Structural and Elastic Properties of Empty-Pore Metalattices Extracted via Nondestructive Coherent Extreme UV Scatterometry and Electron Tomography.

Semiconductor metalattices consisting of a linked network of three-dimensional nanostructures with periodicities on a length scale <100 nm can enable tailored functional properties due to their complex nanostructuring. For example, by controlling both the porosity and pore size, thermal transport in these phononic metalattices can be tuned, making them promising candidates for efficient thermoelectrics or thermal rectifiers. Thus, the ability to characterize the porosity, and other physical properties, of metalattices is critical but challenging, due to their nanoscale structure and thickness. To date, only metalattices with high porosities, close to the close-packing fraction of hard spheres, have been studied experimentally. Here, we characterize the porosity, thickness, and elastic properties of a low-porosity, empty-pore silicon metalattice film (∼500 nm thickness) with periodic spherical pores (∼tens of nanometers), for the first time. We use laser-driven nanoscale surface acoustic waves probed by extreme ultraviolet scatterometry to nondestructively measure the acoustic dispersion in these thin silicon metalattice layers. By comparing the data to finite element models of the metalattice sample, we can extract Young's modulus and porosity. Moreover, by controlling the acoustic wave penetration depth, we can also determine the metalattice layer thickness and verify the substrate properties. Additionally, we utilize electron tomography images of the metalattice to verify the geometry and validate the porosity extracted from scatterometry. These advanced characterization techniques are critical for informed and iterative fabrication of energy-efficient devices based on nanostructured metamaterials.

Directional thermal channeling: A phenomenon triggered by tight packing of heat sources.

Understanding nanoscale thermal transport is critical for nano-engineered devices such as quantum sensors, thermoelectrics, and nanoelectronics. However, despite overwhelming experimental evidence for nondiffusive heat dissipation from nanoscale heat sources, the underlying mechanisms are still not understood. In this work, we show that for nanoscale heat source spacings that are below the mean free path of the dominant phonons in a substrate, close packing of the heat sources increases in-plane scattering and enhances cross-plane thermal conduction. This leads to directional channeling of thermal transport-a novel phenomenon. By using advanced atomic-level simulations to accurately access the lattice temperature and the phonon scattering and transport properties, we finally explain the counterintuitive experimental observations of enhanced cooling for close-packed heat sources. This represents a distinct fundamental behavior in materials science with far-reaching implications for electronics and future quantum devices.

A General and Predictive Understanding of Thermal Transport from 1D- and 2D-Confined Nanostructures: Theory and Experiment.

Heat management is crucial in the design of nanoscale devices as the operating temperature determines their efficiency and lifetime. Past experimental and theoretical works exploring nanoscale heat transport in semiconductors addressed known deviations from Fourier's law modeling by including effective parameters, such as a size-dependent thermal conductivity. However, recent experiments have qualitatively shown behavior that cannot be modeled in this way. Here, we combine advanced experiment and theory to show that the cooling of 1D- and 2D-confined nanoscale hot spots on silicon can be described using a general hydrodynamic heat transport model, contrary to previous understanding of heat flow in bulk silicon. We use a comprehensive set of extreme ultraviolet scatterometry measurements of nondiffusive transport from transiently heated nanolines and nanodots to validate and generalize our ab initio model, that does not need any geometry-dependent fitting parameters. This allows us to uncover the existence of two distinct time scales and heat transport mechanisms: an interface resistance regime that dominates on short time scales and a hydrodynamic-like phonon transport regime that dominates on longer time scales. Moreover, our model can predict the full thermomechanical response on nanometer length scales and picosecond time scales for arbitrary geometries, providing an advanced practical tool for thermal management of nanoscale technologies. Furthermore, we derive analytical expressions for the transport time scales, valid for a subset of geometries, supplying a route for optimizing heat dissipation.

Nondestructive Measurements of the Mechanical and Structural Properties of Nanostructured Metalattices.

Metalattices are artificial 3D solids, periodic on sub-100 nm length scales, that enable the functional properties of materials to be tuned. However, because of their complex structure, predicting and characterizing their properties is challenging. Here we demonstrate the first nondestructive measurements of the mechanical and structural properties of metalattices with feature sizes down to 14 nm. By monitoring the time-dependent diffraction of short wavelength light from laser-excited acoustic waves in the metalattices, we extract their acoustic dispersion, Young's modulus, filling fraction, and thicknesses. Our measurements are in excellent agreement with macroscopic predictions and potentially destructive techniques such as nanoindentation and scanning electron microscopy, with increased accuracy over larger areas. This is interesting because the transport properties of these metalattices do not obey bulk predictions. Finally, this approach is the only way to validate the filling fraction of metalattices over macroscopic areas. These combined capabilities can enable accurate synthesis of nanoenhanced materials.

