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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.

A system that possesses translational symmetry but breaks orientational symmetry is known as a nematic phase. While there are many examples of nematic phases in a wide range of contexts, such as in liquid crystals, complex oxides, and superconductors, of particular interest is the magnetic analogue, where the spin, charge, and orbital degrees of freedom of the electron are intertwined. The difficulty of spin nematics is the unambiguous realization and characterization of the phase. Here we present an entirely new type of magnetic nematic phase, which replaces the basis of individual spins with magnetic helices. The helical basis allows for the direct measurement of the order parameters with soft X-ray scattering and a thorough characterization of the nematic phase and its thermodynamic transitions. We discover two distinct nematic phases with unique spatio-temporal correlation signatures. Using coherent X-ray methods, we find that near the phase boundary between the two nematic phases, fluctuations coexist on the timescale of both seconds and sub-nanoseconds. Additionally, we have determined that the fluctuations occur simultaneously with a reorientation of the magnetic helices, indicating that there is spontaneous symmetry breaking and new degrees of freedom become available. Our results provide a novel framework for characterizing exotic phases and the phenomena presented can be mapped onto a broad class of physical systems.

The unification of quantum mechanics and general relativity has long been elusive. Only recently have empirical predictions of various possible theories of quantum gravity been put to test. The dawn of multi-messenger high-energy astrophysics has been tremendously beneficial, as it allows us to study particles with much higher energies and travelling much longer distances than possible in terrestrial experiments, but more progress is needed on several fronts. A thorough appraisal of current strategies and experimental frameworks, regarding quantum gravity phenomenology, is provided here. Our aim is twofold: a description of tentative multimessenger explorations, plus a focus on future detection experiments. As the outlook of the network of researchers that formed through the COST Action CA18108 "Quantum gravity phenomenology in the multi-messenger approach (QG-MM)", in this work we give an overview of the desiderata that future theoretical frameworks, observational facilities, and data-sharing policies should satisfy in order to advance the cause of quantum gravity phenomenology., Comment: Submitted to CQG for the Focus Issue on "Quantum Gravity Phenomenology in the Multi-Messenger Era: Challenges and Perspectives". Please contact us to express interesst of endorsement of this white paper

A first look is taken at the NIRSpec 1-5 $\mu$m observations from JWST program 1591 that targets 7 objects along the low-mass stellar life cycle with PAH emission. Spectra extracted from a 1.5$^{\prime\prime}$ radius sized circular aperture are explored, showing a wealth of features, including the 3 $\mu$m PAH complex, the PAH-continuum, and atomic and molecular emission lines from HI, He, H$_{\rm 2}$, and other species. CO$_{\rm 2}$- and H$_{\rm 2}$O-ice absorption and CO emission is also seen. Focusing on the bright-PDR position in M17, the PAH CH stretch falls at 3.29 $\mu$m (FWHM=0.04 $\mu$m). Signs of its 1.68 $\mu$m overtone are confused by line emission in all targets. Multi-component decomposition reveals a possible aliphatic deuterated PAH feature centered at 4.65 $\mu$m (FWHM=0.02 $\mu$m), giving [D/H]$_{\rm alip.}$=31$\pm$12.7%. However, there is little sign of its aromatic counterpart between 4.36-4.43 $\mu$m. There is also little sign of PAH-nitrile emission between 4.34-4.39 $\mu$m. A PAH continuum rises from $\sim$1 to 3.2 $\mu$m, after which it jumps by about a factor of 2.5 at 3.6 $\mu$m, with bumps at 3.8, 4.04, and 4.34 $\mu$m adding structure. The CO$_{\rm 2}$ absorption band in M17 is matched with 10:1 H$_{\rm 2}$O:CO$_{\rm 2}$ ice at 10 K. The $v$=0 pure rotational molecular hydrogen population diagram reveals $>$2200 K UV-pumped gas. The hydrogen Pfund series runs from levels 10 to $>$30. Considering Br$\alpha$/Br$\beta$=0.381$\pm$0.01966 and Case B recombination results in A$_{\rm V}{\simeq}$8. CO emission in IRAS21282+5050 originates from 258 K gas. In-depth spectral-spatial analysis of all features and targets are planned for a series of forthcoming papers., Comment: 23 pages, 20 figures, to be published in ApJ

