Infrared–microwave double-resonance spectroscopy of CH<sub>3</sub>OH by use of sidebands of CO<sub>2</sub> laser lines

Zhen-Dong Sun; Fusakazu Matsushima; Shozo Tsunekawa; Kojiro Takagi

doi:10.1364/JOSAB.16.001447

Journal of the Optical Society of America B
Vol. 16,
Issue 9,
pp. 1447-1454
(1999)
•https://doi.org/10.1364/JOSAB.16.001447

Infrared–microwave double-resonance spectroscopy of CH₃OH by use of sidebands of CO₂ laser lines

Zhen-Dong Sun, Fusakazu Matsushima, Shozo Tsunekawa, and Kojiro Takagi

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Zhen-Dong Sun, Fusakazu Matsushima, Shozo Tsunekawa, and Kojiro Takagi, "Infrared–microwave double-resonance spectroscopy of CH₃OH by use of sidebands of CO₂ laser lines," J. Opt. Soc. Am. B 16, 1447-1454 (1999)

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Abstract

An infrared–microwave double-resonance technique using microwave sidebands of ${CO}_{2}$ laser lines as an infrared source has been applied for observation of rotational lines of the methanol molecule. Frequencies of more than 50 rotational lines in the excited $C — O$ stretching vibrational state $(v_{co} = 1)$ have been measured with good precision and have been compared with those reported in infrared studies. Many of them agree within several megahertz, although some lines show differences of >10 MHz. The pressure dependence of the double-resonance signals for two low-J microwave transitions belonging to the ground and the $v_{co} = 1$ states, respectively, have been observed for sample pressures as high as 0.4 Torr. For the former transition the signal has been observed to change its sign at higher pressures. Rate equation analysis explains the observed pressure dependence quantitatively and allows us to understand the physical processes involved in the double resonance.

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${CO}_{2}$ Laser Line	Microwave Frequency of Laser Sidebanda (MHz)	Infrared Transition $(v_{co} = 1 \leftarrow 0)$	$v_{t}$	Rotational Transition $(v_{co} = 1)$	$ν_{obs}$ (MHz)	$Obs . - Calc .$ b (MHz)
$9 P (10)$	-15 980	$14_{4^{+}} \leftarrow 13_{4^{+}}$	0	$15_{3^{+}} \leftarrow 14_{4^{+}}$	74 875.79	7.87
	-15 980	$14_{4^{-}} \leftarrow 13_{4^{-}}$	0	$15_{3^{-}} \leftarrow 14_{4^{-}}$	75 239.09	-0.48
	16 961	$15_{1^{-}} \leftarrow 14_{1^{-}}$	0	$15_{1^{-}} \leftarrow 15_{1^{+}}$	102 649.89	-1.75
$9 P (12)$	-13 910	$13_{1^{-}} \leftarrow 12_{1^{-}}$	0	$13_{1^{-}} \leftarrow 13_{1^{+}}$	781 23.60	2.18
	-8741	$13_{2^{-}} \leftarrow 12_{2^{-}}$	1	$13_{2^{-}} \leftarrow 12_{1^{-}}$	88 971.30	-0.51
	-8789	$13_{2^{+}} \leftarrow 12_{2^{+}}$	1	$13_{2^{+}} \leftarrow 12_{1^{+}}$	95 168.53	-5.08
$9 P (14)$	-16 014	$12_{1^{+}} \leftarrow 11_{1^{+}}$	0	$12_{1^{-}} \leftarrow 12_{1^{+}}$	67 066.53	0.26
$9 P (16)$	15 987	$11_{4^{+}} \leftarrow 10_{4^{+}}$	0	$11_{4^{+}} \leftarrow 12_{3^{+}}$	68 646.78	-23.39
	15 987	$11_{4^{-}} \leftarrow 10_{4^{-}}$	0	$11_{4^{-}} \leftarrow 12_{3^{-}}$	68 548.76	5.44
	-13 274	$11_{1^{+}} \leftarrow 10_{1^{+}}$	1	$12_{2^{+}} \leftarrow 11_{1^{+}}$	47 426.43	-16.03
$9 P (20)$	-16 593	$8_{1^{-}} \leftarrow 7_{1^{-}}$	0	$7_{2^{-}} \leftarrow 8_{1^{-}}$	70 840.60	-0.96
$9 P (28)$	-16 400	$2_{0^{+}} \leftarrow 1_{0^{+}}$	2	$2_{0^{+}} \leftarrow 1_{0^{+}}$	95 145.72	-3.01
$9 P (34)$	121^*	$2_{1^{+}} \leftarrow 2_{1^{-}}$	1	$2_{1^{+}} \leftarrow 1_{1^{+}}$	95 285.69	0.17
	-14 938	$12_{2^{-}} \leftarrow 12_{2^{+}}$	1	$12_{2^{-}} \leftarrow 11_{1^{-}}$	42 152.81	10.00
	17 213	$0_{0^{+}} \leftarrow 1_{0^{+}}$	2	$1_{0^{+}} \leftarrow 0_{0^{+}}$	47 573.32	17.54

