Ambipolar Transport in an Electrochemically Gated Single-Molecule Field-Effect Transistor

Díez‐Pérez, Ismael; Li, Zhihai; Guo, Shaoyin; Madden, Christopher; Huang, Helin; Che, Yanke; Yang, Xiaomei; Zang, Ling; Tao, Nongjian

doi:10.1021/nn302090t

Cited by 71 publications

(61 citation statements)

References 44 publications

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“…As an example, metal complexes can display very low HOMO-LUMO gap and are excellent candidates for achieving ambipolar single molecule field-effect transistors than can be switched between n-type and p-type transport behaviour with a gate voltage. 31 Light controlled metal complexes or the association of complexes with light controlled active units is also promising for conductivity gating. Recently, light-induced modulation of molecular conductance was realized with a porphyrin-C 60 dyad.…”

Section: Discussionmentioning

confidence: 99%

Metal complexes in molecular junctions

Rigaut

2013

Dalton Trans.

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Section: Discussionmentioning

confidence: 99%

Metal complexes in molecular junctions

Rigaut

2013

Dalton Trans.

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“…As a result, many electro-active properties, such as rectification78, negative differential resistance910 and Coulomb blockade11, have been uncovered, indicative of their promising applications in functional electronic devices. Additionally, external stimuli, such as light1213141516, mechanical force1718, magnetic field1920, electrical field212223 and electrochemical potential2425262728, were introduced to modulate the molecular conductivity and thus to tune the properties of functional molecular devices, thereby significantly driving their development. As attested by the giant magnetoresistance effect2930 and photoelectric cooperation3132, a better synergy between such external stimuli and corresponding fabrication of multi-addressable MTJs may further efficiently advance the field of molecular electronics.…”

mentioning

confidence: 99%

“…In addition to this photochromic property, we previously showed that such a ruthenium/DTE association can also perform electrochemical cyclization of the DTE unit in solution at low potential40, in contrast to organic systems4950. Therefore, since it has been successfully demonstrated that molecular conductance can be respectively tuned by light irradiation121314151644 or electrochemical potential2425262728, we were strongly motivated in the association of these two stimuli in a single electronic device to achieve orthogonally modulated MTJs.…”

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confidence: 99%

Orthogonally modulated molecular transport junctions for resettable electronic logic gates

et al. 2014

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Individual molecules have been demonstrated to exhibit promising applications as functional components in the fabrication of computing nanocircuits. Based on their advantage in chemical tailorability, many molecular devices with advanced electronic functions have been developed, which can be further modulated by the introduction of external stimuli. Here, orthogonally modulated molecular transport junctions are achieved via chemically fabricated nanogaps functionalized with dithienylethene units bearing organometallic ruthenium fragments. The addressable and stepwise control of molecular isomerization can be repeatedly and reversibly completed with a judicious use of the orthogonal optical and electrochemical stimuli to reach the controllable switching of conductivity between two distinct states. These photo-/electro-cooperative nanodevices can be applied as resettable electronic logic gates for Boolean computing, such as a two-input OR and a three-input AND-OR. The proof-of-concept of such logic gates demonstrates the possibility to develop multifunctional molecular devices by rational chemical design.

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“…Furthermore, in the calculations we assume that at zero bias (V = 0) the HOMO is on resonance with the Fermi energy. Experimentally, this may require the presence of an electrochemical [29][30][31] or electrostatic 32 gate. However, we would like to stress that this assumption represents the ideal case with the highest rectification.…”

mentioning

confidence: 99%

Design of an efficient coherent multi-site single-molecule rectifier

Perrin

Doelman

Eelkema

et al. 2017

Phys. Chem. Chem. Phys.

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aWe propose the design of a single-molecule diode with a rectification ratio exceeding a million. The employed mechanism is based on coherent resonant charge transport across a molecule that consists of four conjugated sites coupled by non-conjugated bridges. Using density functional theory calculations, we rationalize the design of the molecule and demonstrate the crucial role of aligning the sites at a specific voltage. Rectification ratios are calculated for a series of chemical substituents and demonstrate that with careful molecular design, high rectification ratios can be achieved. Finally, we comment on the shortcomings of our approach, how further improvements can be obtained and discuss some of the experimental challenges.Molecular diodes have been attracting much attention recently, both in self-assembled monolayers 1-7 and on the single-molecule scale. [8][9][10][11][12][13][14][15][16] Even though the rectifier has been the seminal device which launched the field of single-molecule electronics, 17 up to date, their performance have many shortcomings. In particular, their rectification ratios (RR) are orders of magnitude lower than typical semiconducting rectifiers. The highest RR reported experimentally on a single-molecule junction 15 is about 600, and is no match for a semiconducting diode where ratios exceeding 10 6 are common. In that study, a molecular backbone was considered which consisted of two identical, weakly-coupled conjugated parts. In such a system, current flows coherently when both halves are on resonance, i.e., the sites are aligned with each other within the bias window. The alignment of the two sites can be modified by applying a bias voltage and/or by chemical substituents. With proper design, one can align the sites at zero bias, while misaligning them at finite bias, yielding negative differential conductance. 18 One can also align the sites at a finite bias, 15,19-22 and achieve single-molecule rectification.Based on a similar principle, here we investigate theoretically how the rectification ratio of single-molecule diodes can be significantly enhanced by the addition of more sites in series, as shown in as presented in Fig. 1b. Low RR are primarily caused by a high reverse current. Adding more sites in series leads to a strong suppression of the reverse current, thereby drastically improving the RR. However, the addition of sites comes at the cost of an increased molecular complexity and number of model parameters. In this study, we first focus on the design of a molecule which behaves as having four sites in series. For this purpose, we use density functional theory (DFT) calculations. We then investigate how the molecule can be engineered by the means of chemical substitution to align the sites at a particular bias voltage. We eventually show that the molecule designed with four sites represents a drastic improvement compared to a two-site molecule, with RR approaching 10 6 , competitive with siliconbased diodes.1 Design guidelines Fig. 1 depicts the concept of a rectifier...

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Ambipolar Transport in an Electrochemically Gated Single-Molecule Field-Effect Transistor

Cited by 71 publications

References 44 publications

Metal complexes in molecular junctions

Metal complexes in molecular junctions

Orthogonally modulated molecular transport junctions for resettable electronic logic gates

Design of an efficient coherent multi-site single-molecule rectifier

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