Multi-photon absorption (MPA) is of increasing interest for applications in technologically important "windows" of the electromagnetic spectrum (near-infrared III, NIR-III, 1550-1870 nm; and the new 2080-2340 nm region); however, few molecules exist that display strong MPA at these long wavelengths. We herein report the syntheses of the first 2,5,8-s-heptazine-cored organometallic complexes, together with organic analogues. The complexes exhibit outstanding 3PA cross-sections in the NIR-III and exceptional 4PA cross-sections in the new 2080-2340 nm window. We demonstrate that replacing organic donor groups by organometallic units results in an order of magnitude increase in 3PA, the "switching on" of 4PA, and a dramatic improvement in photo-stability. Our results highlight the impressive outcomes possible with an "organometalation" approach to NLO materials design.
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http://dx.doi.org/10.1002/anie.202208168 | DOI Listing |
Nanoscale
January 2025
Department of Chemistry, Faculty of Science, Kyushu University, 744 Motooka, Nishi-ku, Fukuoka 819-0395, Japan.
We report photodissociation processes and spectral measurements upon photoabsorption of size-selected cationic silver clusters, Ag, stored in an ion trap. The experiment shows that small clusters ( ≲ 15) dissociate upon one-photon absorption, whereas larger ones require multiple photons up to five in the present study. The emergence of multi-photon processes is attributed to collisional cooling in the presence of a buffer helium gas in the trap, which competes with size-dependent dissociation rates.
View Article and Find Full Text PDFMicromodification in bulk undoped polymethylmethacrylate (PMMA) by single focused (numerical aperture (NA) = 0.25), 1030-nm 250-fs laser pump pulses was explored by pump self-transmittance; optical, 3D-scanning confocal photoluminescence (PL); Raman micro-spectroscopy; and optical polarimetric and interferometric microscopy. Starting from the threshold pulse energy = 0.
View Article and Find Full Text PDFAdv Funct Mater
October 2024
Department of Chemical and Biomolecular Engineering, University of California, Berkeley, CA 94720, USA.
Traditional deep fluorescence imaging has primarily focused on red-shifting imaging wavelengths into the near-infrared (NIR) windows or implementation of multi-photon excitation approaches. Here, we combine the advantages of NIR and multiphoton imaging by developing a dual-infrared two-photon microscope to enable high-resolution deep imaging in biological tissues. We first computationally identify that photon absorption, as opposed to scattering, is the primary contributor to signal attenuation.
View Article and Find Full Text PDFNanoscale Horiz
January 2025
Department of Chemistry and Centre for Atomic Engineering of Advanced Materials, Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education, Institutes of Physical Science and Information Technology and Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized Materials, Anhui University, Hefei, Anhui, 230601, China.
Recent developments in optical imaging techniques, particularly multi-photon excitation microscopy that allows studies of biological interactions at a deep cellular level, have motivated intensive research in developing multi-photon absorption fluorophores. Biological tissues are optically transparent in the near-infrared region. Therefore, fluorophores that can absorb light in the near-infrared (NIR) region by multi-photon absorption are particularly useful in bio-imaging.
View Article and Find Full Text PDFMulti-photon absorption in the second near-infrared (NIR-II) regime has attracted extensive attention due to biological imaging and frequency-upconverted lasing applications. We report the dispersion of four-photon absorption (4 PA) response in pristine and Ga-doped ZnO single crystals over the spectral range 1180-1350 nm. Femtosecond Z-scan results demonstrate that Ga doping can significantly enhance the 4 PA coefficient β of ZnO.
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