Herein, we demonstrate that meticulous and in-depth analysis of the reaction mechanisms of nanoparticle formation is rewarded by full control of the size, shape, and crystal structure of superparamagnetic iron oxide nanocrystals during synthesis. Starting from two iron sources, iron(II) and iron(III) carbonate, a strict separation of oleate formation from the generation of reactive pyrolysis products and concomitant nucleation of iron oxide nanoparticles was achieved. This protocol enabled us to analyze each step of nanoparticle formation independently in depth. The progress of the entire reaction was monitored via matrix-assisted laser desorption ionization time-of-flight mass spectrometry and gas chromatography, thus providing insight into the formation of various iron oleate species prior to nucleation. Interestingly, due to the intrinsic strongly reductive pyrolysis conditions of the oleate intermediates and redox process in early stages of the synthesis, pristine iron oxide nuclei were composed exclusively from wustite irrespective of the oxidation state of the iron source. Controlling the reaction conditions provided a very broad range of size-and shape-defined monodispersed iron oxide nanoparticles. Curiously, after nucleation, star-shaped nanocrystals were obtained that underwent metamorphism toward cubic-shaped particles. Electron energy loss spectroscopy tomography revealed ex post oxidation of the primary wustite nanocrystal, providing a full 3D image of Fe 2+ and Fe 3+ distribution within. Overall, we developed a highly flexible synthesis, yielding multi-gram amounts of well-defined iron oxide nanocrystals of different sizes and morphologies.

Nanocomposite materials based on highly stable encapsulated superparamagnetic iron oxide nanocrystals (SPIONs) were synthesized and characterized by scattering methods and transmission electron microscopy (TEM). The combination of advanced synthesis and encapsulation techniques using different diblock copolymers and the thiol-ene click reaction for cross-linking the polymeric shell results in uniform hybrid SPIONs homogeneously dispersed in a poly(ethylene oxide) matrix. Small-angle X-ray scattering and TEM investigations demonstrate the presence of mostly single particles and a negligible amount of dyads. Consequently, an efficient control over the encapsulation and synthetic conditions is of paramount importance to minimize the fraction of agglomerates and to obtain uniform hybrid nanomaterials.

Spin-coating is suitable to grow 2D supercrystalline nanoparticle lattices and the lattice type can be changed by using different solvents.

The spin-dependent electrical transport in rigid inorganic-inorganic layered systems is extensively applied for the detection of magnetic fields in data storage. In this work, spin-dependent electrical transport in flexible organicinorganic supercrystals based on superparamagnetic iron oxide nanoparticles is investigated. These nanoparticles are stabilized by oleic acid ligands, which in turn are serving as tunneling barriers between individual magnetic nanoparticles. The resulting tunneling magnetoresistance (TMR) is tunable due to the elastic properties of these organic barriers. Applying external mechanical stress on this composite material will change the average distance between adjacent nanoparticles and will hence determine the resulting TMR-effect amplitude. Thus, measured stress-induced changes in the barrier thickness at sub-nanometer scale allow for determining the mechanical properties of organic barrier molecules in the confined space between the particles. These results provide the foundation for a new type of mechanical sensor.

With the development of X-ray free-electron lasers (XFELs), producing pulses of femtosecond durations comparable with the coherence times of X-ray fluorescence, it has become possible to observe intensity–intensity correlations due to the interference of emission from independent atoms. This has been used to compare durations of X-ray pulses and to measure the size of a focusedX-ray beam, for example. Here it is shown that it is also possible to observe the interference of fluorescence photons through the measurement of the speckle contrast of angle-resolved fluorescence patterns. Speckle contrast is often used as a measure of the degree of coherence of the incident beam or the fluctuations of the illuminated sample as determined from X-ray diffraction patterns formed by elastic scattering, rather than from fluorescence patterns as addressed here. Commonly used approaches to estimate speckle contrast were found to suffer when applied to XFEL-generated fluorescence patterns due to low photon counts and a significant variation of the excitation pulse energy from shot to shot. A new method to reliably estimate speckle contrast under such conditions, using a weighting scheme, is introduced. The method is demonstrated by comparing the speckle contrast of fluorescence observed with pulses of 3 fs to 15 fs duration.