${CO}_{2}$ Laser Line	Microwave Frequency of Laser Sidebanda (MHz)	Infrared Transition $(v_{co} = 1 \leftarrow 0)$	$v_{t}$	Rotational Transition $(v_{co} = 1)$	$ν_{obs}$ (MHz)	$Obs . - Calc .$ b (MHz)
$9 P (6)$	-12 766	$17_{5} \leftarrow 16_{5}$	0	$16_{6} \leftarrow 17_{5}$	93 334.28	-5.80
	14 735	$18_{4} \leftarrow 17_{4}$	0	$18_{4} \leftarrow 19_{3}$	69 671.70	0.53
	-10 016	$18_{- 2} \leftarrow 17_{- 2}$	1	$18_{- 2} \leftarrow 17_{- 1}$	101 151.35	-0.72
	-10 016	$18_{- 2} \leftarrow 17_{- 2}$	1	$19_{- 3} \leftarrow 18_{- 2}$	75 184.45	3.40
$9 P (8)$	-9417	$16_{1} \leftarrow 15_{1}$	0	$16_{2} \leftarrow 16_{1}$	49 908.35	1.60
	8503	$16_{- 3} \leftarrow 15_{- 3}$	1	$15_{- 2} \leftarrow 16_{- 3}$	65 439.36	-5.63
	-14 387	$14_{2} \leftarrow 13_{2}$	2	$13_{3} \leftarrow 14_{2}$	52 228.78	4.93
	8983	$15_{3} \leftarrow 14_{3}$	2	$16_{2} \leftarrow 15_{3}$	43 291.24	3.31
$9 P (10)$	-17 749	$14_{- 7} \leftarrow 13_{- 7}$	1	$15_{- 6} \leftarrow 14_{- 7}$	74 636.39	-1.44
$9 P (12)$	-7704	$13_{2} \leftarrow 12_{2}$	0	$13_{2} \leftarrow 13_{1}$	48 996.95	-0.53
	-15 155	$13_{- 4} \leftarrow 12_{- 4}$	0	$12_{- 5} \leftarrow 13_{- 4}$	92 943.03	3.77
	11 226	$14_{1} \leftarrow 13_{1}$	0	$14_{2} \leftarrow 14_{1}$	49 335.91	-0.93
	-16 081	$14_{- 2} \leftarrow 13_{- 2}$	1	$13_{- 1} \leftarrow 14_{- 2}$	68 086.48	-0.88
	-8341	$12_{3} \leftarrow 11_{3}$	2	$12_{3} \leftarrow 13_{2}$	99 980.74	-9.04
$9 P (14)$	-11 117	$12_{- 6} \leftarrow 11_{- 6}$	1	$11_{- 7} \leftarrow 12_{- 6}$	69 884.78	1.36
$9 P (16)$	-9173	$11_{1} \leftarrow 10_{1}$	0	$11_{2} \leftarrow 11_{1}$	48 392.32	11.81
	11 881	$11_{3} \leftarrow 10_{3}$	0	$12_{2} \leftarrow 11_{3}$	46 350.71	-27.18
