^ecUnical ilot& 332

CARBON DIOXIDE SPECTRAL LINE POSITIONS AND INTENSITIES

CALCULATED FOR THE 2.05 AND 2.7 MICRON REGIONS

ROBERT F. CALFEE AND WILLIAM S. BENEDICT

U. S. DEPARTMENT OF COMMERCE

NATIONAL BUREAU OF STANDARDS
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NATIONAL BUREAU OF STANDARDS

Technical Note 332

ISSUED MARCH 15, 1966

CARBON DIOXIDE SPECTRAL LINE POSITIONS AND INTENSITIES

CALCULATED FOR THE 2.05 AND 2.7 MICRON REGIONS

Robert F. Calfee

Institute for Telecommunication Sciences and Aeronomy * Environmental Science Services Administration

Boulder, Colorado

and

William S. Benedict

Institute for Basic Standards

National Bureau of Standards

Washington, D.C.

This work sponsored by the Advanced Research Projects Agency,

under Contract Number 250-61; Code Number 7400-DO

* Formerly the Central Radio Propagation Laboratory of the

National Bureau of Standards; CRPL was transferred to ESSA

in October 1965, but will temporarily use various NBS publication series pending inauguration of ESSA counterparts.

NBS Technical Notes are designed to supplement the Bureau's regular publications program. They provide a means for making available scientific data that are of transient or limited interest. Technical Notes may be

listed or referred to in the open literature.

For sale by the Superintendent of Documents, U.S. Government Printing Office Washington, D.C, 20402 Price 60*

CONTENTS

1. Introduction 1

2. Frequencies 1

3. Intensities 2

4. Discussion 12

5. References 110

in

CARBON DIOXIDE SPECTRAL LINE

POSITIONS AND INTENSITIES CALCULATED

FOR THE 2. 05 AND 2. 7 MICRON REGIONS

Robert F. Calfee and William S- Benedict

The spectral line positions and intensities for the carbon dioxide

bands occurring in the 2. 05 and 2. 7 micron regions of the infrared spectrum

are listed. Lines with intensities down to 10" cm" /atm cm are listed for a temperature of 296°K.

Keywords: 2. 05\i, 2. 7(jl, carbon dioxide, intensities and line positions.

1

.

Introduction

A precise calculation of the infrared absorption by carbon dioxide depends upon a

knowledge of the position and strength of the individual lines of the spectrum. The absorption spectrum of carbon dioxide has been obtained in considerable detail by Courtoy (1959).

He not only presents spectra of the gas as its isotopes occur in natural abundance, but also

includes results of enhancement by certain of the isotopic molecules. Lists of the identification and position of the absorption lines are also tabulated.

However, in order to make quantitative calculations, it is necessary to have values

for the intensities of individual lines. Furthermore, in several instances Courtoy does not

give an exact value for the position of lines. For these reasons it was necessary to calculate

the intensities and positions of the CO? lines. This report concerns such calculations for

those bands which give rise to absorption in the 2. 05 and 2. 7u regions of carbon dioxide.

2. Frequencies

In this study centrifugal stretching effects are taken into account in calculating the

frequencies and intensities of the spectral lines. The energy values for the upper and lower

states are written in the following manner:

Upper level: v , , =u + J'(J' + 1)B'-J' (J'-Pl) D'

Lower level: v „=vl +J"(J"+1 )B"- J" 2 (J"+1 ) D",

V J V
where V and J denote the vibrational and rotational quantum numbers respectively of a

particular energy level. Here, v is the vibrational contribution; B and D are the usual

rotational constants. If we let a = B' + B", b = B'-B", c = -2(D'+D"), d = D"-D', then for the

P(A J = - 1 ) and R(A J = + 1 ) branches the frequency for a transition between energy levels is:

2 3 4 u{V'J' - V"J") =15 +am + (b+d)m + cm + dm . (1)

3 3 For the Q branch (A J =0), the terms am and cm are replaced by bm and dm ,

respectively. The possible branches depend upon the type of transition (E-E, II- IT, A -A, etc. ).

Values of m are determined by the branch: m = - J" for the P branch, m = J" in the Q branch,

and m = J" + l in the R branch. The possible values of J depend upon the parity of the lower

state; only even values of J are allowed for even parity and only odd values of J are permitted

for odd parity. In the case of molecules with different isotopes of oxygen, the listing of both

parities was included as an artificial means of forcing these bands through a computational

program relying on an even - odd scheme. In (1) V (band origin) is the vibrational energy

difference between the two states, (u - v ,,,,)• For a more thorough discussion of the behavior of linear polyatomic molecules, see Herzberg (1962).

3. Intensities

Line intensities are a combination of the vibrational and rotational contributions

determined by use of the following formulas:

S =(u/u )S S /Q ; (2) ° v r r where

S^gLexp (-E^'/kT); (3) Qr=Sg(2J + l) exp(-E^/kT); (4) E =B"J"(J" + 1) -D"J"

2 (J" + 1) Z

. (5) Here values of S , the vibrational band intensities, have been chosen on a semiv

theoretical basis attempting to fit the total observed intensities. The abundance factor for

the various isotopic species is taken into account in the values listed for S . Values of S v v

for a temperature of 296°K used for each band are listed in the seventh column of tables

