Abstract
The synthesis and crystal structure of rhodamine 590 acid phthalate (RhAP) have been reported. This novel solid-state rhodamine derivative not only has a longer fluorescence lifetime compared to rhodamine solid-state matrixes where emission is quenched but also possesses strong nonlinear optical characteristics. The static and dynamic first- and second-order hyperpolarizabilities were calculated using the time-dependent density functional theory at the B3LYP/6-31+G* level. The computed static values of β and γ of RhAP by the X-ray diffraction (XRD) structure were 31.9 × 10–30 and 199.0 × 10–36 esu, respectively. These values were about 62 times larger than the corresponding values in urea, an already well-known nonlinear optical material. The second-order hyperpolarizability of the compound was determined experimentally by measuring the two-photon absorption cross section using intensity-modulated light fields. The reported compound, excitable at near-infrared, exhibited frequency upconversion with the two-photon absorption coefficient enhanced by two orders of magnitude compared to that of the dye solution. Hosting the dye in the solid, at high concentrations, exploits the nonlinearity of the dye itself as well as results in significant excitonic effects including formation of broad exciton band and superradiance.
Highlights
Organic molecular crystals with strong nonlinear optical (NLO) response have received much attention owing to their potential applications in optoelectronics
The single crystals of rhodamine 590 acid phthalate (RhAP) were grown in an aqueous solution using the solution growth by slow evaporation at room temperature, as already reported.[24−26] The amount of the dye added to the KAP growth solution was approximately 1% of the amount of KAP salt that was added to the aqueous solution to reach saturation
A new nonlinear optical crystal was synthesized in an aqueous solution using a simple solution growth technique at room temperature by including an organic laser dye at high concentrations into the KAP crystal
Summary
Organic molecular crystals with strong nonlinear optical (NLO) response have received much attention owing to their potential applications in optoelectronics. Large molecular hyperpolarizability is one of the basic requirements for NLO applications. Organic dyes have applications in different fields due to their wide spectral range in the visible region.[15] These dyes can be used in solid, liquid, or gas phases, where their concentration and their absorption and gain can be readily controlled. Different solidstate materials like polymers, organic semiconductors, zeolites, sol−gel, and NLO crystals have been used as host media for organic laser dyes. These studies are aimed at the fabrication of dye-doped single-crystal microlasers.[16−29]
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