Creation of reduced graphene oxide based field effect transistors and their utilization in the detection and discrimination of nucleoside triphosphates.

Two low-cost, micropatterned, solution-gated field effect transistors (modified FET and unmodified FET) based on reduced graphene oxide (RGO) were developed and used for detection and discrimination of nucleoside triphosphates (NTPs). The modified FET was realized by simple deposition of a positively charged bis-pyrenyl derivative, py-diIM-py, onto the conducting RGO strips of the unmodified FET. The electrical properties and sensing behaviors of the as-prepared devices were studied comprehensively. Electrical transfer property tests revealed that both of the two FETs exhibit V-shaped ambipolar field effect behavior from p-type region to n-type region. Sensing performance studies demonstrated that modification of the native FET with py-diIM-py improves its sensing ability to NTPs-GTP and ATP in particular. The detection limit of GTP and ATP was as low as 400 nM, which is the lowest value for graphene-based electronic sensors reported so far. Furthermore, based on the cross-reactive responses of the two devices to NTPs, NTPs can be conveniently distinguished via combining use of the two devices. The enhancement of the modifier (py-diIM-py) to the sensing performance of the FET is tentatively attributed to its possible mediation role in sticking onto RGO strips and accumulating analytes by electrostatic association with the relevant species. Because they are sensitive and fast in response, simple and low-cost in preparation, and possibly useful in sensor-array fabrication, the developed sensors show great potential in real-life application.

Constitutional Dynamic Chemistry-based New Concept of Molecular Beacons for High Efficient Development of Fluorescent Probes.

Inspired by the concept of constitutional dynamic chemistry, we propose a new and well-adaptable strategy for developing molecular beacon (MB)-like fluorescent probes. To demonstrate the strategy, we synthesized and used an amino group containing pyrenyl derivative of cholesterol (CP) for the construction of new fluorescent probes with EDTA and sulfuric acid. The probes as created were successfully used for n-hexane purity checking and Ba(2+)and Pb(2+)sensing, respectively.

Towards a new FRET system via combination of pyrene and perylene bisimide: synthesis, self-assembly and fluorescence behavior.

A new fluorescent derivative of cholesterol, N,N'-(N-(2-(3ß-cholest-5-en-3yl-formamido)ethyl) pyrene-1-sulfonamido)ethyl perylene-3,4:9,10-tetracarboxylic acid bisimide (CPPBI), was designed and synthesized. In the design, pyrene (Py) and perylene bisimide (PBI) were specially chosen as the energy donor and the acceptor, respectively. Fluorescence studies revealed that (1) CPPBI shows a strong tendency to form supra-molecular assemblies, (2) the assemblies possess a high efficiency of fluorescence resonance energy transfer (FRET) via intermolecular interactions, and (3) the profile and position of its fluorescence emission are highly dependent upon the nature of its medium, but the medium shows little effect on the efficiency of the energy transfer, suggesting that the chromophores including both Py and PBI units enjoy some rotational and/or translational mobility in the aggregated state of the compound. Temperature- and concentration-dependent (1)H NMR spectroscopy studies revealed that both hydrogen-bonding and π-π stacking play a great role in stabilizing the assemblies of the compound, and confirmed the existence of π-π stacking between the Py moieties and between the PBI residues of the compound, of which the donor and the acceptor may have arranged in an appropriate orientation and at a suitable distance which are the key factors to determine the FRET efficiency. Moreover, the CPPBI-based film possesses unusual photochemical stability, and its emission is sensitive to the presence of some organic vapors, in particular aniline.

N-acetylglucosamine-based efficient, phase-selective organogelators for oil spill remediation.

Two simple, eco-friendly and efficient phase-selective gelators were developed for instant (<45 s) gelation of oil (either commercial fuels or pure organic liquids) from an oil-water mixture at room temperature to combat marine oil spills.

Terthiophene derivatives of cholesterol-based molecular gels and their sensing applications.

