Recently, x-ray illumination, using synchrotron radiation, has been used to manipulate defects, stimulate self-organization and to probe their structure. Here we explore a method of defect-engineering low-dimensional systems using focused laboratory-
scale X-ray sources. We demonstrate an irreversible change in the conducting properties of the 2-dimensional electron gas at the interface between the complex oxide materials LaAlO3 and SrTiO3 by X-ray irradiation. The electrical resistance is monitored during exposure as the irradiated regions are driven into a high resistance state. Our results suggest attention shall be paid on electronic structure modification in X-ray spectroscopic studies and highlight large-area defect manipulation and direct device patterning as possible new fields of application for focused laboratory X-ray sources.
While it is known that the nature and the arrangement of defects in complex oxides have an impact on the material functionalities little is known on control of superconductivity by oxygen interstitial organization in cuprates. Here we report direct c
ompelling evidence for the control of Tc, by manipulation of the superconducting granular networks of nanoscale puddles, made of ordered oxygen stripes, in a single crystal of YBa2Cu3O6.5+y with average formal hole doping p close to 1/8. Upon thermal treatments we were able to switch from a first network of oxygen defects striped puddles with OVIII modulation (qOVIII(a*)=(h+3/8,k,0) and qOVIII(a*)=(h+5/8,k,0)), to second network characterized by OXVI modulation (qOXVI(a*)=(h+7/16,k,0) and qOXVI(a*)=(h+9/16,k,0)), and finally to a third network with puddles of OV periodicity (qOV(a*)=(4/10,1,0) and qOV(a*)=(6/10,1,0)). We map the microscopic spatial evolution of the out of plane OVIII, OXVI and OV puddles nano-size distribution via scanning micro-diffraction measurements. In particular, we calculated the number of oxygen chains (n) and the charge density (holes concentration p) inside each puddle, analyzing areas of 160x80 {mu}m2, and recording 12800 diffraction patterns to reconstruct each spatial map. The high spatial inhomogeneity shown by all the reconstructed spatial maps reflects the intrinsic granular structure that characterizes cuprates and iron-chalcogenides, disclosing the presence of several complex networks of coexisting superconducting domains with different lattice modulations, charge density and different gaps like in the proposed multi-gaps scenario called superstripes.
Despite intensive research a physical explanation of high Tc superconductors remains elusive. One reason for this is that these materials have generally a very complex structure making useless theoretical models for a homogeneous system. Little is kn
own on the control of the critical temperature by the space disposition of defects because of lack of suitable experimental probes. X-ray diffraction and neutron scattering experiments used to investigate y oxygen dopants in YBa2Cu3O 6+y lack of spatial resolution. Here we report the spatial imaging of dopants distribution in-homogeneity in YBa2Cu3O6.67 using scanning nano X-ray diffraction. By changing the X-ray beam size from 1 micron to 300 nm of diameter, the lattice inhomogeneity increases. The ordered oxygen puddles size distribution vary between 6-8 nm using 1x1 {mu}m2 beam, while it is between 5-12 nm with a fat tail using the 300x300 nm2 beam. The increased inhomogeneity at the nanoscale points toward an intrinsic granular complexity.
Oxygen chain fragments are known to appear at the insulator to superconductor transition (SIT) in YBa2Cu3O6+y. However the self organization and the size distribution of oxygen chain fragments is not known. Here we contribute to fill this gap, using
scanning micro X ray diffraction which is a novel imaging method based on advances in focusing synchrotron radiation beam. This novel approach allows us to probe both real-space and k-space of a high-quality YBa2Cu3O6.33 single crystals with Tc=7K. We report compelling evidence for nanoscale striped puddles, with Ortho-II structure, made of chain fragments in the basal Cu(1) plane with local oxygen concentration 0.5. The size of the Ortho-II puddles spans a range between 2 and 9 nanometers. The real space imaging of Ortho-II puddles granular network shows that superconductivity, at low hole-doping regime, occurs in a network of nanoscale oxygen ordered patches, interspersed with oxygen depleted regions. The manipulation by thermal treatments of the striped Ortho II puddles has been investigated focusing on the spontaneous symmetry breaking near the order to disorder phase transition at 350 K.