In the cuprate superconductors, the spatial coherence of the charge density wave (CDW) state grows rapidly below a characteristic temperature $T_\mathrm{CDW}$, the nature of which is debated. We have combined a set of x-ray scattering techniques to study La$_{1.88}$Sr$_{0.12}$CuO$_{4}$ ($T_\mathrm{CDW}$~$\approx$~80\,K) to shed light on this discussion. We observe the emergence of a crystal structure, which is consistent with the CDW modulation in symmetry, well above $T_\mathrm{CDW}$. This global structural change also induces strong fluctuations of local atomic disorder in the intermediate temperature region. At $T_\mathrm{CDW}$, the temperature dependence of this structure develops a kink, while the atomic disorder is minimized. We find that the atomic relaxation dynamics cross over from a cooperative to an incoherent response at $T_\mathrm{CDW}$. These results reveal a rich interplay between the CDWs and atomic fluctuations of distinct spatio-temporal scales. For example, the CDW coherence is enhanced on quasi-elastic timescales by incoherent atomic relaxation.

The exploration of the universe has recently entered a new era thanks to the multi-messenger paradigm, characterized by a continuous increase in the quantity and quality of experimental data that is obtained by the detection of the various cosmic messengers (photons, neutrinos, cosmic rays and gravitational waves) from numerous origins. They give us information about their sources in the universe and the properties of the intergalactic medium. Moreover, multi-messenger astronomy opens up the possibility to search for phenomenological signatures of quantum gravity. On the one hand, the most energetic events allow us to test our physical theories at energy regimes which are not directly accessible in accelerators; on the other hand, tiny effects in the propagation of very high energy particles could be amplified by cosmological distances. After decades of merely theoretical investigations, the possibility of obtaining phenomenological indications of Planck-scale effects is a revolutionary step in the quest for a quantum theory of gravity, but it requires cooperation between different communities of physicists (both theoretical and experimental). This review is aimed at promoting this cooperation by giving a state-of-the art account of the interdisciplinary expertise that is needed in the effective search of quantum gravity footprints in the production, propagation and detection of cosmic messengers., Comment: This review was written by participants of the COST Action CA18108. Further information on the review can be found at https://qg-mm.unizar.es/review/, updated to published version

Piezoelectrics are materials that linearly deform in response to an applied electric field. As a fundamental prerequisite, piezoelectric material must possess a non centrosymmetric crystal structure. For more than a century, this remains the major obstacle for finding new piezoelectric materials. We circumvent this limitation by breaking the crystallographic symmetry, and inducing large and sustainable piezoelectric effects in centrosymmetric materials by electric field induced rearrangement of oxygen vacancies Surprisingly, the results show the generation of extraordinarily large piezoelectric responses d33 ~200,000 pm/V), in cubic fluorite Gd-doped CeO2-x films, which is two orders of magnitude larger than in the presently best known lead based piezoelectric relaxor ferroelectric oxide. These findings open opportunities to design new piezoelectric materials from environmentally friendly centrosymmetric ones.

