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Hio-Ieng Un

Publications and source records attributed to Hio-Ieng Un.

3 recordsLinked to original sources

Controlling the growth of 2D conjugated coordination polymers to induce metallic and spin-dependent transport signatures

Understanding growth evolution and thereby implementing precise microstructural tuning of two-dimensional (2D) conjugated coordination polymers (cCPs) is crucial to achieve efficient electronic conduction towards their full potential and to observe materials' intrinsic properties. However, fundamental understanding of how 2D cCPs films grow remains very limited. Here, we use copper-benzenehexathiol (Cu-BHT) cCP as a model system to unravel the growth evolution of layered films in liquid-liquid interfacial synthesis in order to identify strategies to achieve tuning of structure-property relationships. We find that thin films formed at the early stage of growth in 20 minutes facilitate smoother, denser, and horizontally oriented films, and thereby achieve higher electrical conductivity of > 3000 S/cm with a metallic temperature dependence down to 20 K. They also reveal signatures of quantum interference mediated weak antilocalisation and Kondo-like effect in magnetotransport at low temperatures. These phenomena are not observed when long reaction time was employed. Our findings offer a new perspective for the growth of dynamically reversible self-assemblies, that is different from the traditional paradigm of longer reaction time being associated with higher ordering and performance, and offer a platform to study spin-related transport properties of these materials with higher performance for advanced electronic, thermoelectric, and potential spintronic applications.

cond-mat.mtrl-sci

Unbounded Systematic Error in Thin Film Conductivity Measurements

Electrical conductivity is the most fundamental charge transport parameter, and measurements of conductivity are a basic part of materials characterization for nearly all conducting materials. In thin films, conductivity is often measured in four bar architectures in which the current source and voltage measurement are spatially separated to eliminate systematic error due to contact resistance. Despite the apparent simplicity of these measurements, we demonstrate here that the four bar architecture is subject to significant systematic error arising from the finite conductivity of the metal electrodes. Remarkably, these systematic errors can in some cases become unbounded, producing arbitrarily high measured conductivity at modest true film conductivities, within the range relevant to emerging thin film thermoelectric materials such as conducting polymers. These unbounded errors, which can occur even in properly conducted four-point measurements of patterned films, likely explain literature reports of extremely high conductivities in conducting polymers, and can lead to anomalous scaling in temperature dependent studies, potentially leading to incorrect interpretation of the relevant charge transport mechanism. We characterize the device geometric factors that control these errors, which stand partially at odds with those required for accurate Seebeck coefficient measurements. Our analyses allow us to identify device architectures that provide small systematic errors for conductivity and Seebeck coefficient while still providing a low measurement resistance, critical to reducing noise in thermal voltage measurements. These findings provide important guidelines for accurate measurements in the growing field of thin-film thermoelectric materials.

cond-mat.mtrl-sci

Defect-tolerant electron and defect-sensitive phonon transport in quasi-2D conjugated coordination polymers

Thermoelectric materials, enabling direct waste-heat to electricity conversion, need to be highly electrically conducting while simultaneously thermally insulating. This is fundamentally challenging since electrical and thermal conduction are usually coupled. Here, we discover that quasi-2D conjugated coordination polymer films exhibit this ideal mix of antithetical properties due to coexistence of defect-tolerant charge transport and defect-sensitive heat propagation. The former is highlighted by the highest conductivities > 2000 S cm-1 with metallic temperature dependence observed in disordered films with paracrystallinity > 10%, while the latter manifests in low, temperature-activated lattice thermal conductivities (< 0.38 W m-1 K-1) originating from small-amplitude, quasi-harmonic lattice dynamics with disorder-limited lifetimes and vibrational scattering length on the order of interatomic spacing. Based on temperature-dependent thermoelectric and magnetotransport experiments we identify a two-carrier (hole-electron), ambipolar metallic transport regime as the origin of relatively small Seebeck coefficients in these materials. Our findings identify conjugated coordination polymers as attractive materials for applications in thermoelectric energy harvesting, (bio)electronics and energy storage.

cond-mat.mtrl-sci