Nanowire growth in the standard <111> direction is assumed to occur at a planar catalyst-nanowire interface, but recent reports contradict this picture. Here we show that a nonplanar growth interface is, in fact, a general phenomenon. Both III-V and group IV nanowires show a distinct region at the trijunction with a different orientation whose size oscillates during growth, synchronized with step flow. We develop an explicit model for this structure that agrees well with experiment and shows that the oscillations provide a direct visualization of catalyst supersaturation. We discuss the implications for wire growth and structure.
Measurements of solution-phase crystal growth provide mechanistic information that is helpful in designing and synthesizing nanostructures. Here, we examine the model system of individual Au nanocrystal formation within a defined liquid geometry during electron beam irradiation of gold chloride solution, where radiolytically formed hydrated electrons reduce Au ions to solid Au. By selecting conditions that favor the growth of well-faceted Au nanoprisms, we measure growth rates of individual crystals. The volume of each crystal increases linearly with irradiation time at a rate unaffected by its shape or proximity to neighboring crystals, implying a growth process that is controlled by the arrival of atoms from solution. Furthermore, growth requires a threshold dose rate, suggesting competition between reduction and oxidation processes in the solution. Above this threshold, the growth rate follows a power law with dose rate. To explain the observed dose rate dependence, we demonstrate that a reaction-diffusion model is required that explicitly accounts for the species H(+) and Cl(-). The model highlights the necessity of considering all species present when interpreting kinetic data obtained from beam-induced processes, and suggest conditions under which growth rates can be controlled with higher precision.
ABSTRACT. Since the AD 775 and AD 994 Δ 14 C peak (henceforth M12) was first measured by Miyake et al. (2012Miyake et al. ( , 2013, several possible production mechanisms for these spike have been suggested, but the work of Mekhaldi et al. (2015) shows that a very soft energy spectrum was involved, implying that a strong solar energetic particle (SEP) event (or series of events) was responsible. Here we present Δ 14 C values from AD 721-820 Sequoiadendron giganteum annual tree-ring samples from Sequoia National Park in California, USA, together with Δ 14 C in German oak from 650-670 BC. The AD 721-820 measurements confirm that a sharp Δ 14 C peak exists at AD 775, with a peak height of approximately 15‰ and show that this spike was preceded by several decades of rapidly decreasing Δ 14 C. A sharp peak is also present at 660 BC, with a peak height of about 10‰, and published data ) indicate that it too was preceded by a multi-decadal Δ 14 C decrease, suggesting that solar activity was very strong just prior to both Δ 14 C peaks and may be causally related. During periods of strong solar activity there is increased probability for coronal mass ejection (CME) events that can subject the Earth's atmosphere to high fluencies of solar energetic particles (SEPs). Periods of high solar activity (such as one in October-November 2003) can also often include many large, fast CMEs increasing the probability of geomagnetic storms. In this paper we suggest that the combination of large SEP events and elevated geomagnetic activity can lead to enhanced production of 14 C and other cosmogenic isotopes by increasing the area of the atmosphere that is irradiated by high solar energetic particles.
Recently, it has been confirmed that extreme solar proton events can lead to significantly increased atmospheric production rates of cosmogenic radionuclides. Evidence of such events is recorded in annually resolved natural archives, such as tree rings [carbon-14 (14C)] and ice cores [beryllium-10 (10Be), chlorine-36 (36Cl)]. Here, we show evidence for an extreme solar event around 2,610 years B.P. (∼660 BC) based on high-resolution10Be data from two Greenland ice cores. Our conclusions are supported by modeled14C production rates for the same period. Using existing36Cl ice core data in conjunction with10Be, we further show that this solar event was characterized by a very hard energy spectrum. These results indicate that the 2,610-years B.P. event was an order of magnitude stronger than any solar event recorded during the instrumental period and comparable with the solar proton event of AD 774/775, the largest solar event known to date. The results illustrate the importance of multiple ice core radionuclide measurements for the reliable identification of short-term production rate increases and the assessment of their origins.
The use of liquid cell electron microscopy as a quantitative probe of nanomaterial structures and reactions requires an accurate understanding of how the sample is altered by the imaging electron beam. In particular, changes in the chemical environment due to beam-induced radiolysis can strongly affect processes such as solution-phase nanocrystal synthesis or electrochemical deposition. It is generally assumed that beam effects are uniform throughout the irradiated liquid. Here we show that for a liquid cell filled with water, the inevitable presence of interfaces between water and the surrounding surfaces causes a spatial variation in the energy absorbed by the water near the walls. The mechanism for this effect is that the walls act as a source of secondary and backscattered electrons which diffuse and deposit energy in the water nearby. This increased dose rate then changes the local concentrations of radiolysis species. We quantify and compare the effects for different materials used in practical liquid cells. We show that the dose rate can increase by several times within tens of nanometers of a water/Au interface, locally increasing the concentrations of species such as the hydrated electron. We discuss the implications for materials processes that are typically triggered at the solid-liquid interface.
Control of interfacial morphology in electrochemical processes is essential for applications ranging from nanomanufacturing to batteries. Here, we quantify the evolution of an electrochemical growth front, using liquid cell electron microscopy to access unexplored length and time scales. During galvanostatic deposition of copper from an acidic electrolyte, we find that the growth front initially evolves consistent with kinetic roughening theory. Subsequently, it roughens more rapidly, consistent with diffusion-limited growth physics. However, the onset of roughening is strongly delayed compared to expectations, suggesting the importance of lateral diffusion of ions. Based on these growth regimes, we discuss morphological control and demonstrate the effects of two strategies, pulse plating and the use of electrolyte additives.
Lithium metal is an ideal material for high-energy, cost-effective rechargeable energy storage systems. The thermodynamically unfavorable solid−liquid interface between the lithium metal and organic electrolyte necessitates the formation of an interlayer (SEI) which is known to have significant impact on lithium morphologies. Less well understood is the impact of the current collector substrate on the morphology of electrodeposited lithium. Here we report on the morphology of electrodeposited lithium as a function of the chemical pretreatments of the working electrode. We find that a copper substrate pretreatment with acidic solutions (sulfuric, oxalic, or acetic acid) results in the deposition of close-packed lithium columns with a uniform diameter. A controlled study of the pre-electrodeposited copper surface indicates that the formation of a 5−8 nm thick LiF protective layer on copper substrate from a chemical reaction between adsorbed surface water layer in acidic solutions and LiPF 6 electrolyte is the key process in the electrochemical growth of lithium columns. We anticipate that this simple chemical approach can be generalized as a scalable, low-cost, additive-free substrate treatment method for depositing a LiF protective layer, broadly applicable in the development of uniform lithium films.
[Purpose] This study investigated the effects of Nordic walking on physical functions and depression in frail people aged 70 years and above. [Subjects] Twenty frail elderly individuals ≥70 years old were assigned to either a Nordic walking group (n=8) or general exercise group (n=10). [Methods] The duration of intervention was equal in both groups (3 sessions/week for 12 weeks, 60 min/session). Physical function (balance, upper extremity strength, lower extremity strength, weakness) and depression were examined before and after the interventions. [Results] With the exception of upper extremity muscle strength, lower extremity strength, weakness, balance, and depression after Nordic walking demonstrated statistically significant improvement. However, in the general exercise group, only balance demonstrated a statistically significant improvement after the intervention. There were significant differences in the changes in lower extremity muscle strength, weakness and depression between the groups. [Conclusion] In conclusion, Nordic walking was more effective than general exercise. Therefore, we suggest that Nordic walking may be an attractive option for significant functional improvement in frail people over 70 years old.
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