Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 116, Issue 35, Pages 17163-17168Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1905492116
Keywords
polymers; polyethylene; thermal conductivity; mean free path; ballistic transport
Categories
Funding
- Office of Naval Research Young Investigator Award [N00014-15-1-2688]
- Engineering and Physical Sciences Research Council [EP/K034405/1]
- EPSRC [EP/K034405/1] Funding Source: UKRI
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Thermally conductive polymer crystals are of both fundamental and practical interest for their high thermal conductivity that exceeds that of many metals. In particular, polyethylene fibers and oriented films with uniaxial thermal conductivity exceeding 50 W.m(-1).K-1 have been reported recently, stimulating interest into the underlying microscopic thermal transport processes. While ab initio calculations have provided insight into microscopic phonon properties for perfect crystals, such properties of actual samples have remained experimentally inaccessible. Here, we report the direct observation of thermal phonons with mean free paths up to 200 nm in semicrystalline polyethylene films using transient grating spectroscopy. Many of the mean free paths substantially exceed the crystalline domain sizes measured using small-angle X-ray scattering, indicating that thermal phonons propagate ballistically within and across the nanocrystalline domains; those transmitting across domain boundaries contribute nearly one-third of the thermal conductivity. Our work provides a direct determination of thermal phonon propagation lengths in molecular solids, yielding insights into the microscopic origins of their high thermal conductivity.
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