New nonlinear optical crystal of rhodamine 590 acid phthalate

Sesha Bamini Nariyangadu*, Tenzin Choedak, Ezekiel Joy Padma Malar, Junsheng Chen, Erling Thyrhaug, Pushpendra Kumar, Jinming Zhou, Vidyalakshmi Yechuri, Suman Kalyan Pal, Sven Lidin, Kejalakshmy Namassivayane Thangadhorai, Khadga J. Karki, Tönu Pullerits

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

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 γof 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.

Original languageEnglish
Pages (from-to)20863-20873
Number of pages11
JournalACS Omega
Volume5
Issue number33
DOIs
StatePublished - 25 Aug 2020
Externally publishedYes

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