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Zakharov, Dmitri

Publications and source records attributed to Zakharov, Dmitri.

Photonic Crystal Surface Emitting Diode Lasers with λ near 2 µm

Epitaxially regrown electrically pumped photonic crystal surface emitting lasers (PCSELs) operating near 2 µm were designed and fabricated within a III-V-Sb material system. A high-index-contrast photonic crystal layer was incorporated into the laser heterostructures by air-pocket-retaining epitaxial regrowth. Transmission electron microscopy studies confirmed uniform and continuous AlGaAsSb initial growth over the nano-patterned GaSb surface, followed by the development of the air-pockets. The PCSEL threshold current density had a minimal value of ~170 A/cm 2 in the 160–180 K temperature range when the QW gain spectrum aligned with the Γ 2 band edge of the photonic crystal. The devices operated in a continuous wave regime at 160 K. The divergence and polarization of the multimode laser beam emitted from the 200 µm × 200 µm PCSEL aperture were controlled by filamentation.

36 MATERIALS SCIENCE↗

Revealing the dynamics of the alloying and segregation of Pt-Co nanoparticles via in-situ environmental transmission electron microscopy

Thermal treatment is a general and efficient way to synthesize intermetallic catalysts and may involve complicated physical processes. So far, the mechanisms leading to the size and composition heterogeneity, as well as the phase segregation behavior in Pt-Co nanoparticles (NPs) are still not well understood. Here, via in-situ environmental transmission electron microscopy, the formation dynamics and segregation behaviors of Pt-Co alloyed NPs during the thermal treatment were investigated. It is found that Pt-Co NPs on zeolitic imidazolate frameworks-67-derived nanocarbon (NC) are formed consecutively through both particle migration coalescence and the Ostwald ripening process. The existence of Pt NPs is found to affect the movement of Co NPs during their migration. With the help of theoretical calculations, the correlations between the composition and migration of the Pt and Co during the ripening process were uncovered. Herein, these complex alloying processes are revealed as key factors leading to the heterogeneity of the synthesized Pt-Co alloyed NPs. Under oxidation environment, the Pt-Co NPs become surface faceted gradually, which can be attributed to the oxygen facilitated relatively higher segregation rate of Co from the (111) surface. This work advances the fundamental understanding of design, synthesis, and durability of the Pt-based nanocatalysts.

36 MATERIALS SCIENCE↗

Effect of surface steps on chemical ordering in the subsurface of Cu(Au) solid solutions

Atomic steps are typically assumed to only influence surface phenomena of solids. In contrast, in this paper we show, using in-situ atomic-resolution electron microscopy observations and atomistic modeling, the pronounced effect from surface stepsin inducing compositional and structural evolution in the subsurface of a Cu(Au) solid solution. We find that Au surface segregation results in a stacked sequence of Cu-Au ordered phases in the subsurface. The presence of a monatomic step at the surface induces the formation of an anti-phase boundary that extends from the surface step to deeper layers by maintaining the same composition profile associated with each terrace. The bunching of surface steps induces chemical disordering of the Cu-Au ordered phases in the subsurface region of the bunched steps. These results demonstrate the instant propagation of surface dynamics of atomic steps into the subsurface region and can find broader applicability in utilizing surface defects to tune the composition and structure in the subsurface of alloys.

36 MATERIALS SCIENCE↗

One-dimensional twisted and tubular structures of zinc oxide by semiconductor-catalyzed vapor–liquid–solid synthesis

The exploration of unconventional catalysts for the vapor-liquid-solid synthesis of one-dimensional materials promises to yield new morphologies and functionality. Here, we show, for the model ZnO system, that unusual nanostructures can be produced via a semiconductor (Ge) catalyst. As well as the usual straight nanowires, we describe two other distinct morphologies: twisted nanowires and twisted nanotubes. The twisted nanotubes show large hollow cores and surprisingly high twisting rates, up to 9°/μm, that cannot be easily explained through the Eshelby twist model. A combination of ex situ and in situ transmission electron microscopy measurements suggest that the hollow core results from a competition between growth and etching at the Ge-ZnO interface during synthesis. The twisting rate is consistent with a softening of elastic rigidity. Finally, these results indicate that the use of unconventional, nonmetallic catalysts provides opportunities to synthesize unusual oxide nanostructures with potentially useful properties.

36 MATERIALS SCIENCE↗

Replication Data for: Evolution of steady-state material properties during catalysis: Oxidative coupling of methanol over nanoporous Ag0.03Au0.97

The data underlying this published work have been made publicly available in this repository as part of the IMASC Data Management Plan. This work was supported as part of the Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award # DE-SC0012573.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Atomically Visualizing Elemental Segregation-Induced Surface Alloying and Restructuring

Using in situ transmission electron microscopy that spatially and temporally resolves the evolution of the atomic structure in the surface and subsurface regions, we Find that the surface segregation of Au atoms in a Cu(Au) solid solution results in the nucleation and growth of a (2 × 1) missing-row reconstructed, half-unit-cell thick L1 2 Cu 3 Au(110) surface alloy. Our in situ electron microscopy observations and atomistic simulations demonstrate that the (2 × 1) reconstruction of the Cu 3 Au(110) surface alloy remains as a stable surface structure as a result of the favored Cu-Au diatom configuration.

36 MATERIALS SCIENCE↗

Dislocation nucleation facilitated by atomic segregation

Surface segregation—the enrichment of one element at the surface, relative to the bulk—is ubiquitous to multi-component materials. Using the example of a Cu–Au solid solution, we demonstrate that compositional variations induced by surface segregation are accompanied by misfit strain and the formation of dislocations in the subsurface region via a surface di˙usion and trapping process. The resulting chemically ordered surface regions acts as an e˙ective barrier that inhibits subsequent dislocation annihilation at free surfaces. Using dynamic, atomic-scale resolution electron microscopy observations and theory modelling, we show that the dislocations are highly active, and we delineate the specific atomic-scale mechanisms associated with their nucleation, glide, climb, and annihilation at elevated temperatures. As a result, these observations provide mechanistic detail of how dislocations nucleate and migrate at heterointerfaces in dissimilar-material systems.

36 MATERIALS SCIENCE↗

In situ atomic-scale imaging of the metal/oxide interfacial transformation

Directly probing structure dynamics at metal/oxide interfaces has been a major challenge due to their buried nature.Using environmental transmission electron microscopy,here we report observations of the in-place formation of Cu 2 O/Cu interfaces via the oxidation of Cu, and subsequently probe the atomic mechanisms by which interfacial transformation and grain rotation occur at the interfaces during reduction in an H 2 gas environment. The Cu 2 O→Cu transformation is observed to occur initially along the Cu 2 O/Cu interface in a layer-by-layer manner.The accumulation of oxygen vacancies at the Cu 2 O/Cu interface drives the collapse of the Cu 2 O lattice near the interface region, which results in a tilted Cu 2 O/Cu interface with concomitant Cu 2 O island rotation. Lastly, these results provide unprecedented microscopic detail regarding the redox reactions of supported oxides,which differs fundamentally from the reduction of bulk or isolated oxides that requires the formation of new interfaces between the parent oxide and the reduced phase.

36 MATERIALS SCIENCE↗