TD-DFT Simulation and Experimental Studies of a Mirrorless Lasing of Poly[(9,9-dioctylfluorenyl-2,7-diyl)-co-(1,4-diphenylene-vinylene-2-methoxy-5-{2-ethylhexyloxy}-benzene)]

Abstract

In this work, we investigate the TD-DFT simulation, optical, and mirrorless laser properties of conjugated polymer (CP) Poly[(9,9-dioctylfluorenyl-2,7-diyl)-co-(1,4-diphenylene-vinylene-2-methoxy-5-{2-ethylhexyloxy}-benzene)], also known as (PFO-co-PPV-MEHB) or ADS125GE. TD-DFT calculations were performed for three monomer units with truncated tails using time-dependent density functional theory (TD-DFT) calculations. The calculations showed a highest occupied and lowest unoccupied molecular orbital (HOMO-LUMO) structure and a very high oscillator strength of 6.434 for the singlet-singlet transition at 374.43 nm. Experimentally, the absorption and fluorescence spectra were examined at various concentrations in verity of solvents, such as benzene, toluene, and hexane. The experimental results obtained in hexane were comparable with theoretical UV-VIS spectra calculated under vacuum. Amplified spontaneous emission (ASE) spectra peaked at approximately 509 nm for CO PFO-co-PPV-MEHB in solution and were obtained at suitable concentrations and pump energies. Additionally, the photochemical stability of this CP and coumarin (C510) were compared. Time-resolved spectroscopy (TRS) studies with a sub-nanosecond resolution were performed for the CO under various pump energies. These results showed the excited state dynamics and single-pass optical gain of CO PFO-co-PPV-MEHB.