The development of future valley based electronics or valleytronics requires a high degree of valley polarization (VP) in large area monolayer (1L)-MoS2. Though it is possible to synthesize 1L-MoS2 films with large area coverage, VP property of as-grown films is found to be very poor. Here, we investigate the role of physisorbed air molecules and strain on the luminescence and the VP characteristics of large area monolayer MoS2 grown on various substrates by a microcavity based chemical vapor deposition (CVD) technique. The study shows that the removal of adsorbates from sulfur vacancy ( VS) sites not only suppresses the broad sub-bandgap luminescence feature that typically dominates low temperature photoluminescence (PL) spectra of these films but also significantly enhances VP. Post-growth transfer of the 1L-MoS2 film from sapphire to a SiO2/Si substrate by a polystyrene assisted process is found to be highly effective in improving the polarization characteristic (∼80%) of K-valleys through relaxation of the biaxial tensile strain and the removal of physisorbed air molecules from the VS sites. The process is also found to provide long lasting protection for MoS2 films from air. The finding, thus, creates much needed opportunity to use CVD grown large area 1L-MoS2 for realization of valleytronics of the future.
We have investigated defects in large area monolayer MoS2 films using thermally stimulated current (TSC) spectroscopy. Films are grown on c-sapphire substrates using a microcavity based chemical vapor deposition technique. A theoretical framework to analyze TSC data for a two dimensional semiconductor has been developed. The study reveals the existence of two traps with average activation energies of 670 and 850 meV. The density of these traps shows an increase followed by saturation as the sample goes through repeated thermal cycles in vacuum. Interestingly, the density returns to its initial level when the sample is exposed to the ambient condition for a sufficiently long time, suggesting that these defects are passivated by certain adsorbate groups/molecules in the ambient condition. It has been found that annealing in a sulfur environment substantially reduces the concentration of these traps. This indicates that the traps must be related to sulfur deficiency related defects.
A systematic study of growth, structural, electrical, and luminescence properties of zinc oxide (ZnO) layers grown on c-oriented GaN/sapphire templates by the pulsed laser deposition technique is carried out. A thorough high-resolution x-ray diffraction study reveals that c-ZnO films with high crystalline quality can be grown under certain growth conditions. Screw and edge dislocation densities in these films are found to be as low as 7×108 and 3×1010cm−2, respectively. All layers are found to be unintentionally n-type with ∼1019cm−3 electron concentration and mobility as high as ∼50 cm2 V−1 s−1. Temperature and excitation intensity dependent photoluminescence (PL) studies as functions of the growth conditions are carried out to identify the transition processes behind various luminescence features found in these samples. At low temperatures, PL spectra are marked by sharp neutral donor bound excitonic transitions, their phonon replicas, and two broad luminescence bands at 2.2 and 2.9 eV. These broad bands are attributed to transitions from the (2+/0) oxygen vacancy (VO) and (2+/+/0) zinc-interstitial (Zni) levels, respectively, to the valence band. Thermal energy needed to depopulate these defects is found to be 11 and 385 meV, respectively, for the (2+/0) VO and (2+/+/0) Zni levels. Low temperature PL spectra for the samples grown with relatively high oxygen pressures are featured by the Zn-vacancy (VZn) related neutral acceptor bound excitonic transition, its phonon replicas, and a broad band at 2.75 eV. This band diminishes with increasing temperature and, instead, another broad feature appears at ∼2.1 eV. Our study attributes the 2.75 eV band to transition from the conduction band to (0/−) VZn levels and the 2.1 eV feature to the transition between (−/2−) VZn levels and the valence band. It has been found that all the defect related features can be minimized by adjusting the growth conditions.
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