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The ability to actively regulate heat flow at the nanoscale could be a game changer for applications in thermal management and energy harvesting. Such a breakthrough could also enable the control of heat flow using thermal circuits, in a manner analogous to electronic circuits. Here we demonstrate switchable thermal transistors with an order of magnitude thermal on/off ratio, based on reversible electrochemical lithium intercalation in MoS₂thin films. We use spatially-resolved time-domain thermoreflectance to map the lithium ion distribution during device operation, and atomic force microscopy to show that the lithiated state correlates with increased thickness and surface roughness. First principles calculations reveal that the thermal conductance modulation is due to phonon scattering by lithium rattler modes,c-axis strain, and stacking disorder. This study lays the foundation for electrochemically-driven nanoscale thermal regulators, and establishes thermal metrology as a useful probe of spatio-temporal intercalant dynamics in nanomaterials.

Transmission electron microscopy (TEM) is arguably the most important tool for atomic‐scale material characterization. A significant portion of the energy of transmitted electrons is transferred to the material under study through inelastic scattering, causing inadvertent damage via ionization, radiolysis, and heating. In particular, heat generation complicates TEM observations as the local temperature can affect material properties. Here, the heat generation due to electron irradiation is quantified using both top‐down and bottom‐up approaches: direct temperature measurements using nanowatt calorimeters as well as the quantification of energy loss due to inelastic scattering events using electron energy loss spectroscopy. Combining both techniques, a microscopic model is developed for beam‐induced heating and to identify the primary electron‐to‐heat conversion mechanism to be associated with valence electrons. Building on these results, the model provides guidelines to estimate temperature rise for general materials with reasonable accuracy. This study extends the ability to quantify thermal impact on materials down to the atomic scale.

Polymer‐based materials hold great potential for use in thermoelectric applications but are limited by their poor electrical properties. Through a combination of solution‐shearing deposition and directionally applied solvent treatments, poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) thin films with metallic‐like conductivities can be obtained with high power factors in excess of 800 µW m⁻¹K⁻². X‐ray scattering and absorption data indicate that structural alignment of PEDOT chains and larger‐sized domains are responsible for the enhanced electrical conductivity. It is expected that further enhancements to the power factor can be obtained through device geometry and postdeposition solvent shearing optimization.

Understanding the pathways and time scales underlying electrically driven insulator-metal transitions is crucial for uncovering the fundamental limits of device operation. Using stroboscopic electron diffraction, we perform synchronized time-resolved measurements of atomic motions and electronic transport in operating vanadium dioxide (VO₂) switches. We discover an electrically triggered, isostructural state that forms transiently on microsecond time scales, which is shown by phase-field simulations to be stabilized by local heterogeneities and interfacial interactions between the equilibrium phases. This metastable phase is similar to that formed under photoexcitation within picoseconds, suggesting a universal transformation pathway. Our results establish electrical excitation as a route for uncovering nonequilibrium and metastable phases in correlated materials, opening avenues for engineering dynamical behavior in nanoelectronics.

Understanding the fundamentals of nanoscale heat propagation is crucial for next‐generation electronics. For instance, weak van der Waals bonds of layered materials are known to limit their thermal boundary conductance (TBC), presenting a heat dissipation bottleneck. Here, a new nondestructive method is presented to probe heat transport in nanoscale crystalline materials using time‐resolved X‐ray measurements of photoinduced thermal strain. This technique directly monitors time‐dependent temperature changes in the crystal and the subsequent relaxation across buried interfaces by measuring changes in thec‐axis lattice spacing after optical excitation. Films of five different layered transition metal dichalcogenides MoX₂[X = S, Se, and Te] and WX₂[X = S and Se] as well as graphite and a W‐doped alloy of MoTe₂are investigated. TBC values in the range 10–30 MW m⁻²K⁻¹are found, onc‐plane sapphire substrates at room temperature. In conjunction with molecular dynamics simulations, it is shown that the high thermal resistances are a consequence of weak interfacial van der Waals bonding and low phonon irradiance. This work paves the way for an improved understanding of thermal bottlenecks in emerging 3D heterogeneously integrated technologies.

On‐chip dynamic strain engineering requires efficient micro‐actuators that can generate large in‐plane strains. Inorganic electrochemical actuators are unique in that they are driven by low voltages (≈1 V) and produce considerable strains (≈1%). However, actuation speed and efficiency are limited by mass transport of ions. Minimizing the number of ions required to actuate is thus key to enabling useful “straintronic” devices. Here, it is shown that the electrochemical intercalation of exceptionally few lithium ions into WTe₂causes large anisotropic in‐plane strain: 5% in one in‐plane direction and 0.1% in the other. This efficient stretching of the 2D WTe₂layers contrasts to intercalation‐induced strains in related materials which are predominantly in the out‐of‐plane direction. The unusual actuation of Li_xWTe₂is linked to the formation of a newly discovered crystallographic phase, referred to as Td', with an exotic atomic arrangement. On‐chip low‐voltage (<0.2 V) control is demonstrated over the transition to the novel phase and its composition. Within the Td'‐Li_0.5−δWTe₂phase, a uniaxial in‐plane strain of 1.4% is achieved with a change of δ of only 0.075. This makes the in‐plane chemical expansion coefficient of Td'‐Li_0.5−δWTe₂far greater than of any other single‐phase material, enabling fast and efficient planar electrochemical actuation.