Isotopes of rutherfordium

Rutherfordium (Rf) is a synthetic element, and thus a standard atomic mass cannot be given. Like all synthetic elements, it has no stable isotopes. The first isotope to be synthesized was either ²⁵⁹Rf in 1966 or ²⁵⁷Rf in 1969. There are 15 known radioisotopes from ²⁵³Rf to ²⁶⁸Rf (2 of which, ²⁶⁶Rf and ²⁶⁸Rf, are unconfirmed) and 4 isomers. The longest-lived isotope is ²⁶⁷Rf with an estimated half-life of 5 hours. The longest directly measured half-life is ²⁶³Rf at 11 minutes, and the longest-lived isomer is ^261mRf with a half-life of 81 seconds.

Table

nuclide symbol	Z(p)	N(n)	isotopic mass (u)	half-life	decay mode(s)[1][n 1]	daughter isotope(s)	nuclear spin
	excitation energy
^253Rf	104	149	253.10044(44)#	13(5) ms	SF (51%)	(various)	(7/2)(+#)
					α (49%)	^249No
^253mRf	200(150)# keV			52(14) µs [48(+17−10) µs]	SF	(various)	(1/2)(−#)
^254Rf	104	150	254.10005(30)#	23(3) µs	SF (99.7%)	(various)	0+
					α (.3%)	^250No
^255Rf	104	151	255.10127(12)#	1.64(11) s	SF (52%)	(various)	(9/2−)#
					α (48%)	^251No
^256Rf	104	152	256.101152(19)	6.45(14) ms	SF (96%)	(various)	0+
					α (6%)	^252No
^257Rf	104	153	257.102918(12)#	4.7(3) s	α (79%)	^253No	(1/2+)
					β^+ (18%)	^257Lr
					SF (2.4%)	(various)
^257mRf	114(17) keV			3.9(4) s			(11/2−)
^258Rf	104	154	258.10343(3)	12(2) ms	SF (87%)	(various)	0+
					α (13%)	^254No
^259Rf	104	155	259.10560(8)#	2.8(4) s	α (93%)	^255No	7/2+#
					SF (7%)	(various)
					β^+ (.3%)	^259Lr
^260Rf	104	156	260.10644(22)#	21(1) ms	SF (98%)	(various)	0+
					α (2%)	^256No
^261Rf	104	157	261.10877(5)	68 s[2]	α (76%)	^257No	9/2+#
					β^+ (14%)	^261Lr
					SF (10%)	(various)
^261mRf	70(100)# keV			1.9(4) s[3]	SF (73%)	(various)	3/2+#
					α (27%)	^257No
^262Rf	104	158	262.10993(24)#	2.3(4) s	SF (99.2%)	(various)	0+
					α (.8%)	^258No
^262mRf	600(400)# keV			47(5) ms	SF	(various)	high
^263Rf	104	159	263.1125(2)#	11(3) min	SF (70%)	(various)	3/2+#
					α (30%)	^259No
^264Rf	104	160	264.11388(39)#	1# h	SF	(various)	0+
^265Rf[n 2]	104	161	265.11668(39)#	1.0 min[4]	SF	(various)
^266Rf[n 3][n 4]	104	162	266.11817(50)#	10# h			0+
^267Rf[n 5]	104	163	267.12179(62)#	1.3 h	SF	(various)
^268Rf[n 3][n 6]	104	164	268.12397(77)#	1# h			0+

1. Abbreviations:
   EC: Electron capture
   SF: Spontaneous fission
2. Not directly synthesized, occurs in decay chain of ²⁸⁵Fl
3. Discovery of this isotope is unconfirmed
4. Not directly synthesized, occurs in decay chain of ²⁸²Uut
5. Not directly synthesized, occurs in decay chain of ²⁸⁷Fl
6. Not directly synthesized, occurs in decay chain of ²⁸⁸Uup

Notes

• Values marked # are not purely derived from experimental data, but at least partly from systematic trends. Spins with weak assignment arguments are enclosed in parentheses.
• Uncertainties are given in concise form in parentheses after the corresponding last digits. Uncertainty values denote one standard deviation, except isotopic composition and standard atomic mass from IUPAC, which use expanded uncertainties.