1 and 2.
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Determination of the rotational contribution, S , depends upon a weighting factor g,

based upon the parity; in the case of -even parity g = 1 for even values of J, and g = for odd

values of J. Just the opposite is true for odd parity. The rotational partition functions, Q , r have nearly the same values in all the bands of a particular molecular species. The values

of Q for a temperature of 296°K are as follows: CCX,

16

, Q =263; C016 17

, Q =271 and

r

* r r C016 18

, Q =279. For a linear molecule, the rotational partition function can be taken as

directly proportional to the temperature (Herzberg, 1962). The rotational line strength

factors, Li, depend upon the type of band as well as the values of m which in turn depend

upon J. The following table shows this dependence:

Table 3. Rotational Line Strength Factors

Band

Type

Branch

E- S

n- n

A - A

$ - $

n- s

s- n

P and R m

a- n

p

Q

R

P

Q

R

I m| -1/| m|

(Zm +1), m(m +1)

|m| - 4/|m|

4(2m + l)/m(m-j- 1)

(|mj - l)(|m[ -2)/|mj

(m + 2)(m- l)(2m+ l)/m(m + l)

(m + 2)(m +l)/m

10
It should be noted that in tables 1 and 2 each series of lines with a distinct frequency

formula has been listed as a "separate band" for convenience of computational programming.

Thus in a A- II transition of an asymmetric molecule there would be four sub-bands listed

separately: the P- and R- branches with odd J", the P- and R- branches with even J", and

the corresponding odd and even Q branches. Each "band" has been normalized so that the

sum of states is close to that for the most common case, that of the T.-T, band in the symmetric molecule, with only even J". The rotational line strength factors in table 3 reflect

this unconventional definition of a "band".

The values used for the various other parameters for COH defined above and occurring in ( 1) through (5) are listed for each band in tables 1 and 2. The first column gives a

band number used for identification purposes in this report, the second column shows the

band type, and the isotopic species of the molecule is shown in the third column. The fourth

column indicates the parity of J" (e for even, o for odd). The next three columns (fifth,

sixth, and seventh), give the band origin u (cm ), the vibrational energy of the lower state,

E (cm ), and the vibrational band strength determined for 296°K. The eighth through

thirteenth columns give appropriate values of the molecular constants B", D", a, b, c, and

d. Certain of the weaker bands (II- S, S- II) require the addition of a term, (1 + t, m) in

calculating intensities to take into consideration the Coriolis vibration-rotation interaction.

Values of the empirical constant, t, , depending on the Coriolis interaction and the vibrational transition involved, which provide a satisfactory fit with the experimental data are

listed in the fourteenth column of tables 1 and 2.

Taking into account the values from tables 1 and 2, a program was developed for

computing the rotational energies, E", of the lower state, using values of J through 100,

and at the same time determining the rotational partition function, Q , according to (4).

The frequency and intensity are computed for all the lines in each of the branches again for

values of J through 100, according to (1) and (3).

*

11
Table 4 shows a tabulation of the results of the computations made by an electronic

computer using the appropriate data for the 61 bands of table 1 for the 2. 05u region. The

listing is according to increasing frequency, in cm , in the first column. The second

column gives the computed intensity of the line in cm /(atm-cm) . Note that all numbers

-3

listed are to be multiplied by 1 as indicated by the -3 at the head of this column. The

notation STP refers to the absorber concentration (atm-cm) and not the temperature for

which the values were computed. The energy (cm ), of the lower state including both

vibrational and rotational contributions, is found in the third column. Values of the

rotational line strength factor, L, are listed in the fourth column. The fifth column gives

the identification of the line in terms of the band number, the branch, and the value of J.

Table 5 gives similar information for the 2. 7u region based on the parameters listed in

table 2.

4. Discussion

Recently Burch, Gryvnak and Patty (19 64), have made extensive measurements of

the absorption spectrum in the 2. 05u region. Comparisons with these records have been

used to arrive at values of S , the vibrational band intensities, used to determine the line v

intensities computed for table 4. For the 2. 7|jl region, comparisons with the absorption

spectra published by Burch, Gryvnak and Williams (I960) have been used to assign the values

of S for these bands. With the exception of regions of low absorption, where bands weaker

than those included in the present computations may be expected to make a proportionately

large contribution, the transmission calculated from the line strength listed here agrees

with the measured values of Burch, Gryvnak and Patty (1964) to within a few percent. The

average Lorentz half -width parameter required to give the best agreement is approximately

0. 080 cm /atm for nitrogen broadening and 0. 104 cm /atm for self broadening.

In tables 4 and 5, the calculated line intensities for all lines having intensities of -7 -1 10 cm /(atm-cm) and greater have been listed. Since the experimental spectra with

which comparisons were made were observed at a temperature of 296°K, the intensity values were calculated and listed for this same temperature.

12
For extremely long optical paths, weaker lines due to higher J values and for other

bands not treated here will appear. However, for absorption paths through the earth's

atmosphere, all the significant carbon dioxide lines in the 2. 05 and 2 . 7(jl regions of the

spectrum will be found in the tables of this report.

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5. References

Burch, Darrell E. , David Gryvnak and DudleyWilliams (I960), Infrared Absorption by Carbon

Dioxide, Scientific Report No. II(AFCRL-255).

Burch, Darrell E. , David Gryvnak and Richard

R. Patty (1964), Absorption by CO Between 4500

and 5400 cm" , Philco Scientific Report No. U2955.

Courtoy, Charles P. (1959), Spectre Infrarouge,

A Grand Dispersion et Constantes Moleculaires

Du CO , Annales de la Societe Scientifique de

Bruxelles, 73, 5-203.

Herzberg, G. (1962), Molecular Spectra and

Molecular Structure II Infrared and Raman Spectra

of Polyatomic Molecules (Van Nostrand, New York,

1962)

110

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