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Optimized hierarchical equations of motion theory for Drude dissipation and efficient implementation to nonlinear spectroscopies
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10.1063/1.3653479
/content/aip/journal/jcp/135/16/10.1063/1.3653479
http://aip.metastore.ingenta.com/content/aip/journal/jcp/135/16/10.1063/1.3653479
View: Figures

Figures

Image of FIG. 1.
FIG. 1.

The deviation spectrum function δC N (ω) of Drude bath, plotted in terms of δC N (ω)/Δ N versus ω/Γ N (γ) for some selected values of {N, βγ}, where Δ N is given via Eq. (8) and Γ N (γ) is by the approximate of Eq. (12).

Image of FIG. 2.
FIG. 2.

βΓ N (γ) and versus βγ.

Image of FIG. 3.
FIG. 3.

Evolution of the reduced spin system density matrix elements, with the same parameters as Fig. 8 of Ref. 45; i.e., ε/V = 1, λ/V = 0.25, γ/V = 5, and βV = 50. The accuracy control parameters are {Γ N s , κ N } = {2.6, 3.6} for N = 4 and {4.7, 8.5} for N = 8, as indicated. The converged dynamics are identical to that of N = 10 whose {Γ N s , κ N } = {6.3, 12.0}.

Image of FIG. 4.
FIG. 4.

Dispersed transient absorption coefficient signals of the model dimer system (see text): (a) Linear absorption (A) and emission (E) signals; (b) Nonlinear absorptive component; (c) Nonlinear emissive component. The pump field is a transform-limited 50 fs-pulse of finite intensity (see text), centered at ω = ε; i.e., Δω ≡ ω − ε = 0, as indicated by the arrow in panel (a). At T = 298 K, N = 1 is in the numerically accurate range, with {Γ N s , κ N } = {8.3, 8.7} as indicated.

Image of FIG. 5.
FIG. 5.

Same as Fig. 4, but at T = 77 K, where N = 1 is in the semi-quantitative range, with {Γ N s , κ N } = {2.4, 2.4}, as indicated.

Image of FIG. 6.
FIG. 6.

Two-dimensional spectroscopy of the same dimer system of Fig. 4 at T = 298 K, reported in Δω1 = ω1 − ε and Δω3 = ω3 − ε. All pulsed fields are operated in weak and impulsive limit.

Image of FIG. 7.
FIG. 7.

The Δω1 = 0 slices of the absorptive and emissive panels of Fig. 6. This figure resembles the impulsive pump counterpart of Fig. 4.

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/content/aip/journal/jcp/135/16/10.1063/1.3653479
2011-10-31
2014-04-18
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Optimized hierarchical equations of motion theory for Drude dissipation and efficient implementation to nonlinear spectroscopies
http://aip.metastore.ingenta.com/content/aip/journal/jcp/135/16/10.1063/1.3653479
10.1063/1.3653479
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