Journal
CHEMPHYSCHEM
Volume 14, Issue 15, Pages 3532-3542Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cphc.201300447
Keywords
density functional calculations; donor-acceptor systems; fluorescence; hydrogen bonds; photochemistry
Funding
- National Science Foundation [ECCS-0925712, CHE-0840431, CHE-0832622]
- US National Academy of Sciences [PGA-P210877]
- National Academy of Sciences of Ukraine [1.4.1.B/153, VC/157]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [0832622] Funding Source: National Science Foundation
- Div Of Electrical, Commun & Cyber Sys
- Directorate For Engineering [0925712] Funding Source: National Science Foundation
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The synthesis, linear photophysical, two-photon absorption (2PA), femtosecond transient absorption, and superfluorescence properties of a new symmetrical squaraine derivative (1) are reported. Steady-state linear spectral and photochemical properties, fluorescence lifetimes, and excitation anisotropy of 1 were investigated in various organic solvents. High fluorescence quantum yields (approximate to 0.7) and very high photostability (photodecomposition quantum yields approximate to 10(-6)-10(-8)) were observed. An open-aperture Z-scan method was used to obtain 2PA spectra of 1 over a broad spectral range (maximum 2PA cross section approximate to 1000 GM). Excited-state absorption (ESA) and gain was observed by femtosecond transient absorption spectroscopy, in which both reached a maximum at approximately 500 fs. Squaraine 1 exhibits efficient superfluorescence. The quantum chemical study of 1 revealed the simulated vibronic nature of the 1PA and 2PA spectra were in good agreement with experimental data; this may provide the ability to predict potential advanced photonic materials.
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