$9 P (26)$	-11 831	$2_{0} \leftarrow 1_{0}$	2	$2_{0} \leftarrow 1_{0}$	95 109.71	1.45
$9 P (30)$	-16 528	$2_{0} \leftarrow 1_{0}$	0	$1_{1} \leftarrow 2_{0}$	64 199.93	2.67
$9 P (34)$	121^*	$2_{1} \leftarrow 2_{1}$	0	$2_{1} \leftarrow 1_{1}$	95 708.44	-2.10
	121^*	$2_{1} \leftarrow 2_{1}$	0	$2_{2} \leftarrow 2_{1}$	47 879.89	-6.26
	-17 322	$12_{2} \leftarrow 12_{2}$	0	$12_{2} \leftarrow 12_{1}$	48 674.30	-27.28
	-17 360	$8_{1} \leftarrow 8_{1}$	0	$8_{2} \leftarrow 8_{1}$	47 882.63	-1.72
	-16 449	$2_{1} \leftarrow 3_{1}$	2	$2_{1} \leftarrow 1_{1}$	95 087.98	9.40
	-12 547	$1_{- 1} \leftarrow 2_{- 1}$	2	$2_{- 1} \leftarrow 1_{- 1}$	95 138.91	-19.71
$9 P (36)$	-7577	$13_{- 5} \leftarrow 13_{- 5}$	0	$13_{- 5} \leftarrow 14_{- 4}$	46 077.90	1.00
	-7786	$18_{2} \leftarrow 18_{2}$	0	$18_{2} \leftarrow 18_{1}$	49 994.07	0.68
	-12 408	$16_{4} \leftarrow 16_{4}$	0	$15_{5} \leftarrow 16_{4}$	81 034.04	-2.86
	-13 678	$16_{- 3} \leftarrow 16_{- 3}$	0	$17_{- 2} \leftarrow 16_{- 3}$	78 050.80	13.92
	-16 582	$19_{6} \leftarrow 19_{6}$	0	$20_{5} \leftarrow 19_{6}$	50 844.77	-1.83
	-18 242	$19_{2} \leftarrow 19_{2}$	0	$19_{2} \leftarrow 19_{1}$	49 713.69	0.31
	10 406	$13_{- 3} \leftarrow 13_{- 3}$	0	$13_{- 3} \leftarrow 12_{- 4}$	78 007.35	6.45
	10 406	$13_{- 3} \leftarrow 13_{- 3}$	0	$13_{- 3} \leftarrow 14_{- 2}$	72 275.16	-3.30
$9 P (38)$	16 000	$20_{- 6} \leftarrow 20_{- 6}$	1	$19_{- 5} \leftarrow 20_{- 6}$	70 562.80	-8.64
$9 P (40)$	8556	$19_{3} \leftarrow 19_{3}$	1	$19_{3} \leftarrow 20_{4}$	68 955.42	-5.54
$9 P (42)$	133^*	$4_{1} \leftarrow 5_{1}$	0	$4_{2} \leftarrow 4_{1}$	47 820.38	-2.81
	133^*	$4_{1} \leftarrow 5_{1}$	0	$5_{0} \leftarrow 4_{1}$	79 089.58	-2.87

