Ambipolar Charge Transport Characteristics Research Articles

Benzopyrano-Fused Phenanthridine-Based Columnar Mesogens: Synthesis, Self-organization and Charge-Transport Properties.

Columnar mesogens constitute a fascinating class of supramolecular nano-architectures owing to the exceptional properties induced by their self-assembling behavior. Extending the π-conjugated core in such systems by incorporating heteroatoms extensively influences their mesomorphic, photophysical properties, etc., presenting them as potential candidates for optoelectronic applications. In the present work, a series of novel nitrogen and oxygen-incorporated chromenonaphthophenanthridine-based elliptical dimers have been synthesized through tandem Pictet-Spengler cyclization followed by ipso-aromatic substitution in one-pot. Mesophase characterization has been carried out by employing POM, DSC, and X-ray diffraction studies. Photophysical properties were investigated using UV-vis and emission spectroscopy. Furthermore, the charge transport properties were analyzed by time-of-flight measurements, and the observed ambipolar mobilities were found to be of the order of 10-3 cm2 V-1 s-1 . The high solubility, excellent thermal stability, self-organizing properties, and ambipolar charge transport characteristics make them promising candidates for applications in organic electronics.

Organic Single-Crystalline p–n Heterojunctions for High-Performance Ambipolar Field-Effect Transistors and Broadband Photodetectors

Organic semiconducting single crystals are ideal building blocks for organic field-effect transistors (OFETs) and organic photodetectors (OPDs) because they can potentially exhibit the best charge transport and photoelectric properties in organic materials. Nevertheless, it is usual for single-crystal OFETs to be built from one kind of organic material in which the dominant transport is either electron or hole; such OFETs show unipolar charge transport. Furthermore, single-crystal OPDs present high performance only in restricted regions because of the limited absorption of one-component single crystals. In an ideal situation, devices which comprise both electron- and hole-transporting single crystals with complementary absorptions, such as single-crystalline p-n heterojunctions (SCHJs), can permit broadband photoresponse and ambipolar charge transport. In this paper, a solution-processing crystallization strategy to prepare an SCHJ composed of C60 and 6,13-bis(triisopropylsilylethynyl)pentacene (TIPS-PEN) was shown. These SCHJs demonstrated ambipolar charge-transport characteristics in OFETs with a balanced performance of 2.9 cm2 V-1 s-1 for electron mobility and 2.7 cm2 V-1 s-1 for hole mobility. This demonstration is the first of single-crystal OFETs in which both electron and hole mobilities were over 2.5 cm2 V-1 s-1. OPDs fabricated upon as-prepared SCHJs exhibited highly sensitive photoconductive properties ranging from ultraviolet to visible and further to near-infrared regions as a result of complementary absorption between C60 and TIPS-PEN, thereby attaining photoresponsivities that are among the highest reported values within the OPDs. This work would provide valuable references for developing novel SCHJ systems to achieve significant progress in high-performance ambipolar OFETs and broadband OPDs.

Dicyanodistyrylbenzene-Based Copolymers for Ambipolar Organic Field-Effect Transistors with Well-Balanced Hole and Electron Mobilities

We report three types of dicyanodistyrylbenzene (DCS)-based copolymers (PBDT-DCS, PT-DCS, and PNDI-DCS), which present highly balanced ambipolar charge transport characteristics in organic field-effect transistors (OFETs). The introduction of the DCS moiety in a polymer backbone not only lowers the lowest unoccupied molecular orbital (LUMO) level but also increases the crystalline ordering via interchain dipole–dipole interactions. As a result, the LUMO levels for PBDT-DCS, PT-DCS, and PNDI-DCS were decreased to −3.76, −4.00, and −3.99 eV, respectively, which is beneficial for efficient electron injection from Au electrode for improving ambipolar charge transport. The determined hole/electron mobilities of the OFETs were 0.064/0.014, 0.492/0.181, and 0.420/0.447 cm2/(V s) for PBDT-DCS, PT-DCS, and PNDI-DCS, respectively, after thermal annealing at 250 °C. By incorporating the electron-deficient naphthalene diimide (NDI) unit in the copolymers, the n-channel transport was enhanced, with decreasing frontier...

