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Quantum and Phonon Interference-Enhanced Molecular-Scale Thermoelectricity.

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We enhanced thermoelectric performance in molecular junctions by suppressing heat transport and boosting electrical properties. This strategy significantly improves the thermoelectric figure of merit (ZT) for waste heat energy conversion.

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Area of Science:

  • Nanoscale science and engineering
  • Materials science
  • Condensed matter physics

Background:

  • High-performance thermoelectric materials are crucial for waste heat energy conversion.
  • Simultaneous control of electron and phonon transport in molecular junctions is key.
  • Existing molecular junctions show limited thermoelectric efficiency.

Purpose of the Study:

  • To systematically improve the room-temperature thermoelectric figure of merit (ZT) of molecular junctions.
  • To achieve this by engineering both thermal and electrical transport properties.
  • To explore the potential of functionalized organic molecules for thermoelectric applications.

Main Methods:

  • Utilized dinitro functionalization to modify oligo(phenylene-ethynylene) (OPE2), biphenyl-dithiol (BDT), and bipyridyl molecular junctions.
  • Investigated the effects of functionalization on phonon interference (PI) and quantum interference.
  • Measured thermoelectric figure of merit (ZT), Seebeck coefficient, and thermal conductance.

Main Results:

  • Achieved record ZT values up to 2.4 in dinitro-functionalized OPE2 (DOPE2), a significant increase from ~10^-6.
  • Dinitro functionalization enhanced ZT in BDT and bipyridyl junctions, with Seebeck coefficients reaching -470 microV/K.
  • Demonstrated suppressed phonon thermal conductance due to destructive PI and conserved efficiency in parallel molecular configurations.

Conclusions:

  • Simultaneous engineering of electron and phonon transport via functionalization is a viable strategy for high-performance thermoelectrics.
  • Nitro group functionalization offers a generic route to enhance Seebeck coefficient and ZT by enabling resonance transport.
  • These findings pave the way for organic molecules in thermoelectric energy harvesting and cooling applications.