Controlling Multiphoton Absorption Efficiency by Chromophore Packing in Metal-Organic Frameworks

David C. Mayer, Aurora Manzi, Raghavender Medishetty, Benedikt Winkler, Christian Schneider, Gregor Kieslich, Alexander Pöthig, Jochen Feldmann, Roland A. Fischer

Research output: Contribution to journalArticlepeer-review

55 Scopus citations

Abstract

Coordination polymers show great potential for the tailored design of advanced photonic applications by employing crystal chemistry concepts. One challenge for achieving a rational design of nonlinear optically active MOF materials is deriving fundamental structure-property relations of the interplay between the photonic properties and the spatial arrangements of optically active chromophores within the network. We here investigate two-photon-absorption (TPA)-induced photoluminescence of two new MOFs based on a donor-acceptor tetraphenylphenylenediamine (tPPD) chromophore linker (H4TPBD) and Zn(II) and Cd(II) as metal centers. The TPA efficiencies are controlled by the network topologies, degree of interpenetration, packing densities, and the specific spatial arrangement of the chromophores. The effects can be rationalized within the framework of established excited-state theories of molecular crystals. The results presented here demonstrate the key effect of chromophore orientation on the nonlinear optical properties of crystalline network compounds and allow for establishing quantitative design principles for efficient TPA materials.

Original languageEnglish
Pages (from-to)11594-11602
Number of pages9
JournalJournal of the American Chemical Society
Volume141
Issue number29
DOIs
StatePublished - 24 Jul 2019

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