Full-field imaging of thermal and acoustic dynamics in an individual nanostructure using tabletop high harmonic beams.

Imaging charge, spin, and energy flow in materials is a current grand challenge that is relevant to a host of nanoenhanced systems, including thermoelectric, photovoltaic, electronic, and spin devices. Ultrafast coherent x-ray sources enable functional imaging on nanometer length and femtosecond timescales particularly when combined with advances in coherent imaging techniques. Here, we combine ptychographic coherent diffractive imaging with an extreme ultraviolet high harmonic light source to directly visualize the complex thermal and acoustic response of an individual nanoscale antenna after impulsive heating by a femtosecond laser. We directly image the deformations induced in both the nickel tapered nanoantenna and the silicon substrate and see the lowest-order generalized Lamb wave that is partially confined to a uniform nanoantenna. The resolution achieved-sub-100 nm transverse and 0.5-Å axial spatial resolution, combined with ≈10-fs temporal resolution-represents a significant advance in full-field dynamic imaging capabilities. The tapered nanoantenna is sufficiently complex that a full simulation of the dynamic response would require enormous computational power. We therefore use our data to benchmark approximate models and achieve excellent agreement between theory and experiment. In the future, this work will enable three-dimensional functional imaging of opaque materials and nanostructures that are sufficiently complex that their functional properties cannot be predicted.

Full Characterization of the Mechanical Properties of 11-50 nm Ultrathin Films: Influence of Network Connectivity on the Poisson's Ratio.

Precise characterization of the mechanical properties of ultrathin films is of paramount importance for both a fundamental understanding of nanoscale materials and for continued scaling and improvement of nanotechnology. In this work, we use coherent extreme ultraviolet beams to characterize the full elastic tensor of isotropic ultrathin films down to 11 nm in thickness. We simultaneously extract the Young's modulus and Poisson's ratio of low-k a-SiC:H films with varying degrees of hardness and average network connectivity in a single measurement. Contrary to past assumptions, we find that the Poisson's ratio of such films is not constant but rather can significantly increase from 0.25 to >0.4 for a network connectivity below a critical value of ∼2.5. Physically, the strong hydrogenation required to decrease the dielectric constant k results in bond breaking, lowering the network connectivity, and Young's modulus of the material but also decreases the compressibility of the film. This new understanding of ultrathin films demonstrates that coherent EUV beams present a new nanometrology capability that can probe a wide range of novel complex materials not accessible using traditional approaches.

Nondestructive Measurement of the Evolution of Layer-Specific Mechanical Properties in Sub-10 nm Bilayer Films.

We use short wavelength extreme ultraviolet light to independently measure the mechanical properties of disparate layers within a bilayer film for the first time, with single-monolayer sensitivity. We show that in Ni/Ta nanostructured systems, while their density ratio is not meaningfully changed from that expected in bulk, their elastic properties are significantly modified, where nickel softens while tantalum stiffens, relative to their bulk counterparts. In particular, the presence or absence of the Ta capping layer influences the mechanical properties of the Ni film. This nondestructive nanomechanical measurement technique represents the first approach to date able to distinguish the properties of composite materials well below 100 nm in thickness. This capability is critical for understanding and optimizing the strength, flexibility and reliability of materials in a host of nanostructured electronic, photovoltaic, and thermoelectric devices.

A new regime of nanoscale thermal transport: Collective diffusion increases dissipation efficiency.

Understanding thermal transport from nanoscale heat sources is important for a fundamental description of energy flow in materials, as well as for many technological applications including thermal management in nanoelectronics and optoelectronics, thermoelectric devices, nanoenhanced photovoltaics, and nanoparticle-mediated thermal therapies. Thermal transport at the nanoscale is fundamentally different from that at the macroscale and is determined by the distribution of carrier mean free paths and energy dispersion in a material, the length scales of the heat sources, and the distance over which heat is transported. Past work has shown that Fourier's law for heat conduction dramatically overpredicts the rate of heat dissipation from heat sources with dimensions smaller than the mean free path of the dominant heat-carrying phonons. In this work, we uncover a new regime of nanoscale thermal transport that dominates when the separation between nanoscale heat sources is small compared with the dominant phonon mean free paths. Surprisingly, the interaction of phonons originating from neighboring heat sources enables more efficient diffusive-like heat dissipation, even from nanoscale heat sources much smaller than the dominant phonon mean free paths. This finding suggests that thermal management in nanoscale systems including integrated circuits might not be as challenging as previously projected. Finally, we demonstrate a unique capability to extract differential conductivity as a function of phonon mean free path in materials, allowing the first (to our knowledge) experimental validation of predictions from the recently developed first-principles calculations.