Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 3, Issue 9, Pages 1222-1228Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jz300222h
Keywords
Molecular Structure; Quantum Chemistry; General Theory
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Funding
- Air Force Office of Scientific Research (AFOSR) [FA9550-10-1-0558]
- DARPA ZOE [W31R4Q09-1-0012]
- NSF via the PREM [0934212, CHE 0832622]
- Direct For Mathematical & Physical Scien
- Division Of Materials Research [934212] Funding Source: National Science Foundation
- Division Of Chemistry
- Direct For Mathematical & Physical Scien [0832622] Funding Source: National Science Foundation
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The two-photon absorption (2PA) spectrum of an organic single crystal is reported. The crystal is grown by self-nucleation of a subsaturated hot solution of acetonitrile, and is composed of an asymmetrical donor-a-acceptor cyanine-like dye molecule. To our knowledge, this is the first report of the 2PA spectrum of single crystals made from a cyanine-like dye. The linear and nonlinear properties of the single crystalline material are investigated and compared with the molecular properties of a toluene solution of its monomeric form. The maximum polarization-dependent 2PA coefficient of the single crystal is 52 +/- 9 cm/GW, which is more than twice as large as that for the inorganic semiconductor CdTe with a similar absorption edge. The optical properties, linear and nonlinear, are strongly dependent upon incident polarization due to anisotropic molecular packing. X-ray diffraction analysis shows a-stacking dimers formation in the crystal, similar to H-aggregates. Quantum chemical calculations demonstrate that this dimerization leads to the splitting of the energy bands and the appearance of new red-shifted 2PA bands when compared to the solution of monomers. This trend is opposite to the blue shift in the linear absorption spectra upon H-aggregation.
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