Observation of aligned dipoles and angular chromism of exciplexes in organic molecular heterostructures.

The dipole characteristics of Frenkel excitons and charge-transfer excitons between donor and acceptor molecules in organic heterostructures such as exciplexes are important in organic photonics and optoelectronics. For the bilayer of the organic donor 4,4',4''-tris[(3-methylphenyl)phenylamino]triphenylamine and acceptor 2,4,6-tris(biphenyl-3-yl)-1,3,5-triazine molecules, the exciplexes form aligned dipoles perpendicular to the Frenkel excitons, as observed in back focal plane photoluminescence images. The angular chromism of exciplexes observed in the 100 meV range indicates possible delocalization and angle-sensing photonic applications. The blue shift of the peak position and increase in the linewidth of photoluminescene spectra with increasing excitation power are caused by the repulsive aligned exciplex dipole moments with a long lifetime (4.65 µs). Electroluminescence spectra of the exciplex from organic light-emitting diodes using the bilayer are blue-shifted with increasing bias, suggesting unidirectional alignment of the exciplex dipole moments. The observation of exciplex dipole moment alignments across molecular interfaces can facilitate the controlled coupling of exciton species and increase efficiency of organic light-emitting diodes.

Charge-Transfer Effect and Enhanced Photoresponsivity of WS2- and MoSe2-Based Field Effect Transistors with π-Conjugated Polyelectrolyte.

The characteristics of field effect transistors (FETs) fabricated using two-dimensional (2D) transition-metal dichalcogenides (TMDCs) can be modulated by surface treatment of the active layers. In this study, an ionic π-conjugated polyelectrolyte, poly(9,9-bis(4'-sulfonatobutyl)fluorene-alt-1,4-phenylene) potassium (FPS-K), was used for the surface treatment of MoSe2 and WS2 FETs. The photoluminescence (PL) intensities of monolayer (1L)-MoSe2 and 1L-WS2 clearly decreased, and the PL peaks were red-shifted after FPS-K treatment, suggesting a charge-transfer effect. In addition, the n-channel current of both the MoSe2 and WS2 FETs increased and the threshold voltage (Vth) shifted negatively after FPS-K treatment owing to the charge-transfer effect. The photoresponsivity of the MoSe2 FET under light irradiation (λex = 455 nm) increased considerably, from 5300 A W-1 to approximately 10 000 A W-1, after FPS-K treatment, and similar behavior was observed in the WS2 FET. The results can be explained in terms of the increase in electron concentration due to photogating. The external quantum efficiency and photodetectivity of both FETs were also enhanced by the charge-transfer effect resulting from surface treatment with FPS-K containing mobile cations (K+) and fixed anions (SO3-), as well as by the photogating effect. The variation in charge-carrier density due to the photogating and charge-transfer effects is estimated to be approximately 2 × 1012 cm-2. The results suggest that π-conjugated polyelectrolytes such as FPS-K can be a promising candidate for the passivation of TMDC-based FETs and obtaining enhanced photoresponsivity.