Kathleen Hoogeboom-Pot

A New Regime of Nanoscale Thermal Transport: Collective Diffusion Increases Dissipation Efficiency

Significance A complete description of nanoscale thermal transport is a fundamental problem that has defied understanding for many decades. Here, we uncover a surprising new regime of nanoscale thermal transport where, counterintuitively, nanoscale heat sources cool more quickly when placed close together than when they are widely separated. This increased cooling efficiency is possible when the separation between nanoscale heat sources is comparable to the average mean free paths of the dominant heat-carrying phonons. This finding suggests new approaches for addressing the significant challenge of thermal management in nanosystems, with design implications for integrated circuits, thermoelectric devices, nanoparticle-mediated thermal therapies, and nanoenhanced photovoltaics for improving clean-energy technologies. 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.

Probing limits of acoustic nanometrology using coherent extreme ultraviolet light

Photoacoustic nanometrology using coherent extreme ultraviolet (EUV) light detection is a unique and powerful tool for probing ultrathin films with a wide range of mechanical properties and thicknesses well under 100 nm. In this technique, short wavelength acoustic waves are generated through laser excitation of a nano-patterned metallic grating, and then probed by diffracting coherent EUV beams from the dynamic surface deformation. Both longitudinal and surface acoustic waves within thin films and metallic nanostructures can be observed using EUV light as a phase-sensitive probe. The use of nanostructured metal transducers enables the generation of particularly short wavelength surface acoustic waves, which truly confine the measurement within the ultrathin film layer of interest, to thicknesses < 50 nm for the first time. Simultaneous measurement of longitudinal and transverse surface wave velocities yields both the Young’s modulus and Poisson’s ratio of the film. In the future, this approach will make possible precise mechanical characterization of nanostructured systems at sub-10 nm length scales.

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.

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 Youngs modulus and Poissons 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 Poissons 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 Youngs 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.

Characterization of ultrathin films by laser-induced sub-picosecond photoacoustics with coherent extreme ultraviolet detection

Photoacoustic spectroscopy is a powerful tool for characterizing thin films. In this paper we demonstrate a new photoacoustic technique that allows us to precisely characterize the mechanical properties of ultrathin films. We focus an ultrafast laser onto a nano-patterned thin film sample, launching both surface acoustic waves (SAWs) and longitudinal acoustic waves (LAWs). Coherent extreme ultraviolet pulses are then used to probe the propagation dynamics of both the SAWs and LAWs. The resulting photoacoustic signal on both short (picosecond) and long (nanosecond) time scales yields important information. In the first 100ps, a fast oscillation followed by an echo signal corresponds to LAWs traveling inside the nanostructures and the thin film, from which the LAW velocities in the two materials can be extracted. On longer time-scales, SAW oscillations are observed. By combining the measured SAW frequency with the wavelength (determined by the nanostructure period) the SAW velocity can be accurately determined, even for very short wavelength surface acoustic waves with very small penetration depths. Using this technique, the elastic properties, including the Youngs modulus and Poisson ratio for the thin film, can be obtained in a single measurement, this technique can be extended to sub-10nm thin films.

Reliable characterization of materials and nanostructured systems <<50nm using coherent EUV beams

Coherent extreme ultraviolet beams from tabletop high harmonic generation offer revolutionary capabilities for observing nanoscale systems on their intrinsic length and time scales. By launching and monitoring acoustic waves in such systems, we fully characterize sub-10nm films and find that the Poisson’s ratio of low-k dielectric materials does not stay constant as often assumed, but increases when bond coordination is bellow a critical value. Within the same measurement, by following the heat dissipation dynamics from nano-gratings of width 20-1000nm and different periodicities, we confirm the effects of the newly identified collectively-diffusive regime, where close-spaced nanowires cool faster than widely-spaced ones.

Mechanical and thermal properties of nanomaterials at sub-50nm dimensions characterized using coherent EUV beams

Coherent extreme ultraviolet beams from tabletop high harmonic generation offer several revolutionary capabilities for observing nanoscale systems on their intrinsic length and time scales. By launching and monitoring hypersonic acoustic waves in such systems, we characterize the mechanical properties of sub-10nm layers and find that the material densities remain close to their bulk values while their elastic properties are significantly modified. Moreover, within the same measurement, by following the heat dissipation dynamics from 30-750nm-wide nanowires, we uncover a new thermal transport regime in which closely-spaced nanoscale heat sources can surprisingly cool more efficiently than widelyspaced heat sources of the same size.