Research output: Contribution to Journal/Magazine › Journal article › peer-review
Research output: Contribution to Journal/Magazine › Journal article › peer-review
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TY - JOUR
T1 - Interplay between quantum interference and conformational fluctuations in single-molecule break junctions
AU - Berritta, Marco
AU - Manrique, David Zsolt
AU - Lambert, Colin J.
PY - 2015/1/21
Y1 - 2015/1/21
N2 - We theoretically explored the combined role of conformational fluctuations and quantum interference in determining the electrical conductance of single-molecule break junctions. In particular we computed the conductance of a family of methylsulfide-functionalized trans-alpha,omega-diphenyloligoene molecules, with terminal phenyl rings containing meta or para linkages, for which (at least in the absence of fluctuations) destructive interference in the former is expected to decrease their electrical conductance compared with the latter. We compared the predictions of density functional theory (DFT), in which fluctuational effects are absent, with results for the conformationally-averaged conductance obtained from an ensemble of conformations obtained from classical molecular dynamics. We found that junctions formed from these molecules exhibit distinct transport regimes during junction evolution and the signatures of quantum interference in these molecules survive the effect of conformational fluctuations. Furthermore, the agreement between theory and experiment is significantly improved by including conformational averaging.
AB - We theoretically explored the combined role of conformational fluctuations and quantum interference in determining the electrical conductance of single-molecule break junctions. In particular we computed the conductance of a family of methylsulfide-functionalized trans-alpha,omega-diphenyloligoene molecules, with terminal phenyl rings containing meta or para linkages, for which (at least in the absence of fluctuations) destructive interference in the former is expected to decrease their electrical conductance compared with the latter. We compared the predictions of density functional theory (DFT), in which fluctuational effects are absent, with results for the conformationally-averaged conductance obtained from an ensemble of conformations obtained from classical molecular dynamics. We found that junctions formed from these molecules exhibit distinct transport regimes during junction evolution and the signatures of quantum interference in these molecules survive the effect of conformational fluctuations. Furthermore, the agreement between theory and experiment is significantly improved by including conformational averaging.
KW - CHARGE-TRANSPORT
KW - ELECTRONIC TRANSPORT
KW - CONDUCTANCE
KW - DEPENDENCE
KW - PARALLEL
KW - WIRES
KW - INTERFACE
KW - EVOLUTION
KW - DYNAMICS
KW - SYMMETRY
U2 - 10.1039/c4nr05316h
DO - 10.1039/c4nr05316h
M3 - Journal article
VL - 7
SP - 1096
EP - 1101
JO - Nanoscale
JF - Nanoscale
SN - 2040-3364
IS - 3
ER -