Nucleosynthesis

Super-heavy elements such as rutherfordium are produced by bombarding lighter elements in particle accelerators that induces fusion reactions. Whereas most of the isotopes of rutherfordium can be synthesized directly this way, some heavier ones have only been observed as decay products of elements with higher atomic numbers.^[5]

Depending on the energies involved, the former are separated into "hot" and "cold". In hot fusion reactions, very light, high-energy projectiles are accelerated toward very heavy targets (actinides), giving rise to compound nuclei at high excitation energy (~40–50 MeV) that may either fission or evaporate several (3 to 5) neutrons.^[5] In cold fusion reactions, the produced fused nuclei have a relatively low excitation energy (~10–20 MeV), which decreases the probability that these products will undergo fission reactions. As the fused nuclei cool to the ground state, they require emission of only one or two neutrons, and thus, allows for the generation of more neutron-rich products.^[6] The latter is a distinct concept from that of where nuclear fusion claimed to be achieved at room temperature conditions (see cold fusion).^[7]

Hot fusion studies

The synthesis of rutherfordium was first attempted in 1964 by the team at Dubna using the hot fusion reaction of neon-22 projectiles with plutonium-242 targets:

242
94Pu + 22
10Ne → 264−x
104Rf + 3 or 5 n.

The first study produced evidence for a spontaneous fission with a 0.3 second half-life and another one at 8 seconds. While the former observation was eventually retracted, the latter eventually became associated with the ²⁵⁹Rf isotope.^[8] In 1966, the Soviet team repeated the experiment using a chemical study of volatile chloride products. They identified a volatile chloride with eka-hafnium properties that decayed fast through spontaneous fission. This gave strong evidence for the formation of RfCl₄, and although a half-life was not accurately measured, later evidence suggested that the product was most likely ²⁵⁹Rf. The team repeated the experiment several times over the next few years, and in 1971, they revised the spontaneous fission half-life for the isotope at 4.5 seconds.^[8]

In 1969, researchers at the University of California led by Albert Ghiorso, tried to confirm the original results reported at Dubna. In a reaction of curium-248 with oxygen-16, they were unable to confirm the result of the Soviet team, but managed to observe the spontaneous fission of ²⁶⁰Rf with a very short half-life of 10–30 ms:

248
96Cm + 16
8O → 260
104Rf + 4 n.

In 1970, the American team also studied the same reaction with oxygen-18 and identified ²⁶¹Rf with a half-life of 65 seconds (later refined to 75 seconds).^[9][10] Later experiments at the Lawrence Berkeley National Laboratory in California also revealed the formation of a short-lived isomer of ²⁶²Rf (which undergoes spontaneous fission with a half-life of 47 ms),^[11] and spontaneous fission activities with long lifetimes tentatively assigned to ²⁶³Rf.^[12]

Diagram of the experimental set-up used in the discovery of isotopes ²⁵⁷Rf and ²⁵⁹Rf

The reaction of californium-249 with carbon-13 was also investigated by the Ghiorso team, which indicated the formation of the short-lived ²⁵⁸Rf (which undergoes spontaneous fission in 11 ms):^[13]

249
98Cf + 13
6C → 258
104Rf + 4 n.

In trying to confirm these results by using carbon-12 instead, they also observed the first alpha decays from ²⁵⁷Rf.^[13]

The reaction of berkelium-249 with nitrogen-14 was first studied in Dubna in 1977, and in 1985, researchers there confirmed the formation of the ²⁶⁰Rf isotope which quickly undergoes spontaneous fission in 28 ms:^[8]

249
97Bk + 14
7N → 260
104Rf + 3 n.

In 1996 the isotope ²⁶²Rf was observed in LBNL from the fusion of plutonium-244 with neon-22:

244
94Pu + 22
10Ne → 266−x
104Rf + 4 or 5 n.

The team determined a half-life of 2.1 seconds, in contrast to earlier reports of 47 ms and suggested that the two half-lives might be due to different isomeric states of ²⁶²Rf.^[14] Studies on the same reaction by a team at Dubna, lead to the observation in 2000 of alpha decays from ²⁶¹Rf and spontaneous fissions of ^261mRf.^[15]

The hot fusion reaction using a uranium target was first reported at Dubna in 2000:

238
92U + 26
12Mg → 264−x
104Rf + x n (x = 3, 4, 5, 6).

They observed decays from ²⁶⁰Rf and ²⁵⁹Rf, and later for ²⁵⁹Rf. In 2006, as part of their program on the study of uranium targets in hot fusion reactions, the team at LBNL also observed ²⁶¹Rf.^[15][16][17]

Cold fusion studies

The first cold fusion experiments involving element 104 were done in 1974 at Dubna, by using light titanium-50 nuclei aimed at lead-208 isotope targets:

208
82Pb + 50
22Ti → 258−x
104Rf + x n (x = 1, 2, or 3).

