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Direct measurements of collisionally broadened Raman linewidths of CO2 S-branch transitions
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Image of FIG. 1.
FIG. 1.

(a) CO2 ps-RCARS spectra shown for two probe time delays at P = 1 atm and T = 295 K, normalized to the respective peak intensities in each spectrum. (b) ps-RCARS signal integrated over the J = 10, 24, and 40 rotational lines as a function of probe time delay along with single-exponential fits (solid lines) to the decays.

Image of FIG. 2.
FIG. 2.

Measured CO2 collisional self-broadening linewidths for three S-branch lines at 295 K as a function of pressure. The symbols denote the experimental measurements, and the solid lines are linear fits.

Image of FIG. 3.
FIG. 3.

Collisional self-broadening coefficients of CO2 (S-branch) rotational Raman lines at T = 295 K. Measurements made for this work (○) include error bars representing one standard deviation associated with linear fits to data analogous to those shown in Fig. 2 . The dashed curve represents a best-fit ECS-P approximation to the experimental results. Also shown are reported experimental Raman broadening coefficient measurements (■) of Jammu et al. [Ref. 10 ] and semi-classical theoretical coefficients (●) reported by Rosenmann et al. [Ref. 7 ] based on averaged experimental data; associated error bars represent extrema of these experimental values.

Image of FIG. 4.
FIG. 4.

Probe-delayed (Δt = 200 ps) ps-RCARS spectrum of 30% CO2 in N2 at T = 295 K and P = 1 atm.

Image of FIG. 5.
FIG. 5.

Measured CO2 rotational Raman linewidths broadened by N2 at three different mixture ratios at T = 295 K and P = 1 atm.

Image of FIG. 6.
FIG. 6.

Extracted linewidth data for CO2–N2 collisional broadening at T = 295 K and P = 1 atm. Also shown is the theoretical calculation by Rosenmann et al. [Ref. 7 ]. Shown in the inset is the linear curve fitting for the J = 8, 24, 34 lines using Eq. (5) to obtain the limiting value of .


Generic image for table
Table I.

Measured collisional self-broadening coefficients (HWHM), γ J, J+2, at 295 K for the CO2 S-branch transitions. Numbers in parentheses correspond to one-standard-deviation uncertainties in last digits.


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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Direct measurements of collisionally broadened Raman linewidths of CO2S-branch transitions