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Measuring the three-dimensional (3D) distribution of chemistry in nanoscale matter is a longstanding challenge for metrological science. The inelastic scattering events required for 3D chemical imaging are too rare, requiring high beam exposure that destroys the specimen before an experiment completes. Even larger doses are required to achieve high resolution. Thus, chemical mapping in 3D has been unachievable except at lower resolution with the most radiation-hard materials. Here, high-resolution 3D chemical imaging is achieved near or below one nanometer resolution in a Au-Fe$_3$O$_4$ metamaterial, Co$_3$O$_4$ - Mn$_3$O$_4$ core-shell nanocrystals, and ZnS-Cu$_{0.64}$S$_{0.36}$ nanomaterial using fused multi-modal electron tomography. Multi-modal data fusion enables high-resolution chemical tomography often with 99\% less dose by linking information encoded within both elastic (HAADF) and inelastic (EDX / EELS) signals. Now sub-nanometer 3D resolution of chemistry is measurable for a broad class of geometrically and compositionally complex materials.

Efforts to map atomic-scale chemistry at low doses with minimal noise using electron microscopes are fundamentally limited by inelastic interactions. Here, fused multi-modal electron microscopy offers high signal-to-noise ratio (SNR) recovery of material chemistry at nano- and atomic- resolution by coupling correlated information encoded within both elastic scattering (high-angle annular dark field (HAADF)) and inelastic spectroscopic signals (electron energy loss (EELS) or energy-dispersive x-ray (EDX)). By linking these simultaneously acquired signals, or modalities, the chemical distribution within nanomaterials can be imaged at significantly lower doses with existing detector hardware. In many cases, the dose requirements can be reduced by over one order of magnitude. This high SNR recovery of chemistry is tested against simulated and experimental atomic resolution data of heterogeneous nanomaterials.

Magic-sized clusters (MSCs) are renowned for their identical size and closed-shell stability that inhibit conventional nanoparticle (NP) growth processes. Though MSCs have been of increasing interest, understanding the reaction pathways toward their nucleation and stabilization is an outstanding issue. In this work, we demonstrate that high concentration synthesis (1000 mM) promotes a well-defined reaction pathway to form high-purity MSCs (greater than 99.9 percent). The MSCs are resistant to typical growth and dissolution processes. Based on insights from in-situ X-ray scattering analysis, we attribute this stability to the accompanying production of a large, hexagonal organic-inorganic mesophase (greater than 100 nm grain size) that arrests growth of the MSCs and prevents NP growth. At intermediate concentrations (500 mM), the MSC mesophase forms, but is unstable, resulting in NP growth at the expense of the assemblies. These results provide an alternate explanation for the high stability of MSCs. Whereas the conventional mantra has been that the stability of MSCs derives from the precise arrangement of the inorganic structures (i.e., closed-shell atomic packing), we demonstrate that anisotropic clusters can also be stabilized by self-forming fibrous mesophase assemblies. At lower concentration (less than 200 mM or greater than 16 acid-to-metal), MSCs are further destabilized and NPs formation dominates that of MSCs. Overall, the high concentration approach intensifies and showcases inherent concentration-dependent surfactant phase behavior that is not accessible in conventional (i.e., dilute) conditions. This work provides not only a robust method to synthesize, stabilize, and study identical MSC products, but also uncovers an underappreciated stabilizing interaction between surfactants and clusters., Comment: main text - 24 pages, 8 figures. SI - 35 pages, 30 figures, 6 tables

Structural transformations in molecules and solids have generally been studied in isolation, while intermediate systems have eluded characterization. We show that a pair of CdS cluster isomers provides an advantageous experimental platform to study isomerization in well-defined atomically precise systems. The clusters coherently interconvert over an est. 1 eV energy barrier with a 140 meV shift in their excitonic energy gaps. There is a diffusionless, displacive reconfiguration of the inorganic core (solid-solid transformation) with first order (isomerization-like) transformation kinetics. Driven by a distortion of the ligand binding motifs, the presence of hydroxyl species changes the surface energy via physisorption, which determines phase stability in this system. This reaction possesses essential characteristics of both solid-solid transformations and molecular isomerizations, and bridges these disparate length scales., Comment: Main text - 17 pages, 4 figures, SI - 65 pages, 10 figures, 6 tables

Electron tomography in materials science has flourished with the demand to characterize nanoscale materials in three dimensions (3D). Access to experimental data is vital for developing and validating reconstruction methods that improve resolution and reduce radiation dose requirements. This work presents five high-quality scanning transmission electron microscope (STEM) tomography datasets in order to address the critical need for open access data in this field. The datasets represent the current limits of experimental technique, are of high quality, and contain materials with structural complexity. Included are tomographic series of a hyperbranched Co2P nanocrystal, platinum nanoparticles on a carbon nanofibre imaged over the complete 180{\deg} tilt range, a platinum nanoparticle and a tungsten needle both imaged at atomic resolution by equal slope tomography, and a through-focal tilt series of PtCu nanoparticles. A volumetric reconstruction from every dataset is provided for comparison and development of post-processing and visualization techniques. Researchers interested in creating novel data processing and reconstruction algorithms will now have access to state of the art experimental test data., Comment: 3 figures, 10 datasets