Water‐Processable Multiwalled Nanotube: Phenol‐Induced Reversible Oxidation Process and Ambipolar Charge Transport Property

AbstractDue to the fascinating electronic, thermal, and mechanical properties of single‐walled carbon nanotubes (SWCNTs), extensive efforts have been devoted to the development of SWCNT‐based materials. These materials' semiconducting properties and related applications, such as field‐effect transistors (FETs), have been investigated by researchers for many years. However, despite the significant progress achieved, it remains challenging to separate semiconducting and metallic nanotubes from the mixtures of as‐grown SWCNTs. In a few studies, composites of water‐processable phenol formaldehyde resin/multiwalled carbon nanotubes (MWCNTs) have been found to exhibit a quasireversible oxidation process and to behave as semiconductors or field‐effect transistors. This finding has rarely been reported for MWCNTs, and it differs greatly from findings regarding intrinsic semiconductive SWCNTs. Significantly, field‐effect transistors fabricated with MWCNT composites as their semiconductor active layers have shown ambipolar charge transport characteristics. The results provide a high value‐added application pathway for the application of polymer/MWCNTs as the FET materials for electronic devices that offer higher performance at a lower cost.

Facile fabrication of phenothiazine-tetracyanoquinodimethane co-crystal microwires with ambipolar charge transport characteristics

Novel co-crystal microwires based on phenothiazine (PTZ) and tetracyanoquinodimethane (TCNQ) have been fabricated using a facile solution method and fully characterized. The microwires had well-defined shapes, smooth surfaces and high crystalline. Moreover, the co-crystal microwires exhibited a significant absorption at wavelengths between 900 and 2400nm owing to the charge-transfer interaction between PTZ and TCNQ. The prototype field-effect transistor with the bottom-gate was directly constructed, exhibiting typical ambipolar charge transport characteristics.

Regioirregular ambipolar naphthalenediimide‐based alternating polymers: Synthesis, characterization, and application in field‐effect transistors

ABSTRACTIn this work, we report the synthesis, characterization, and application of two regioirregular naphthalenediimide (NDI)‐based alternating conjugated polymers, namely P1 and P2, in which nitrile‐substituted moiety, 2,3‐bis(thiophen‐2‐yl)acrylonitrile and NDI moiety act as donor and acceptor unit, respectively. The two regioirregular polymers possess low‐lying LUMO energy levels of −3.92 eV for P1 and −3.96 eV for P2. Both polymers possess typical dual‐band UV−Vis−NIR absorption profiles of NDI‐based polymers, and show broadened and red‐shifted absorption spectra in the solid state compared with those in solutions. Field‐effect transistor devices with top‐gate bottom‐contact configuration were used to evaluate the polymers' semiconducting properties. The two polymers exhibited promising and air‐stable ambipolar charge transport characteristics. Thin film microstructure investigations (AFM and 2D‐GIXRD) suggest both polymers formed continuous and smooth thin films, and adopted predominantly face‐on molecular packing in the solid state. © 2017 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2017, 55, 3627–3635

Enhanced ambipolar charge transport in staggered carbon nanotube field-effect transistors for printed complementary-like circuits

Semiconducting single-walled carbon nanotubes (semi-SWNTs) are attractive as they can be used enable high-performance nano-electronic devices. We report the enhanced ambipolar charge transport characteristics of the semi-SWNT field-effect transistors (FETs) based on a top-gated staggered device structure. SWNTs were selectively dispersed in non-polar organic solvents and sorted by a π-conjugated polymer wrapping method. The sorted semi-SWNTs solution was used simply to form a well-percolated CNT-network, and the top-gate and bottom-contact FETs showed relatively high and equivalent electron and hole mobilities with very high on/off-current ratios and steep subthreshold slopes. The equivalent ambipolar charge transport behavior of semi-SWNTs was used to demonstrate a reliable complementary-like electronic circuits. The inverters showed a good switching threshold near the ideal point at half the driving bias, high gain, low hysteresis, and stability under repeatable operating conditions. They can thus be broadly applied as a fundamental circuit element in printed and flexible electronics.

Modulation of ambipolar charge transport characteristics in side-chain polystyrenes as host materials for solution processed OLEDs

A series of side-chain polystyrenes was developed as ambipolar hosts for solution processed organic light emitting diodes (OLEDs). The series was derived from the hole-only transport host molecule 1,3-Bis(N-carbazolyl)benzene (mCP). Electron transport ability was incorporated into the host polymers by the introduction of electron-poor heterocycles (pyridine or triazine) and extending delocalization of the lowest unoccupied molecular orbital (LUMO). The materials were tested in Ir-based green OLED devices with all organic layers processed from solution. Devices with the polymer combining triazine and carbazole on its side-chain exhibited a low luminance on-set voltage of 3.0 V and a current efficacy of 28.9 cd/A, which was more than 10 times higher than for devices with the mCP-based polymer (1.6 cd/A). The increase in performance is most likely due to an improvement of charge balance in the emissive layer, showing that our ambipolar polymers are good candidates for further wet-process optoelectronic applications.

