TY - JOUR
T1 - Local Atomic Heat Currents and Classical Interference in Single-Molecule Heat Conduction
AU - Chen, Renai
AU - Sharony, Inon
AU - Nitzan, Abraham
N1 - Publisher Copyright:
Copyright © 2020 American Chemical Society.
PY - 2020/6/4
Y1 - 2020/6/4
N2 - We consider interference effects in vibrational heat conduction across single-molecule junctions. Previous theoretical descriptions of such effects have relied on the quantum Landauer-type expression for heat transport by harmonic molecules, and such observations are sometimes termed "quantum interference". Here we demonstrate via classical atomistic simulations of heat conduction in benzenedithiol single-molecule junctions that the room-temperature effect is essentially classical. In fact, classical simulations and quantum evaluation of room-temperature heat conduction in these systems yield similar results. Simulations of para-, meta-, and ortho-connected benzenedithiols between gold substrates yield conductions in the order para > ortho > meta, which is similar to trends found in the electronic conduction of these structures. The (essentially classical) interference origin of this ordering is indicated by the similarity of the quantum and classical behaviors of these systems.
AB - We consider interference effects in vibrational heat conduction across single-molecule junctions. Previous theoretical descriptions of such effects have relied on the quantum Landauer-type expression for heat transport by harmonic molecules, and such observations are sometimes termed "quantum interference". Here we demonstrate via classical atomistic simulations of heat conduction in benzenedithiol single-molecule junctions that the room-temperature effect is essentially classical. In fact, classical simulations and quantum evaluation of room-temperature heat conduction in these systems yield similar results. Simulations of para-, meta-, and ortho-connected benzenedithiols between gold substrates yield conductions in the order para > ortho > meta, which is similar to trends found in the electronic conduction of these structures. The (essentially classical) interference origin of this ordering is indicated by the similarity of the quantum and classical behaviors of these systems.
UR - http://www.scopus.com/inward/record.url?scp=85086481333&partnerID=8YFLogxK
U2 - 10.1021/acs.jpclett.0c00471
DO - 10.1021/acs.jpclett.0c00471
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C2 - 32375004
AN - SCOPUS:85086481333
SN - 1948-7185
VL - 11
SP - 4261
EP - 4268
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
IS - 11
ER -