Date of Award

Spring 1-1-2017

Document Type

Dissertation

Degree Name

Doctor of Philosophy (PhD)

Department

Physics

First Advisor

Margaret M. Murnane

Second Advisor

Henry C. Kapteyn

Third Advisor

Mahmoud Hussein

Fourth Advisor

Minhyea Lee

Fifth Advisor

Ronggui Yang

Abstract

Advances in nanofabrication have pushed the characteristic dimensions of nanosystems well below 100nm, where physical properties are often significantly different from their bulk counterparts, and accurate models are lacking. Critical technologies such as thermoelectrics for energy harvesting, nanoparticle-mediated thermal therapy, nano-enhanced photovoltaics, and efficient thermal management in integrated circuits depend on our increased understanding of the nanoscale. However, traditional microscopic characterization tools face fundamental limits at the nanoscale. Theoretical efforts to build a fundamental picture of nanoscale thermal dynamics lack experimental validation and still struggle to account for newly reported behaviors. Moreover, precise characterization of the elastic behavior of nanostructured systems is needed for understanding the unique physics that become apparent in small-scale systems, such as thickness-dependent or fabrication-dependent elastic properties. In essence, our ability to fabricate nanosystems has outstripped our ability to understand and characterize them.

In my PhD thesis, I present the development and refinement of coherent extreme ultraviolet (EUV) nanometrology, a novel tool used to probe material properties at the intrinsic time- and length-scales of nanoscale dynamics. By extending ultrafast photoacoustic and thermal metrology techniques to very short probing wavelengths using tabletop coherent EUV beams from high-harmonic upconversion (HHG) of femtosecond lasers, coherent EUV nanometrology allows for a new window into nanoscale physics, previously unavailable with traditional techniques. Using this technique, I was able to probe both thermal and acoustic dynamics in nanostructured systems with characteristic dimensions below 50nm with high temporal (sub-ps) and spatial (<10pm vertical) resolution, including the smallest heat sources probed (20nm) and thinnest film (10.9nm) fully mechanically characterized to date.

By probing nanoscale thermal transport (i.e. cooling) of periodic hot nanostructures down to 20nm in characteristic dimension in both 1D (nanolines) and 2D (nanocubes) geometries, I uncovered a new surprising regime of nanoscale thermal transport called the "collectively-diffusive regime". In this regime, nanoscale hot spots cool faster when placed closer together than when farther apart. This is a consequence of the interplay between both the size and spacing of the nanoscale heat sources with the phonon spectrum of a material. This makes our technique one of the only experimental routes to directly probe the dynamics of phonons in complex materials, which is critical to both technological applications and fundamental condensed matter physics. I developed a proof of concept model and used it to extract the first experimental differential conductivity phonon mean free path (MFP) spectra for silicon and sapphire, which compare well with first-principles calculations. However, a complete picture of the physics is still elusive. Thus, I developed a computational solver for the phonon Boltzmann transport equation in realistic experimental geometries. Using this approach, I successfully found confirmation of the influence of the period in thermal transport from periodic heat sources: a smaller periodicity can enhance the heat dissipation efficiency. This result is qualitatively consistent with the results of the "collectively-diffusive regime", but more work is needed for a full theoretical quantitative picture of the experimental results.

In other work, I used coherent EUV nanometrology to simultaneously measure, in a non-contact and non-destructive way, Young's modulus and, for the first time, Poisson's ratio of ultra-thin films. I successfully extracted the full elastic tensor of the thinnest films to date (10.9nm). Moreover, by using our technique on a series of low-k dielectric sub-100nm SiC:H films, I uncovered an unexpected transition from compressible

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