Deconvolution of Atomic Photoabsorption Spectra: a match between theory and experiment
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1 Deconvolution of Atomic Photoabsorption Spectra: a match between theory and experiment T. N. Chang and Y. X. Luo Department of Physics and Astronomy, University of Southern California Los Angeles, CA , USA H. S. Fung and T. S. Yih Department of Physics, National Central University, Chung-Li, TAIWAN ROC We present in this paper an extension of a recently proposed deconvolution procedure to compare directly the theoretical and experimental spectrum of a doubly excited ultra-narrow and nearly symmetric resonance in atomic photoabsorption. Our discussion is based on a set of analytical relations in terms of the variations of i) the ratio between the resonance width Γ and the experimental energy resolution Ω in the limit when Γ/Ω 1 and ii) the column density nl of the media in a photoabsorption experiment. PACS number(s): 32.80Fb, Jz, Dz. I. Introduction In an attempt to estimate the width of a narrow isolated doubly excited resonance from measured spectra in the absence of an ultrahigh-energy resolution, Fang and Chang [1] have recently proposed a deconvolution procedure which enables a direct extrapolation to inþnite energy resolution using a set of explicit analytical relations in terms of the ratio R of the resonant width Γ and the experimental energy resolution Ω in the limit of R = Γ/Ω 1. This procedure applies well for a photoionization experiment when the photoion and/or the photoelectron are measured directly. Unlike the photoionization, the resonant spectra in a photoabsorption experiment is determined by detecting the light attenuation through a medium. It is known that the measured cross section is signiþcantly affected by the column density nl of the medium and the experimental monochromator (or slit) function F [2]. The photoabsorption cross-section σ Pa (E) at a photon energy E is determined experimentally using the Beer-Lambert law, I(E) =I o (E) e nlσpa (E). (1) where I o is the intensity of the incident light, I is the attenuated intensity of the transmitted light, and nl is the column density. At a photon energy E, I o and I can be expressed in terms of the slit function F centered at E and characterized by an energy resolution Ω, i.e., Z I o (E) = i o F(E 0 E; Ω) de 0 (2) and Z I(E) = i o F(E 0 E; Ω) e nl σ(e) de 0, (3) 1
2 where σ is the cross section at an inþnite energy resolution (i.e., at Ω =0). FromEqs.(1-3), the measured resonance structure in a photoabsorption experiment is represented by a convoluted spectrum in the form of σ Pa (E) = 1 Z ln ( F(E 0 E; Ω) e nl σ(e0) de 0 ). (4) nl As expected, when nl 0, the cross section takes the same form of the photoionization given by Eq. (3) of Ref. [1], i.e., σ Pa σ Pi,where Z σ Pi (E) = σ(e 0 ) F(E 0 E; Ω) de 0. (5) The slit function F may be approximated at the center by a Gaussian distribution G and modiþed at its tail by a Lorentzian distribution L. It can be expressed by a weighted combination of G and L [1, 3], i.e., F(E; Ω,w g,w`) =w g G(E; Ω)+w` L(E; Ω), (6) where the sum of w g and w` equals one. (G and L are given explicitly by Eq. (4) of Ref. [1].) There is no well established general procedure to determine the weighting factors w g and w` experimentally in the absence of ultrahigh energy resolution. Based on the analytical relations discussed in the next section, we shall propose a procedure leading to the determination of w g and w`. The density effect in photoabsorption can be easily illustrated by the variation of the convoluted spectra of an isolated resonance with changing nl and Ω. For simplicity, we will limit our discussion using a Fano-type of resonance described by an asymmetry parameter q and the smoothly varying background cross section σ b, i.e., [4] σ(e) =σ b (q + ²) ² 2, (7) where the reduced energy ² =(E E r )/( 1Γ)isdeÞnedintermsoftheenergyE 2 r and the width Γ of the resonance. The cross section σ is expected to reach its peak value σ max = σ b (1 + q 2 )andazeroatenergies E max = E r (Γ/q) and E min = E r 1 (Γq), (8) 2 respectively. Figure 1 presents a number of selected convoluted photoionization spectra using Eq. (5) with R ranging from 1/10 to1/25 and a slit function F represented either by a Gaussian distribution G or a Lorentzian distribution L. These spectra correspond to a Þctitious resonance derived from Eq. (7) with E r =2.110 Ry,σ b = 1.0 Mb,q 2 = 2500, and Γ = 10 6 Ry. As expected, for a given ratio R, the peak cross section σ max corresponding to the spectrum convoluted using Gaussian distribution is substantially higher than the one using Lorentzian distribution. The density effect in photoabsorption measurement is unambiguous demonstrated by the substantial reduction in peak cross sections shown in Fig. 2 when the same spectrum is convoluted using Eq. (4) with a column density nl = Mb 1. 2