N-type organic electrochemical transistors with stability in water.

Organic electrochemical transistors (OECTs) are receiving significant attention due to their ability to efficiently transduce biological signals. A major limitation of this technology is that only p-type materials have been reported, which precludes the development of complementary circuits, and limits sensor technologies. Here, we report the first ever n-type OECT, with relatively balanced ambipolar charge transport characteristics based on a polymer that supports both hole and electron transport along its backbone when doped through an aqueous electrolyte and in the presence of oxygen. This new semiconducting polymer is designed specifically to facilitate ion transport and promote electrochemical doping. Stability measurements in water show no degradation when tested for 2 h under continuous cycling. This demonstration opens the possibility to develop complementary circuits based on OECTs and to improve the sophistication of bioelectronic devices.

Donor-acceptor co-assembled supramolecular nanofibers with high and well-balanced ambipolar charge transport properties under ambient conditions.

Single-bundle nanofiber based OFETs were fabricated from co-assembled supramolecular nanofibers which comprise TCAT and PDI-13, using a simple gelation method. The co-assembled supramolecular nanoarchitecture was fully characterized by means of optical microscopy, TEM, SEM, 2D-GIWAXS and so on. The devices exhibited typical ambipolar charge transport characteristics with very well-balanced hole and electron mobilities as well as high photoresponsivity under ambient conditions.

Fusing N-heteroacene analogues into one "kinked" molecule with slipped two-dimensional ladder-like packing.

An unexpected "kinked" N-heteroacene with a slipped two-dimensional ladder-like packing feature is produced from the conventional condensation reaction. The as-obtained compound [2,2']bi(5,12-bis(TIPS)piperazin-3-one[2,3-b]phenazine) (2BPP) consists of two identical backbones (5,12-bis(TIPS)piperazin-3-one[2,3-b]phenazine), which are fused together through a C[double bond, length as m-dash]C double bond and two intramolecular H-bonds. A study on the charge carrier transport indicates that a 2BPP single crystal has a hole mobility up to 0.3 cm2 V-1 s-1, while theoretical calculations suggest that this compound might possess potential well-balanced ambipolar charge-transport characteristics.

(3E,8E)-3,8-Bis(2-oxoindolin-3-ylidene)naphtho-[1,2-b:5,6-b']difuran-2,7(3H,8H)-dione (INDF) based polymers for organic thin-film transistors with highly balanced ambipolar charge transport characteristics.

Two donor-acceptor (D-A) conjugated polymers, PINDFTT and PINDFBT, based on a novel electron acceptor, (3E,8E)-3,8-bis(2-oxoindolin-3-ylidene)naphtho-[1,2-b:5,6-b']difuran-2,7(3H,8H)-dione (INDF), are synthesized for solution processed organic thin-film transistors. Both polymers exhibited highly balanced ambipolar characteristics with hole and electron mobilities up to 0.51 cm(2) V(-1) s(-1) and 0.50 cm(2) V(-1) s(-1), respectively.

Ambipolar charge-transport properties in 4,10-dihalogenated anthanthrone crystals: a theoretical study

Good ambipolar charge-transport characteristics have been revealed for the halogenated anthanthrone crystals by DFT and MD calculations.

Charge Transport Properties of Perylene–TCNQ Crystals: The Effect of Stoichiometry

In this work we have revisited the charge-transfer crystal system perylene–TCNQ and found that this complex can crystallize with a 2:1 stoichiometric ratio in addition to the 1:1 and 3:1 stoichiometries previously observed. The vibrational and electronic properties of these perylene–TCNQ charge-transfer crystals have been investigated by means of Raman scattering measurements and density functional theory calculations. Electrical measurements were also performed by preparing organic field-effect transistors (OFETs) from the crystals. The Raman spectra in the low-frequency range (below 200 cm–1) are found to be unique to the specific crystal structure and can therefore be used to determine the stoichiometry. The Raman data and the X-ray diffraction measurements indicate that at room temperature the amount of charge transferred to the TCNQ molecule is less than 0.2e for all three compounds, and is nearly the same in P1T1 and P2T1 but is slightly larger in P3T1. The electronic structure calculations suggest good intrinsic charge transport properties for both holes and electrons in P1T1 and P2T1 and only for holes in P3T1. Ambipolar charge transport characteristics were found for P2T1 and hole and electron charge transport characteristics were found in P3T1 and P1T1, respectively.

