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Laser Physics Letters

Femtosecond four-wave mixing spectroscopy on CdS crystal at room temperature

Иванин Константин Валерьевич, Andrey V. Leontyev, Vladimir S. Lobkov, Victor G. Nikiforov, К. М. Салихов, В. В. Самарцев, Georgy M. Safiullin

Published Jun 2, 2009• 10 citations
Publisher

Abstract

The results of the femtosecond four-wave mixing measurements performed on the CdS crystal at room temperature are reported. The dephasing time T d = 180 fs was obtained. The anti-Stokes shift of the primary photon echo spectrum with respect to the excitation spectrum was observed. The some peculiarities of the coherent responses decay curves indicate that this optical dephasing is due to the exciton-exciton interaction. The stimulated photon echo decay curves appear to have a fast decay component (the time constant of approximately 4.5 ps) in case the energy of exciting pulses exceeds the threshold value of 0.4 μJ.

DOI
10.1002/lapl.200910054

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The results of the femtosecond four-wave mixing measurements performed on the CdS crystal at room temperature are reported. The dephasing time T d = 180 fs was obtained. The anti-Stokes shift of the primary photon echo spectrum with respect to the excitation spectrum was observed. The some peculiarities of the coherent responses decay curves indicate that this optical dephasing is due to the exciton-exciton interaction. The stimulated photon echo decay curves appear to have a fast decay component (the time constant of approximately 4.5 ps) in case the energy of exciting pulses exceeds the threshold value of 0.4 μJ.
Femtosecond four-wave mixing coherent specstroscopy in CdS crystal on 790 nm at room temperature is analyzed. It is stated that the optical dephasing time is equal to 180 fs. Some specific features of the coherent responses' decay curves indicate that this optical dephasing is due to exciton-exciton interaction. The stimulated photon echo decay curves appear to have a fast decay component (the time constant of approximately 4.5 ps), in case when the energy of exciting pulses exceeds the threshold value of 0.4 μJ.
Time-resolved and integrated degenerated four-wave mixing experiments with two-photon excitation at a wavelength of 600–710 nm on a 30–40 μm thick cadmium sulfide crystal are presented for a temperature range from 5 to 300 K. A photon echo is observed showing quantum beats both at positive and negative delay times τ with a period of 0.7–0.8 ps. The signal decays exponentially with time constants of ≈170 fs at τ>0 and half as large at τ<0, independent of temperature. The results are discussed in terms of the decay of a high-density gas of e–h pairs, excitons and excitonic molecules highly out of equilibrium.
The dephasing of excitonic localized states is investigated in CdSx{\mathrm{CdS}}_{\mathit{x}}CdSx​${\mathrm{Se}}_{1\mathrm{\ensuremath{-}}\mathit{x}}$ mixed crystals at 2 K with low intensity femtosecond optical pulses. We observe a fast relaxation process which is first reported here. It is shown to be related to the creation of localized biexcitons via the exciton-biexciton transitions which act as an additional dephasing mechanism with a time constant ${\mathit{T}}_{2}^{\mathrm{ex}\mathrm{\ensuremath{-}}\mathrm{bi}}$ of 700 fs. The coherence between excitonic and biexcitonic states, which manifests by 800 fs period beats, is studied in detail. A simple model is presented which describes both the fast initial decay and the beating behavior.
We report femtosecond photon echo and four-wave mixing measurements performed on GaAs/AlGaAs heterostructure at room temperature. In femtosecond photon echo experiment the dephasing time was obtained, found to vary between 40 and 55 fs depending on carrier density. The dependence showed a power-law behavior T 2 ∝ N -0.22 , which indicates that major phase coherence loss is due to screened Coulomb electron-electron interaction. Transient grating experiments yielded the electron diffusion coefficient value of 200 cm 2 /s and electron relaxation time equal to 3 ns.
Phase relaxation of optical excitations in condensed matter can be studied by coherent four—wave—mixing experiments in the time domain without requiring assumptions on the spectral properties of the material. For inhomogeneously broadened transitions, three laser pulses at times t = 0, t = t21 and t = T with wave vectors k1, k2 and k3, respectively, generate a stimulated photon echo pulse, emitted time—delayed at t = T+t21 in the momentum—matching direction according to k3+k2−k1. As a function of t21 the echo amplitude decays due to scattering events, described by the dephasing time constant T2 [1].