Visualizing electroluminescence process in light-emitting electrochemical cells.

Electroluminescence occurs via recombination reactions between electrons and holes, but these processes have not been directly evaluated. Here, we explore the operation dynamics of ionic liquid-based light-emitting electrochemical cells (LECs) with stable electroluminescence by multi-timescale spectroscopic measurements synchronized with the device operation. Bias-modulation spectroscopy, measuring spectral responses to modulated biases, reveals the bias-dependent behavior of p-doped layers varying from growth to saturation and to recession.

A Versatile and Simple Approach to Generate Light Emission in Semiconductors Mediated by Electric Double Layers.

The light-emitting device is the primary device for current light sources. In principle, conventional light-emitting devices need heterostructures and/or intentional carrier doping to form a p-n junction. This junction formation is, however, very difficult to achieve for most emerging semiconductors, and the fabrication of light-emitting devices is invariably a significant challenge.

High Current Injection into Dynamic p-n Homojunction in Polymer Light-Emitting Electrochemical Cells.

Ions and electrons in blends of polymer-electrolyte can work in ensemble to operate light-emitting electrochemical cells (LECs), in which the unique features of in situ formed p-n homojunctions offer efficient charge injection and transport. However, electrochemical features give rise to significant stability and speed issues due to limited electrochemical stability and low ion mobility, resulting in low brightness and a slow response of LECs. Here, these issues are overcome by the separate control of ionic and electronic charges, using a simple driving pulse superimposed on a small base voltage; ions with slow response are rearranged by a constant base voltage, while a high-voltage pulse, superimposed upon the base, injects electrons/holes which have fast response, with minimal effect on the ions.

Protonation-induced red-coloured circularly polarized luminescence of [5]carbohelicene fused by benzimidazole.

Benzimidazole-fused [5]carbohelicene ([5]HeliBI) was newly synthesized to examine the spectroscopic and chiroptical properties. The reversible protonation and deprotonation processes of [5]HeliBI were successfully investigated using (1)H NMR, absorption and fluorescence spectral measurements. We also confirmed the circularly polarized luminescence of protonated [5]HeliBI (H(+)-[5]HeliBI).

Synthetic Control of the Excited-State Dynamics and Circularly Polarized Luminescence of Fluorescent "Push-Pull" Tetrathia[9]helicenes.

A series of fluorescent "push-pull" tetrathia[9]helicenes based on quinoxaline (acceptor) fused with tetrathia[9]helicene (donor) derivatives was synthesized for control of the excited-state dynamics and circularly polarized luminescence (CPL) properties. In this work, introduction of a quinoxaline onto the tetrathia[9]helicene skeleton induced the "push-pull" character, which was enhanced by further introduction of an electron-releasing Me2 N group or an electron-withdrawing NC group onto the quinoxaline unit (denoted as Me2 N-QTTH and NC-QTTH, respectively). These trends were successfully discussed in terms of by electrochemical measurements and density functional theory (DFT) calculations.

Ambipolar light-emitting organic single-crystal transistors with a grating resonator.

Electrically driven organic lasers are among the best lasing devices due to their rich variety of emission colors as well as other advantages, including printability, flexibility, and stretchability. However, electrically driven lasing in organic materials has not yet been demonstrated because of serious luminescent efficiency roll-off under high current density. Recently, we found that the organic ambipolar single-crystal transistor is an excellent candidate for lasing devices because it exhibits less efficient roll-off, high current density, and high luminescent efficiency.

Ultrafast photoinduced electron transfer in face-to-face charge-transfer π-complexes of planar porphyrins and hexaazatriphenylene derivatives.

Charge-transfer (CT) π-complexes are formed between planar porphyrins and 1,4,5,8,9,12-hexaazatriphenylene (HAT) derivatives with large formation constants (, 10 M), exhibiting broad CT absorption bands. The unusually large formation constants result from close face-to-face contact between two planar π-planes of porphyrins and HAT derivatives. The redox potentials of porphyrins and HAT derivatives measured by cyclic voltammetry indicate that porphyrins and HAT derivatives act as electron donors and acceptors, respectively.

Formation of one-dimensional helical columns and excimerlike excited states by racemic quinoxaline-fused [7]carbohelicenes in the crystal.

A series of quinoxaline-fused [7]carbohelicenes (HeQu derivatives) was designed and synthesized to evaluate their structural and photophysical properties in the crystal state. The quinoxaline units were expected to enhance the light-emitting properties and to control the packing structures in the crystal. The electrochemical and spectroscopic properties and excited-state dynamics of these compounds were investigated in detail.

Hall-effect measurements probing the degree of charge-carrier delocalization in solution-processed crystalline molecular semiconductors.

Intramolecular structure and intermolecular packing in crystalline molecular semiconductors should have profound effects on the charge-carrier wave function, but simple drift mobility measurements are not very sensitive to this. Here we show that differences in the Hall resistance of two soluble pentacene derivatives can be explained with different degrees of carrier delocalization being limited by thermal lattice fluctuations. A combination of Hall measurements, optical spectroscopy, and theoretical simulations provides a powerful probe of structure-property relationships at a molecular level.

Band-like temperature dependence of mobility in a solution-processed organic semiconductor.

The mobility mu of solution-processed organic semiconductors has improved markedly to room-temperature values of 1-5 cm(2) V(-1) s(-1). In spite of their growing technological importance, the fundamental open question remains whether charges are localized onto individual molecules or exhibit extended-state band conduction like those in inorganic semiconductors. The high bulk mobility of 100 cm(2) V(-1) s(-1) at 10 K of some molecular single crystals provides clear evidence that extended-state conduction is possible in van-der-Waals-bonded solids at low temperatures.

High yield, single droplet electrode arrays for nanoscale printed electronics.

In this work we demonstrate two building blocks of a scalable manufacturing technology for nanoscale electronic devices based on direct-write printing: an architecture for high-yield printing of electrode gaps with 100 nm dimension and a low-temperature silver complex ink for integration of organic materials with high conductivity metal interconnects. We use single printed droplets that are made to dewet slowly from each other to allow reliable, high yield patterning even in the presence of certain surface defects.