Meltable, Glass-Forming, Iron Zeolitic Imidazolate Frameworks.

We describe the first meltable iron-based zeolitic imidazolate framework (ZIF), denoted MUV-24. This material, elusive from direct synthesis, is obtained from the thermal treatment of [Fe3(im)6(Him)2], which yields Fe(im)2 upon loss of the neutral imidazole molecules. Different crystalline phase transformations are observed upon further heating, until the material melts at 482 °C. Vitrification upon cooling of the liquid phase gives rise to the first Fe-metal-organic framework glass. X-ray total scattering experiments show that the tetrahedral environment of the crystalline solids is maintained in the glass, whereas nanoindentation measurements reveal an increase in Young's modulus, in agreement with stiffening upon vitrification.

Preparation, Single-Molecule Manipulation, and Energy Transfer Investigation of a Polyfluorene-graft-DNA polymer.

Conjugated polymers have been intensively studied due to their unique optical and electronic properties combined with their physical flexibility and scalable bottom up synthesis. Although the bulk qualities of conjugated polymers have been extensively utilized in research and industry, the ability to handle and manipulate conjugated polymers at the nanoscale lacks significantly behind. Here, the toolbox for controlled manipulation of conjugated polymers was expanded through the synthesis of a polyfluorene-DNA graft-type polymer (poly(F-DNA)). The polymer possesses the characteristics associated with the conjugated polyfluorene backbone, but the protruding single-stranded DNA provides the material with an exceptional addressability. This study demonstrates controlled single-molecule patterning of poly(F-DNA), as well as energy transfer between two different polymer-DNA conjugates. Finally, highly efficient DNA-directed quenching of polyfluorene fluorescence was shown.

Observation of Attractive and Repulsive Polarons in a Bose-Einstein Condensate.

The problem of an impurity particle moving through a bosonic medium plays a fundamental role in physics. However, the canonical scenario of a mobile impurity immersed in a Bose-Einstein condensate (BEC) has not yet been realized. Here, we use radio frequency spectroscopy of ultracold bosonic ^{39}K atoms to experimentally demonstrate the existence of a well-defined quasiparticle state of an impurity interacting with a BEC. We measure the energy of the impurity both for attractive and repulsive interactions, and find excellent agreement with theories that incorporate three-body correlations, both in the weak-coupling limits and across unitarity. The spectral response consists of a well-defined quasiparticle peak at weak coupling, while for increasing interaction strength, the spectrum is strongly broadened and becomes dominated by the many-body continuum of excited states. Crucially, no significant effects of three-body decay are observed. Our results open up exciting prospects for studying mobile impurities in a bosonic environment and strongly interacting Bose systems in general.

Decoherence of Impurities in a Fermi Sea of Ultracold Atoms.

We investigate the decoherence of ^{40}K impurities interacting with a three-dimensional Fermi sea of ^{6}Li across an interspecies Feshbach resonance. The decoherence is measured as a function of the interaction strength and temperature using a spin-echo atom interferometry method. For weak to moderate interaction strengths, we interpret our measurements in terms of scattering of K quasiparticles by the Fermi sea and find very good agreement with a Fermi liquid calculation. For strong interactions, we observe significant enhancement of the decoherence rate, which is largely independent of temperature, pointing to behavior that is beyond the scattering of quasiparticles in the Fermi liquid picture.

Unravelling the complex formation mechanism of HfO2 nanocrystals using in situ pair distribution function analysis.

Hafnia, HfO2, which is a wide band gap semiconducting oxide, is much less studied than the chemically similar zirconia (ZrO2). Here, we study the formation of hafnia nanocrystals from hafnium tetrachloride in methanol under solvothermal conditions (248 bar, 225-450 °C) using complementary in situ powder X-ray diffraction (PXRD) and Pair Distribution Function (PDF) analysis. The main structural motif of the precursor solution (HfCl4 dissolved in methanol) is a Hf oxide trimer with very similar local structure to that of m-HfO2. Different measurements on precursor solutions show large intensity variation for the Hf-Cl correlations signifying different extents of HCl elimation. A few seconds of heating lead to a correlation appearing at 3.9 Å corresponding to corner-sharing Hf-polyhedra in a disordered solid matrix. During the next minutes (depending on temperature) the disordered structure rearranges and the nearest neighbour Hf-Hf distance contracts while the Hf-O coordination number increases. After approximately 90 seconds (at T = 250 °C) the structural rearrangement terminates and 1-2 nm nanocrystals of m-HfO2 nucleate. Initially the m-HfO2 nanocrystals have significant disorder as reflected in large Hf atomic displacement parameter (ADP) values, but as the nanocrystals grow to 5-6 nm in size during extended heating, the Hf ADPs decrease toward the values obtained for ordered bulk structures. The nanocrystal growth is not well modelled by the Johnson-Mehl-Avrami expression reflecting that multiple complex chemical processes occur during this highly nonclassical nanocrystal formation under solvothermal conditions.