The measurement of a spontaneous fission activity was assigned to ²⁵⁶Rf,^[18] while later studies done at the Gesellschaft für Schwerionenforschung Institute (GSI), also measured decay properties for the isotopes ²⁵⁷Rf, and ²⁵⁵Rf.^[19][20]

In 1974 researchers at Dubna investigated the reaction of lead-207 with titanium-50 to produce the isotope ²⁵⁵Rf.^[21] In a 1994 study at GSI using the lead-206 isotope, ²⁵⁵Rf as well as ²⁵⁴Rf were detected. ²⁵³Rf was similarly detected that year when lead-204 was used instead.^[20]

Decay studies

Most isotopes with an atomic mass below 262 have also observed as decay products of elements with a higher atomic number, allowing for refinement of their previously measured properties. Heavier isotopes of rutherfordium have only been observed as decay products. For example, a few alpha decay events terminating in ²⁶⁷Rf were observed in the decay chain of darmstadtium-279 since 2004:

279
110Ds → 275
108Hs + α → 271
106Sg + α → 267
104Rf + α.

This further underwent spontaneous fission with a half-life of about 1.3 h.^[22][23][24]

Investigations on the synthesis of the dubnium-263 isotope in 1999 at the University of Bern revealed events consistent with electron capture to form ²⁶³Rf. A rutherfordium fraction was separated, and several spontaneous fission events with long half-lives of about 15 minutes were observed, as well as and alpha decays with half-lives of about 10 minutes.^[12] Reports on the decay chain of flerovium-285 in 2010 showed five sequential alpha decays that terminate in ²⁶⁵Rf, which further undergoes spontaneous fission with a half-life of 152 seconds.^[25]

Some experimental evidence was obtained in 2004 for an even heavier isotope, ²⁶⁸Rf, in the decay chain of an isotope of ununpentium:

288
115Uup → 284
113Uut + α → 280
111Rg + α → 276
109Mt + α → 272
107Bh + α → 268
105Db + α ? → 268
104Rf + ν
e.

However, the last step in this chain was uncertain. After observing the five alpha decay events that generate dubnium-268, spontaneous fission events were observed with a long half-life. It is unclear whether these events were due to direct spontaneous fission of ²⁶⁸Db, or ²⁶⁸Db produced electron capture events with long half-lives to generate ²⁶⁸Rf. If the latter is produced and decays with a short half-life, the two possibilities cannot be distinguished.^[26] Given that the electron capture of ²⁶⁸Db cannot be detected, these spontaneous fission events may be due to ²⁶⁸Rf, in which case the half-life of this isotope cannot be extracted.^[27][28]

According to a 2007 report on the synthesis of ununtrium, the isotope ²⁸²113 was observed to undergo a similar decay to form ²⁶⁶Db, which undergoes spontaneous fission with a half-life of 22 minutes. Given that the electron capture of ²⁶⁶Db cannot be detected, these spontaneous fission events may be due to ²⁶⁶Rf, in which case the half-life of this isotope cannot be extracted.^[29][30]

Nuclear isomerism

Currently suggested decay level scheme for ²⁵⁷Rf^g,m from the studies reported in 2007 by Hessberger et al. at GSI^[31]

Several early studies on the synthesis of ²⁶³Rf have indicated that this nuclide decays primarily by spontaneous fission with a half-life of 10–20 minutes. More recently, a study of hassium isotopes allowed the synthesis of atoms of ²⁶³Rf decaying with a shorter half-life of 8 seconds. These two different decay modes must be associated with two isomeric states, but specific assignments are difficult due to the low number of observed events.^[12]

During research on the synthesis of rutherfordium isotopes utilizing the ²⁴⁴Pu(²²Ne,5n)²⁶¹Rf reaction, the product was found to undergo exclusive 8.28 MeV alpha decay with a half-life of 78 seconds. Later studies at GSI on the synthesis of copernicium and hassium isotopes produced conflicting data, as ²⁶¹Rf produced in the decay chain was found to undergo 8.52 MeV alpha decay with a half-life of 4 seconds. Later results indicated a predominant fission branch. These contradictions led to some doubt on the discovery of copernicium. The first isomer is currently denoted ^261aRf (or simply ²⁶¹Rf) whilst the second is denoted ^261bRf (or ^261mRf). However, it is thought that the first nucleus belongs to a high-spin ground state and the latter to a low-spin metastable state.^[32] The discovery and confirmation of ^261bRf provided proof for the discovery of copernicium in 1996.^[33]