Electronic functionalities in materials from silicon to transition metal oxides are to a large extent controlled by defects and their relative arrangement. Outstanding examples are the oxides of copper, where defect order is correlated with their hig
h superconducting transition temperatures. The oxygen defect order can be highly inhomogeneous, even in optimal superconducting samples, which raises the question of the nature of the sample regions where the order does not exist but which nonetheless form the glue binding the ordered regions together. Here we use scanning X-ray microdiffraction (with beam 300 nm in diameter) to show that for La2CuO4+y, the glue regions contain incommensurate modulated local lattice distortions, whose spatial extent is most pronounced for the best superconducting samples. For an underdoped single crystal with mobile oxygen interstitials in the spacer La2O2+y layers intercalated between the CuO2 layers, the incommensurate modulated local lattice distortions form droplets anticorrelated with the ordered oxygen interstitials, and whose spatial extent is most pronounced for the best superconducting samples. In this simplest of high temperature superconductors, there are therefore not one, but two networks of ordered defects which can be tuned to achieve optimal superconductivity. For a given stoichiometry, the highest transition temperature is obtained when both the ordered oxygen and lattice defects form fractal patterns, as opposed to appearing in isolated spots. We speculate that the relationship between material complexity and superconducting transition temperature Tc is actually underpinned by a fundamental relation between Tc and the distribution of ordered defect networks supported by the materials.
The disposition of defects in metal oxides is a key attribute exploited for applications from fuel cells and catalysts to superconducting devices and memristors. The most typical defects are mobile excess oxygens and oxygen vacancies, and can be mani
pulated by a variety of thermal protocols as well as optical and dc electric fields. Here we report the X-ray writing of high-qualitysuperconducting regions, derived from defect ordering, in the superoxygenated layered cuprate, La2CuO4+y. Irradiation of a poor superconductor prepared by rapid thermal quenching results first in growth of ordered regions, with an enhancement of superconductivity becoming visible only after a waiting time, as is characteristic of other systems such as ferroelectrics, where strain must be accommodated for order to become extended. However, in La2CuO4+y, we are able to resolve all aspects of the growth of (oxygen) intercalant order, including an extraordinary excursion from low to high and back to low anisotropy of the ordered regions. We can also clearly associate the onset of high quality superconductivity with defect ordering in two dimensions. Additional experiments with small beams demonstrate a photoresist-free, single-step strategy for writing functional materials.
Temperature dependent single-crystal x-ray diffraction (XRD) in transmission mode probing the bulk of the newly discovered K0.8Fe1.6Se2 superconductor (Tc = 31.8 K) using synchrotron radiation is reported. A clear evidence of intrinsic phase separati
on at 520 K between two competing phases, (i) a first majority magnetic phase with a ThCr2Si2-type tetragonal lattice modulated by the iron vacancy ordering and (ii) a minority non-magnetic phase having an in-plane compressed lattice volume and a weak superstructure, is reported. The XRD peaks due to the Fe vacancy ordering in the majority phase disappear by increasing the temperature at 580 K, well above phase separation temperature confirming the order-disorder phase transition. The intrinsic phase separation at 520K between a competing first magnetic phase and a second non-magnetic phase in the normal phase both having lattice superstructures (that imply different Fermi surface topology reconstruction and charge density) is assigned to a lattice-electronic instability of the K0.8Fe1.6Se2 system typical of a system tuned at a Lifshitz critical point of an electronic topological transition that gives a multi-gaps superconductor tuned a shape resonance.
The tetragonal-to-orthorhombic structural phase transition (SPT) in LaFeAsO (La-1111) and SmFeAsO (Sm-1111) single crystals measured by high resolution x-ray diffraction is found to be sharp while the RFeAsO (R=La, Nd, Pr, Sm) polycrystalline samples
show a broad continuous SPT. Comparing the polycrystalline and the single crystal 1111 samples, the critical exponents of the SPT are found to be the same while the correlation length critical exponents are found to be very different. These results imply that the lattice fluctuations in 1111 systems change in samples with different surface to volume ratio that is assigned to the relieve of the temperature dependent superlattice misfit strain between active iron layers and the spacer layers in 1111 systems. This phenomenon that is missing in the AFe2As2 (A=Ca, Sr, Ba) 122 systems, with the same electronic structure but different for the thickness and the elastic constant of the spacer layers, is related with the different maximum superconducting transition temperature in the 1111 (55 K) versus 122 (35 K) systems and implies the surface reconstruction in 1111 single crystals.
We report the temperature dependent x-ray powder diffraction of the FeAs-based superconductors in the range between 300 K and 95 K. In the case of NdOFeAs we have detected the structural phase transition from the tetragonal phase, with P4/nmm space g
roup, to the orthorhombic phase,with Cmma space group, over a broad temperature range from 150 K to 120 K, centered at T0 137K. This transition is reduced, by about 30K, by the internal chemical pressure going from LaOFeAs to NdOFeAs. On the contrary the superconducting critical temperature increases from 27K to 51 K going from LaOFeAs to NdOFeAs doped samples. The FeAs layers in all undoped 1111 and 122 systems suffer a tensile misfit strain. The tensile misfit strain is reduced in 1111 and in 122 samples and at optimum doping the misfit strain is close to zero. This result shows that the normal striped orthorhombic Cmma phase competes with the superconducting tetragonal phase. In the orthorhombic clusters the charges can move only along the stripes in the b direction and are localized by the magnetic interaction.
