Modeling of non-Lorentzian two-photon absorption line shape in dipolar chromophore

We present a new approach to modeling of homogeneous line shape in two-photon absorption (2PA) spectra of chromophores with large permanent dipole moment difference between the ground- and excited electronic states using numerical solution of stochastic two-level density matrix equation of motion. Good agreement with experimental 2PA line shapes is obtained for S1←S0 transition of Styryl 9M, which allows us to estimate that the permanent dipole moment difference varies in this chromophore within the S1←S0 band in the range, Δμ = 12 - 25 D.

[1]  Mikhail Drobizhev,et al.  Narrowing of the homogeneous two-photon absorption line width in two-level dipolar system , 2008, SPIE OPTO.

[2]  Richard L. Sutherland,et al.  Excited-state characterization and effective three-photon absorption model of two-photon-induced excited-state absorption in organic push-pull charge-transfer chromophores , 2005 .

[3]  M. Drobizhev,et al.  Photon energy upconversion in porphyrins: one-photon hot-band absorption versus two-photon absorption , 2003 .

[4]  S. Mukamel.  Principles of Nonlinear Optical Spectroscopy , 1995 .

[5]  M. Drobizhev,et al.  Color hues in red fluorescent proteins are due to internal quadratic Stark effect. , 2009, The journal of physical chemistry. B.

[6]  Ajaya K. Singh,et al.  Relaxation Dynamics in the Excited States of LDS-821 in Solution , 2001 .

[7]  Zhi‐zhan Xu,et al.  Carrier-envelope phase dependence of few-cycle ultrashort laser pulse propagation in a polar molecule medium. , 2007, Physical review letters.

[8]  H. Ågren,et al.  Quantum-classical modeling of nonlinear pulse propagation in a dissolved two-photon active chromophore. , 2006, The journal of physical chemistry. B.

[9]  D. Wiersma,et al.  Femtosecond non-Markovian optical dynamics in solution. , 1991, Physical review letters.

[10]  A. Myers.  Molecular electronic spectral broadening in liquids and glasses. , 1998, Annual review of physical chemistry.

[11]  M. Drobizhev,et al.  Two-photon absorption standards in the 550-1600 nm excitation wavelength range. , 2008, Optics express.

[12]  Aleksander Rebane,et al.  Quantitative Prediction of Two-Photon Absorption Cross Section Based on Linear Spectroscopic Properties† , 2008 .

[13]  Aleksander Rebane,et al.  Environment-sensitive two-photon dye , 2008, Organic Photonics + Electronics.

[14]  I. Khoo.  Nonlinear Organic Liquid-Cored Fiber Array for All-Optical Switching and Sensor Protection Against Short-Pulsed Lasers , 2008, IEEE Journal of Selected Topics in Quantum Electronics.

[15]  Aleksander Rebane,et al.  Optimizing two-photon absorption for volumetric optical data storage , 2007 .