A detailed spectroscopic study of the production of ²⁵⁷Rf nuclei using the reaction ²⁰⁸Pb(⁵⁰Ti,n)²⁵⁷Rf allowed the identification of an isomeric level in ²⁵⁷Rf. The work confirmed that ^257gRf has a complex spectrum with 15 alpha lines. A level structure diagram was calculated for both isomers.^[34] Similar isomers were reported for ²⁵⁶Rf also.^[35]

Future experiments

The team at GSI are planning to perform first detailed spectroscopic studies on the isotope ²⁵⁹Rf. It will be produced in the new reaction:

$\,^{238}_{92}\mathrm{U}\ + \,^{24}_{12}\mathrm{Mg}\to \,^{259}_{104}\mathrm{Rf}\ + 3 \,^{1}_{0}\mathrm{n}$

Chemical yields of isotopes

Cold fusion

The table below provides cross-sections and excitation energies for cold fusion reactions producing rutherfordium isotopes directly. Data in bold represents maxima derived from excitation function measurements. + represents an observed exit channel.

Projectile	Target	CN	1n	2n	3n
^50Ti	^208Pb	^258Rf	38.0 nb, 17.0 MeV	12.3 nb, 21.5 MeV	660 pb, 29.0 MeV
^50Ti	^207Pb	^257Rf	4.8 nb
^50Ti	^206Pb	^256Rf	800 pb, 21.5 MeV	2.4 nb, 21.5 MeV
^50Ti	^204Pb	^254Rf	190 pb, 15.6 MeV
^48Ti	^208Pb	^256Rf	380 pb, 17.0 MeV

Hot fusion

The table below provides cross-sections and excitation energies for hot fusion reactions producing rutherfordium isotopes directly. Data in bold represents maxima derived from excitation function measurements. + represents an observed exit channel.

Projectile	Target	CN	3n	4n	5n
^26Mg	^238U	^264Rf		240 pb	1.1 nb
^22Ne	^244Pu	^266Rf		+	4.0 nb
^18O	^248Cm	^266Rf		+	13.0 nb

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• Isotope masses from:
  • M. Wang; G. Audi; A. H. Wapstra; F. G. Kondev; M. MacCormick; X. Xu; et al. (2012). "The AME2012 atomic mass evaluation (II). Tables, graphs and references." (PDF). Chinese Physics C 36 (12): 1603–2014. Bibcode:2012ChPhC..36....3M. doi:10.1088/1674-1137/36/12/003.
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• Isotopic compositions and standard atomic masses from:
  • J. R. de Laeter; J. K. Böhlke; P. De Bièvre; H. Hidaka; H. S. Peiser; K. J. R. Rosman; P. D. P. Taylor (2003). "Atomic weights of the elements. Review 2000 (IUPAC Technical Report)". Pure and Applied Chemistry 75 (6): 683–800. doi:10.1351/pac200375060683.
  • M. E. Wieser (2006). "Atomic weights of the elements 2005 (IUPAC Technical Report)". Pure and Applied Chemistry 78 (11): 2051–2066. doi:10.1351/pac200678112051. Lay summary.
• Half-life, spin, and isomer data selected from the following sources. See editing notes on this article's talk page.
  • G. Audi; A. H. Wapstra; C. Thibault; J. Blachot; O. Bersillon (2003). "The NUBASE evaluation of nuclear and decay properties" (PDF). Nuclear Physics A 729 (1): 3–128. Bibcode:2003NuPhA.729....3A. doi:10.1016/j.nuclphysa.2003.11.001.
  • National Nuclear Data Center. "NuDat 2.1 database". Brookhaven National Laboratory. Retrieved September 2005.
  • N. E. Holden (2004). "Table of the Isotopes". In D. R. Lide. CRC Handbook of Chemistry and Physics (85th ed.). CRC Press. Section 11. ISBN 978-0-8493-0485-9.

External links

• http://www.radiochemistry.org/periodictable/elements/isotopes_data/104.html
• http://www-phynu.cea.fr/science_en_ligne/carte_potentiels_microscopiques/choix/isotopes/z104_eng.html
• http://www.springermaterials.com/docs/info/978-3-540-70609-0_7730.html