}$ level manifold. The Ps cloud excitation is obtained with a UV laser pulse in an experimental vacuum chamber in presence of guiding magnetic field of 25 mT and an average electric field of 300 V/cm. The indication of the $2^3\text{S}$ state production is obtained from a novel analysis technique of single-shot positronium annihilation lifetime spectra. Its production efficiency relative to the total amount of formed Ps is evaluated by fitting a simple rate equations model to the experimental data and found to be $ (2.1 \pm 1.3) \, \% $.

The characteristics of low energy antiproton annihilations on nuclei (e.g. hadronization and product multiplicities) are not well known, and Monte Carlo simulation packages that use different models provide different descriptions of the annihilation events. In this study, we measured the particle multiplicities resulting from antiproton annihilations on nuclei. The results were compared with predictions obtained using different models in the simulation tools GEANT4 and FLUKA. For this study, we exposed thin targets (Cu, Ag and Au) to a very low energy antiproton beam from CERN's Antiproton Decelerator, exploiting the secondary beamline available in the AEgIS experimental zone. The antiproton annihilation products were detected using emulsion films developed at the Laboratory of High Energy Physics in Bern, where they were analysed at the automatic microscope facility. The fragment multiplicity measured in this study is in good agreement with results obtained with FLUKA simulations for both minimally and heavily ionizing particles.

The existence of charge density wave (CDW) correlations in cuprate superconductors has now been established. However, the nature of the ground state order has remained uncertain because disorder and the presence of superconductivity typically limit the CDW correlation lengths to a dozen unit cells or less. Here we explore the CDW correlations in YBa2Cu3Ox (YBCO) ortho-II and ortho-VIII crystals, which belong to the cleanest available cuprate family, at magnetic fields in excess of the resistive upper critical field (Hc2) where the superconductivity is heavily suppressed. We find an incommensurate, unidirectional CDW with a well-defined onset at a critical field strength that is proportional to Hc2. It is related to but distinct from the short-range bidirectional CDW that exists at zero magnetic field. The unidirectional CDW possesses a long inplane correlation length as well as significant correlations between neighboring CuO2 planes, yielding a correlation volume that is at least 2 - 3 orders of magnitude larger than that of the zero-field CDW. This is by far the largest CDW correlation volume observed in any cuprate crystal and so is presumably representative of the high-field ground-state of an "ideal" disorder-free cuprate.

Charge density wave (CDW) correlations have recently been shown to universally exist in cuprate superconductors. However, their nature at high fields inferred from nuclear magnetic resonance is distinct from that measured by x-ray scattering at zero and low fields. Here we combine a pulsed magnet with an x-ray free electron laser to characterize the CDW in YBa2Cu3O6.67 via x-ray scattering in fields up to 28 Tesla. While the zero-field CDW order, which develops below T ~ 150 K, is essentially two-dimensional, at lower temperature and beyond 15 Tesla, another three-dimensionally ordered CDW emerges. The field-induced CDW onsets around the zero-field superconducting transition temperature, yet the incommensurate in-plane ordering vector is field-independent. This implies that the two forms of CDW and high-temperature superconductivity are intimately linked.

We investigated the crystal structure and lattice excitations of the ternary intermetallic stannide Ca3Ir4Sn13 using neutron and x-ray scattering techniques. For T > T* ~ 38 K the x-ray diffraction data can be satisfactorily refined using the space group Pm-3n. Below T* the crystal structure is modulated with a propagation vector of q = (1/2, 1/2, 0). This may arise from a merohedral twinning in which three tetragonal domains overlap to mimic a higher symmetry, or from a doubling of the cubic unit cell. Neutron diffraction and neutron spectroscopy results show that the structural transition at T* is of a second-order, and that it is well described by mean-field theory. Inelastic neutron scattering data point towards a displacive structural transition at T* arising from the softening of a low-energy phonon mode with an energy gap of Delta(120 K) = 1.05 meV. Using density functional theory the soft phonon mode is identified as a 'breathing' mode of the Sn12 icosahedra and is consistent with the thermal ellipsoids of the Sn2 atoms found by single crystal diffraction data.