The interaction of many-body systems with intense light pulses may lead to novel emergent phenomena far from equilibrium. Recent discoveries, such as the optical enhancement of the critical temperature in certain superconductors and the photo-stabilization of hidden phases, have turned this field into an important research frontier. Here, we demonstrate nonthermal charge-density-wave (CDW) order at electronic temperatures far greater than the thermodynamic transition temperature. Using time- and angle-resolved photoemission spectroscopy and time-resolved X-ray diffraction, we investigate the electronic and structural order parameters of an ultrafast photoinduced CDW-to-metal transition. Tracking the dynamical CDW recovery as a function of electronic temperature reveals a behaviour markedly different from equilibrium, which we attribute to the suppression of lattice fluctuations in the transient nonthermal phonon distribution. A complete description of the system's coherent and incoherent order-parameter dynamics is given by a time-dependent Ginzburg-Landau framework, providing access to the transient potential energy surfaces., Comment: 23 pages, 14 figures

Thanks to the remarkable developments of ultrafast science, one of today's challenges is to modify material state by controlling with a light pulse the coherent motions that connect two different phases. Here we show how strain waves, launched by electronic and structural precursor phenomena, determine a macroscopic transformation pathway for the semiconducting-to-metal transition with large volume change in bistable Ti$_3$O$_5$ nanocrystals. Femtosecond powder X-ray diffraction allowed us to quantify the structural deformations associated with the photoinduced phase transition on relevant time scales. We monitored the early intra-cell distortions around absorbing metal dimers, but also long range crystalline deformations dynamically governed by acoustic waves launched at the laser-exposed Ti$_3$O$_5$ surface. We rationalize these observations with a simplified elastic model, demonstrating that a macroscopic transformation occurs concomitantly with the propagating acoustic wavefront on the picosecond timescale, several decades earlier than the subsequent thermal processes governed by heat diffusion., Comment: 30 pages (including supplementary text), 5 main figures, 9 supplementary figures; corrected author list

Inkjet printing of 8% Y2O3-stabilized ZrO2 (YSZ) thin films is achieved by designing a novel water-based reactive ink for Drop-on-Demand (DoD) inkjet printing. The ink formulation is based on a novel chemical strategy that consists of a combination of metal oxide precursors (zirconium alkoxide and yttrium salt), water and a nucleophilic agent, i.e. n-methyldiethanolamine (MDEA). This chemistry leads to metal-organic complexes with long term ink stability and high precision printability. Ink rheology and chemical reactivity are analyzed and controlled in terms of metal-organic interactions in the solutions. Thin dense nanocrystalline YSZ film below 150 nm are obtained by low temperature calcination treatments (400-500 {\deg}C), making the deposition suitable for a large variety of substrates, including silicon, glass and metals. Thin films and printed patterns achieve full densification with no lateral shrinkage and high ionic conductivity., Comment: 30 pages,6 figures, 2 tables, open access

Currently, additive manufacturing of ceramics by stereolithography (SLA) is limited to single materials and by a poor thickness resolution that strongly depends on the ceramic particles-UV light interaction. Combining selective laser curing with inkjet printing represents a novel strategy to overcome these constrains. Nonetheless, this approach requires UV-curable inks that allow hardening of the printed material and sintering to high density. In this work, we report how to design an ink for inkjet printing of yttria stabilized zirconia (YSZ) which can be impressed by addition of UV-curable monomers. We especially show how the formulation of the inks and particularly the UV-monomer concentration impacts the printability and the UV-curing. This leads to prints that are resistant to solvent washing first and densify to 96% dense YSZ layers after sintering.

Water dispersion of nanometric yttria stabilized zirconia (YSZ) particles synthesized by continuous hydrothermal synthesis are transferred into nanoinks for thin film deposition. YSZ nanoparticles are synthesized in supercritical conditions resulting in highly dispersed crystals of 10 nm in size. The rheology of the colloid is tailored to achieve inkjet printability (Z) by using additives for regulating viscosity and surface tension. Inks with a wide range of properties are produced. A remarkable effect of nanoparticles on the ink printability is registered even at solid load < 1% vol. In particular, nanoparticles hinder the droplet formation at low values of the printability while suitable jetting is observed at high Z values, i.e. Z ca. 20. For the optimized inks, we achieve high quality printing with lateral and thickness resolution of 70 um and ca. 250 nm respectively, as well as self levelling effect with a reduction of the substrate roughness. Densification is achieved at sintering temperatures below 1200 C.

