55 research outputs found
Grain engineering for improved charge carrier transport in two-dimensional lead-free perovskite field-effect transistors
Controlling crystal growth and reducing the number of grain boundaries are crucial to maximize the charge carrier transport in organic-inorganic perovskite field-effect transistors (FETs). Herein, the crystallization and growth kinetics of a Sn(ii)-based 2D perovskite, using 2-thiopheneethylammonium (TEA) as the organic cation spacer, were effectively regulated by the hot-casting method. With increasing crystalline grain size, the local charge carrier mobility is found to increase moderately from 13 cm2 Vâ1 sâ1 to 16 cm2 Vâ1 sâ1, as inferred from terahertz (THz) spectroscopy. In contrast, the FET operation parameters, including mobility, threshold voltage, hysteresis, and subthreshold swing, improve substantially with larger grain size. The optimized 2D (TEA)2SnI4 transistor exhibits hole mobility of up to 0.34 cm2 Vâ1 sâ1 at 295 K and a higher value of 1.8 cm2 Vâ1 sâ1 at 100 K. Our work provides an important insight into the grain engineering of 2D perovskites for high-performance FETs
Organic Electron Acceptors Comprising a DicyanomethyleneâBridged Acridophosphine Scaffold: The Impact of the Heteroatom
Stable twoâelectron acceptors comprising a dicyanomethyleneâbridged acridophosphine scaffold were synthesized and their reversible reduction potentials were efficiently tuned through derivatization of the phosphorus center. Xâray crystallographic analysis combined with NMR, UV/Vis, IR spectroscopic, and electrochemical studies, supported by theoretical calculations, revealed the crucial role of the phosphorus atom for the unique redox, structural, and photophysical properties of these compounds. The results identify the potential of these electron deficient scaffolds for the development of functional nâtype materials and redox active chromophores upon further functionalization
New strong organic acceptors by cycloaddition of TCNE and TCNQ to donor-substituted cyanoalkynes
Donor-substituted 1,1,2,4,4-pentacyanobuta-1,3-dienes and a cyclohexa-2,5-diene-1,4-diylidene-expanded derivative were prepared by a [2 + 2] cycloaddition of tetracyanoethene (TCNE) or 7,7,8,8-tetracyanoquinodimethane (TCNQ) to anilino-substituted cyanoalkynes, followed by retro-electrocyclisation; they feature intense bathochromically-shifted intramolecular chargetransfer bands and undergo their first one-electron reductions at potentials similar to those reported for TCNE and TCNQ
Stability of odd versus even electron gas-phase (quasi)molecular ions derived from pyridine-substituted N-heterotriangulenes
Electrospray ionisation of N-heterotriangulenes (i.e. dimethylmethylene-bridged triphenylamines) with up to three pyridyl groups at their periphery, produces the true radical cation ([M]+*) and the protonated molecule ([M+H]+) simultaneously. These ions are studied as model systems to illustrate the stability alternation of odd- versus even-electron ions in energy-dependent collision-induced dissociation (CID) experiments. All ions show the same fragmentation pattern, the consecutive loss of three methyl radicals (*CH3) from the dimethylmethylene bridges of the central triangulene core. [M]+* ions dissociate at much lower collision energies than their [M+H]+ counterparts. The radical cation forms a singlet fragment with an extended aromatic system that is energetically favoured. Ab initio and density functional theory calculations support this interpretation and allow the assignment of the electronic structure of the fragment ions. Consecutive collision-induced dissociations provide a better match with theory when studied with an ion trap, rather than a linear quadrupole. This is attributed to the resonant nature of the excitation of intermediate ions
OnâSurface Assembly of Hydrogenâ and HalogenâBonded Supramolecular GraphyneâLike Networks
Demonstrated here is a supramolecular approach to fabricate highly ordered monolayered hydrogenâ and halogenâbonded graphyneâlike twoâdimensional (2D) materials from triethynyltriazine derivatives on Au(111) and Ag(111). The 2D networks are stabilized by Nâ
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HâC(sp) bonds and Nâ
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BrâC(sp) bonds to the triazine core. The structural properties and the binding energies of the supramolecular graphynes have been investigated by scanning tunneling microscopy in combination with densityâfunctional theory calculations. It is revealed that the Nâ
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BrâC(sp) bonds lead to significantly stronger bonded networks compared to the hydrogenâbonded networks. A systematic analysis of the binding energies of triethynyltriazine and triethynylbenzene derivatives further demonstrates that the X3âsynthon, which is commonly observed for bromobenzene derivatives, is weaker than the X6âsynthon for our bromotriethynyl derivatives
Impact of Electronic Coupling, Symmetry, and Planarization on One- and Two-Photon Properties of Triarylamines with One, Two, or Three Diarylboryl Acceptors
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