Photophysics and Spin-Physics Studies on Persistent Upconversion Luminescence from Nonlinearly Polarizable Ferroelectric-Like Lattice Prepared by Orderly Packing Donor–Acceptor Structures under Multiphoton Excitation

Yixuan Dou, Catherine Demangeat, Miaosheng Wang, Bogdan Dryzhakov, Kwang Sup Lee, André Jean Attias, Bin Hu

Research output: Contribution to journalArticlepeer-review

2 Scopus citations

Abstract

The ultralong-lived upconversion luminescence with the lifetime of 0.48 s in a broad spectral range (530–650 nm) is observed in CD49 (9-(3-(5-bromopyridin-3-yl)prop-2-yn-1-yl)-9H-carbazole) crystal designed with donor–acceptor (carbazole–pyridine) structures under infrared excitation, simultaneously accompanied with second harmonic generation (SHG). This phenomenon indicates orderly packing donor–acceptor structures form a nonlinearly polarizable ferroelectric-like lattice with ultralong-lived light-emitting states, leading to much prolonged nonlinear optical behaviors. The persistent upconversion luminescence together with SHG is largely reduced when lowering crystallinity. This implies that nonlinearly polarizable ferroelectric-like lattice provides the necessary condition to generate persistent upconversion luminescence. Evidently, persistent upconversion luminescence becomes completely lacking when only using ultralong-lived light-emitting states without nonlinearly polarizable ferroelectric-like lattice, exampled by 4-(dimethylamino)benzonitrile dispersed in polyvinyl alcohol matrix. Magneto-photoluminescence shows that persistent upconversion luminescence is essentially a super-delayed fluorescence from crystalline intermolecular charge-transfer excitons formed in the nonlinearly polarizable ferroelectric-like lattice. Magnetodielectrics indicate crystalline intermolecular charge-transfer excitons are coupled with nonlinearly polarizable ferroelectric-like lattice, leading to prolonged nonlinear optical behaviors shown as persistent upconversion luminescence through super delayed fluorescence. Therefore, crystalline intermolecular charge-transfer excitons formed in nonlinearly polarizable ferroelectric-like lattice provide an interesting platform to generate prolonged nonlinear optical behaviors toward developing persistent upconversion luminescence under multiphoton excitation.

Original languageEnglish
Article number2102002
JournalAdvanced Optical Materials
Volume10
Issue number5
DOIs
StatePublished - Mar 4 2022
Externally publishedYes

Keywords

  • crystalline charge-transfer excitons
  • ferroelectric lattices
  • multiphoton upconversion luminescence
  • persistent upconversion luminescence
  • super-delayed fluorescence

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