Quantitative current-voltage characteristics in molecular junctions from first principles

Pierre Darancet, Jonathan R. Widawsky, Hyoung Joon Choi, Latha Venkataraman, Jeffrey B. Neaton

Research output: Contribution to journalArticle

57 Citations (Scopus)

Abstract

Using self-energy-corrected density functional theory (DFT) and a coherent scattering-state approach, we explain current-voltage (IV) measurements of four pyridine-Au and amine-Au linked molecular junctions with quantitative accuracy. Parameter-free many-electron self-energy corrections to DFT Kohn-Sham eigenvalues are demonstrated to lead to excellent agreement with experiments at finite bias, improving upon order-of-magnitude errors in currents obtained with standard DFT approaches. We further propose an approximate route for prediction of quantitative IV characteristics for both symmetric and asymmetric molecular junctions based on linear response theory and knowledge of the Stark shifts of junction resonance energies. Our work demonstrates that a quantitative, computationally inexpensive description of coherent transport in molecular junctions is readily achievable, enabling new understanding and control of charge transport properties of molecular-scale interfaces at large bias voltages.

Original languageEnglish
Pages (from-to)6250-6254
Number of pages5
JournalNano letters
Volume12
Issue number12
DOIs
Publication statusPublished - 2012 Dec 12

Fingerprint

Current voltage characteristics
Density functional theory
electric potential
density functional theory
Coherent scattering
Bias voltage
Pyridine
Transport properties
Amines
coherent scattering
Charge transfer
pyridines
amines
eigenvalues
Electrons
flux density
transport properties
routes
Electric potential
energy

All Science Journal Classification (ASJC) codes

  • Bioengineering
  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanical Engineering

Cite this

Darancet, Pierre ; Widawsky, Jonathan R. ; Choi, Hyoung Joon ; Venkataraman, Latha ; Neaton, Jeffrey B. / Quantitative current-voltage characteristics in molecular junctions from first principles. In: Nano letters. 2012 ; Vol. 12, No. 12. pp. 6250-6254.
@article{ea3a8d896b54482497123ecc231ce99a,
title = "Quantitative current-voltage characteristics in molecular junctions from first principles",
abstract = "Using self-energy-corrected density functional theory (DFT) and a coherent scattering-state approach, we explain current-voltage (IV) measurements of four pyridine-Au and amine-Au linked molecular junctions with quantitative accuracy. Parameter-free many-electron self-energy corrections to DFT Kohn-Sham eigenvalues are demonstrated to lead to excellent agreement with experiments at finite bias, improving upon order-of-magnitude errors in currents obtained with standard DFT approaches. We further propose an approximate route for prediction of quantitative IV characteristics for both symmetric and asymmetric molecular junctions based on linear response theory and knowledge of the Stark shifts of junction resonance energies. Our work demonstrates that a quantitative, computationally inexpensive description of coherent transport in molecular junctions is readily achievable, enabling new understanding and control of charge transport properties of molecular-scale interfaces at large bias voltages.",
author = "Pierre Darancet and Widawsky, {Jonathan R.} and Choi, {Hyoung Joon} and Latha Venkataraman and Neaton, {Jeffrey B.}",
year = "2012",
month = "12",
day = "12",
doi = "10.1021/nl3033137",
language = "English",
volume = "12",
pages = "6250--6254",
journal = "Nano Letters",
issn = "1530-6984",
publisher = "American Chemical Society",
number = "12",

}

Darancet, P, Widawsky, JR, Choi, HJ, Venkataraman, L & Neaton, JB 2012, 'Quantitative current-voltage characteristics in molecular junctions from first principles', Nano letters, vol. 12, no. 12, pp. 6250-6254. https://doi.org/10.1021/nl3033137

Quantitative current-voltage characteristics in molecular junctions from first principles. / Darancet, Pierre; Widawsky, Jonathan R.; Choi, Hyoung Joon; Venkataraman, Latha; Neaton, Jeffrey B.

In: Nano letters, Vol. 12, No. 12, 12.12.2012, p. 6250-6254.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Quantitative current-voltage characteristics in molecular junctions from first principles

AU - Darancet, Pierre

AU - Widawsky, Jonathan R.

AU - Choi, Hyoung Joon

AU - Venkataraman, Latha

AU - Neaton, Jeffrey B.

PY - 2012/12/12

Y1 - 2012/12/12

N2 - Using self-energy-corrected density functional theory (DFT) and a coherent scattering-state approach, we explain current-voltage (IV) measurements of four pyridine-Au and amine-Au linked molecular junctions with quantitative accuracy. Parameter-free many-electron self-energy corrections to DFT Kohn-Sham eigenvalues are demonstrated to lead to excellent agreement with experiments at finite bias, improving upon order-of-magnitude errors in currents obtained with standard DFT approaches. We further propose an approximate route for prediction of quantitative IV characteristics for both symmetric and asymmetric molecular junctions based on linear response theory and knowledge of the Stark shifts of junction resonance energies. Our work demonstrates that a quantitative, computationally inexpensive description of coherent transport in molecular junctions is readily achievable, enabling new understanding and control of charge transport properties of molecular-scale interfaces at large bias voltages.

AB - Using self-energy-corrected density functional theory (DFT) and a coherent scattering-state approach, we explain current-voltage (IV) measurements of four pyridine-Au and amine-Au linked molecular junctions with quantitative accuracy. Parameter-free many-electron self-energy corrections to DFT Kohn-Sham eigenvalues are demonstrated to lead to excellent agreement with experiments at finite bias, improving upon order-of-magnitude errors in currents obtained with standard DFT approaches. We further propose an approximate route for prediction of quantitative IV characteristics for both symmetric and asymmetric molecular junctions based on linear response theory and knowledge of the Stark shifts of junction resonance energies. Our work demonstrates that a quantitative, computationally inexpensive description of coherent transport in molecular junctions is readily achievable, enabling new understanding and control of charge transport properties of molecular-scale interfaces at large bias voltages.

UR - http://www.scopus.com/inward/record.url?scp=84870890087&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84870890087&partnerID=8YFLogxK

U2 - 10.1021/nl3033137

DO - 10.1021/nl3033137

M3 - Article

C2 - 23167709

AN - SCOPUS:84870890087

VL - 12

SP - 6250

EP - 6254

JO - Nano Letters

JF - Nano Letters

SN - 1530-6984

IS - 12

ER -