Photofragmentation-laser induced fluorescence: a new method for detecting atmospheric trace gases

M. O. Rodgers; K. Asai; D. D. Davis

doi:10.1364/AO.19.003597

Applied Optics
Vol. 19,
Issue 21,
pp. 3597-3605
(1980)
•https://doi.org/10.1364/AO.19.003597

Photofragmentation-laser induced fluorescence: a new method for detecting atmospheric trace gases

M. O. Rodgers, K. Asai, and D. D. Davis

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M. O. Rodgers, K. Asai, and D. D. Davis, "Photofragmentation-laser induced fluorescence: a new method for detecting atmospheric trace gases," Appl. Opt. 19, 3597-3605 (1980)

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Abstract

A new method for the in situ detection of nonfluorescing molecular species is proposed: photofragmentation-laser induced fluorescence (PF-LIF). In this approach, the species to be detected is first laser photolyzed at a wavelength λ₁, producing one or more vibrationally excited photofragments. Before vibrational relaxation occurs, one of these photofragments is pumped into a bonding excited state by a second laser pulse centered at wavelength λ₂. Fluorescence is sampled at a wavelength λ₃, where λ₃ < λ₂ and λ₁. This pumping configuration thus permits massive discrimination against Rayleigh and Raman scattering as well as white noise fluorescence from the laser wavelengths λ₁ and λ₂. The technique should be both highly sensitive and selective for numerous atmospheric trace gases. Specific sampling schemes for detecting NO₂, NO₃, and HNO₂ are proposed. Various noise sources and chemical interferences are discussed. Specific calculations that estimate the sensitivity of the PF-LIF system for detecting NO₂, NO₃, and HNO₂ are given.

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Term	Variables	Ref.
$E_{λ_{2}} = 3.4 \times 10^{- 2}$	$P_{λ_{2}} = 2.1 \times 10^{15} photons$	Assumed
	$σ_{λ_{2}} = 8 \times 10^{- 18} {cm}^{2}$	18
	$σ_{λ_{1}} = 0.5 {cm}^{2}$	Assumed
E_f = 7.1 × 10⁻³	k_f = 6.3 × 10⁶ sec⁻¹	19
	k_d = 0	20
	k_q = 1.7 × 10⁻¹⁰ cm³/sec	21
	[M] = 5.2 × 10¹⁸ cm⁻³	22
E_d = 1.4 × 10⁻⁴	$γ_{λ_{3}} = 0.16$	23
	$Y_{λ_{3}} = 0.09$	Assumed
	$Z_{λ_{3}} = 0.05$	Assumed
	$ϕ_{λ_{3}} = 0.20$	Assumed
E_e = 1.0		Assumed
V = 7.5 × 10⁻¹ cm³	$a_{λ_{1}} = 0.5 {cm}^{2}$	Assumed
	l = 1.5 cm	Assumed

Species	$P_{λ_{1}} (\times 1 0^{16})$	$σ_{λ_{1}} {({cm}^{2})}^{11}$	f_i (×10⁻²)	Q	F	$E_{λ_{1}}$
NO₂	1.1	1.3 × 10⁻¹⁹	1.5	1.012	1.0	4.3 × 10⁻⁵
HNO₂	8.9	1.2 × 10⁻¹⁹	1	0.914	1.0	1.9 × 10⁻⁴
NO₃	7.4	5.5 × 10⁻¹⁸	2	0.3513	1.0	3.9 × 10⁻³

Species	Concentration	Number of laser shots (min at 20 Hz)	Estimated signal counts	Estimated24 noise counts	Signal real noise	Signal25 statistical noise
NO₂	5 × 10⁸	6000 (5 min)	20	0.5	40:1	4.5:1
	2.5 × 10⁸	12000 (10 min)	20	1	20:1	4.5:1
	7.5 × 10⁷	24000 (20 min)	12	2	6:1	3.5:1
HNO₂	5 × 10⁸	6000 (5 min)	46	0.25	184:1	6.8:1
	1.25 × 10⁸	12000 (10 min)	23	0.5	46:1	4.8:1
	2.5 × 10⁷	12000 (10 min)	30	1	30:1	5.5:1
NO₃	2.5 × 10⁷	12000 (10 min)	30	1	30:1	5.5:1
	7.5 × 10⁶	24000 (20 min)	20	2	10:1	4.5:1
	2.5 × 10⁶	24000 (20 min)	7	2	3.5:1	2.6:1

Term	Variables	Ref.
$E_{λ_{2}} = 3.4 \times 10^{- 2}$	$P_{λ_{2}} = 2.1 \times 10^{15} photons$	Assumed
	$σ_{λ_{2}} = 8 \times 10^{- 18} {cm}^{2}$	18
	$σ_{λ_{1}} = 0.5 {cm}^{2}$	Assumed
E_f = 7.1 × 10⁻³	k_f = 6.3 × 10⁶ sec⁻¹	19
	k_d = 0	20
	k_q = 1.7 × 10⁻¹⁰ cm³/sec	21
	[M] = 5.2 × 10¹⁸ cm⁻³	22
E_d = 1.4 × 10⁻⁴	$γ_{λ_{3}} = 0.16$	23
	$Y_{λ_{3}} = 0.09$	Assumed
	$Z_{λ_{3}} = 0.05$	Assumed
	$ϕ_{λ_{3}} = 0.20$	Assumed
E_e = 1.0		Assumed
V = 7.5 × 10⁻¹ cm³	$a_{λ_{1}} = 0.5 {cm}^{2}$	Assumed
	l = 1.5 cm	Assumed

Species	$P_{λ_{1}} (\times 1 0^{16})$	$σ_{λ_{1}} {({cm}^{2})}^{11}$	f_i (×10⁻²)	Q	F	$E_{λ_{1}}$
NO₂	1.1	1.3 × 10⁻¹⁹	1.5	1.012	1.0	4.3 × 10⁻⁵
HNO₂	8.9	1.2 × 10⁻¹⁹	1	0.914	1.0	1.9 × 10⁻⁴
NO₃	7.4	5.5 × 10⁻¹⁸	2	0.3513	1.0	3.9 × 10⁻³

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Applied Optics