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Exceptionally High Two-Photon Absorption Cross Sections in Quinoidal Diazaacene-Bithiophene Derivatives
Gabriel Sauter1, Antonia Papapostolou2, Audrey Pollien1,3
1Physikalisch-Chemisches Institut, Universität Heidelberg, Im Neuenheimer Feld 253, 69120, Heidelberg, Germany.
This study reveals exceptionally large two-photon absorption (2PA) cross sections in novel heterophenoquinones. These findings highlight their potential for advanced optical applications.
Area of Science:
- Materials Science
- Quantum Chemistry
- Optoelectronics
Background:
- Two-photon absorption (2PA) is crucial for advanced optical materials.
- Organic chromophores are being explored for their 2PA properties.
- Heterophenoquinones offer unique electronic structures.
Purpose of the Study:
- To investigate the 2PA properties of (azaacene-annulated) heterophenoquinones.
- To correlate molecular structure with 2PA cross sections.
- To elucidate the mechanism behind strong 2PA.
Main Methods:
- Synergistic experimental and theoretical analyses.
- Measurement of 2PA cross sections across a broad spectral range.
- Quantum chemical calculations for mechanism elucidation.
Main Results:
- Exceptionally large 2PA cross sections observed, up to 51770 GM in the 850-950 nm range.
- Significant 2PA cross sections (up to 4100 GM) found in the 1400-1600 nm range.
- Experimental findings supported and explained by quantum chemical calculations.
Conclusions:
- The studied heterophenoquinones exhibit outstanding 2PA performance for their molecular size.
- High oscillator strength and coupling to excited states drive the large 2PA cross sections.
- The acceptor-π-donor-π-acceptor motif facilitates strong 2PA and optimal molecular alignment.
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