Robust Bipolar Light Emission and Charge Transport in Symmetric Molecular Junctions

Tefashe, Ushula M.; Nguyen, Quang Trong; Lafolet, Frédéric; Lacroix, Jean; McCreery, Richard L.

doi:10.1021/jacs.7b02563

Cited by 56 publications

(102 citation statements)

References 25 publications

(83 reference statements)

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“…Thus, tunneling transport is determined for Rucomplexes bridging a gap of about 4 nm, i. e. corresponding to the distance between two AuNP, while in longer wires thermally activated hopping is the dominant transport mechanism. This finding is in notable agreement with reports from other groups [31,32,35]. Thus, the respective device design of Next we discuss the impact of this finding on the electrical switching ability of few Ru(MPTP)2-AuNP compared to single Ru(MPTP)2-AuNP devices.…”

Section: Electrical Properties Of Ru(tp)2-complex Devicessupporting

confidence: 91%

Impact of device design on the electronic and optoelectronic properties of integrated Ru-terpyridine complexes

Mennicken¹,

Peter²,

Kaulen³

et al. 2021

Preprint

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The performance of nanoelectronic and molecular electronic devices relies strongly on the employed functional units and their addressability, which is often a matter of appropriate interfaces and device design. Here, we compare two promising designs to build up solid-state electronic devices utilizing the same functional unit. Optically addressable Ru-terpyridine complexes were incorporated in supramolecular wires or employed as ligands of gold nanoparticles and contacted by nanoelectrodes. The resulting small area nanodevices were thoroughly electrically characterized as a function of temperature and light exposure. Differences in the resulting device conductance could be attributed to the device design and the respective transport mechanism: thermally activated hopping conduction in case of Ru-terpyridine wire devices or sequential tunneling in nanoparticle-based devices. Furthermore, the conductance switching of nanoparticle-based devices upon 530 nm irradiation was attributed to plasmon-induced metal-to-ligand charge-transfer in the Ru-terpyridine complexes used as switching ligands. Finally, our results reveal a superior device performance of nanoparticle-based devices compared to molecular wire devices based on Ru-terpyridine complexes as functional units.

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Section: Electrical Properties Of Ru(tp)2-complex Devicessupporting

confidence: 91%

Impact of device design on the electronic and optoelectronic properties of integrated Ru-terpyridine complexes

Mennicken¹,

Peter²,

Kaulen³

et al. 2021

Preprint

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“…Materials and Sample Preparation : Bottom electrode contacts were patterned on diced, fused quartz chips (Quartz Unlimited LLC, nanograde polish), as shown in Figure B, by sequential electron beam evaporation (Kurt J. Lesker PVD75) of Cr (4 nm), Au (30 nm), and eC (10 nm, from spectroscopic grade graphite) through a shadow mask following a previously established procedure. [6c,9] AQ diazonium tetrafluoroborate was prepared and stored at 4 °C using the 2‐aminoanthraquinone precursor (Sigma‐Aldrich) as described previously . BTB diazonium ions were prepared from the amino precursor (BTAB, synthesized at the University of Paris by Prof. Jean‐Christophe et al) in situ prior to electrochemical grafting using tert ‐butyl nitrite (Sigma‐Aldrich) as an oxidizing agent .…”

Section: Methodsmentioning

confidence: 99%

“…In addition to optical spectroscopy used to verify MJ structure, illumination of MJs can produce an electronic response, and current through a MJ can result in light emission . The single‐component MJs studied to date show relatively weak photoeffects such as internal photoemission (IPE)[5a,e,f] and conductance changes,[5b] due in part to weak optical absorption by the thin molecular layer.…”

Section: Summary Of Voc and Jsc Values Measured With A 407 Nm Laser Imentioning

confidence: 99%

“…MJs of single‐component layers of AQ and BTB, along with bilayer devices of BTB–AQ and AQ–BTB, were fabricated on patterned quartz/Cr 4 /Au 30 /C 10 substrates with C 10 /Au 20 top contacts using established techniques[3,6a,9] to achieve arrays of MJs (Figure B, subscripts indicate layer thicknesses in nm determined with atomic force microscopy (AFM)). Figure C displays a schematic energy level diagram for the bilayer BTB–AQ molecular device under zero bias showing the highest occupied (HOMO) and lowest unoccupied molecular orbitals (LUMO) of the BTB and AQ bilayer MJs (estimated with Gaussian 09 [B3LYP/6‐31G(d)] for the free molecules) with the electron beam deposited carbon (eC) electrode contacts.…”

Section: Summary Of Voc and Jsc Values Measured With A 407 Nm Laser Imentioning

confidence: 99%

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Photocurrent, Photovoltage, and Rectification in Large‐Area Bilayer Molecular Electronic Junctions

