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Main Authors: Nwosu, Ikechukwu D, Matasović, Lujo, Ramos, Tárcius N, Phuoc, Nguyen Le, Londi, Giacomo, Gillett, Alexander J, Toolan, Daniel T W, Smith, Charles T, Whitehead, George F S, Blanchard-Desce, Mireille, Daniel, Jonathan, Linnolahti, Mikko, Olivier, Yoann, Romanov, Alexander S
Format: Preprint
Published: 2026
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Online Access:https://arxiv.org/abs/2603.05039
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author Nwosu, Ikechukwu D
Matasović, Lujo
Ramos, Tárcius N
Phuoc, Nguyen Le
Londi, Giacomo
Gillett, Alexander J
Toolan, Daniel T W
Smith, Charles T
Whitehead, George F S
Blanchard-Desce, Mireille
Daniel, Jonathan
Linnolahti, Mikko
Olivier, Yoann
Romanov, Alexander S
author_facet Nwosu, Ikechukwu D
Matasović, Lujo
Ramos, Tárcius N
Phuoc, Nguyen Le
Londi, Giacomo
Gillett, Alexander J
Toolan, Daniel T W
Smith, Charles T
Whitehead, George F S
Blanchard-Desce, Mireille
Daniel, Jonathan
Linnolahti, Mikko
Olivier, Yoann
Romanov, Alexander S
contents Advanced photonic materials showing two-photon absorption (2PA) have been widely explored to develop three-dimensional imaging, micro and nanofabrication, all-optical switching, lithography on a nanoscale and many other enabling technologies. These all require nonlinear absorption chromophores with intrinsic 2PA cross-sections and long-term photo-and thermal stability. Here, we disclose the very first example of the dipolar carbenemetal-amide (CMA) material showing a enhanced 2PA cross-section up to 105 GM. Overall molecular design considerations such as extended $π$-conjugation (to increase polarizability), minimizing the singlet-triplet energy gap ($Δ$E ST ), and using heavy metal atoms are the first design principles to obtain bright one-and two-photon excited thermally activated delayed fluorescence (TADF) material, showing one of the highest radiative rate of 2.18$\bullet$10 6 s -1 across CMA materials. Bright red CMA 2P-TADF material shows excellent photostability (LT 50 = 3 h) to 20 mW femtosecond pulsed laser excitation at 1000 nm, encouraging further CMA exploration for future applications in advanced photonic technologies requiring third-order nonlinear optical properties.
format Preprint
id arxiv_https___arxiv_org_abs_2603_05039
institution arXiv
publishDate 2026
record_format arxiv
spellingShingle Enhanced Third-Order Optical Nonlinearity in a Dipolar Carbene-Metal-Amide Material with Two-Photon Excited Delayed Fluorescence
Nwosu, Ikechukwu D
Matasović, Lujo
Ramos, Tárcius N
Phuoc, Nguyen Le
Londi, Giacomo
Gillett, Alexander J
Toolan, Daniel T W
Smith, Charles T
Whitehead, George F S
Blanchard-Desce, Mireille
Daniel, Jonathan
Linnolahti, Mikko
Olivier, Yoann
Romanov, Alexander S
Chemical Physics
Advanced photonic materials showing two-photon absorption (2PA) have been widely explored to develop three-dimensional imaging, micro and nanofabrication, all-optical switching, lithography on a nanoscale and many other enabling technologies. These all require nonlinear absorption chromophores with intrinsic 2PA cross-sections and long-term photo-and thermal stability. Here, we disclose the very first example of the dipolar carbenemetal-amide (CMA) material showing a enhanced 2PA cross-section up to 105 GM. Overall molecular design considerations such as extended $π$-conjugation (to increase polarizability), minimizing the singlet-triplet energy gap ($Δ$E ST ), and using heavy metal atoms are the first design principles to obtain bright one-and two-photon excited thermally activated delayed fluorescence (TADF) material, showing one of the highest radiative rate of 2.18$\bullet$10 6 s -1 across CMA materials. Bright red CMA 2P-TADF material shows excellent photostability (LT 50 = 3 h) to 20 mW femtosecond pulsed laser excitation at 1000 nm, encouraging further CMA exploration for future applications in advanced photonic technologies requiring third-order nonlinear optical properties.
title Enhanced Third-Order Optical Nonlinearity in a Dipolar Carbene-Metal-Amide Material with Two-Photon Excited Delayed Fluorescence
topic Chemical Physics
url https://arxiv.org/abs/2603.05039