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Mairi McCauley

Publications and source records attributed to Mairi McCauley.

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Platform and Framework for Time-Resolved Nanoscale Thermal Transport Measurements in STEM

Understanding heat transport at the nanometer scale is critical for semiconductor devices, quantum materials, and thermal management of nanostructures, yet direct local measurements of thermal conductivity and heat capacity remain scarce. We developed a laser-excitation system integrated into a scanning transmission electron microscope (STEM) for nanoscale thermal transport measurements using ultra-high-resolution electron energy-loss spectroscopy (EELS). A fiber-coupled laser is introduced via a modified aperture mechanism, enabling flexible holder geometries and large tilt angles without optical elements in the polepiece gap. Synchronization of pulsed laser excitation with an externally gated direct electron detector provides temporal resolution about 50 ns at <10 meV energy resolution. Local temperatures are determined via the principle of detailed balance, and thermal transport parameters are extracted by fitting a forward-time central-space heat diffusion model including radiative losses. For amorphous carbon films, we obtain a thermal conductivity of 1.24 $\frac{W}{m\cdot K}$ and a heat capacity of 821 $\frac{J}{kg\cdot K}$, consistent with literature. This framework enables time-resolved nanoscale measurements of thermal transport in materials and devices.

cond-mat.mtrl-sci

Tuning the Electronic States of Bi2Se3 Films with Large Spin-Orbit Interaction Using Molecular Heterojunctions

An electric bias can shift the Fermi level along the Dirac cone of a topological insulator and modify its charge transport, but tuning the electronic states and spin-orbit interaction (SOI) without destroying the surface topology is challenging. Here, we show that thin film Bi2Se3/n-p (p-n) molecular diodes form ordered interfaces where charge transfer and orbital re-hybridisation result in a decrease (increase) of the carrier density and improved mobility. In Bi2Se3 the spin-orbit lifetime, t_so, is 0.13 ps, which is comparable to the strongest spin-orbit materials. This lifetime drops further to 0.06 ps (0.09 ps) with the addition of p-n (n-p) molecular diodes, at the limit of measurable values. This strengthened spin-orbit interaction occurs even though molecules are made of light elements and increase the mean free path of the charge carriers by almost 50%, indicating changes to the Berry curvature and/or Rashba splitting around the hybridisation points. Raman spectroscopy gives evidence that the coupling effect may be controlled by optical irradiation, opening a pathway towards the design of heavy-light element hybrids with optically tunable quantum transport.

cond-mat.mtrl-sci

Control of 2D plasmons in the topological insulator Bi2Se3 with highly crystalline C60 overlayers

Topological Insulators (TIs) present an interesting materials platform for nanoscale, high frequency devices because they support high mobility, low scattering electronic transport within confined surface states. However, a robust methodology to control the properties of surface plasmons in TIs has yet to be developed. We propose that charge transfer between Bi$_2$Se$_3$ and crystalline C$_{60}$ films may provide tunable control of the two-dimensional plasmons in Bi$_2$Se$_3$. We have grown heterostructures of Bi$_2$Se$_3$/C$_{60}$ with exceptional crystallinity. Electron energy loss spectroscopy (EELS) reveals significant hybridisation of $π$ states at the interface, despite the expectation for only weak van der Waals interactions, including quenching of 2D plasmons. Momentum-resolved EELS measurements are used to probe the plasmon dispersion, with Density Functional Theory predictions providing an interpretation of results based on interfacial charge dipoles. Our measurements suggest a robust methodology for tuneable TI interfaces that can be engineered for plasmonic applications in computing, communications and sensing.

cond-mat.mes-hall