Spontaneous Supercrystal Formation During a Strain-Engineered Metal-Insulator Transition.

Mott metal-insulator transitions possess electronic, magnetic, and structural degrees of freedom promising next-generation energy-efficient electronics. A previously unknown, hierarchically ordered, and anisotropic supercrystal state is reported and its intrinsic formation characterized in-situ during a Mott transition in a Ca2RuO4 thin film. Machine learning-assisted X-ray nanodiffraction together with cryogenic electron microscopy reveal multi-scale periodic domain formation at and below the film transition temperature (TFilm ≈ 200-250 K) and a separate anisotropic spatial structure at and above TFilm. Local resistivity measurements imply an intrinsic coupling of the supercrystal orientation to the material's anisotropic conductivity. These findings add a new degree of complexity to the physical understanding of Mott transitions, opening opportunities for designing materials with tunable electronic properties.

Real-space imaging of periodic nanotextures in thin films via phasing of diffraction data.

New properties and exotic quantum phenomena can form due to periodic nanotextures, including Moire patterns, ferroic domains, and topologically protected magnetization and polarization textures. Despite the availability of powerful tools to characterize the atomic crystal structure, the visualization of nanoscale strain-modulated structural motifs remains challenging. Here, we develop nondestructive real-space imaging of periodic lattice distortions in thin epitaxial films and report an emergent periodic nanotexture in a Mott insulator. Specifically, we combine iterative phase retrieval with unsupervised machine learning to invert the diffuse scattering pattern from conventional X-ray reciprocal-space maps into real-space images of crystalline displacements. Our imaging in PbTiO3/SrTiO3 superlattices exhibiting checkerboard strain modulation substantiates published phase-field model calculations. Furthermore, the imaging of biaxially strained Mott insulator Ca2RuO4 reveals a strain-induced nanotexture comprised of nanometer-thin metallic-structure wires separated by nanometer-thin Mott-insulating-structure walls, as confirmed by cryogenic scanning transmission electron microscopy (cryo-STEM). The nanotexture in Ca2RuO4 film is induced by the metal-to-insulator transition and has not been reported in bulk crystals. We expect the phasing of diffuse X-ray scattering from thin crystalline films in combination with cryo-STEM to open a powerful avenue for discovering, visualizing, and quantifying the periodic strain-modulated structures in quantum materials.

Femtosecond laser produced periodic plasma in a colloidal crystal probed by XFEL radiation.

With the rapid development of short-pulse intense laser sources, studies of matter under extreme irradiation conditions enter further unexplored regimes. In addition, an application of X-ray Free-Electron Lasers (XFELs) delivering intense femtosecond X-ray pulses, allows to investigate sample evolution in IR pump - X-ray probe experiments with an unprecedented time resolution. Here we present a detailed study of the periodic plasma created from the colloidal crystal. Both experimental data and theory modeling show that the periodicity in the sample survives to a large extent the extreme excitation and shock wave propagation inside the colloidal crystal. This feature enables probing the excited crystal, using the powerful Bragg peak analysis, in contrast to the conventional studies of dense plasma created from bulk samples for which probing with Bragg diffraction technique is not possible. X-ray diffraction measurements of excited colloidal crystals may then lead towards a better understanding of matter phase transitions under extreme irradiation conditions.

Publisher Correction: Seeded X-ray free-electron laser generating radiation with laser statistical properties.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Seeded X-ray free-electron laser generating radiation with laser statistical properties.

The invention of optical lasers led to a revolution in the field of optics and to the creation of such fields of research as quantum optics. The reason was their unique statistical and coherence properties. The emerging, short-wavelength free-electron lasers (FELs) are sources of very bright coherent extreme-ultraviolet and X-ray radiation with pulse durations on the order of femtoseconds, and are presently considered to be laser sources at these energies. FELs are highly spatially coherent to the first-order but in spite of their name, behave statistically as chaotic sources. Here, we demonstrate experimentally, by combining Hanbury Brown and Twiss interferometry with spectral measurements that the seeded XUV FERMI FEL-2 source does indeed behave statistically as a laser. The results may be useful for quantum optics experiments and for the design and operation of next generation FEL sources.

Structural Changes in a Single GaN Nanowire under Applied Voltage Bias.

GaN nanowires (NWs) are promising building blocks for future optoelectronic devices and nanoelectronics. They exhibit stronger piezoelectric properties than bulk GaN. This phenomena may be crucial for applications of NWs and makes their study highly important. We report on an investigation of the structure evolution of a single GaN NW under an applied voltage bias along polar [0001] crystallographic direction until its mechanical break. The structural changes were investigated using coherent X-ray Bragg diffraction. The three-dimensional (3D) intensity distributions of the NWs without metal contacts, with contacts, and under applied voltage bias in opposite polar directions were analyzed. Coherent X-ray Bragg diffraction revealed the presence of significant bending of the NWs already after metal contacts deposition, which was increased at applied voltage bias. Employing analytical simulations based on elasticity theory and a finite element method (FEM) approach, we developed a 3D model of the NW bending under applied voltage. From this model and our experimental data, we determined the piezoelectric constant of the GaN NW to be about 7.7 pm/V in [0001] crystallographic direction. The ultimate tensile strength of the GaN NW was obtained to be about 1.22 GPa. Our work demonstrates the power of in operando X-ray structural studies of single NWs for their effective design and implementation with desired functional properties.

Ptychographic X-Ray Imaging of Colloidal Crystals.

Ptychographic coherent X-ray imaging is applied to obtain a projection of the electron density of colloidal crystals, which are promising nanoscale materials for optoelectronic applications and important model systems. Using the incident X-ray wavefield reconstructed by mixed states approach, a high resolution and high contrast image of the colloidal crystal structure is obtained by ptychography. The reconstructed colloidal crystal reveals domain structure with an average domain size of about 2 µm. Comparison of the domains formed by the basic close-packed structures, allows us to conclude on the absence of pure hexagonal close-packed domains and confirms the presence of random hexagonal close-packed layers with predominantly face-centered cubic structure within the analyzed part of the colloidal crystal film. The ptychography reconstruction shows that the final structure is complicated and may contain partial dislocations leading to a variation of the stacking sequence in the lateral direction. As such in this work, X-ray ptychography is extended to high resolution imaging of crystalline samples.