We demonstrate the use of a scanning transmission electron microscope (STEM) equipped with a monochromator and an electron energy loss (EEL) spectrometer as a powerful tool to study localized surface plasmons in metallic nanoparticles. We find that plasmon modes can be influenced by changes in nanostructure geometry and electron beam damage and show that it is possible to delineate the two effects through optimization of specimen preparation techniques and acquisition parameters. The results from the experimental mapping of bright and dark plasmon energies are in excellent agreement with the results from theoretical modeling.

During the past decade, significant progress has been made in the field of resonant optics ranging from fundamental aspects to concrete applications. While several techniques have been introduced for the fabrication of highly defined metallic nanostructures, the synthesis of complex, free-standing three-dimensional (3D) structures is still an intriguing, but so far intractable, challenge. In this study, we demonstrate a 3D direct-write synthesis approach that addresses this challenge. Specifically, we succeeded in the direct-write fabrication of 3D nanoarchitectures via electron-stimulated reactions, which are applicable on virtually any material and surface morphology. By that, complex 3D nanostructures composed of highly compact, pure gold can be fabricated, which reveal strong plasmonic activity and pave the way for a new generation of 3D nanoplasmonic architectures that can be printed on-demand.

Magnetically doped topological insulators enable the quantum anomalous Hall effect (QAHE) which provides quantized edge states for lossless charge transport applications [1][2][3][4][5][6][7][8][9]. The edge states are hosted by a magnetic energy gap at the Dirac point[2] but all attempts to observe it directly have been unsuccessful. The size of this gap is considered the clue to overcoming the present limitations of the QAHE, which so far occurs only at temperatures one to two orders of magnitude below its principle limit set by the ferromagnetic Curie temperature T C [8,9]. Here, we use low temperature photoelectron spectroscopy to unambiguously reveal the magnetic gap of Mn-doped Bi 2 Te 3 films which is present only below T C . Surprisingly, the gap turns out to be ∼ 90 meV wide, which not only exceeds k B T at room temperature but is also 5 times larger than predicted by density functional theory [10]. By an exhaustive multiscale structure characterization we show that this enhancement is due to a remarkable structure modification induced by Mn doping. Instead of a disordered impurity system, it forms an alternating sequence of septuple and quintuple layer blocks, where Mn is predominantly incorporated in the center of the septuple layers. This self-organized heterostructure substantially enhances the wave-function overlap and the size of the magnetic gap at the Dirac point, as recently predicted [11]. Mn-doped Bi 2 Se 3 forms a similar heterostructure, however, only a large, albeit nonmagnetic gap is formed. We explain both differences based on the higher spin-orbit interaction in Bi 2 Te 3 with the most important consequence of a magnetic anisotropy perpendicular to the films, whereas for Bi 2 Se 3 the spin-orbit interaction it is too weak to overcome the dipole-dipole interaction. Our findings provide crucial insights for pushing the lossless transport properties of topological insulators towards room-temperature applications.We thank B. Henne, F. Wilhelm, and A. Rogalev for support of the XANES and EX-AFS measurements at ID 12 and BM23 beam lines of the ESRF, V. Holý for advices on the structure model, W. Grafeneder for the TEM sample preparation and G. Bihlmayer and A. Ernst for helpful discussions. S.A.K and J.M. are grateful for support from CEDAMNF (CZ.02.1.01/0.0/0.0/15 003/0000358) of Czech ministry MSMT.

No abstract

For three types of colloidal magnetic nanocrystals, we demonstrate that postsynthetic cation exchange enables tuning of the nanocrystal’s magnetic properties and achieving characteristics not obtainable by conventional synthetic routes. While the cation exchange procedure, performed in solution phase approach, was restricted so far to chalcogenide based semiconductor nanocrystals, here ferrite-based nanocrystals were subjected to a Fe2+ to Co2+ cation exchange procedure. This allows tracing of the compositional modifications by systematic and detailed magnetic characterization. In homogeneous magnetite nanocrystals and in gold/magnetite core shell nanocrystals the cation exchange increases the coercivity field, the remanence magnetization, as well as the superparamagnetic blocking temperature. For core/shell nanoheterostructures a selective doping of either the shell or predominantly of the core with Co2+ is demonstrated. By applying the cation exchange to FeO/CoFe2O4 core/shell nanocrystals the Neél temperature of the core material is increased and exchange-bias effects are enhanced so that vertical shifts of the hysteresis loops are obtained which are superior to those in any other system.

No abstract

The detection of gas species with high sensitivity is a significant task for fundamental sciences as well as for industrial applications. Similarly, the ongoing trend for device miniaturization brings new challenges for advanced fabrication including on-demand functionality tuning. Following this motivation, here the additive, direct-write fabrication of freestanding 3D nanoarchitectures is introduced, which can be brought into mechanical resonance via electric AC fields. Specifically, this study focuses on the 3D nanostructure synthesis, the subsequent determination of Young's modulus, and demonstrates a postgrowth procedure, which can precisely tune the material modulus. As-fabricated resonators reveal a Young's modulus of 9-13 GPa, which can be increased by a factor greater than 5. Next, the electric readout of the resonance behavior is demonstrated via electric current measurement as an essential element for the resonance sensor applications. Finally, the implications of gas-physisorption and gas-chemisorption on the resonance frequencies are studied, representing a proof-of-principle for sensing applications by the here presented approach.

The authors use focused electron-beam-induced Pt deposition from a gaseous (CH3)3CH3C5H4Pt precursor for the fabrication of electrically conductive structures consisting of Pt nanocrystals embedded in a carbon containing matrix. Recently it has been demonstrated that the electrical resistivity of such deposits can be strongly improved via postgrowth electron irradiation. This study shows very strong evidence that incompletely and nondissociated precursor molecules incorporated within the deposits during deposition are the key elements for efficient e-beam curing. During the early stages of e-beam curing these fragments are further dissociated, which leads to slight growth of the Pt nanocrystals. This is further supported by variable growth regime experiments during deposition which can be used to enhance the incorporation of incompletely and nondissociated precursor molecules, resulting in higher curing efficiencies and lower electrical resistivities. The absence of a predominant graphitization of the surrounding carbon matrix during this dissociation dominated curing regime suggests strongly that the observed resistivity decrease is mainly caused by the formation of preferred tunnel percolation paths due to reduced intercrystallite distances. Furthermore, it is shown that deposit height and the electron-beam energy used for curing should be adapted to each other to achieve the fastest curing time and the lowest electrical resistivities. Such optimized procedures allow then for curing rates higher than 1.5 μm2 min−1 and resistivity decreased to 5 ± 0.4 × 104 μΩ cm, representing an improvement of up to 3 orders of magnitude.