Low-temperature solution-processed wavelength-tunable perovskites for lasing

Low-temperature solution-processed materials that show optical gain and can be embedded into a wide range of cavity resonators are attractive for the realization of on-chip coherent light sources. Organic semiconductors and colloidal quantum dots are considered the main candidates for this application. However, stumbling blocks in organic lasing include intrinsic losses from bimolecular annihilation and the conflicting requirements of high charge carrier mobility and large stimulated emission; whereas challenges pertaining to Auger losses and charge transport in quantum dots still remain. Herein, we reveal that solution-processed organic-inorganic halide perovskites (CH3NH3PbX3 where X = Cl, Br, I), which demonstrated huge potential in photovoltaics, also have promising optical gain. Their ultra-stable amplified spontaneous emission at strikingly low thresholds stems from their large absorption coefficients, ultralow bulk defect densities and slow Auger recombination. Straightforward visible spectral tunability (390-790 nm) is demonstrated. Importantly, in view of their balanced ambipolar charge transport characteristics, these materials may show electrically driven lasing.

Small band gap polymers incorporating a strong acceptor, thieno[3,2-b]thiophene-2,5-dione, with p-channel and ambipolar charge transport characteristics

Novel small band gap semiconducting polymers incorporating thienothiophenedione exhibit high hole mobilities of ∼1.38 cm2V−1s−1.

Solution‐Grown Organic Single‐Crystalline p‐n Junctions with Ambipolar Charge Transport

Organic single-crystalline p-n junctions are grown from mixed solutions. First, C60 crystals (n-type) form and, subsequently, C8-BTBT crystals (p-type) nucleate heterogeneously on the C60 crystals. Both crystals continue to grow simultaneously into single-crystalline p-n junctions that exhibit ambipolar charge transport characteristics. This work provides a platform to study organic single-crystalline p-n junctions.

Preparation and ambipolar transistor characteristics of co-crystal microrods of dibenzotetrathiafulvalene and tetracyanoquinodimethane

Co-crystal microrods of dibenzotetrathiafulvalene (DBTTF) and tetracyanoquinodimethane (TCNQ) molecules with the mixed-stack structure were prepared via a facile solution process and fully characterized. The as-prepared microrods were directly used for fabricating prototype devices, which exhibited typical ambipolar charge transport characteristics. The result indicated that the co-crystal microrods of DBTTF-TCNQ were potentially useful for miniaturized devices.

Fullerene/Cobalt Porphyrin Hybrid Nanosheets with Ambipolar Charge Transporting Characteristics

A novel supramolecular nanoarchitecture, comprising C(60)/Co porphyrin nanosheets, was prepared by a simple liquid-liquid interfacial precipitation method and fully characterized by means of optical microscopy, AFM, STEM, TEM, and XRD. It is established that the highly crystalline C(60)/Co porphyrin nanosheets have a simple (1:1) stoichiometry, and when incorporated in bottom-gate, bottom-contact field-effect transistors (FETs), they show ambipolar charge transport characteristics.

Prediction of Remarkable Ambipolar Charge-Transport Characteristics in Organic Mixed-Stack Charge-Transfer Crystals

We have used density functional theory calculations and mixed quantum/classical dynamics simulations to study the electronic structure and charge-transport properties of three representative mixed-stack charge-transfer crystals, DBTTF-TCNQ, DMQtT-F(4)TCNQ, and STB-F(4)TCNQ. The compounds are characterized by very small effective masses and modest electron-phonon couplings for both holes and electrons. The hole and electron transport characteristics are found to be very similar along the stacking directions; for example, in the DMQtT-F(4)TCNQ crystal, the hole and electron effective masses are as small as 0.20 and 0.26 m(0), respectively. This similarity arises from the fact that the electronic couplings of both hole and electron are controlled by the same superexchange mechanism. Remarkable ambipolar charge-transport properties are predicted for all three crystals. Our calculations thus provide strong indications that mixed-stack donor-acceptor materials represent a class of systems with high potential in organic electronics.