Ultrafast light pulses can modify the electronic properties of quantum materials by perturbing the underlying, intertwined degrees of freedom. In particular, iron-based superconductors exhibit a strong coupling among electronic nematic fluctuations, spins, and the lattice, serving as a playground for ultrafast manipulation. Here we use time-resolved x-ray scattering to measure the lattice dynamics of photo-excited BaFe2As2. Upon optical excitation, no signature of an ultrafast change of the crystal symmetry is observed, but the lattice oscillates rapidly in time due to the coherent excitation of an A1g mode that modulates the Fe-As-Fe bond angle. We directly quantify the coherent lattice dynamics and show that even a small photo-induced lattice distortion can induce notable changes in the electronic and magnetic properties. Our analysis implies that transient structural modification can generally be an effective tool for manipulating the electronic properties of multi-orbital systems, where electronic instabilities are sensitive to the orbital character of bands near the Fermi level.

We study the zero-point and thermal ionic motion in La$_2$CuO$_4$ by means of high-resolution neutron diffraction experiments. Our results demonstrate anisotropic motion of O and to a lesser extent of Cu ions, both consistent with the structure of coupled CuO$_6$ octahedra, and quantify the relative effects of zero-point and thermal contributions to ionic motion. By substitution of $^{18}$O, we find that the oxygen isotope effect on the lattice dimensions is small and negative ($-0.01\%$), while the isotope effect on the ionic displacement parameters is significant ($-6$ to $50\%$). We use our results as input for theoretical estimates of the distribution of magnetic interaction parameters, $J$, in an effective one-band model for the cuprate plane. We find that ionic motion causes only small ($1\%$) effects on the average value $\langle J\rangle$, which vary with temperature and O isotope, but results in dramatic ($10$-$20\%$) fluctuations in $J$ values that are subject to significant ($8$-$12\%$) isotope effects. We demonstrate that this motional broadening of $J$ can have substantial effects on certain electronic and magnetic properties in cuprates., Comment: 13 pages, 9 figures

We report room-temperature electric field noise measurements combined with in-situ surface characterization and cleaning of a microfabricated ion trap. We used a single-ion electric field noise sensor in combination with surface cleaning and analysis tools, to investigate the relationship between electric field noise from metal surfaces in vacuum and the composition of the surface. These experiments were performed in a novel setup that integrates ion trapping capabilities with surface analysis tools. We find that surface cleaning of an aluminum-copper surface significantly reduces the level of electric field noise, but the surface does not need to be atomically clean to show noise levels comparable to those of the best cryogenic traps. The post-cleaning noise levels are low enough to allow fault-tolerant trapped-ion quantum information processing on a microfabricated surface trap., Comment: 13 pages, 4 figures

We use small angle neutron scattering to study the superconducting vortex lattice in La$_{2-x}$Sr$_x$CuO$_4$ as a function of doping and magnetic field. We show that near optimally doping the vortex lattice coordination and the superconducting coherence length $\xi$ are controlled by a van-Hove singularity crossing the Fermi level near the Brillouin zone boundary. The vortex lattice properties change dramatically as a spin-density-wave instability is approached upon underdoping. The Bragg glass paradigm provides a good description of this regime and suggests that SDW order acts as a novel source of disorder on the vortex lattice., Comment: Accepted in Phys. Rev. B

Efficient self-interference of single-photons emitted by a sideband-cooled Barium ion is demonstrated. First, the technical tools for performing efficient coupling to the quadrupolar transition of a single $^{138}$Ba$^{+}$ ion are presented. We show efficient Rabi oscillations of the internal state of the ion using a highly stabilized 1.76 $\mu m$ fiber laser resonant with the S$_{1/2}$-D$_{5/2}$ transition. We then show sideband cooling of the ion's motional modes and use it as a means to enhance the interference contrast of the ion with its mirror-image to up to 90%. Last, we measure the dependence of the self-interference contrast on the mean phonon number, thereby demonstrating the potential of the set-up for single-atom thermometry close to the motional ground state., Comment: 6 pages, 6 figures