3 II. Peak Cross Sections For an ultra-narrow and nearly symmetric resonance, the peak cross section σ max is very well approximated by the cross section at E = E r, i.e., σ max σ(e r ), since, from Eq. (8), the energy corresponding to the peak cross section, i.e., E max, equals approximately the resonant energy E r as the difference E max E r is substantially smaller than the resonance width, i.e., as q 2 À 1 and Γ q Γ. In a photoionization experiment, σmax Pi Z = σ(e 0 ) F(E 0 E r ; Ω) de 0. (9) Although Eq. (5) is not in general integrable for an arbitrary energy E, Eq. (9) can be integrated analytically. For a Lorentzian distribution, and for a Gaussian distribution, σ L max = σ b (1 + q 2 R)/(1 + R) (10) σ G max = σ b (1 + π 1/2 (q 2 1))Re R2 F c (R), (11) where F c (x) =1 (2/ π) R x 0 e y2 dy is the complementary error function. For a nearly symmetric ultra-narrow resonance, such as the Þctitious resonance shown in Figs. 1 and 2, our calculation shows that the approximate σ max at E = E r, derived from Eqs. (10) and (11), are within 0.05% of the exact peak cross sections determined from the numerically calculated spectra using Eq. (5). In a photoabsorption experiment, the peak cross section σ max can also be approximated similarly from Eq. (4) as σ pa max = 1 nl Z ln ( F(E 0 E r ; Ω) e nl σ(e0) de 0 ). (12) Figure 3 shows that the approximate peak cross sections σ max, represented by the nearly straight lines obtained from Eq. (12) are in close agreement with the exact peak cross sections at R = 1, 1, 1 and 1 for a number of column densities nl derived directly from the numerically calculated convoluted spectra using Eqs. (4) and (5) for photoabsorption and photoionization (i.e., when nl = 0), respectively. In general, Eq. (12) can not be integrated analytically due to the exponential term e nlσ. However, when e nlσ is expanded into an inþnite series, each individual term becomes integrable and σ max can be expressed in terms of a polynomial in R, i.e., where σ max σ Pa (E = E r )=q 2 σ b X(R, nl), (13) X(R, nl) = X i=1( 1) i+1 ξ i (ρ) R i (14) 3
4 and ρ is a parameter given by ρ = nlq 2 σ b. (15) For a Lorentzian distribution, the Þrst few expansion coefficients are ξ 1 = ρ ρ ρ ρ4 (16) ξ 2 = ρ ρ ρ ρ4 (17) ξ 3 = ρ ρ ρ ρ4 (18) ξ 4 = 1 ρ + ρ ρ ρ4 (19) ξ 5 = ρ ρ ρ ρ4, (20) and for a Gaussian distribution ξ 1 = π(1 1 4 ρ ρ ρ ρ4 ) (21) ξ 2 =2 π( 1 2 ρ 1 4 ρ ρ ρ4 + ) (22) ξ 3 = π(1 7 4 ρ +( π 3 )ρ2 ( π 4 )ρ3 +( π 8 )ρ4 ) (23) ξ 4 = 4 3 (1 ρ) π(ρ 2ρ2 +( π 4 )ρ3 ( π 4 )ρ4 + ) (24) ξ 5 = π( ρ +( π)ρ2 ( π 4 )ρ3 +( π 24 + π2 5 )ρ4 ). (25) Under a typical experimental condition, even at a fairly low column density nl, the parameter ρ may be close to or greater than unity as q 2 À 1. Consequently, the peak cross section σ max can be estimated approximately from Eq. (13) only if R is very small and the number of contributing ξ i terms is limited. More discussion will be given in section III. 4
5 III. Proposed Procedures A. Determination of w` and w g in photoionization When Γ Ω (or, R 1), for a nearly symmetric resonance with q 2 À 1, theobserved σ max = w`σ L max + w g σ G max can be expressed approximately according to Eqs. (10) and (11) as or, σ max varies linearly as functions of 1/Ω. Asaresult, σ max (w` + w g π 1/2 )(q 2 σ b )R, (26) (w` + w g π 1/2 )(q 2 Γσ b )=S 1, (27) where S 1 is the slope determined experimentally by a plot of σ max vs. 1/Ω according to Eq. (12). In addition, according to Eq. (17) of Ref. [1], (1.3282w` w g )(q 2 Γσ b )=S 2, (28) where S 2 is also a slope determined experimentally by a procedure detailed in Ref. [1]. Eqs. (27) and (28), together with w` + w g = 1, offer an unambiguous procedure to determine the weighting factors w` and w g in a photoionization experiment. B. Determination of q 2 σ b and Γ. Figure 4 shows that the approximate peak cross sections, σ E=Er, obtained from the analytical expression Eq. (13) remain in close agreement with the numerically calculated σ E=Er from Eq. (12) and the exact σ max from Eq. (4) for a value of ρ = nlq 2 σ b as large as Clearly, as ρ increases to a value of 2.5, Eq. (13) is no longer applicable. Since Ω (not R) is an experimentally measured variable, we shall now work with an alternative polynomial, in stead of the polynomial X(R, nl), for σ max, i.e., where Y (η,nl)takestheform σ max = (q 2 σ b Γ) Y (η,nl), (29) Y (η,nl)= X i=1( Γ) i 1 ξ i (ρ) η i (30) and η = 1/Ω. (31) Our proposed procedure starts with a best Þt of the measured σ max at a number of energy resolutions to an expression σ max (η; nl) = X µ=1 α µ (nl) η µ. (32) 5
