Direct reconstruction of the two-dimensional pair distribution function in systems with angular correlations

An x-ray scattering approach to determine the two-dimensional (2D) pair distribution function (PDF) in partially ordered 2D systems is proposed. We derive relations between the structure factor and PDF that enable quantitative studies of positional and bond-orientational (BO) order in real space. We apply this approach in the x-ray study of a liquid crystal (LC) film undergoing the smectic-hexatic phase transition, to analyze the interplay between the positional and BO order during the temperature evolution of the LC film. We analyze the positional correlation length in different directions in real space.Comment: 23 pages, 8 figure

Statistical properties of a free-electron laser revealed by the Hanbury Brown and Twiss interferometry

We present a comprehensive experimental analysis of statistical properties of the self-amplified spontaneous emission (SASE) free-electron laser (FEL) FLASH at DESY in Hamburg by means of Hanbury Brown and Twiss (HBT) interferometry. The experiments were performed at the FEL wavelengths of 5.5 nm, 13.4 nm, and 20.8 nm. We determined the 2-nd order intensity correlation function for all wavelengths and different operation conditions of FLASH. In all experiments a high degree of spatial coherence (above 50%) was obtained. Our analysis performed in spatial and spectral domains provided us with the independent measurements of an average pulse duration of the FEL that were below 60 fs. To explain complicated behaviour of the 2-nd order intensity correlation function we developed advanced theoretical model that includes the presence of multiple beams and external positional jitter of the FEL pulses. By this analysis we determined that in most experiments several beams were present in radiating field and in one of the experiments external positional jitter was about 25% of the beam size. We envision that methods developed in our study will be used widely for analysis and diagnostics of the FEL radiation.Comment: 29 pages, 14 figures, 3 table

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 even to the creation of completely new fields of research such as quantum optics. The reason was their unique statistical and coherence properties. The newly emerging, short-wavelength free-electron lasers (FELs) are sources of very bright coherent extreme-ultraviolet (XUV) and x-ray radiation with pulse durations on the order of femtoseconds, and are presently considered to be laser sources at these energies. Most existing FELs are highly spatially coherent but in spite of their name, they behave statistically as chaotic sources. Here, we demonstrate experimentally, by combining Hanbury Brown and Twiss (HBT) interferometry with spectral measurements that the seeded XUV FERMI FEL-2 source does indeed behave statistically as a laser. The first steps have been taken towards exploiting the first-order coherence of FELs, and the present work opens the way to quantum optics experiments that strongly rely on high-order statistical properties of the radiation.Comment: 24 pages, 10 figures, 37 reference

Spatially resolved fluorescence of caesium lead halide perovskite supercrystals reveals quasi-atomic behavior of nanocrystals

We correlate spatially resolved fluorescence (-lifetime) measurements with X-ray nanodiffraction to reveal surface defects in supercrystals of self-assembled cesium lead halide perovskite nanocrystals and study their effect on the fluorescence properties. Upon comparison with density functional modeling, we show that a loss in structural coherence, an increasing atomic misalignment between adjacent nanocrystals, and growing compressive strain near the surface of the supercrystal are responsible for the observed fluorescence blueshift and decreased fluorescence lifetimes. Such surface defect-related optical properties extend the frequently assumed analogy between atoms and nanocrystals as so-called quasi-atoms. Our results emphasize the importance of minimizing strain during the self-assembly of perovskite nanocrystals into supercrystals for lighting application such as superfluorescent emitters

Quantum Imaging with Incoherently Scattered Light from a Free-Electron Laser

The advent of accelerator-driven free-electron lasers (FEL) has opened new avenues for high-resolution structure determination via diffraction methods that go far beyond conventional x-ray crystallography methods. These techniques rely on coherent scattering processes that require the maintenance of first-order coherence of the radiation field throughout the imaging procedure. Here we show that higher-order degrees of coherence, displayed in the intensity correlations of incoherently scattered x-rays from an FEL, can be used to image two-dimensional objects with a spatial resolution close to or even below the Abbe limit. This constitutes a new approach towards structure determination based on incoherent processes, including Compton scattering, fluorescence emission or wavefront distortions, generally considered detrimental for imaging applications. Our method is an extension of the landmark intensity correlation measurements of Hanbury Brown and Twiss to higher than second-order paving the way towards determination of structure and dynamics of matter in regimes where coherent imaging methods have intrinsic limitations

A hybrid optoelectronic Mott insulator

The coupling of electronic degrees of freedom in materials to create "hybridized functionalities" is a holy grail of modern condensed matter physics that may produce versatile mechanisms of control. Correlated electron systems often exhibit coupled degrees of freedom with a high degree of tunability which sometimes lead to hybridized functionalities based on external stimuli. However, the mechanisms of tunability and the sensitivity to external stimuli are determined by intrinsic material properties which are not always controllable. A Mott metal-insulator transition (MIT) is technologically attractive due to the large changes in resistance, tunable by doping, strain, electric fields, and orbital occupancy but not, in and of itself, controllable with light. Here, an alternate approach is presented to produce optical functionalities using a properly engineered photoconductor/strongly correlated hybrid heterostructure. This approach combines a photoconductor, which does not exhibit an MIT, with a strongly correlated oxide, which is not photoconducting. Due to the intimate proximity between the two materials, the heterostructure exhibits giant volatile and nonvolatile, photoinduced resistivity changes with substantial shifts in the MIT transition temperatures. This approach can be extended to other judicious combinations of strongly correlated materials