Selective detection of uranium by laser-induced fluorescence: a potential remote-sensing technique. 1: Optical characteristics of uranyl geologic targets

J. P. deNeufville; A. Kasdan; R. J. L. Chimenti

doi:10.1364/AO.20.001279

Applied Optics
Vol. 20,
Issue 8,
pp. 1279-1296
(1981)
•https://doi.org/10.1364/AO.20.001279

Selective detection of uranium by laser-induced fluorescence: a potential remote-sensing technique. 1: Optical characteristics of uranyl geologic targets

J. P. deNeufville, A. Kasdan, and R. J. L. Chimenti

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J. P. deNeufville, A. Kasdan, and R. J. L. Chimenti, "Selective detection of uranium by laser-induced fluorescence: a potential remote-sensing technique. 1: Optical characteristics of uranyl geologic targets," Appl. Opt. 20, 1279-1296 (1981)

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Abstract

The remote sensing of laser-induced uranyl ion fluorescence is examined as a potential indicator of uranium occurring in geologic materials at the earth’s surface. The lifetime and brightness of the fluorescence from a wide variety of rocks, minerals, and soils are reported. The distinctive characteristics of uranyl ion absorption and fluorescence were observed in diverse geologic materials such as chalcedonies and opals containing 15–3000 ppm of uranium and in surface coatings of uranyl minerals such as metaautunite, liebigite, and andersonite. The conditions which permit the excitation and selective detection of uranyl ion fluorescence from such targets are described.

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Mineral	Composition	Crystal structure	Fluorescence
Mineral	Composition	Crystal structure	Intensity	Color
Autunite	Ca(UO₂)₂(PO₄)₂· 10–12 H₂O	Tetragonal	Strong	Yellow-green
Metaautunite	Ca(UO₂)₂(PO₄)₂· 8 H₂O	Tetragonal	Strong	Yellow-green
Metauranocircite	Ba(UO₂)₂(PO₄)₂· 8 H₂O	Tetragonal	Strong	Yellow-green
Saléeite	Mg(UO₂)₂(PO₄)₂· 8–10 H₂O	Tetragonal	Strong	Yellow-green
Uranospinite	Ca(UO₂)₂(AsO₄)₂· 10 H₂O	Tetragonal	Strong	Yellow-green
Zippeite	(UO₂)₂(SO₄)(OH)₂· 4 H₂O	Orthorhombic	Strong	Yellow-green
Schroeckingerite	NaCa₃(UO₂)(CO₃)₃(SO₄)F · 10 H₂O	Orthorhombic	Strong	Blue-green
Liebigite	Cao(UO₂)(CO₃)₃· 10 H₂O	Orthorhombic	Strong	Blue-green
Andersonite	Na₂Ca(UO₂)(CO₃)₃· 6 H₂O	Rhombohedral	Strong	Blue-green
Uranophane	Ca(UO₂)₂(SiO₃)₂(OH)₂· 5 H₂O	Monoclinic	Weak/none	(Yellow-green)
β-uranophane	Ca(UO₂)₂(SiO₃)₂(OH)₂· 5 H₂O	Monoclinic	Weak/none	(Yellow-green)
Tyuyamunite	Ca(UO₂)₂(VO₄)₂· 5–8 H₂O	Orthorhombic	Weak/none	(Yellow-green)
Carnotite	K₂(UO₂)₂(VO₄)₂· 1–3 H₂O	Monoclinic	Weak/none	(Yellow-green)
Torbenite	Cu(UO₂)₂(PO₄)₂· 10 H₂O	Tetragonal	None	—
Metatorbernite	Cu(UO₂)₂(PO₄)₂· 8 H₂O	Tetragonal	None	—

	Glass number
	1	2	3	4
Calculated composition,
Wt. %
SiO₂	60.19	61.63	61.63	61.63
B₂O₃	16.24	16.63	16.63	16.63
K₂O	21.02	21.52	21.52	21.52
As₂O₃	0.191	0.196	0.196	0.196
Na₂O₂	0.35	0.004
UO₂	2	0.02	0.002	0.0002
U	1.76	0.0176	0.0018	0.00018
U analysis31	1.4	0.014	0.0017	0.0002
Density,30 g · cm⁻³	2.544	2.419	2.510	2.511
Refractive index30 at 5896 Å	1.51302	1.50473	1.51022	1.51031
C₀, U atoms · cm⁻³	1.12 × 10²⁰	1.08 × 10¹⁸	1.12 × 10¹⁶	1.12 × 10¹⁶