Femtosecond time-resolved x-ray diffraction is employed to study the dynamics of the periodic lattice distortion (PLD) associated with the charge-density-wave (CDW) in K0.3MoO3. Using a multi-pulse scheme we show the ability to extend the lifetime of coherent oscillations of the PLD about the undistorted structure through re-excitation of the electronic states. This suggests that it is possible to enter a regime where the symmetry of the potential energy landscape corresponds to the high symmetry phase but the scattering pathways that lead to the damping of coherent dynamics are still controllable by altering the electronic state population. The demonstrated control over the coherence time offers new routes for manipulation of coherent lattice states., Comment: 18 pages, 5 figures, including supplementary information

The ability to control the structure of a crystalline solid on ultrafast timescales bears enormous potential for information storage and manipulation or generating new functional states of matter [1]. In many materials where the ultrafast control of crystalline structures has been explored, optical excitation pushes materials towards their less ordered high temperature phase [2{9] as electronically driven ordered phases melt and possible concomitant structural modifications relax. Nonetheless, for a few select materials it has been shown that photoexcitation can slightly enhance the amplitude of an electronic ordering phenomenon (i.e. its electronic order parameter) [9{13]. Here we show via femtosecond hard X-ray diffraction that photodoping of the perovskite EuTiO3 transiently increases the order parameter associated with a purely structural [14] phase transition represented by the antiferrodistortive rotation of the oxygen octahedra. This can be understood from an ultrafast charge-transfer induced reduction of the Goldschmidt tolerance factor [15], which is a fundamental control parameter for the properties of perovskites, Comment: 11 pages, 3 figures

The ultrafast dynamics of the octahedral rotation in Ca:SrTiO3 is studied by time resolved x-ray diffraction after photo excitation over the band gap. By monitoring the diffraction intensity of a superlattice reflection that is directly related to the structural order parameter of the soft-mode driven antiferrodistortive phase in Ca:SrTiO3, we observe a ultrafast relaxation on a 0.2 ps timescale of the rotation of the oxygen octahedron, which is found to be independent of the initial temperaure despite large changes in the corresponding soft-mode frequency. A further, much smaller reduction on a slower picosecond timescale is attributed to thermal effects. Time-dependent density-functional-theory calculations show that the fast response can be ascribed to an ultrafast displacive modification of the soft-mode potential towards the normal state, induced by holes created in the oxygen 2p states.

We use femtosecond x-ray diffraction to study the structural response of charge and orbitally ordered Pr$_{1-x}$Ca$_x$MnO$_3$ thin films across a phase transition induced by 800 nm laser pulses. By investigating the dynamics of both superlattice reflections and regular Bragg peaks, we disentangle the different structural contributions and analyze their relevant time-scales. The dynamics of the structural and charge order response are qualitatively different when excited above and below a critical fluence $f_c$. For excitations below $f_c$ the charge order and the superlattice is only partially suppressed and the ground state recovers within a few tens of nanosecond via diffusive cooling. When exciting above the critical fluence the superlattice vanishes within approximately half a picosecond followed by a change of the unit cell parameters on a 10 picoseconds time-scale. At this point all memory from the symmetry breaking is lost and the recovery time increases by many order of magnitudes due to the first order character of the structural phase transition.

Recent experiments have shown that the high temperature incommensurate (I) charge density wave (CDW) phase of 1T-TaS2 can be photoinduced from the lower temperature, nearly commensurate (NC) CDW state. Here we report a time-resolved x-ray diffraction study of the growth process of the photoinduced I-CDW domains. The layered nature of the material results in a marked anisotropy in the size of the photoinduced domains of the I-phase. These are found to grow self-similarly, their shape remaining unchanged throughout the growth process. The photoinduced dynamics of the newly formed I-CDW phase was probed at various stages of the growth process using a double pump scheme, where a first pump creates I-CDW domains and a second pump excites the newly formed I-CDW state. We observe larger magnitudes of the coherently excited I-CDW amplitude mode in smaller domains, which suggests that the incommensurate lattice distortion is less stable for smaller domain sizes., Comment: 8 pages, 8 figures