Three novel terthiophene derivatives of cholesterol (TtGC, TtLPC, TtDPC), of which the two building blocks are linked by a structure of glycine, l-phenylalanine, or d-phenylalanine, respectively, were designed and prepared, and their gelation behaviors in 26 liquids were tested. It was demonstrated that the compounds show different gelation abilities with the variation of the linker structures even though the variation is small. FTIR, (1)H NMR, and UV-vis measurements revealed that intermolecular hydrogen bonding and van der Waals interaction are the main driving forces for the gel formation. As for TtDPC, CD and AFM measurements revealed that it aggregated into chiral structures of left-helical feature in benzene. Importantly, the morphologies of the gel networks could be subtly adjusted via alteration of the gelator concentration. Considering the brightness in fluorescence and the unique micro/nanostructures of the gel networks, a fluorescent film (film 1) was fabricated by simple dip-coating of TtDPC/benzene solution (before gelation) onto a glass plate surface. Fluorescent studies demonstrated that the film is photochemically unstable. Two hours UV irradiation of the film results in film 2, which is almost fluorescent silence. However, the presence of HAc vapor or the vapors of some other volatile organic liquids induces new fluorescence emission, laying the foundation for creating a turn-on type fluorescent sensor of the organic vapors. Furthermore, as a new type of low-molecular-mass gelators (LMMGs), of which oligothiophene was employed as a building block, the present study has provided a possibility to explore the photo-/electronic applications of oligothiophenes via a molecular gel strategy.

Surface-enhanced molecular spectroscopy (SEMS) based on perfect-absorber metamaterials in the mid-infrared.

Surface-enhanced infrared absorption spectroscopy has attracted increased attention for direct access to molecular vibrational fingerprints in the mid-infrared. Perfect-absorber metamaterials (PAMs) with multi-band spectral responses and significant enhancement of the local near-field intensity were developed to improve the intrinsic absorption cross sections of absorption spectrum to identify the vibrational spectra of biomolecules. To verify its performance, the proposed infrared PAM array was used to identify the molecular stretches of a Parylene C film. The resonant responses of the infrared PAMs were accurately tuned to the vibrational modes of the C = C target bonds. The vibrational stretches of the C = C moiety were observed and the auto-fluorescence mechanisms of the Parylene C film were monitored. The unique properties of the PAMs indicate that this approach is a promising strategy for surface-enhanced molecular absorption spectroscopy (SEMS) in the mid-infrared region and for the tracking of characteristic molecular vibrational modes.

Ultrasensitive and selective sensing of heavy metal ions with modified graphene.

Swift fabrication of a non-covalently modified reduced graphene oxide electronic sensor has been developed. An unparalleled detection limit is demonstrated for Hg(2+), down to the picomolar range.

A diketopyrrolopyrrole-thiazolothiazole copolymer for high performance organic field-effect transistors.

A diketopyrrolopyrrole-thiazolothiazole copolymer with a short π-π stacking distance (3.52 Å), due to the introduction of heteroaromatic rings, exhibits a high charge mobility above 3.40 cm(2) V(-1) s(-1) at a relatively gentle annealing temperature.

An expedient synthesis of fused heteroacenes bearing a pyrrolo[3,2-b]pyrrole core.

Two linear fused heteroacenes bearing a pyrrolo[3,2-b]pyrrole core have been synthesized via a novel reductive ring closure methodology in three steps and in good overall yield. Preliminary OFET results showed that dinaphtho[2,3-b:2',3'-f]pyrrolo[3,2-b]pyrrole (DNPP) is a potential candidate for organic electronics.

Diketopyrrolopyrrole-containing quinoidal small molecules for high-performance, air-stable, and solution-processable n-channel organic field-effect transistors.

We report the synthesis, characterization, and application of a novel series of diketopyrrolopyrrole (DPP)-containing quinoidal small molecules as highly efficient n-type organic semiconductors in thin film transistors (TFTs). The first two representatives of these species exhibit maximum electron mobility up to 0.55 cm(2) V(-1) s(-1) with current on/current off (I(on)/I(off)) values of 10(6) for 1 by vapor evaporation, and 0.35 cm(2) V(-1) s(-1) with I(on)/I(off) values of 10(5)-10(6) for 2 by solution process in air, which is the first demonstration of DPP-based small molecules offering only electron transport characteristics in TFT devices. The results indicate that incorporation of a DPP moiety to construct quinoidal architecture is an effective approach to enhance the charge-transport capability.