To deposit an ultrathin dielectric onto WSe2, monolayer titanyl phthalocyanine (TiOPc) is deposited by molecular beam epitaxy as a seed layer for atomic layer deposition (ALD) of Al2O3 on WSe2. TiOPc molecules are arranged in a flat monolayer with 4-fold symmetry as measured by scanning tunneling microscopy. ALD pulses of trimethyl aluminum and H2O nucleate on the TiOPc, resulting in a uniform deposition of Al2O3, as confirmed by atomic force microscopy and cross-sectional transmission electron microscopy. The field-effect transistors (FETs) formed using this process have a leakage current of 0.046 pA/μm(2) at 1 V gate bias with 3.0 nm equivalent oxide thickness, which is a lower leakage current than prior reports. The n-branch of the FET yielded a subthreshold swing of 80 mV/decade.
Ambient NO2 adsorption onto copper(II) phthalocyanine (CuPc) monolayers is observed using ultrahigh vacuum (UHV) scanning tunneling microscopy (STM) to elucidate the molecular sensing mechanism in CuPc chemical vapor sensors. For low doses (1 ppm for 5 min) of NO2 at ambient temperatures, isolated chemisorption sites on the CuPc metal centers are observed in STM images. These chemisorbates almost completely desorb from the CuPc monolayer after annealing at 100 °C for 30 min. Conversely, for high NO2 doses (10 ppm for 5 min), the NO2 induces a fracture of the CuPc domains. This domain fracture can only be reversed by annealing above 150 °C, which is consistent with dissociative chemisorption into NO and atomic O accompanied by surface restructuring. This high stability implies that the domain fracture results from tightly bound adsorbates, such as atomic O. Existence of atomic O on or under the CuPc layer, which results in domain fracture, is revealed by XPS analysis and ozone-dosing experiments. The observed CuPc domain fracturing is consistent with a mechanism for the dosimetric sensing of NO2 and other reactive gases by CuPc organic thin film transistors (OTFTs).
To fabricate practical devices based on semiconducting two-dimensional (2D) materials, the source, channel, and drain materials are exposed to ambient air. However, the response of layered 2D materials to air has not been fully elucidated at the molecular level. In the present report, the effects of air exposure on transition metal dichalcogenides (TMD) and metal dichalcogenides (MD) are studied using ultrahigh-vacuum scanning tunneling microscopy (STM). The effects of a 1-day ambient air exposure on MBE-grown WSe, chemical vapor deposition (CVD)-grown MoS, and MBE SnSe are compared. Both MBE-grown WSe and CVD-grown MoS display a selective air exposure response at the step edges, consistent with oxidation on WSe and adsorption of hydrocarbon on MoS, while the terraces and domain/grain boundaries of both TMDs are nearly inert to ambient air. Conversely, MBE-grown SnSe, an MD, is not stable in ambient air. After exposure in ambient air for 1 day, the entire surface of SnSe is decomposed to SnO and SeO, as seen with X-ray photoelectron spectroscopy. Since the oxidation enthalpy of all three materials is similar, the data is consistent with greater oxidation of SnSe being driven by the weak bonding of SnSe.
Current logic devices rely on 3D architectures, such as the tri-gate field effect transistor (finFET), which utilize the (001) and (110) crystal faces simultaneously thus requiring passivation methods for the (110) face in order to ensure a pristine 3D surface prior to further processing. Scanning tunneling microscopy (STM), x-ray photoelectron spectroscopy (XPS), and correlated electrical measurement on MOSCAPs were utilized to compare the effects of a previously developed in situ pre-atomic layer deposition (ALD) surface clean on the InGaAs (001) and (110) surfaces. Ex situ wet cleans are very effective on the (001) surface but not the (110) surface. Capacitance voltage indicated the (001) surface with no buffered oxide etch had a higher C(max) hypothesized to be a result of poor nucleation of HfO2 on the native oxide. An in situ pre-ALD surface clean employing both atomic H and trimethylaluminum (TMA) pre-pulsing, developed by Chobpattana et al. and Carter et al. for the (001) surface, was demonstrated to be effective on the (110) surface for producing low D(it) high C(ox) MOSCAPs. Including TMA in the pre-ALD surface clean resulted in reduction of the magnitude of the interface state capacitance. The XPS studies show the role of atomic H pre-pulsing is to remove both carbon and oxygen while STM shows the role of TMA pre-pulsing is to eliminate H induced etching. Devices fabricated at 120 °C and 300 °C were compared.
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