The Prototypical magnetic memory shape alloy Ni$_2$MnGa undergoes various phase transitions as a function of temperature, pressure, and doping. In the low-temperature phases below 260 K, an incommensurate structural modulation occurs along the [110] direction which is thought to arise from softening of a phonon mode. It is not at present clear how this phenomenon is related, if at all, to the magnetic memory effect. Here we report time-resolved measurements which track both the structural and magnetic components of the phase transition from the modulated cubic phase as it is brought into the high-symmetry phase. The results suggest that the photoinduced demagnetization modifies the Fermi surface in regions that couple strongly to the periodicity of the structural modulation through the nesting vector. The amplitude of the periodic lattice distortion, however, appears to be less affected by the demagnetizaton., Comment: 7 pages, 4 figures

Femtosecond time-resolved X-ray diffraction is used to study a photo-induced phase transition between two charge density wave (CDW) states in 1T-TaS$_2$, namely the nearly commensurate (NC) and the incommensurate (I) CDW states. Structural modulations associated with the NC-CDW order are found to disappear within 400 fs. The photo-induced I-CDW phase then develops through a nucleation/growth process which ends 100 ps after laser excitation. We demonstrate that the newly formed I-CDW phase is fragmented into several nanometric domains that are growing through a coarsening process. The coarsening dynamics is found to follow the universal Lifshitz-Allen-Cahn growth law, which describes the ordering kinetics in systems exhibiting a non-conservative order parameter., Comment: 6 pages, 5 figures

We employ time-resolved resonant x-ray diffraction to study the melting of charge order and the associated insulator-metal transition in the doped manganite Pr$_{0.5}$Ca$_{0.5}$MnO$_3$ after resonant excitation of a high-frequency infrared-active lattice mode. We find that the charge order reduces promptly and highly nonlinearly as function of excitation fluence. Density functional theory calculations suggest that direct anharmonic coupling between the excited lattice mode and the electronic structure drive these dynamics, highlighting a new avenue of nonlinear phonon control.

Aims. The high energy spectrum of 3C 273 is usually understood in terms of inverse-Compton emission in a relativistic leptonic jet. This model predicts variability patterns and delays that could be tested with simultaneous observations from the radio to the GeV range. Methods. The instruments IBIS, SPI, JEM-X on board INTEGRAL, PCA on board RXTE, and LAT on board Fermi have enough sensitivity to follow the spectral variability of 3C 273 from the keV to the GeV. We looked for correlations between the different energy bands, including radio data at 37 GHz collected at the Mets\"ahovi Radio Observatory and built quasi-simultaneous multiwavelength spectra in the high energy domain when the source is flaring either in the X-rays or in the {\gamma} rays. Results. Both temporal and spectral analysis suggest a two-component model to explain the complete high energy spectrum. X-ray emission is likely dominated by a Seyfert-like component while the {\gamma}-ray emission is dominated by a blazar-like component produced by the relativistic jet. The variability of the blazar-like component is discussed, comparing the spectral parameters in the two different spectral states. Changes of the electron Lorentz factor are found to be the most likely source of the observed variability., Comment: 11 pages, 9 figures

The densification, delamination and crack growth behavior in a Ce$_{0.9}$Gd$_{0.1}$O$_{1.95}$ (CGO) and (La$_{0.85}$Sr$_{0.15})_{0.9}$MnO$_{3}$ (LSM) multi-layer ceramic sample was studied using in situ X-ray tomographic microscopy (microtomography), to investigate the critical dynamics of crack propagation and delamination in a multilayered sample. Naturally occurring defects, caused by the sample preparation process, are shown not to be critical in sample degradation. Instead defects are nucleated during the debinding step. Crack growth is significantly faster along the material layers than perpendicular to them, and crack growth and delamination only accelerates when sintering occurs., Comment: 9 pages, 8 figures