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Conformational relaxation of -conjugated polymer radical anion on picosecond scale
34.T. Hasegawa, Y. Iwasa, T. Koda, H. Kishida, Y. Tokura, S. Wada, H. Tashiro, H. Tachibana, and M. Matsumoto, Phys. Rev. B 54, 11365 (1996).
51.Artificial peak shift which arises from the overlap between a peak and a slope was confirmed not to appear by using this protocol. No distinct difference was found for the use of Lorentzian function instead of Gaussian.
52.It is well-known that polysilane tend to be degraded via main chain scission, e.g., upon exposure to UV light, resulting in the blueshift and decrease in transition of neutral polymers. We note that this degradation effect on the observed spectrum change is negligibly small, which is supported by the fact that the transmitted light intensity without beam (a reference light for transient spectroscopy) was constant during ca. 3000 beam shots (Fig. S1, Ref. 53), there was no significant difference in the backwards- or second-scanned kinetics, and our picosecond pulse radiolysis system can, with the help of double pulse detection scheme, minimize the effect of steady-state PA change.
See EPAPS Document No. for transmitted light intensity used as reference during picosecond pulse radiolysis of PBPS, experimental estimation of
and rate constant:
obtained at 1300 nm, time-dependent
: standard deviation of Gaussian function expressed in Eq. (6)
, and the experiments of smaller PBPS concentrations (0.02 and
). For more information on EPAPS, see http://www.aip.org/pubservs/epaps.html
56.M. Smoluchowski, Z. Phys. Chem. 92, 129 (1917).
58.F. C. Grozema, R. J. O. M. Hoofman, L. P. Candeias, M. P. De Haas, J. M. Warman, and L. D. A. Siebbeles, J. Phys. Chem. A 107, 5976 (2003).
62.M. J. Frisch, G. W. Trucks, H. B. Schlegel et al., GAUSSIAN 03, Revision C.02, Gaussian, Inc., Wallingford, CT, 2004. The complete reference is on EPAPS (Ref. 53). The MD was performed by MOPAC program.
63.The hexamer of oligosilane of which substituent was replaced by methyl instead of -butylphenyl was employed from the reason of computational resource limitation. The end of the chain was also caped by methyl because of the same reason. The effect of substituents on extinction coefficient and transition energy is significant especially for phenyl-group due to the mixing (Refs. 3 and 8) and transition [A. Sharma, U. Lourderaj, G. Deepak, and N. Sathyamurthy, J. Phys. Chem. B 109, 15860 (2005)]; however, we adopted the present model to focus on the conformational dynamics of Si backbone.
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