The coarsening of catalytically active metal clusters is often accelerated by the presence of gases, but the role played by gas molecules is difficult to ascertain and varies from system to system. We use scanning tunnelling microscopy to follow the CO-induced coalescence of Pd adatoms supported on the Fe3O4(001) surface at room temperature, and find Pd-carbonyl species to be responsible for mobility in this system. Once these reach a critical density, clusters nucleate; subsequent coarsening occurs through cluster diffusion and coalescence. Whereas CO induces the mobility in the Pd/Fe3O4 system, surface hydroxyls have the opposite effect. Pd atoms transported to surface OH groups are no longer susceptible to carbonyl formation and remain isolated. Following the evolution from well-dispersed metal adatoms into clusters, atom-by-atom, allows identification of the key processes that underlie gas-induced mass transport.
High-pressure high-temperature (HPHT) nanodiamonds originate from grinding of diamond microcrystals obtained by HPHT synthesis. Here we report on a simple two-step approach to obtain as small as 1.1 nm HPHT nanodiamonds of excellent purity and crystallinity, which are among the smallest artificially prepared nanodiamonds ever shown and characterized. Moreover we provide experimental evidence of diamond stability down to 1 nm. Controlled annealing at 450 °C in air leads to efficient purification from the nondiamond carbon (shells and dots), as evidenced by X-ray photoelectron spectroscopy, Raman spectroscopy, photoluminescence spectroscopy, and scanning transmission electron microscopy. Annealing at 500 °C promotes, besides of purification, also size reduction of nanodiamonds down to ∼1 nm. Comparably short (1 h) centrifugation of the nanodiamonds aqueous colloidal solution ensures separation of the sub-10 nm fraction. Calculations show that an asymmetry of Raman diamond peak of sub-10 nm HPHT nanodiamonds can be well explained by modified phonon confinement model when the actual particle size distribution is taken into account. In contrast, larger Raman peak asymmetry commonly observed in Raman spectra of detonation nanodiamonds is mainly attributed to defects rather than to the phonon confinement. Thus, the obtained characteristics reflect high material quality including nanoscale effects in sub-10 nm HPHT nanodiamonds prepared by the presented method.
The Ångström-sized probe of the scanning transmission electron microscope can visualize and collect spectra from single atoms. This can unambiguously resolve the chemical structure of materials, but not their isotopic composition. Here we differentiate between two isotopes of the same element by quantifying how likely the energetic imaging electrons are to eject atoms. First, we measure the displacement probability in graphene grown from either 12C or 13C and describe the process using a quantum mechanical model of lattice vibrations coupled with density functional theory simulations. We then test our spatial resolution in a mixed sample by ejecting individual atoms from nanoscale areas spanning an interface region that is far from atomically sharp, mapping the isotope concentration with a precision better than 20%. Although we use a scanning instrument, our method may be applicable to any atomic resolution transmission electron microscope and to other low-dimensional materials.
Gold deposited on the Fe3O4(001) surface at room temperature was studied using scanning tunneling microscopy (STM) and x-ray photoelectron spectroscopy (XPS). This surface forms a (√2 × √2)R45° reconstruction, where pairs of Fe and neighboring O ions are slightly displaced laterally producing undulating rows with "narrow" and "wide" hollow sites. At low coverages, single Au adatoms adsorb exclusively at the narrow sites, with no significant sintering up to annealing temperatures of 400 °C. We propose the strong site preference to be related to charge and orbital ordering within the first subsurface layer of Fe3O4(001)-(√2 × √2)R45°. Because of its high thermal stability, this could prove an ideal model system for probing the chemical reactivity of single atomic species.
In this work we demonstrate that a free-standing van der Waals heterostructure, usually regarded as a flat object, can exhibit an intrinsic buckled atomic structure resulting from the interaction between two layers with a small lattice mismatch. We studied a freely suspended membrane of well-aligned graphene on a hexagonal boron nitride (hBN) monolayer by transmission electron microscopy (TEM) and scanning TEM (STEM). We developed a detection method in the STEM that is capable of recording the direction of the scattered electron beam and that is extremely sensitive to the local stacking of atoms. A comparison between experimental data and simulated models shows that the heterostructure effectively bends in the out-of-plane direction, producing an undulated structure having a periodicity that matches the moiré wavelength. We attribute this rippling to the interlayer interaction and also show how this affects the intralayer strain in each layer.
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