Proton Collective Quantum Tunneling Induces Anomalous Thermal Conductivity of Ice under Pressure
Open accessAbstract
Proton tunneling is believed to be nonlocal in ice, but its range has been shown to be limited to only a few molecules. Here, we measured the thermal conductivity of ice under pressure up to 50 GPa and found it increases with pressure until 20 GPa but decreases at higher pressures. We attribute this nonmonotonic thermal conductivity to the collective tunneling of protons at high pressures, supported by large-scale quantum molecular dynamics simulations. The collective tunneling loops span several picoseconds in time and are as large as nanometers in space, which match the phonon periods and wavelengths, leading to strong phonon scattering at high pressures. Our results show direct evidence of global quantum motion existing in high-pressure ice and provide a new perspective to understanding the coupling between phonon propagation and atomic tunneling.
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The 1/e2 beam radius of 30 μm in the measurement results in negligible sensitivity of TDTR signals to in-plane thermal conductivity Λ// at frequencies higher than 4 MHz.
“However, the 1/e 2 beam radius of 30 µ m in our measurement results in a negligible sensitivity of signals to Λ // at f higher than 4 MHz (see Supplemental Material [25]).”
From Boundary conditions dictate frequency dependence of thermal conductivity in silicon (2025) · cites this paper as [25]
The TDTR measurement passage (section labeled Abstract; page unavailable) mentions a sensitivity analysis but identifies metal-transducer thickness and heat capacity as the main sources of uncertainty. Searches for the 30 μm beam radius, frequencies above 4 MHz, and sensitivity to in-plane thermal conductivity found no passage addressing the claimed relationship. (LLM, conf=0.74)
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Cited by
Sorted by citations
Boundary conditions dictate frequency dependence of thermal conductivity in silicon
Liu, Y., Li, Q., Liu, F., Wang, X., & Sun, B. (2025) · Applied Physics Reviews · doi:10.1063/5.0254248 · Cited by 4 · see citing works
“WemeasuredΛ of Si and G of the Al/Si interface in as-prepared samples by TDTR [22, 23], a non-contact pump-probe technique to characterize thermal transport in a variety of materials [37–39].”
Self-citationBoundary conditions dictate frequency dependence of thermal conductivity in silicon
Liu, Y., Li, Q., Liu, F., Wang, X., & Sun, B. (2024) · arXiv · doi:10.48550/arxiv.2412.02227 · Cited by 2 · see citing works
“WemeasuredΛ of Si and G of the Al/Si interface in as-prepared samples by TDTR [22, 23], a non-contact pump-probe technique to characterize thermal transport in a variety of materials [37–39].”
Self-citation
- Authors
- Wang, Y., Luo, R., Chen, J., Zhou, X., Wang, S., Wu, J., Kang, F., Yu, K., & Sun, B.
- Affiliations
- Tsinghua–Berkeley Shenzhen Institute (CN)
- Southern University of Science and Technology (CN)
- Lawrence Berkeley National Laboratory (US)
- Corresponding author
- Wang, Yufeng
- Luo, Ripeng
- ORCID
- Venue
- Physical Review Letters
- Publisher
- American Physical Society (APS)
- Published
- 2024-06-26
- Volume
- 132
- Issue
- 26
- Pages
- 264101-264101
- ISSN
- 0031-9007 (ISSN-L)
- 1079-7114
- OpenAlex
- W4400036464
- Cited by
- 10
- References
- 1
- Citations by year
- 2026: 3 · 2025: 6 · 2024: 1
- FWCI
- 2.58
- Type
- journal article
- Language
- en
- Open access
- green
- arxiv.org
- Licence
- Locations
- Physical Review Letters (publishedVersion)
- PubMed (publishedVersion)
- arXiv (Cornell University) (submittedVersion)
- eScholarship (California Digital Library) (submittedVersion, cc-by)
- OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
- arXiv (Cornell University)
- Funders
- National Natural Science Foundation of China (52161145502, 12004211, 22103048)
- Shenzhen Science and Technology Innovation Program (RCYX20200714114643187, WDZC20200821100123001)
- Tsinghua Shenzhen International Graduate School (QD2021008N, JC2021008, HW2020009)
- U.S. Department of Energy (DE-AC02-05-CH11231)
- Office of Science
- Basic Energy Sciences
- Division of Materials Sciences and Engineering
- Israel Science Foundation
- Topics
- Physical Sciences › Earth and Planetary Sciences › Geophysics › High-pressure geophysics and materials
- Physical Sciences › Materials Science › Materials Chemistry › Material Dynamics and Properties
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Quantum, superfluid, helium dynamics
- Keywords
- proton tunneling, ice, thermal conductivity, high pressure, phonon scattering, quantum molecular dynamics, high-pressure ice
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