MoS presents a promising low-cost catalyst for the hydrogen evolution reaction (HER), but the understanding about its active sites has remained limited. Here we present an unambiguous study of the catalytic activities of all possible reaction sites of MoS, including edge sites, sulfur vacancies, and grain boundaries. We demonstrate that, in addition to the well-known catalytically active edge sites, sulfur vacancies provide another major active site for the HER, while the catalytic activity of grain boundaries is much weaker. The intrinsic turnover frequencies (Tafel slopes) of the edge sites, sulfur vacancies, and grain boundaries are estimated to be 7.5 s (65-75 mV/dec), 3.2 s (65-85 mV/dec), and 0.1 s (120-160 mV/dec), respectively. We also demonstrate that the catalytic activity of sulfur vacancies strongly depends on the density of the vacancies and the local crystalline structure in proximity to the vacancies. Unlike edge sites, whose catalytic activity linearly depends on the length, sulfur vacancies show optimal catalytic activities when the vacancy density is in the range of 7-10%, and the number of sulfur vacancies in high crystalline quality MoS is higher than that in low crystalline quality MoS, which may be related with the proximity of different local crystalline structures to the vacancies.
Control of ion energy distributions (IEDs) onto the surface of wafers is an ongoing challenge in microelectronics fabrication. The use of capacitively coupled plasmas (CCPs) using multiple radio frequency (rf) power sources provides many opportunities to customize IEDs. In dual-frequency CCPs using a fundamental frequency and its second harmonic, varying the relative voltages, powers, and phases between the fundamental and second harmonic biases have demonstrated potential as control mechanisms for the shape of the IEDs. In this paper, we report on computational and experimental investigations of IED control in dual-frequency and triple-frequency CCPs where the phase between the fundamental and second harmonic frequency voltage waveform is used as a control variable. The operating conditions were 5–40 mTorr (0.67–5.33 Pa) in Ar and Ar/CF4/O2 gas mixtures. By changing the phase between the applied rf frequency and its second harmonic, the Electrical Asymmetric Effects was significant and not only shifted the dc self-bias but also affected plasma uniformity. When changing phases of higher harmonics, the energies and widths of the IEDs could be controlled. With the addition of a 3rd high-frequency source, the plasma density increased and uniformity improved. Computed results for IEDs were compared with experimental results using an ion energy analyzer in systems using rf phase locked power supplies.
Doppler-free saturation spectroscopy provides a very powerful method to obtain detailed information about the electronic structure of the atom through measurement of the spectral line profile. This is achieved through a significant decrease in the Doppler broadening and essentially an elimination of the instrument broadening inherent to passive spectroscopic techniques. In this paper we present the technique and associated physics of Doppler-free saturation spectroscopy in addition to how one selects the appropriate transition. Simulations of H spectra are presented to illustrate the increased sensitivity to both electric field and electron density measurements.
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