Sample	Lifetime (μsec)		Yield
Sample	Range at 298 K	Value at 77 K	Yield
Uranyl minerals
Bulk minerals
Andersonite	460–269	800(460)^a	0.57
Metaautunite	85–257	253(188),	0.74
		231(257),	0.8,
		285(228)	0.8
Liebigite	400	960	0.42
Schroekingerite	490–571	870(490)	0.56
Metauranocircite	171–200	—	—
Efflorescent films	308–398	—	—
Uranyl in siliceous hosts
Opals and silica	171–486	—	—
Glass (1.5 wt. %)	270	570	0.49

Parameter	Value
Excitation wavelength λ_L	4250 Å
Refractive index n_m⁶	1.6
Transmissivity at λ_L, η_L	0.95
Transmissivity at λ_F, η_F	0.95
Fluorescence yield ϕ	0.8
Fluorescence decay rate Γ	4.38 × 10³ sec⁻¹
Absorption coefficient α(λ_L)	350 ± 100 cm⁻¹
Thickness L	30 μm
$\int_{0}^{\infty} \frac{λ_{L}}{λ} g (λ) d λ$	0.86

Sample	Description	Uranium content, ppm	Fluorescence amptitude	Relative fluorescence brightness, ppm A	Fluorescence lifetime, Γ⁻¹, μsec
Uranyl mineral samples:
U-119	Handpicked flakes of metaautunite from Daybreak Mine, Spokane County, Wash.^b; used as fluorescance brightness standard.		1.87 × 10⁶	10⁶^a	248
U-131	Andersonite-rich zones in sandstone sample from Monte-Christo Mine, Moab, Utah^b			2.54 × 10⁵	571
U-132	Metauranocircite crystals on one surface of rock sample from Anne Creek Mine, Lawrence County, S.D.^b			1.04 × 10⁶	200
U-133	Sandstone with crystals of andersonite on one surface from Grants, N.M.^b			2.99 × 10⁵	628
U-169	Tyuyamunite with geothite from Nevada		<2^d	—	—
U-141	Sandstone fragments and powder containing liebigite from White Canyon # 1 Mine, San Juan County, Utah^b			1.74 × 10⁵	400
U-146	Autunite from Mt. Spokane, Wash. (probably meta-autunite due to dehydration during sample storage); purchased from Wards Natural Scientific Establishment (WNSE); “Museum Collection of Short Wave Fluorescent Minerals” 8			1.21 × 10⁶	257
U-162	Autunite from pegmatite quarry, Haddam, Conn.^c			6.63 × 10⁵	86
U-163	Autunite from pegmatite quarry, Portland, Conn.^c		9.9 × 10³^d		171
U-164	Uranoapatite, Ruggles Mine, Grafton, N.H.^c		77.6^d		86
U-165	Metauranocircite from Bergen Falkenstein, Voightland, Saxony, Germany^c			8.72 × 10⁵	171
U-167	Schroeckingerite from Wamsutter, Wyo.^c			4.56 × 10⁵	571
U-118	Uranophane from Mitchell County, N.C., purchased from WNSE			25	171
Samples of rocks and minerals (mostly siliceous) and optic al glass containing fluorescent uranyl ions in dilute concentrations:
U-27	Vein filling of milky hyalite opal from Spruce Pine, N.C.^b	58		8.8 × 10³	429
U-50	Opalite from Virgin Valley, Humboldt County, Nev. WSNE “Museum Collection of Long Wavelength Fluorescent Minerals” 1	460^e		3.74 × 10⁵	486
U-54	Vein filling of glassy hyalite opal in pegmatite from Spruce Pine N.C., WSNE; long wavelength minerals 5; contains ~3 × 10³ ppm U and ~5 × 10³ ppm Cu by semiquantitative electron microprobe analysis	3 × 10³		4.33 × 10⁵	371
U-134	Common opal from near Casper, Wyo.^b	63^e		1.66 × 10⁴	429
U-138	Hyalite opal on geothite and iron phosphate from Polk County, Ark.^b			52	171
U-150	Chalcedony geode from near Deming, N.Mex.^b	18^e		2.6 × 10³	171
U-153	Hyalite opal from Scenic, S.Dak.^b	180^e		1.38 × 10⁴	143
U-155	Opalite on spar, Casper Mountain, S. Dak.^c			5.3 × 10³	343
U-156	Agate, Calico Mountain, Calif.^c			8.77 × 10³	171
U-157	Opalite from Bad Rivers Mountains, Ariz.^c	24^e		1.19 × 10³	457
U-158	Chalcedony concretion, Dugway Proving Ground, Utah^c	15^e		6.26 × 10³	257
U-159	Opalite on calcite from Utah^c			3.66 × 10⁴	286
U-151	Red Horn Coral from Woodland, Utah^c		17.1^d		200
Other fluorescent rocks and minerals:
U-143	Carpathite, Fourth of July Mine, San Benito Co., Calif.^b			21.7	1030