Smith

McCreery

2018

Adv Elect Materials

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between two electrode contacts, referred to as a "molecular junction (MJ)". [1] A MJ may employ a single organic substituent or repeating units (e.g., an oligomer) to achieve variations in the electronic response depending on structure and molecular layer thickness. [2] Alternatively, MJs may contain two or more molecular layers differing in structure and orbital energies to create multilayered MJs with novel electronic behaviors. As examples, bilayer MJs integrate electron donor and acceptor layers in a single oligomer to achieve an electronic rectifier, [2e,3] and trilayers that further incorporate mobile Li + ions can act as a redox active memory or energy storage device with total thickness <15 nm. [4] Understanding the relationship between the structure, orbital energies, and electronic behavior of both single and multilayer MJs is paramount to engineering new ME devices for a potentially broad range of electronic functions.In addition to optical spectroscopy used to verify MJ structure, illumination of MJs can produce an electronic response, [5] and current through a MJ can result in light emission. [6] The single-component MJs studied to date show relatively weak photoeffects such as internal photoemission (IPE) [5a,e,f ] and conductance changes, [5b] due in part to weak optical absorption by the thin molecular layer. We recently reported PCs at zero bias for eight single-component carbon/molecule/carbon MJs with varying molecular structure. While the PCs correlated with transport properties across a range of structures, the external quantum efficiencies were small, in the range of 10 −5 to 10 −4 photoelectrons/incident photon. [7] In contrast to symmetric current density versus bias voltage (JV) behavior observed with single-component layers, bilayer MJs with an electron accepting layer that is subsequently overlaid with an electron donating layer between symmetric sp 2 carbon contacts exhibit nonlinear, asymmetric JV responses with rectification ratios (RR) of 10-290 for different bilayer combinations. [3] The bilayer introduced asymmetry into a previously symmetric single-layer device, and the rectification direction could be reversed by changing the order of the molecular layers. The current investigation examines photoeffects in molecular bilayers (10-15 nm total thickness) with two main motivations. First, the photoresponse of the MJs should reveal relationships between internal energy levels of both the molecules and the associated contacts in completed, functioning MJs. Second, sensitivity to light is a potentially useful function in ME, and bilayer devices may be good candidates for photodetectors. Unlike the common semiconductor photodetectors, Bilayer donor-acceptor molecular junctions are successfully fabricated with active layer thickness <15 nm to study the mechanism of photo-induced charge transport. The bilayer devices exhibit lifetimes greater than 1 h with laser irradiation, and a strong dependence of the sign and magnitude of the photovoltage and photocurrent on structure and order ...

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“…These Raman bands are attributed to the stretching of C=C and C=N bonds of the pyridine rings. 24,[26][27][28] After electrodeposition of 50 cycles, the Raman spectrum of ZnOnw/Fe II electrodes as revealed in It exhibits two additional broad bands at around 1530 and 1095 cm -1 as showed in Figure 2d. The band at 1095 cm -1 is assigned to the second-order modes of wurtzite ZnO and hence is typical of ZnO NWs.…”

Section: Resultsmentioning

confidence: 98%

ZnO Nanowires as a Promotor of High Photoinduced Efficiency and Voltage Gain for Cathode Battery Recharging

Lecarme

Consonni

Lafolet

et al. 2019

ACS Appl. Energy Mater.

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In recent years, intensive efforts have been focused on the conversion and storage of solar energy in a single device. In this work, we report the use of ZnO-based electrodes in the form of monolayer or nanowires as a light inducer for battery recharging. Two transition metal complexes of ruthenium(II) and iron(II) are grafted onto the ZnO-based electrode to tune the efficiency of the system. We explore the influence of both the ZnO morphology and nature of the transition metal complex on the light induced voltage and faradaic efficiency toward electrochemical storage. The resulting ZnO-based electrodes have all been found to be electrochemically photoactive and their functionalized ZnO nanowire counterpart has shown the best results. Once the ruthenium complex has been grafted, a high potential gain between dark and illumination conditions of 1.3 V is reached, which is associated with a modest faradaic efficiency of 50%. However, in the presence of the iron complex, a favorable potential gain of 700 mV is obtained and advantageously combined with a faradic efficiency of 100%. These results undoubtedly highlight the remarkable synergy between photoactive ZnO, especially in the form of nanowires, and a redox center allowing it to be applied for a photorechargeable battery device.

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Robust Bipolar Light Emission and Charge Transport in Symmetric Molecular Junctions

Cited by 56 publications

References 25 publications

Impact of device design on the electronic and optoelectronic properties of integrated Ru-terpyridine complexes

Impact of device design on the electronic and optoelectronic properties of integrated Ru-terpyridine complexes

Photocurrent, Photovoltage, and Rectification in Large‐Area Bilayer Molecular Electronic Junctions

ZnO Nanowires as a Promotor of High Photoinduced Efficiency and Voltage Gain for Cathode Battery Recharging

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