Infrared radio-frequency double-resonance spectroscopy of molecular vibrational-overtone bands using a Fabry–Perot cavity-absorption cell

Chikako Ishibashi; Ryuji Saneto; Hiroyuki Sasada

doi:10.1364/JOSAB.18.001019

Journal of the Optical Society of America B
Vol. 18,
Issue 7,
pp. 1019-1030
(2001)
•https://doi.org/10.1364/JOSAB.18.001019

Infrared radio-frequency double-resonance spectroscopy of molecular vibrational-overtone bands using a Fabry–Perot cavity-absorption cell

Chikako Ishibashi, Ryuji Saneto, and Hiroyuki Sasada

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Chikako Ishibashi, Ryuji Saneto, and Hiroyuki Sasada, "Infrared radio-frequency double-resonance spectroscopy of molecular vibrational-overtone bands using a Fabry–Perot cavity-absorption cell," J. Opt. Soc. Am. B 18, 1019-1030 (2001)

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Abstract

Infrared (ir) radio-frequency (rf) double-resonance spectroscopy was carried out on the vibrational-overtone band of methyl iodide molecules $({CH}_{3} I) .$ An optical Fabry-Perot cavity was employed as an absorption cell to record saturated ir spectral lines even by a small-power extended-cavity diode laser with a high sensitivity and a wide tunability in the presence of a rf field. These features allowed investigation of molecules strongly coupled with monochromatic and bichromatic rf fields, or dressed molecules, at various rf power levels and detuning frequencies for a variety of ir and rf transitions. At appropriate energy-level schemes, quantum-interference effects were observed. All resultant spectra showed good agreement with dressed-state theoretical calculations, indicating that the present spectrometer is valid for precise investigation of dressed molecules.

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Case	Rf Frequencies	Energy Diagrams	Observed and Calculated Spectra
A	$ω = ω_{12}$	Fig. 2	Figs. 8 and 10
A	$ω = ω_{12} + δ$	Fig. 2	Figs. 9 and 11
B	$ω = ω_{12} + δ = ω_{34} - δ$	Fig. 3	Fig. 12
C	$ω_{α} = ω_{12},$ $ω_{β} = ω_{34}$	Fig. 4	Fig. 13
D	$ω_{α} = ω_{34} + δ,$ $ω_{β} = ω_{34} - δ$	Fig. 5	Fig. 14

Line	Frequency	Transition Dipole Moment
1+	$ω_{13} + \frac{δ + Ω^{'}}{2}$	$μ_{13} cos θ$
$1 c$	$ω_{13} + \frac{δ}{2}$	$μ_{13} (sin θ cos θ)^{1 / 2}$
1-	$ω_{13} + \frac{δ - Ω^{'}}{2}$	$μ_{13} sin θ$
C +	$\frac{ω_{13} + ω_{24} + Ω^{'}}{2}$	$(μ_{13} μ_{24} sin θ cos θ)^{1 / 2}$
C-	$\frac{ω_{13} + ω_{24} - Ω^{'}}{2}$	$(μ_{13} μ_{24} sin θ cos θ)^{1 / 2}$
2+	$ω_{24} - \frac{δ - Ω^{'}}{2}$	$- μ_{24} sin θ$
$2 c$	$ω_{24} - \frac{δ}{2}$	$μ_{24} (sin θ cos θ)^{1 / 2}$
2-	$ω_{24} - \frac{δ + Ω^{'}}{2}$	$μ_{24} cos θ$

Case	Rf Frequencies	Energy Diagrams	Observed and Calculated Spectra
A	$ω = ω_{12}$	Fig. 2	Figs. 8 and 10
A	$ω = ω_{12} + δ$	Fig. 2	Figs. 9 and 11
B	$ω = ω_{12} + δ = ω_{34} - δ$	Fig. 3	Fig. 12
C	$ω_{α} = ω_{12},$ $ω_{β} = ω_{34}$	Fig. 4	Fig. 13
D	$ω_{α} = ω_{34} + δ,$ $ω_{β} = ω_{34} - δ$	Fig. 5	Fig. 14

Line	Frequency	Transition Dipole Moment
1+	$ω_{13} + \frac{δ + Ω^{'}}{2}$	$μ_{13} cos θ$
$1 c$	$ω_{13} + \frac{δ}{2}$	$μ_{13} (sin θ cos θ)^{1 / 2}$
1-	$ω_{13} + \frac{δ - Ω^{'}}{2}$	$μ_{13} sin θ$
C +	$\frac{ω_{13} + ω_{24} + Ω^{'}}{2}$	$(μ_{13} μ_{24} sin θ cos θ)^{1 / 2}$
C-	$\frac{ω_{13} + ω_{24} - Ω^{'}}{2}$	$(μ_{13} μ_{24} sin θ cos θ)^{1 / 2}$
2+	$ω_{24} - \frac{δ - Ω^{'}}{2}$	$- μ_{24} sin θ$
$2 c$	$ω_{24} - \frac{δ}{2}$	$μ_{24} (sin θ cos θ)^{1 / 2}$
2-	$ω_{24} - \frac{δ + Ω^{'}}{2}$	$μ_{24} cos θ$

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Journal of the Optical Society of America B