Abstract
In this study, we explore photoinduced electron transport through a molecule weakly coupled to two electrodes by combining first-principles quantum chemistry calculations with a Pauli master equation approach that accounts for many-electron states. In the incoherent limit, we demonstrate that energy-level alignment of triplet and charged states plays a crucial role, even when the rate of intersystem crossing is much smaller than the rate of fluorescence. Furthermore, the field intensity dependence and an upper bound to the photoinduced electric current can be analytically derived in our model. Under an optical field, the conductance spectra (charge stability diagrams) exhibit unusual Coulomb diamonds, which are associated with molecular excited states, and their widths can be expressed in terms of energies of the molecular electronic states. This study offers new directions for exploring optoelectronic response in nanoelectronics.
| Original language | English |
|---|---|
| Pages (from-to) | 5015-5023 |
| Number of pages | 9 |
| Journal | Nano Letters |
| Volume | 18 |
| Issue number | 8 |
| DOIs | |
| Publication status | Published - Aug 8 2018 |
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Keywords
- energy conversion
- Jablonksi diagram
- Molecular electronics
- optoelectronics
- quantum transport
ASJC Scopus subject areas
- Bioengineering
- Chemistry(all)
- Materials Science(all)
- Condensed Matter Physics
- Mechanical Engineering
Cite this
Photoinduced Anomalous Coulomb Blockade and the Role of Triplet States in Electron Transport through an Irradiated Molecular Transistor. / Fu, Bo; Mosquera, Martín A.; Schatz, George C; Ratner, Mark A; Hsu, Liang Yan.
In: Nano Letters, Vol. 18, No. 8, 08.08.2018, p. 5015-5023.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Photoinduced Anomalous Coulomb Blockade and the Role of Triplet States in Electron Transport through an Irradiated Molecular Transistor
AU - Fu, Bo
AU - Mosquera, Martín A.
AU - Schatz, George C
AU - Ratner, Mark A
AU - Hsu, Liang Yan
PY - 2018/8/8
Y1 - 2018/8/8
N2 - In this study, we explore photoinduced electron transport through a molecule weakly coupled to two electrodes by combining first-principles quantum chemistry calculations with a Pauli master equation approach that accounts for many-electron states. In the incoherent limit, we demonstrate that energy-level alignment of triplet and charged states plays a crucial role, even when the rate of intersystem crossing is much smaller than the rate of fluorescence. Furthermore, the field intensity dependence and an upper bound to the photoinduced electric current can be analytically derived in our model. Under an optical field, the conductance spectra (charge stability diagrams) exhibit unusual Coulomb diamonds, which are associated with molecular excited states, and their widths can be expressed in terms of energies of the molecular electronic states. This study offers new directions for exploring optoelectronic response in nanoelectronics.
AB - In this study, we explore photoinduced electron transport through a molecule weakly coupled to two electrodes by combining first-principles quantum chemistry calculations with a Pauli master equation approach that accounts for many-electron states. In the incoherent limit, we demonstrate that energy-level alignment of triplet and charged states plays a crucial role, even when the rate of intersystem crossing is much smaller than the rate of fluorescence. Furthermore, the field intensity dependence and an upper bound to the photoinduced electric current can be analytically derived in our model. Under an optical field, the conductance spectra (charge stability diagrams) exhibit unusual Coulomb diamonds, which are associated with molecular excited states, and their widths can be expressed in terms of energies of the molecular electronic states. This study offers new directions for exploring optoelectronic response in nanoelectronics.
KW - energy conversion
KW - Jablonksi diagram
KW - Molecular electronics
KW - optoelectronics
KW - quantum transport
UR - http://www.scopus.com/inward/record.url?scp=85049896273&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85049896273&partnerID=8YFLogxK
U2 - 10.1021/acs.nanolett.8b01838
DO - 10.1021/acs.nanolett.8b01838
M3 - Article
VL - 18
SP - 5015
EP - 5023
JO - Nano Letters
JF - Nano Letters
SN - 1530-6984
IS - 8
ER -