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Single-photon pumping and two-photon probing spectroscopy for the determination of absorption cross-sections in an organic semiconductor

Xinping Zhang, Yajun Xia, and Richard H. Friend

Open Access Open Access

Abstract

We investigate the bleaching of two-photon absorption by single-photon excitation using femtosecond transient absorption measurements on the prototypical polyfluorene (F8), and thus introduce single-photon pumping and two-photon probing spectroscopy for the determination of absorption cross-sections in an organic semiconductor. Single-photon excitation at 3.1 eV rearranges the population distributions on the singlet excited state (1Bu ) and on the ground state (1Ag ), and probe pulses at 1.55 eV will thus be absorbed both by the singlet excited state through a single-photon process and by the partially depopulated ground state for two-photon transition from 1Ag to mAg . As a result, the two-photon absorption will be partially bleached, introducing a modulation to the total transient absorption. Probe intensity dependence of the transient absorption enables simultaneous determination of the two-photon absorption (mAg ←1Ag ) and exciton absorption (kAg ←1Bu ) cross-sections at 1.55 eV.

©2005 Optical Society of America

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Figures (5)
Fig. 1.
Fig. 1. Transition mechanisms related to the transient absorption in single-photon pumping (at 2ω) and two-photon probing (at 2ω) spectroscopy.

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Fig. 2.
Fig. 2. Absorption spectrum of the F8/p-Xylene solution with a concentration of 0.1 mg/ml. Inset: the chemical structure of F8.

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Fig. 3.
Fig. 3. Dependence of the TA dynamics on the probe (1.55 eV) intensities at a pump (3.1 eV) intensity of 96 μJ/cm2. The filled circles are TA dynamics measurements at 2 eV for the lifetime comparison. The calculation of the absorption cross-sections have been performed for a delay of 4 ps, as marked by the dash-dotted vertical line.

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Fig. 4.
Fig. 4. Pump intensity dependence of the TA dynamics at the two-photon frequency. The pump fluence at 3.1 eV was changed from 22 μJ/cm2 to 176 μJ/cm2 with the probe fluence at 1.55 eV fixed at (a) 199 μJ/cm2 and (b) 1.99 mJ/cm2, respectively. (c) Comparison between the measurements in (a) and (b) with the simulations using the measured absorption cross-sections.

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Fig. 5.
Fig. 5. Simulated contour lines showing the absolute values of the TA (|ΔT/T|) as a function of the pump and the probe fluences.

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Equations (7)

Equations on this page are rendered with MathJax. Learn more.

∂ N 2 ∂ t = − N 2 τ 2 + N 1 P 1
N 2 ( t ) = N 0 P 1 τ 2 1 + P 1 τ 2 [ 1 − e − ( 1 τ 2 + P 1 ) τ P ] · e − ( t − τ P ) τ 2 ,
∂ N 3 ∂ t = − N 3 τ 3 + N 1 P 2
∂ N 2 ∂ t = − N 2 τ 2 + N 3 τ 3 − N 2 P 3
N 0 ≈ N 1 + N 2 + N 3
d I ω dz = − β 1 I ω − β 2 I ω 2 .
Δ T T = I ω on I ω off − 1
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