TITLE

Resonant third-harmonic generation in all-trans β-carotene: The vibronic origins of the third-order nonlinear susceptibility in the visible region

AUTHOR(S)
van Beek, J. B.; Kajzar, F.; Albrecht, A. C.
PUB. DATE
November 1991
SOURCE
Journal of Chemical Physics;11/1/1991, Vol. 95 Issue 9, p6400
SOURCE TYPE
Academic Journal
DOC. TYPE
Article
ABSTRACT
The dispersion of the modulus of the third-order nonlinear susceptibility, |χ(3)zzzz(-3ω;ω,ω,ω)|, of an all-trans β-carotene doped polystyrene thin film has been measured by third-harmonic generation throughout the 1 1Bu absorption band of the β-carotene. The observed dispersion is interpreted in terms of a three-electronic state model including explicit regard to six Franck–Condon active normal modes in the resonant electronic state. Both the sum-over-states method and, equivalently, the time domain approach are used. A fit of the three-state model to the data shows that the large nonlinear susceptibility of β-carotene in this wavelength range can be explained by strong dipole coupling between the strong one-photon allowed 1 1Bu state and a nearby two-photon allowed n 1Ag state. The electric dipole transition moment between the 1 1Bu excited state and the n 1Ag excited state, located at 22 200 cm-1, was determined to be 31 D.
ACCESSION #
7619501

 

Related Articles

  • Potential energy curves and dipole transition moments to the ground state of the system Ar[sup *](3p[sup 5]4s, [sup 3]P, [sup 1]P)+Ne. Petsalakis, Ioannis D.; Buenker, Robert J.; Lieberman, Heinz-Peter; Alekseyev, Aleksey B.; Devdariani, Alexander Z.; Theodorakopoulos, Giannoula // Journal of Chemical Physics;10/8/2000, Vol. 113 Issue 14 

    Relativistic core-potential calculations have been carried out on Ω states resulting from the interaction of Ar[sup *](3p[sup 5]4s, [sup 3]P, [sup 1]P) with ground state Ne atoms. The results yield the correct asymptotic limits for the atomic states of Ar while shallow minima (700-800 cm-1)...

  • Rotationally resolved ultraviolet–ultraviolet double resonance study of the nonplanar E state of acetylene. Lundberg, James K.; Jonas, David M.; Rajaram, Bhavani; Chen, Yongqin; Field, Robert W. // Journal of Chemical Physics;11/15/1992, Vol. 97 Issue 10, p7180 

    In centrosymmetric molecules such as acetylene, one expects one-photon and two-photon spectroscopy to be mutually exclusive by the gu electric dipole selection rule. An ultraviolet–ultraviolet double resonance (UVUVDR) spectrum of the 74 000–78 000 cm-1 region of acetylene,...

  • Excited-state dipole moments of SO2. II. Heitz, S.; Schmalzigaug, K.; von Moers, F.; Hese, A. // Journal of Chemical Physics;11/15/1992, Vol. 97 Issue 10, p7174 

    Determination of electric dipole moments on SO2 molecules in the region of the A 1A2 and B 1B1 states is reported. The Stark splittings and shifts of single rovibronic lines in several vibronic bands were measured by high-resolution laser spectroscopy in a supersonic molecular beam....

  • Theoretical dipole moment functions involving the a 3Π and a’ 3Σ+ states of carbon monoxide. Peterson, Kirk A.; Woods, R. Claude // Journal of Chemical Physics;10/1/1990, Vol. 93 Issue 7, p5029 

    Potential energy and dipole moment functions have been calculated for the first two excited electronic states of CO by several ab initio methods using large Gaussian basis sets. Similar calculations on the ground state have also been performed to provide a basis for comparison. The types of...

  • Structural Properties of Polyimides and the Mechanism of Carrier Photogeneration in Polyimide-Based Molecular Complexes. Aleksandrova, E. L. // Optics & Spectroscopy;Jul2002, Vol. 93 Issue 1, p118 

    The relation of photophysical parameters (quantum yields of carrier photogeneration and Coulomb-coupled pair formation, thermalization radius, and dipole moments in an excited state) to features of chemical structure, such as the ionization potential of a donor fragment and the electron affinity...

  • Intervalence transition in triarylamine mixed-valence systems: A time-dependent density functional theory study. Coropceanu, V.; Malagoli, M.; Andre´, J. M.; Bre´das, J. L. // Journal of Chemical Physics;12/8/2001, Vol. 115 Issue 22, p10409 

    A theoretical model is developed to describe the intervalence transitions in the mixed-valence N,N,N,[sup ′]N[sup ′]-tetrakis(4-methoxyphenyl)-1, 4-benzenediamine system. The excited-state energies and transition dipole moments are evaluated by means of time-dependent density...

  • Excited-state dipole moments of SO2. von Moers, F.; Schmalzigaug, K.; Schmoldt, A.; Heitz, S.; Hese, A. // Journal of Chemical Physics;6/1/1990, Vol. 92 Issue 11, p6391 

    High resolution ultraviolet spectroscopy of SO2 in a cold supersonic beam is reported. The behavior of single rovibronic lines of the E band (305 nm) and the 322 nm band was investigated in an electric field of up to 12 kV/cm. The dipole moment of the 1 A1 state was determined to be 1.85 (0.03)...

  • Reverse saturable absorption of short polarized light pulses. Band, Yehuda B. // Journal of Chemical Physics;12/1/1985, Vol. 83 Issue 11, p5453 

    We describe the absorption characteristics of polarized light pulses of short temporal duration in media with a ground state absorption cross section and large excited state absorption cross section. The effects of rotational diffusion, pulse depletion, finite pulse propagation time, and...

  • Electronic properties of an organometallic d 0 precatalyst in the ground and excited states. Loukova, G. V.; Milov, A. A.; Vasiliev, V. P.; Smirnov, V. A. // Doklady Physical Chemistry;Nov2007, Vol. 417 Issue 1, p293 

    The article discusses the study which examined the dipole moments of the metallocene precatalyst in the ground and excited states in different media typical of catalysis and organometallic synthesis. The dipole moments will be estimated by combined photophysical methods and quantum-chemical...

Share

Read the Article

Courtesy of VIRGINIA BEACH PUBLIC LIBRARY AND SYSTEM

Sorry, but this item is not currently available from your library.

Try another library?
Sign out of this library

Other Topics