Transition ( $v_{co} = 1 \leftarrow 0,$ $v_{t} = 0$ )	$α_{g}$ (cm^-1 Torr^-1)	$S_{if}$ (cm^-2 atm^-1)	\|μ(1, 0)\| (debye)
E, $2_{0} \leftarrow 1_{0}$	$0.042 \pm 0.004$	$0.078 \pm 0.007$	$0.184 \pm 0.018$
E, $1_{- 1} \leftarrow 2_{- 1}$	$0.038 \pm 0.004$	$0.070 \pm 0.007$	$0.201 \pm 0.02$
Average			$0.192 \pm 0.019$

$\| x \| / 2 π$ (MHz)	Power of ${CO}_{2}$ Laser Sideband P (mW)	$\| x_{m} \| / 2 π$ (MHz)	Microwave Power $P_{m}$ (mW)
Scheme 1
0.276	3.9	1.52	7.3
0.228	2.7
Scheme 2
0.376	9.5	2.21	5.3
0.316	6.7

${CO}_{2}$ Laser Line	Microwave Frequency of Laser Sidebanda (MHz)	Infrared Transition $(v_{co} = 1 \leftarrow 0)$	$v_{t}$	Rotational Transition $(v_{co} = 1)$	$ν_{obs}$ (MHz)	$Obs . - Calc .$ b (MHz)
$9 P (10)$	-15 980	$14_{4^{+}} \leftarrow 13_{4^{+}}$	0	$15_{3^{+}} \leftarrow 14_{4^{+}}$	74 875.79	7.87
	-15 980	$14_{4^{-}} \leftarrow 13_{4^{-}}$	0	$15_{3^{-}} \leftarrow 14_{4^{-}}$	75 239.09	-0.48
	16 961	$15_{1^{-}} \leftarrow 14_{1^{-}}$	0	$15_{1^{-}} \leftarrow 15_{1^{+}}$	102 649.89	-1.75
$9 P (12)$	-13 910	$13_{1^{-}} \leftarrow 12_{1^{-}}$	0	$13_{1^{-}} \leftarrow 13_{1^{+}}$	781 23.60	2.18
	-8741	$13_{2^{-}} \leftarrow 12_{2^{-}}$	1	$13_{2^{-}} \leftarrow 12_{1^{-}}$	88 971.30	-0.51
	-8789	$13_{2^{+}} \leftarrow 12_{2^{+}}$	1	$13_{2^{+}} \leftarrow 12_{1^{+}}$	95 168.53	-5.08
$9 P (14)$	-16 014	$12_{1^{+}} \leftarrow 11_{1^{+}}$	0	$12_{1^{-}} \leftarrow 12_{1^{+}}$	67 066.53	0.26
$9 P (16)$	15 987	$11_{4^{+}} \leftarrow 10_{4^{+}}$	0	$11_{4^{+}} \leftarrow 12_{3^{+}}$	68 646.78	-23.39
	15 987	$11_{4^{-}} \leftarrow 10_{4^{-}}$	0	$11_{4^{-}} \leftarrow 12_{3^{-}}$	68 548.76	5.44
	-13 274	$11_{1^{+}} \leftarrow 10_{1^{+}}$	1	$12_{2^{+}} \leftarrow 11_{1^{+}}$	47 426.43	-16.03
$9 P (20)$	-16 593	$8_{1^{-}} \leftarrow 7_{1^{-}}$	0	$7_{2^{-}} \leftarrow 8_{1^{-}}$	70 840.60	-0.96
$9 P (28)$	-16 400	$2_{0^{+}} \leftarrow 1_{0^{+}}$	2	$2_{0^{+}} \leftarrow 1_{0^{+}}$	95 145.72	-3.01
$9 P (34)$	121^*	$2_{1^{+}} \leftarrow 2_{1^{-}}$	1	$2_{1^{+}} \leftarrow 1_{1^{+}}$	95 285.69	0.17
	-14 938	$12_{2^{-}} \leftarrow 12_{2^{+}}$	1	$12_{2^{-}} \leftarrow 11_{1^{-}}$	42 152.81	10.00
	17 213	$0_{0^{+}} \leftarrow 1_{0^{+}}$	2	$1_{0^{+}} \leftarrow 0_{0^{+}}$	47 573.32	17.54

Abstract

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Figures (10)

Tables (4)

Equations (10)

Journal of the Optical Society of America B