RESUMEN
In this manuscript, we combine experimental and computational approaches to study the atomic layer deposition (ALD) of dielectrics on MoS2 surfaces for a very common class of ALD precursors, the alkylamines. More specifically, we study the thermal ALD of TiO2 from TDMAT and H2O. Depositions on as-produced chemical vapor deposition MoS2 flakes result in discontinuous films. Surface treatment with mercaptoethanol (ME) does not improve the surface coverage, and DFT calculations show that ME reacts very weakly with the MoS2 surface. However, creation of sulfur vacancies on the MoS2 surface using Ar ion beam irradiation results in much improved surface coverage for films with a nominal thickness of 6 nm, and the calculations show that TDMAT reacts moderately with either single or extended sulfur vacancies. ME also reacts with the vacancies, and defect-rich surfaces treated with ME provide an equally good surface for the nucleation of ALD TiO2 films. The computational studies however reveal that the creation of surface vacancies results in the introduction of gap states that may deteriorate the electronic properties of the stack. Treatment with ME results in the complete removal of the gap states originating from the most commonly found single vacancies and reduces substantially the density of states for double and line vacancies. As a result, we provide a pathway for the deposition of high-quality ALD dielectrics on the MoS2 surfaces, which is required for the successful integration of these 2D materials in functional devices.
RESUMEN
Optical cavities can enhance and control light-matter interactions. This level of control has recently been extended to the nanoscale with single emitter strong coupling even at room temperature using plasmonic nanostructures. However, emitters in static geometries, limit the ability to tune the coupling strength or to couple different emitters to the same cavity. Here, we present tip-enhanced strong coupling (TESC) with a nanocavity formed between a scanning plasmonic antenna tip and the substrate. By reversibly and dynamically addressing single quantum dots, we observe mode splitting up to 160 meV and anticrossing over a detuning range of ~100 meV, and with subnanometer precision over the deep subdiffraction-limited mode volume. Thus, TESC enables previously inaccessible control over emitter-nanocavity coupling and mode volume based on near-field microscopy. This opens pathways to induce, probe, and control single-emitter plasmon hybrid quantum states for applications from optoelectronics to quantum information science at room temperature.
RESUMEN
In this work, we studied the evolution and transport of the native oxides during the atomic layer deposition (ALD) of TiO2 on GaAs(100) from tetrakis dimethyl amino titanium and H2O. Arsenic oxide transport through the TiO2 film and removal during the ALD process was investigated using transmission Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). Experiments were designed to decouple these processes by utilizing their temperature dependence. A 4 nm TiO2 layer was initially deposited on a native oxide surface at 100 °C. Ex situ XPS confirmed that this step disturbed the interface minimally. An additional 3 nm TiO2 film was subsequently deposited at 150 to 250 °C with and without an intermediate thermal treatment step at 250 °C. Arsenic and gallium oxide removal was confirmed during this second deposition, leading to the inevitable conclusion that these oxides traversed at least 4 nm of film so as to react with the precursor and its surface reaction/decomposition byproducts. XPS measurements confirmed the relocation of both arsenic and gallium oxides from the interface to the bulk of the TiO2 film under normal processing conditions. These results explain the continuous native oxide removal observed for alkyl-amine precursor-based ALD processes on III-V surfaces and provide further insight into the mechanisms of film growth.
RESUMEN
This manuscript describes a simple process for fabricating gold-based, multi-layered, surface-enhanced Raman scattering (SERS) substrates that can be applied to a variety of different nanostructures, while still providing multi-layer enhancement factors comparable to those previously achieved only with optimized silver/silver oxide/silver substrates. In particular, gold multi-layered substrates generated by atomic layer deposition (ALD) have been fabricated and characterized in terms of their optimal performance, revealing multi-layer enhancements of 2.3-fold per spacer layer applied. These substrates were fabricated using TiO2 as the dielectric spacer material between adjacent gold layers, with ALD providing a conformal thin film with high surface coverage and low thickness. By varying the spacer layer thicknesses from sub-monolayer (non-contiguous) films through multiple TiO2 layer thick films, the non-monotonic spacer layer thickness response has been elucidated, revealing the importance of thin, contiguous dielectric spacer layers for optimal enhancement. Furthermore, the extended shelf life of these gold multi-layered substrates was characterized, demonstrating usable lifetimes (i.e. following storage in ambient conditions) of greater than five months, with the further potential for simple limited electrochemical regeneration even after this time.
RESUMEN
A thermal atomic layer deposition (ALD) process with tetrakis(dimethylamino) titanium and H2O as reagents has been used to deposit TiO2 films on native oxide and etched InAs(100) surfaces at 200 °C. TiO2 was deposited on etched InAs(100) surface without the formation of undesirable interfacial layers. X-ray photoelectron spectroscopy (XPS) data on a series of films of increasing thickness deposited on surfaces covered with native oxide has shown that the surface arsenic oxides are removed within the first 2-3 nm of film deposition. The indium oxides, however, after an initial reduction seem to persist and increase in intensity with film thickness. For a 6.4-nm-thick TiO2 film, XPS depth profile data demonstrate an accumulation of indium oxides at the TiO2 film surface. When the topmost layer of the indium/TiO2 film is removed, then a sharp interface between the TiO2 film and the InAs substrate is detected. This observation demonstrates that the surface oxides diffuse through fairly thick TiO2 films and may subsequently be removed by reaction with the precursor and amine byproducts of the ALD reaction. These findings underscore the importance of diffusion in understanding the so-called "interface clean-up" reaction and its potential impact on the fabrication of high-quality InAs and other Group III-V-based MOS devices.