Strong overtones modes in inelastic electron tunneling spectroscopy with cross-conjugated molecules: a prediction from theory

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Standard

Strong overtones modes in inelastic electron tunneling spectroscopy with cross-conjugated molecules : a prediction from theory. / Jørgensen, Jacob Lykkebo; Gagliardi, Alessio; Pecchia, Alessandro; Solomon, Gemma C.

I: A C S Nano, Bind 7, Nr. 10, 2013, s. 9183-9194.

Publikation: Bidrag til tidsskriftTidsskriftartikelForskningfagfællebedømt

Harvard

Jørgensen, JL, Gagliardi, A, Pecchia, A & Solomon, GC 2013, 'Strong overtones modes in inelastic electron tunneling spectroscopy with cross-conjugated molecules: a prediction from theory', A C S Nano, bind 7, nr. 10, s. 9183-9194. https://doi.org/10.1021/nn4037915

APA

Jørgensen, J. L., Gagliardi, A., Pecchia, A., & Solomon, G. C. (2013). Strong overtones modes in inelastic electron tunneling spectroscopy with cross-conjugated molecules: a prediction from theory. A C S Nano, 7(10), 9183-9194. https://doi.org/10.1021/nn4037915

Vancouver

Jørgensen JL, Gagliardi A, Pecchia A, Solomon GC. Strong overtones modes in inelastic electron tunneling spectroscopy with cross-conjugated molecules: a prediction from theory. A C S Nano. 2013;7(10):9183-9194. https://doi.org/10.1021/nn4037915

Author

Jørgensen, Jacob Lykkebo ; Gagliardi, Alessio ; Pecchia, Alessandro ; Solomon, Gemma C. / Strong overtones modes in inelastic electron tunneling spectroscopy with cross-conjugated molecules : a prediction from theory. I: A C S Nano. 2013 ; Bind 7, Nr. 10. s. 9183-9194.

Bibtex

@article{daae67ec06ce4ff295d44a3afafbc462,
title = "Strong overtones modes in inelastic electron tunneling spectroscopy with cross-conjugated molecules: a prediction from theory",
abstract = "Cross-conjugated molecules are known to exhibit destructive quantum interference, a property that has recently received considerable attention in single-molecule electronics. Destructive quantum interference can be understood as an antiresonance in the elastic transmission near the Fermi energy and leading to suppressed levels of elastic current. In most theoretical studies, only the elastic contributions to the current are taken into account. In this paper, we study the inelastic contributions to the current in cross-conjugated molecules and find that while the inelastic contribution to the current is larger than for molecules without interference, the overall behavior of the molecule is still dominated by the quantum interference feature. Second, an ongoing challenge for single molecule electronics is understanding and controlling the local geometry at the molecule-surface interface. With this in mind, we investigate a spectroscopic method capable of providing insight into these junctions for cross-conjugated molecules: inelastic electron tunneling spectroscopy (IETS). IETS has the advantage that the molecule interface is probed directly by the tunneling current. Previously, it has been thought that overtones are not observable in IETS. Here, overtones are predicted to be strong and, in some cases, the dominant spectroscopic features. We study the origin of the overtones and find that the interference features in these molecules are the key ingredient. The interference feature is a property of the transmission channels of the π system only, and consequently, in the vicinity of the interference feature, the transmission channels of the σ system and the π system become equally transmissive. This allows for scattering between the different transmission channels, which serves as a pathway to bypass the interference feature. A simple model calculation is able to reproduce the results obtained from atomistic calculations, and we use this to interpret these findings.",
author = "J{\o}rgensen, {Jacob Lykkebo} and Alessio Gagliardi and Alessandro Pecchia and Solomon, {Gemma C.}",
year = "2013",
doi = "10.1021/nn4037915",
language = "English",
volume = "7",
pages = "9183--9194",
journal = "A C S Nano",
issn = "1936-0851",
publisher = "American Chemical Society",
number = "10",

}

RIS

TY - JOUR

T1 - Strong overtones modes in inelastic electron tunneling spectroscopy with cross-conjugated molecules

T2 - a prediction from theory

AU - Jørgensen, Jacob Lykkebo

AU - Gagliardi, Alessio

AU - Pecchia, Alessandro

AU - Solomon, Gemma C.

PY - 2013

Y1 - 2013

N2 - Cross-conjugated molecules are known to exhibit destructive quantum interference, a property that has recently received considerable attention in single-molecule electronics. Destructive quantum interference can be understood as an antiresonance in the elastic transmission near the Fermi energy and leading to suppressed levels of elastic current. In most theoretical studies, only the elastic contributions to the current are taken into account. In this paper, we study the inelastic contributions to the current in cross-conjugated molecules and find that while the inelastic contribution to the current is larger than for molecules without interference, the overall behavior of the molecule is still dominated by the quantum interference feature. Second, an ongoing challenge for single molecule electronics is understanding and controlling the local geometry at the molecule-surface interface. With this in mind, we investigate a spectroscopic method capable of providing insight into these junctions for cross-conjugated molecules: inelastic electron tunneling spectroscopy (IETS). IETS has the advantage that the molecule interface is probed directly by the tunneling current. Previously, it has been thought that overtones are not observable in IETS. Here, overtones are predicted to be strong and, in some cases, the dominant spectroscopic features. We study the origin of the overtones and find that the interference features in these molecules are the key ingredient. The interference feature is a property of the transmission channels of the π system only, and consequently, in the vicinity of the interference feature, the transmission channels of the σ system and the π system become equally transmissive. This allows for scattering between the different transmission channels, which serves as a pathway to bypass the interference feature. A simple model calculation is able to reproduce the results obtained from atomistic calculations, and we use this to interpret these findings.

AB - Cross-conjugated molecules are known to exhibit destructive quantum interference, a property that has recently received considerable attention in single-molecule electronics. Destructive quantum interference can be understood as an antiresonance in the elastic transmission near the Fermi energy and leading to suppressed levels of elastic current. In most theoretical studies, only the elastic contributions to the current are taken into account. In this paper, we study the inelastic contributions to the current in cross-conjugated molecules and find that while the inelastic contribution to the current is larger than for molecules without interference, the overall behavior of the molecule is still dominated by the quantum interference feature. Second, an ongoing challenge for single molecule electronics is understanding and controlling the local geometry at the molecule-surface interface. With this in mind, we investigate a spectroscopic method capable of providing insight into these junctions for cross-conjugated molecules: inelastic electron tunneling spectroscopy (IETS). IETS has the advantage that the molecule interface is probed directly by the tunneling current. Previously, it has been thought that overtones are not observable in IETS. Here, overtones are predicted to be strong and, in some cases, the dominant spectroscopic features. We study the origin of the overtones and find that the interference features in these molecules are the key ingredient. The interference feature is a property of the transmission channels of the π system only, and consequently, in the vicinity of the interference feature, the transmission channels of the σ system and the π system become equally transmissive. This allows for scattering between the different transmission channels, which serves as a pathway to bypass the interference feature. A simple model calculation is able to reproduce the results obtained from atomistic calculations, and we use this to interpret these findings.

U2 - 10.1021/nn4037915

DO - 10.1021/nn4037915

M3 - Journal article

VL - 7

SP - 9183

EP - 9194

JO - A C S Nano

JF - A C S Nano

SN - 1936-0851

IS - 10

ER -

ID: 92065146