Research ArticleOPTICS

Deconvolution of optical multidimensional coherent spectra

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Science Advances  01 Jun 2018:
Vol. 4, no. 6, eaar7697
DOI: 10.1126/sciadv.aar7697
  • Fig. 1 Pulse sequence of a 2D photon echo and visualization of optical transformation.

    (A) The pulse sequence applied in the 2D photon echo spectroscopy. (B) Visualization of the transformation from an object O(x′, y′) to an image I(x, y) using the convolution with the PSF cf. Eq. 2.

  • Fig. 2 Photon echo spectra and data extracted from T = 0 ps.

    (A and B) Normalized experimental photon echo spectra (absolute value) for T = 0 ps and T = 20 ps at 5 K. (C) Reconstructed relaxation Green’s function for T = 0 ps at 5 K. (D) Absolute value of line-shape function L(Δω, ω) for 20 K. (E and F) Rescaled line-shape function L(Δω, ω)/|L(0, ω)| for 5 and 20 K, respectively, with the corresponding oscillator strength L(0, ω) and D(ω) given as inset. In (D), (E), and (F), the gray lines mark the area with low reconstruction error.

  • Fig. 3 Reconstructed and simulated relaxation Green’s function at 20 K.

    (A and B) Reconstructed relaxation Green’s functions G1, ω2; T) for the initial energy ℏω1 and the final energy ℏω2 for T = 10 ps and T = 20 ps at 20 K. (C and D) Corresponding simulated relaxation Green’s functions. (The exciton–acoustic-phonon scattering in the second order Born-Markov approximation overestimates the relaxation times by a factor of 2 at 20 K (25); therefore, we use T = 5 and 10 ps from theory for the comparison.) In (A) and (B), the green contour line shows off-diagonal contribution at T = 0 ps, its presence indicates areas that may contain large artifacts and spurious features. Diagonal and horizontal lines provide visual guidance.

  • Fig. 4 Reconstructed and simulated relaxation Green’s function at 5 K.

    (A and B) Reconstructed relaxation Green’s functions G1, ω2; T) for the initial energy ℏω1 and the final energy ℏω2 for T = 10 ps and T = 20 ps at 5 K. (C and D) Corresponding simulated relaxation Green’s functions. In (A) and (B), the green contour line shows off-diagonal contribution at T = 0 ps, and its presence indicates areas that may contain large artifacts and spurious features. Diagonal and horizontal lines provide visual guidance.

Supplementary Materials

  • Supplementary material for this article is available at http://advances.sciencemag.org/cgi/content/full/4/6/eaar7697/DC1

    Supplementary Text: Reconstruction algorithms

    Supplementary Text: Derivation of material model

    fig. S1. Different reconstructed Green’s function G1, ω2; T) at 5 K and T = 10 ps.

    fig. S2. Contributing pathways to the photon echo signal.

  • Supplementary Materials

    This PDF file includes:

    • Supplementary Text: Reconstruction algorithms
    • Supplementary Text: Derivation of material model
    • fig. S1. Different reconstructed Green’s function G(ω1, ω2; T) at 5 K and T = 10 ps.
    • fig. S2. Contributing pathways to the photon echo signal.

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