U-148	Aragonite from Pecos Valley, N.Mex., WNSE; short wavelength 4; UV-induced phosphorescence has lifetime of order 100 msec and very broadband emission spectrum	5^f		26	343
U-149	Hackmanite from Mt. St. Hilaire, Quebec, WNSE; short wavelength 6; green emission under short wavelength excitation suggests that uranyl fluorescence may dominate under such conditions			2.8 × 10²	143
U-152	Powellite from Randsburg, Calif.^c		3.3^d		200
U-145	Calcite from Franklin, N.J.; WNSE short wavelength 10		2.6^d		114
U-144	Willemite from Franklin, N.J.; WNSE short wave 6			3.8 × 10⁴	800
U-104	Esperite and willemite from Franklin, N.J.^c			4.97 × 10⁴	1060
U-97	Rhodonite, franklinite, and willemite from Franklin, N.J.^c			2.15 × 10⁴	200
U-95	Massive gem willemite from Franklin, N.J.^c			1.27 × 10⁴	1200
U-87	Sample of zinc ore from Franklin, N.J. containing esperite some willemite, trace, of calcite^c			4.8 × 10⁴	971
U-55	Calcite (stalactite) from near Missoula, Mont, WNSE; long wave 6		89.3^d		343
U-57	Mineral sample of trona from near Westvaco, Wyo., WNSE; longwave 8		5.5^d		286
U-58	Mineral sample of calcite (septaria) from Toole County, Utah, WNSE; longwave 9		41.5^d		171
U-59	Sample of chalcedony, pseudomorphous after coral from Tampa Bay, Fla., WNSE; longwave 10			5.2 × 10²	171
U-60	Turretella agate from near Wamsutter, Wyo., WNSE; longwave 11		11^d		257
U-61	Sample of shortite [Na₂Ca₂(CO₃)₃] from Green River, Wyo., WNSE; longwave 12; area fraction of fluorescence could not be estimated		10^d		57
U-62	Scapolite sample from Harcourt Township, Ontario, Can., WNSE; longwave 13		<2^d
Soils from uraniferous and nonuraniferous terrains^d^,^f
U-4	Surface soil sample from immediate vicinity of open-pit uranium mine near Three Rivers, Tex.^b		6
U-8	Like U-4		6
U-10	Like U-4		6
U-11	Like U-4		6
U-12	Like U-4		6
U-13	Like U-4		6
U-21	Like U-4		6
U-5	Like U-4		4
U-14	Like U-4		4
U-17	Like U-4		4
U-18	Like U-4		4
U-19	Like U-4	1400	4
U-20	Like U-4		4
U-3	Like U-4	23	2
U-1	Tailings from uranium mill near Three Rivers, Tex.^b	200	2
U-2	Like U-1	48	10		293
U-9	Floor of open-pit uranium mine near Three Rivers, Tex.^b	260	10		143
U-15	Surface soil sample from prior ore pad, open-pit uranium mine near Three Rivers, Tex.^b	88	10		214
U-16	Like U-15	9	2
U-6	Like U-15	4100	6
U-7	Like U-15	2200	2
	Samples U-29 through U-48 are a series of standard soil samples purchased from Wards National Scientific Establishment, Soil Types—45W 6550 ^d
U-29	Gravelly soil, Rochester, N.Y.	<2	<2
U-30	Residual soil from granite, Spruce Pine, N.C.	2	<2
U-31	Sandy soil, Irondequoit, N.Y.	<2	<2
U-32	Wind-blown sand, Webster, N.Y.	2	<2
U-33	Beach sand, Rochester, N.Y.	2	<2
U-34	Slit, Industry, N.Y.	2	<2
U-35	Fire clay, Golden, Colo.	4	<2
U-36	Loess, Kansas City, Kan.	2	<2
U-37	Adobe, Deming, N.Mex.	2	<2
U-38	Sandy Loam, Irondequoit, N.Y.	<2	<2
U-39	Clay loam, East Bloomfield, N.Y.	2	<2
U-40	Silt loam, Avon, N.Y.	<2	<2
U-41	Residual soil from mica schist, Mitchell Co., N.C.	<2	<2
U-42	Residual soil from limonite, Birmingham, Ala.	7	<2
U-43	Residual soil from siliceous oolite, State College, Penn.	<2	<2
U-44	Residua] soil from hornblende schist, Mithcell Co., N.C.	3	<2
U-45	Greensand, Birmingham, N.J.	<2	<2
U-46	Peat, Somerset, England	<2	<2
U-47	Peat moss, Junius, N.Y.	<2	<2
U-48	Muck, Wayne County, N.Y.	4	<2
U-65-U-84	Surface soil samples are collected^b on a grid above a deeply buried uranium ore deposit in West Highland, Wyo.; none of these samples showed a detectable level of fluorescence within the selective window	≤4^f	≤2^d

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Applied Optics