We report on muon spin rotation studies of the noncentrosymmetric heavy fermion antiferromagnet CeRhSi$_3$. A drastic and monotonic suppression of the internal fields, at the lowest measured temperature, was observed upon an increase of external pressure. Our data suggest that the ordered moments are gradually quenched with increasing pressure, in a manner different from the pressure dependence of the N\'eel temperature. At $\unit{23.6}{kbar}$, the ordered magnetic moments are fully suppressed via a second-order phase transition, and $T_{\rm{N}}$ is zero. Thus, we directly observed the quantum critical point at $\unit{23.6}{kbar}$ hidden inside the superconducting phase of CeRhSi$_3$.

We present small angle neutron scattering studies of the vortex lattice (VL) in CeCoIn5 with magnetic fields applied parallel (H) to the antinodal [100] and nodal [110] directions. For H || [100], a single VL orientation is observed, while a 90 degree reorientation transition is found for H || [110]. For both field orientations and VL configurations we find a distorted hexagonal VL with an anisotropy, Gamma = 2.0 +/- 0.05. The VL form factor shows strong Pauli paramagnetic effects similar to what have previously been reported for H || [001]. At high fields, above which the upper critical field (Hc2) becomes a first-order transition, an increased disordering of the VL is observed., Comment: 5 pages, 4 figures

We report an absorption spectroscopy experiment and the observation of electromagnetically induced transparency from a single trapped atom. We focus a weak and narrowband Gaussian light beam onto an optically cooled Barium ion using a high numerical aperture lens. Extinction of this beam is observed with measured values of up to 1.3 %. We demonstrate electromagnetically induced transparency of the ion by tuning a strong control beam over a two-photon resonance in a three-level lambda-type system. The probe beam extinction is inhibited by more than 75 % due to population trapping., Comment: 4 pages, 3 figures

From small-angle neutron scattering studies of the flux line lattice (FLL) in CeCoIn5, with magnetic field applied parallel to the crystal c-axis, we obtain the field- and temperature-dependence of the FLL form factor, which is a measure of the spatial variation of the field in the mixed state. We extend our earlier work [A.D. Bianchi et al. 2008 Science 319, 177] to temperatures up to 1250 mK. Over the entire temperature range, paramagnetism in the flux line cores results in an increase of the form factor with field. Near H_c2 the form factor decreases again, and our results indicate that this fall-off extends outside the proposed FFLO region. Instead, we attribute the decrease to a paramagnetic suppression of Cooper pairing. At higher temperatures, a gradual crossover towards more conventional mixed state behavior is observed., Comment: Submitted to New Journal of Physics, 13 pages, 4 figures

We report measurements of an intensity-field correlation function of the resonance fluorescence of a single trapped Ba+ ion. Detection of a photon prepares the atom in its ground state and we observe its subsequent evolution under interaction with a laser field of well defined phase. We record the regression of the resonance fluorescence source field. This provides a direct measurement of the field of the radiating dipole of a single atom and exhibits its strong non-classical behavior. In the experimental setup an interference measurement is conditioned on a fluorescence photon detection. The third-order correlation function thus recorded demonstrates an aspect of wave-particle duality at the single-atom, single-photon level., Comment: 4 pages, 4 figures, accepted in PRL

We observe quantum interference of photons emitted by two continuously laser-excited single ions, independently trapped in distinct vacuum vessels. High contrast two-photon interference is observed in two experiments with different ion species, calcium and barium. Our experimental findings are quantitatively reproduced by Bloch equation calculations. In particular, we show that the coherence of the individual resonance fluorescence light field is determined from the observed interference.