Bias-driven conductance increase with length in porphyrin tapes

A key goal in molecular electronics has been to find molecules that facilitate efficient charge transport over long distances. Normally, molecular wires become less conductive with increasing length. Here, we report a series of fused porphyrin oligomers for which the conductance increases substantia...

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Главные авторы: Leary, E, Limburg, B, Alanazy, A, Sangtarash, S, Grace, I, Swada, K, Esdaile, L, Noori, M, González, M, Rubio-Bollinger, G, Sadeghi, H, Hodgson, A, Agraı T, N, Higgins, S, Lambert, C, Anderson, H, Nichols, R
Формат: Journal article
Язык:English
Опубликовано: American Chemical Society 2018
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author Leary, E
Limburg, B
Alanazy, A
Sangtarash, S
Grace, I
Swada, K
Esdaile, L
Noori, M
González, M
Rubio-Bollinger, G
Sadeghi, H
Hodgson, A
Agraı T, N
Higgins, S
Lambert, C
Anderson, H
Nichols, R
author_facet Leary, E
Limburg, B
Alanazy, A
Sangtarash, S
Grace, I
Swada, K
Esdaile, L
Noori, M
González, M
Rubio-Bollinger, G
Sadeghi, H
Hodgson, A
Agraı T, N
Higgins, S
Lambert, C
Anderson, H
Nichols, R
author_sort Leary, E
collection OXFORD
description A key goal in molecular electronics has been to find molecules that facilitate efficient charge transport over long distances. Normally, molecular wires become less conductive with increasing length. Here, we report a series of fused porphyrin oligomers for which the conductance increases substantially with length by >10-fold at a bias of 0.7 V. This exceptional behavior can be attributed to the rapid decrease of the HOMO-LUMO gap with the length of fused porphyrins. In contrast, for butadiyne-linked porphyrin oligomers with moderate inter-ring coupling, a normal conductance decrease with length is found for all bias voltages explored (±1 V), although the attenuation factor (β) decreases from ca. 2 nm-1 at low bias to <1 nm-1 at 0.9 V, highlighting that β is not an intrinsic molecular property. Further theoretical analysis using density functional theory underlines the role of intersite coupling and indicates that this large increase in conductance with length at increasing voltages can be generalized to other molecular oligomers.
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spelling oxford-uuid:b2c17b15-8ef8-40cb-88af-65b42dc893e72022-03-27T04:14:04ZBias-driven conductance increase with length in porphyrin tapesJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:b2c17b15-8ef8-40cb-88af-65b42dc893e7EnglishSymplectic Elements at OxfordAmerican Chemical Society2018Leary, ELimburg, BAlanazy, ASangtarash, SGrace, ISwada, KEsdaile, LNoori, MGonzález, MRubio-Bollinger, GSadeghi, HHodgson, AAgraı T, NHiggins, SLambert, CAnderson, HNichols, RA key goal in molecular electronics has been to find molecules that facilitate efficient charge transport over long distances. Normally, molecular wires become less conductive with increasing length. Here, we report a series of fused porphyrin oligomers for which the conductance increases substantially with length by >10-fold at a bias of 0.7 V. This exceptional behavior can be attributed to the rapid decrease of the HOMO-LUMO gap with the length of fused porphyrins. In contrast, for butadiyne-linked porphyrin oligomers with moderate inter-ring coupling, a normal conductance decrease with length is found for all bias voltages explored (±1 V), although the attenuation factor (β) decreases from ca. 2 nm-1 at low bias to <1 nm-1 at 0.9 V, highlighting that β is not an intrinsic molecular property. Further theoretical analysis using density functional theory underlines the role of intersite coupling and indicates that this large increase in conductance with length at increasing voltages can be generalized to other molecular oligomers.
spellingShingle Leary, E
Limburg, B
Alanazy, A
Sangtarash, S
Grace, I
Swada, K
Esdaile, L
Noori, M
González, M
Rubio-Bollinger, G
Sadeghi, H
Hodgson, A
Agraı T, N
Higgins, S
Lambert, C
Anderson, H
Nichols, R
Bias-driven conductance increase with length in porphyrin tapes
title Bias-driven conductance increase with length in porphyrin tapes
title_full Bias-driven conductance increase with length in porphyrin tapes
title_fullStr Bias-driven conductance increase with length in porphyrin tapes
title_full_unstemmed Bias-driven conductance increase with length in porphyrin tapes
title_short Bias-driven conductance increase with length in porphyrin tapes
title_sort bias driven conductance increase with length in porphyrin tapes
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