In order to fully understand nanoscale heat transport it is necessary to spectrally characterize phonon transmission in nanostructures. Towards this goal we have developed a microfabricated phonon spectrometer. We utilize microfabricated superconducting tunnel junction-based (STJ) phonon transducers for the emission and detection of tunable, non-thermal, and spectrally resolved acoustic phonons, with frequencies ranging from ~100 to ~870 GHz, in silicon microstructures. We show that phonon spectroscopy with STJs offers a spectral resolution of ~15-20 GHz, which is ~20 times better than thermal conductance measurements, for probing nanoscale phonon transport. The STJs are Al-AlxOy-Al tunnel junctions and phonon emission and detection occurs via quasiparticle excitation and decay transitions that occur in the superconducting films. We elaborate on the design geometry and constraints of the spectrometer, the fabrication techniques, and the low-noise instrumentation that are essential for successful application of this technique for nanoscale phonon studies. We discuss the spectral distribution of phonons emitted by an STJ emitter and the efficiency of their detection by an STJ detector. We demonstrate that the phonons propagate ballistically through a silicon microstructure, and that submicron spatial resolution is realizable in a design such as ours. Spectrally resolved measurements of phonon transport in nanoscale structures and nanomaterials will further the engineering and exploitation of phonons, and thus have important ramifications for nanoscale thermal transport as well as the burgeoning field of nanophononics., Comment: This is an author-created, un-copyedited version of an article accepted for publication in New Journal of Physics. IOP Publishing Ltd is not responsible for any errors or omissions in this version of the manuscript or any version derived from it

The Galaxy Evolution Explorer (GALEX) satellite has obtained high time resolution ultraviolet photometry during a large flare on the M4 dwarf star GJ 3685A. Simultaneous NUV (1750 - 2800A) and FUV (1350 - 1750A) time-tagged photometry with time resolution better than 0.1 s shows that the overall brightness in the FUV band increased by a factor of 1000 in 200 s. Under the assumption that the NUV emission is mostly due to a stellar continuum, and that the FUV flux is shared equally between emission lines and continuum, then there is evidence for two distinct flare components for this event. The first flare type is characterized by an exponential increase in flux with little or no increase in temperature. The other involves rapid increases in both temperature and flux. While the decay time for the first flare component may be several hours, the second flare event decayed over less than 1 minute, suggesting that there was little or no confinement of the heated plasma.

We present a survey of coronal forbidden lines detected in Far Ultraviolet Spectroscopic Explorer (FUSE) spectra of nearby stars. Two strong coronal features, Fe XVIII 974 A and Fe XIX 1118 A, are observed in 10 of the 26 stars in our sample. Various other coronal forbidden lines, observed in solar flares, also were sought but not detected. The Fe XVIII feature, formed at log T (K) = 6.8, appears to be free of blends, whereas the Fe XIX line can be corrupted by a C I multiplet. FUSE observations of these forbidden iron lines at spectral resolution R ~ 15,000 provides the opportunity to study dynamics of hot coronal plasmas. We find that the velocity centroid of the Fe XVIII feature deviates little from the stellar rest frame, confirming that the hot coronal plasma is confined. The observed line widths generally are consistent with thermal broadening at the high temperatures of formation and show little indication of additional turbulent broadening. The fastest rotating stars, 31 Com, alpha Aur Ab, and AB Dor, show evidence for excess broadening beyond the thermal component and the photospheric v sin i. The anomalously large widths in these fast rotating targets may be evidence for enhanced rotational broadening consistent with emission from coronal regions extending an additional delta R ~ 0.4-1.3 R_star above the stellar photosphere or represent the turbulent broadening caused by flows along magnetic loop structures. For the stars in which Fe XVIII is detected, there is an excellent correlation between the observed Rontgensatellit} (ROSAT) 0.2-2.0 keV soft X-ray flux and the coronal forbidden line flux. As a result, Fe XVIII is a powerful new diagnostic of coronal thermal conditions and dynamics that can be utilized to study high temperature plasma processes in late-type stars., Comment: 29 pages, 7 figures, AASTEX v5.0, accepted by ApJ

gamma Cas (B0.5e) is known to be a unique X-ray source because ot its moderate L_x, hard X-ray spectrum, and light curve punctuated by ubiquitous flares and slow undulations. Its X-ray peculiarities have led to a controversy concerning their origin: either from wind infall onto a putative degenerate companion, as for typical Be/X-ray binaries, or from the Be star per se. Recent progress has been made to address this: (1) the discovery that gamma Cas is an eccentric binary system (P = 203.59 d) with unknown secondary type, (2) the accumulation of RXTE data at 9 epochs in 1996-2000, and (3) the collation of robotic telescope B, V-band photometric observations over 4 seasons. The latter show a 3%, cyclical flux variation with cycle lengths 55-93 days. We find that X-ray fluxes at all 9 epochs show random variations with orbital phase. This contradicts the binary accretion model, which predicts a substantial modulation. However,these fluxes correlate well with the cyclical optical variations. Also, the 6 flux measurements in 2000 closely track the interpolated optical variations between the 2000 and 2001 observing seasons. Since the optical variations represent a far greater energy than that emitted as X-rays, the optical variability cannot arise from X-ray reprocessing. However, the strong correlation between the two suggests that they are driven by a common mechanism. We propose that this mechanism is a cyclical magnetic dynamo excited by a Balbus-Hawley instability located within the inner part of the circumstellar disk. In our model, variations in the field strength directly produce the changes in the magnetically related X-ray activity. Turbulence associated with the dynamo results in changes to the density distribution within the disk and creates the observed optical variations., Comment: 30 dbl-spaced pages, Latex, plus 11 figures. Accepted by ApJ