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<p>Thermal transport through molecules has been exceptionally difficult to measure robustly. This is despite many intriguing theoretical predictions such as thermal diodes or gated thermal conduction, with consequent useful applications. Here, we present a significant development in time-resolved photothermal measurements using the extreme plasmonic enhancement of light inside molecular nanogaps to follow thermal transport on the nanoscale. We exploit free-standing sheets of close-packed nanoparticles, which are locally heated using mid-infrared pulses, and track their cooling by lateral transport on microsecond timescales. The rate of thermal relaxation is found to be dependent on nanogap composition, measured for a series of thiolated aromatic molecules. Observed trends in thermal conductivity with molecular length and contact strength are broadly reproduced by non-equilibrium molecular dynamics simulations. However, we find additional consideration of molecular interactions and dynamic disorder are crucial in fully understanding our experimental findings.</p>

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Thermal transport through molecular monolayers in plasmonic nanogaps

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年5月22日

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  • Fiona Bell,
  • Erfan Norouzi Farahani,
  • Yeeun Roh,
  • Sara Sangtarash,
  • Zhenyao Jiang,
  • Hatef Sadeghi,
  • Jeremy J. Baumberg

摘要

Thermal transport through molecules has been exceptionally difficult to measure robustly. This is despite many intriguing theoretical predictions such as thermal diodes or gated thermal conduction, with consequent useful applications. Here, we present a significant development in time-resolved photothermal measurements using the extreme plasmonic enhancement of light inside molecular nanogaps to follow thermal transport on the nanoscale. We exploit free-standing sheets of close-packed nanoparticles, which are locally heated using mid-infrared pulses, and track their cooling by lateral transport on microsecond timescales. The rate of thermal relaxation is found to be dependent on nanogap composition, measured for a series of thiolated aromatic molecules. Observed trends in thermal conductivity with molecular length and contact strength are broadly reproduced by non-equilibrium molecular dynamics simulations. However, we find additional consideration of molecular interactions and dynamic disorder are crucial in fully understanding our experimental findings.