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• W2069966312 abstract "We used a variety of nonlinear optical (NLO) spectroscopies for studying the excited states order and primary photoexcitations in disubstituted polyacetylene (DPA). The NLO spectroscopies include ultrafast pump-probe photomodulation in a broad spectral range of 0.2--2.5 eV, two-photon absorption in the range of 3.2--4.2 eV, and electroabsorption (EA) in the range of 2.3--4.1 eV. For completeness we also measured the linear-absorption and photoluminescence spectra. We found that the primary photoexcitations in DPA are singlet excitons with three photoinduced absorption (PA) bands, ${text{PA}}_{0}$ at 0.6 eV, ${text{PA}}_{1}$ at 1 eV, and ${text{PA}}_{2}$ at 1.6 eV, respectively, and a stimulated emission band at $ensuremath{sim}2.5text{ }text{eV}$. This is in contrast to other $ensuremath{pi}$-conjugated polymers where the singlet excitons are characterized by two PA bands and a stimulated emission (SE) band. We conclude that in addition to the four essential excited states known to determine the NLO spectra of $ensuremath{pi}$-conjugated polymers, namely, $1{A}_{g}$, $1{B}_{u}$, $text{m}{A}_{g}$, and $text{n}{B}_{u}$; in DPA there is another important complex of states at $ensuremath{sim}3.3text{ }text{eV}$ that contains almost degenerate states with odd and even parity symmetries (dubbed here transverse excited state or TES) that is probably reminiscent of the $2{A}_{g}$ state in unsubstituted trans-polyacetylene, which lies in between the $1{B}_{u}$ and $text{m}{A}_{g}$ of which dipole moment has a strong component perpendicular to the chain direction. In support for this model we found that the depolarization ratio of the EA spectrum drastically changes around the TES from a value of $ensuremath{sim}2$ for $ensuremath{hbar}ensuremath{omega}<3text{ }text{eV}$ to $ensuremath{sim}0.5$ for $ensuremath{hbar}ensuremath{omega}>3.3text{ }text{eV}$." @default.
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• W2069966312 date "2010-05-04" @default.
• W2069966312 modified "2023-09-24" @default.
• W2069966312 title "Nonlinear optical spectroscopy of excited states in disubstituted polyacetylene" @default.
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• W2069966312 doi "https://doi.org/10.1103/physrevb.81.205103" @default.
• W2069966312 hasPublicationYear "2010" @default.
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