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Vibrational ladder climbing in carboxy-hemoglobin: Effects of the protein environment
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10.1063/1.4799271
/content/aip/journal/jcp/138/14/10.1063/1.4799271
http://aip.metastore.ingenta.com/content/aip/journal/jcp/138/14/10.1063/1.4799271
View: Figures

Figures

Image of FIG. 1.
FIG. 1.

Loop diagram, describing the strong pulse pump interaction followed by a weak probe pulse. For details see text.

Image of FIG. 2.
FIG. 2.

Pulse envelope, total vibrational energy, and vibrational population P ν(t) in the CO-stretch in carboxy-hemeoglobine for a typical set of parameters: τ0 = 100 fs, ω0 = 1980.0 cm−1, ϕ = −0.1 ps2, and a peak power .

Image of FIG. 3.
FIG. 3.

Energy transfer achieved by linearly chirped laser pulses as a function of detuning form the center of the absorption band Δω0 and the chirp parameter ϕ with a pulse duration of τ0 = 100 fs (a)–(d) and τ0 = 300 fs (e)–(h), and a peak power of (a), (b), (e), and (f) and (c), (d), (g), and (h).

Image of FIG. 4.
FIG. 4.

Optimal detuning δopt of the excitation laser with respect to the center of the absorption band, required to obtain maximum vibrational energy transfer as a function of the peak power. The chirp parameter is set to ϕ′′ = −0.1ps2 (full lines), and compared to an unchirped (Fourier-transform limited) (dashed lines).

Image of FIG. 5.
FIG. 5.

Effect of chirp parameter ϕ and fluctuations onto vibrational excitation of HbCO. Optimal detunings for ϕ′′ = −0.1ps2 were used and a peak power of .

Image of FIG. 6.
FIG. 6.

Distribution of vibrational populations after strong IR pulse excitation, using different pulse lengths including or suppressing protein fluctuations. The other pulse parameters are ϕ′′ = −0.1 ps2, , and the corresponding optimal detunings.

Image of FIG. 7.
FIG. 7.

(Red) Distribution of vibrational populations after strong IR pulse interaction, for different pulse lengths and chirp parameters. Optimal detunings for ϕ′′ = −0.1 ps2 were used and a peak power of . (Blue) As above, but the vibrational populations are calculated by weighting the individual wavepackets by the projection onto the laser polarization axis.

Image of FIG. 8.
FIG. 8.

Differential transient absorption spectra (see Eq. (24) ) for different pulse lengths and chirp parameters, as indicated. Optimal detunings for ϕ′′ = −0.1ps2 were used and a peak power of .

Image of FIG. 9.
FIG. 9.

(Top panel) Simulated differential transient absorption signal , using different pulse intensities, based on an orientational averaging and averaging over the spatial beam profile (Eq. (25) ). A pulse duration of τ = 100 fs, a detuning of Δω = −61.7 cm−1, and a chirp parameter ϕ′′ = −3.2 × 10−2ps2 were used. (Bottom panel) Experimental spectra, taken from Ref. 23 and based on the same set of parameters.

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/content/aip/journal/jcp/138/14/10.1063/1.4799271
2013-04-11
2014-04-23
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Vibrational ladder climbing in carboxy-hemoglobin: Effects of the protein environment
http://aip.metastore.ingenta.com/content/aip/journal/jcp/138/14/10.1063/1.4799271
10.1063/1.4799271
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