Issue 23, 2024

Exceptional three- to six-photon absorption at organometallic dendrimers

Abstract

The light-intensity dependence of multi-photon absorption (MPA) affords outstanding spatial control. Furthermore, compared to the higher-energy photons needed for analogous linear absorption, the lower-energy photons involved in MPA often correspond to important wavelengths, such as those of the biological and telecommunications “windows”. It is therefore of crucial importance to develop molecules that exhibit outstanding MPA cross-sections. However, although progress has been made with two-photon absorption, there is currently a dearth of efficient instantaneous n-photon absorbers (n > 2), a key reason being the scarcity of structure–property studies required to understand higher-order MPA. We herein report systematically-varied metallodendrimers up to third-generation in size, together with their nonlinear absorptive responses over the spectral range 600–2520 nm. We show that the dendrimers exhibit exceptional instantaneous three- to six-photon absorption cross-sections, with maximal values increasing with dendrimer generation and installation of solubilizing group, and we report that changing the groups at the dendrimer periphery can shift the wavelengths of the nPA maxima. We also describe time-dependent DFT studies that have facilitated assignment of the key linear and nonlinear transitions and disclosed the crucial role of the metal in the outstanding MPA performance.

Graphical abstract: Exceptional three- to six-photon absorption at organometallic dendrimers

Supplementary files

Article information

Article type
Edge Article
Submitted
17 Feb 2024
Accepted
13 May 2024
First published
14 May 2024
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY license

Chem. Sci., 2024,15, 8731-8739

Exceptional three- to six-photon absorption at organometallic dendrimers

L. Zhang, M. Morshedi, T. Schwich, R. Kobayashi and M. G. Humphrey, Chem. Sci., 2024, 15, 8731 DOI: 10.1039/D4SC01127A

This article is licensed under a Creative Commons Attribution 3.0 Unported Licence. You can use material from this article in other publications without requesting further permissions from the RSC, provided that the correct acknowledgement is given.

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