6 By comparing Eq. (32) to Eq. (29), the Þtted coefficients α µ for a given nl is independent of Ω. In addition, the ratio of two Þtted values of α µ at two different column densities equals to the ratio of two ξ µ, i.e., α µ (nl) α µ (n 0 l 0 ) = ξ µ(ρ) ξ µ (ρ 0 ). (33) Since σ max is a slowly varying function of η, a number of experimentally determined ratios between several pairs of α 1 obtained at different column densities should be sufficient to Þt adequately a value of q 2 σ b.withabestþtted q 2 σ b, the resonant width Γ can be determined readily from Eq. (13) or (29). IV. Results and Discussion Figure 5 presents the variation of the simulated photoabsorption peak cross sections σ max as a function of 1/Ω at several column densities. It is derived from the convoluted spectra numerically calculated from Eq. (4) for a Þctitious resonance with a width Γ = Ry, q 2 = 400, and σ b =0.015 Mb. Following the procedure outlined in section III.B, for each nl, a parameter α 1 is Þrst least-square Þtted from Eq. (29). Second, from Eq. (30), we obtain a best Þtted value of 5.42 Mb and 5.54 Mb for q 2 σ b using the Lorentzian and Gaussian distribution, respectively. Finally, Eq. (13) leads to a width of Ry (Lorentzian) and Ry (Gaussian). The 10% error introduced in this application is not unexpected due to values of ρ which exceed unity for some of the column densities. The deconvolution procedure proposed in this paper works best when q 2 À 1. It clearly posts a difficult experimental challenge as it also requires simultaneously a small parameter ρ = nlq 2 σ b when a small column density nl may adversely reduce the signal to noise ratio in a photoabsorption experiment. In spite of this difficulty, the procedure proposed above offers a realistic possibility to take advantage of the density effect, in an attempt to determine experimentally the width of an ultra-narrow and nearly symmetric atomic resonance which can not be measured directly otherwise. Acknowledgments This work is partially supported by the National Science Council of Taiwan under contract NSC M (TSY) and by NSF Grant No. PHY (TNC). References [1] T.K.FangandT.N.Chang,Phys.Rev.A57, 4407(1998). [2] R.D.HudsonandV.L.Carter,J.Op.Soc.Am.58, 227 (1968); W. F. Chan, G. Cooper, andc. E. Brion, Phys. Rev. A44, 186 (1991). [3] K. Schulz, G. Kaindl, M. Domke, J. D. Bozek, P. A. Heimann, A. S. Schlachter, and J. M. Rost, Phys. Rev. Lett. 77, 3086 (1996). [4] U. Fano, Phys. Rev. 124, 1866 (1961). 6
7 Figure captions Figure 1. Figure 2. Convoluted photoionization spectra using Eq. (5) with R ranging from 1/10 to1/25. Convoluted photoabsorption spectra using Eq. (4) with R ranging from 1/10 to1/25 and a column density nl =0.001 Mb 1. Figure 3. Comparison between σ max (nearly straight lines) obtained from Eq. (12) and the exact peak cross sections at R = 1, 1, 1 and for a number of column densities nl derived directly from the numerically calculated convoluted spectra using Eqs. (4) and (5) for photoabsorption and photoionization (i.e., when nl = 0), respectively. Figure 4. Figure 5. Comparison of the approximate peak cross sections, σ E=Er, obtained from the analytical expression Eq. (13), the numerically calculated σ E=Er from Eq. (12) and the exact σ max from Eq. (4). Variation of simulated photoabsorption peak cross sections σ max (from Eq. (4)) as a function of 1/Ω at column densities ranging from 0.07 Mb 1 to 0.23 Mb 1. (Only Lorentzian data are shown.) 7
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Deconvolution of Atomic Photoabsorption Spectra: a Match between Theory and Experiment
Journal of the Chinese Chemical Society, 2001, 48, 347-351 347 Deconvolution of Atomic Photoabsorption Spectra: a Match between Theory Experiment Tu-nan Chang a * ( ), Yuxiang Luo a ( ), Hok-Sum Fung b
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