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Megan Cowie

Publications and source records attributed to Megan Cowie.

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Towards Atom-by-Atom Fabrication: Mechanosynthetic donation and abstraction

Enabled by inverted-mode scanning tunneling microscopy (IM-STM) and the use of functionalized molecular tools, we demonstrate positionally-controlled mechanosynthetic addition (donation) of carbon and subtraction (abstraction) of silicon atoms on a model build site: atomically clean and crystalline Si(100). The resulting structures represent the first demonstrations of an emerging ability to manipulate radical chemistry with positional control of specific atoms and moieties in 3D. Furthermore, by comparing the behavior of molecular tools designed for atomic donation versus abstraction, we highlight general principles governing molecular tool design for selective and reliable mechanosynthetic functionality.

cond-mat.mtrl-sci

Atomically precise mechanosynthesis of carbon structures on hydrogenated Si(100) by inverted-mode STM

The ability to build atomically precise structures on surfaces with complete control over both atomic placement and chemical bonding remains a central challenge in nanoscale fabrication. Here, we demonstrate simultaneous spatial and chemical control over the mechanosynthetic fabrication of carbon structures. Using inverted-mode STM, C$_2$ units are donated from surface-deposited molecules to pre-patterned reactive sites on a hydrogen-passivated Si(100) surface. We demonstrate single-site C$_2$ donation, spatially patterned multi-site C$_2$ donation, and the stepwise assembly of polyyne structures through successive C-C bond formation. Together, these results establish controlled mechanosynthetic donation as a foundational capability for programmable atomically precise fabrication.

cond-mat.mtrl-sci

Inverted-Mode Scanning Tunneling Microscopy for Atomically Precise Fabrication

Scanning Tunneling Microscopy (STM) enables fabrication of atomically precise structures with unique properties and growing technological potential. However, reproducible manipulation of covalently bonded atoms requires control over the atomic configuration of both sample and probe - a longstanding challenge in STM. Here, we introduce inverted-mode STM, an approach that enables mechanically controlled chemical reactions for atomically precise fabrication. Tailored molecules on a Si(100) surface image the probe apex, and the usual challenge of understanding the probe structure is effectively solved. The molecules can also react with the probe, with the two sides of the tunnel junction acting as reagents positioned with sub-angstrom precision. This allows abstraction or donation of atoms from or to the probe apex. We demonstrate this by using a novel alkynyl-terminated molecule to reproducibly abstract hydrogen atoms from the probe. The approach is expected to extend to other elements and moieties, opening a new avenue for scalable atomically precise fabrication.

cond-mat.mes-hall

Spatially resolved dielectric loss at the Si/SiO$_2$ interface

The Si/SiO$_2$ interface is populated by isolated trap states which modify its electronic properties. These traps are of critical interest for the development of semiconductor-based quantum sensors and computers, as well as nanoelectronic devices. Here, we study the electric susceptibility of the Si/SiO$_2$ interface with nm spatial resolution using frequency-modulated atomic force microscopy to measure a patterned dopant delta-layer buried 2 nm beneath the silicon native oxide interface. We show that surface charge organization timescales, which range from 1-150 ns, increase significantly around interfacial states. We conclude that dielectric loss under time-varying gate biases at MHz and sub-MHz frequencies in metal-insulator-semiconductor capacitor device architectures is highly spatially heterogeneous over nm length scales. Supplemental GIFs can be found at https://doi.org/10.6084/m9.figshare.25546687

cond-mat.mtrl-sci

Spatially resolved random telegraph fluctuations of a single trap at the Si/SiO2 interface

We use electrostatic force microscopy to spatially resolve random telegraph noise at the Si/SiO$_2$ interface. Our measurements demonstrate that two-state fluctuations are localized at interfacial traps, with bias-dependent rates and amplitudes. These two-level systems lead to correlated carrier number and mobility fluctuations with a range of characteristic timescales; taken together as an ensemble, they give rise to a $1/f$ power spectral trend. Such individual defect fluctuations at the Si/SiO$_2$ interface impair the performance and reliability of nanoscale semiconductor devices, and will be a significant source of noise in semiconductor-based quantum sensors and computers. The fluctuations measured here are associated with a four-fold competition of rates, including slow two-state switching on the order of seconds and, in one state, fast switching on the order of nanoseconds which is associated with energy loss.

cond-mat.mes-hall

Single-dopant band bending fluctuations in MoSe$_2$ measured with electrostatic force microscopy

In this work, we experimentally demonstrate two-state fluctuations in a metal-insulator-semiconductor (MIS) device formed out of a metallic atomic force microscopy tip, vacuum gap, and multilayer MoSe$_2$ sample. We show that noise in this device is intrinsically bias-dependent due to the bias-dependent surface potential, and does not require that the frequency or magnitude of individual dopant fluctuations are themselves bias-dependent. Finally, we measure spatial nonhomogeneities in band bending (charge reorganization) timescales.

cond-mat.mes-hall

How high is a MoSe$_2$ monolayer?

Transition metal dichalcogenides (TMDCs) have attracted significant attention for optoelectronic, photovoltaic and photoelectrochemical applications. The properties of TMDCs are highly dependent on the number of stacked atomic layers, which is usually counted post-fabrication, using a combination of optical methods and atomic force microscopy (AFM) height measurements. Here, we use photoluminescence spectroscopy and three different AFM methods to demonstrate significant discrepancies in height measurements of exfoliated MoSe$_2$ flakes on SiO$_2$ depending on the method used. We highlight that overlooking effects from electrostatic forces, contaminants and surface binding can be misleading when measuring the height of a MoSe$_2$ flake. These factors must be taken into account as a part of the protocol for counting TMDC layers.

physics.app-ph

Charge carrier inversion in a doped thin film organic semiconductor island

Inducing an inversion layer in organic semiconductors is a highly nontrivial, but critical, achievement for producing organic field-effect transistor (OFET) devices, which rely on the generation of inversion, accumulation, and depletion regimes for successful operation. In recent years, a major milestone was reached: an OFET was made to successfully operate in the inversion-mode for the first time. Here, we develop a pulsed bias technique to characterize the dopant type of any organic material system, without prior knowledge or characterization of the material in question. We use this technique on a pentacene/PTCDI heterostructure and thus deduce that pentacene is n-doped by impurities. Additionally, through tip-induced band-bending, we generate inversion, depletion, and accumulation regimes over a 20~nm radius, three monolayer thick n-doped pentacene island. Our findings demonstrate that nanometer-scale lateral extent and thickness are sufficient for an OFET device to operate in the inversion regime.

cond-mat.mes-hall