Superheavy Element Research Superheavy Element Research
www.superheavies.de
c.e.duellmann@gsi.de
Superheavy Element Research
News from GSI and Mainz
Christoph E. Düllmann
Johannes Gutenberg University Mainz
GSI Helmholtzzentrum für Schwerionenforschung GmbH, Darmstadt
Helmholtz Institute Mainz
FIAS Colloquium
Frankfurt Institute of Advanced Studies, Frankfurt, Germany, October 20, 2011
The next 60 minutes:
• Superheavy elements – Brief introduction, introduction status of
the field
• Facilities + program at GSI, U. Mainz, HIM
• Research at the TASCA gas-filled recoil separator
– Physics Example
Search for Element 120
– Chemistry Example
Element 114: noble metal or noble gas?
• Bi Brief fwrap-up
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
82
50
Peak of
Calcium
20
Map of the Nuclear Landscape
Peak of Tin
Uranium Summit
Peak of Lead
20 82 126
Flerov & Ilyinov (1986)
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Potential
ene ergy / MMeV
Influence of shell effects on fission barrier
2.5 MeV
~0.5 MeV LD + shell
no barrier!
Cf
250 50
98 152
LD 250 25098 98152
SSg
268 268106162 106 162
298 114184
298
114 114184
macroscopic barrier:
Disappears at Z ~ 104!
Deformation β2 after A. Sobiczewski / S. Hofmann
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Potential
ene ergy / MMeV
Influence of shell effects on fission barrier
LD + shell
no barrier!
Cf
250 50
98 152
LD 250 25098 98152
SSg
268 268106162 106 162
298 114184
298
114 114184
macroscopic barrier:
Disappears at Z ~ 104!
with shell structure:
spherical � deformed ground state
fi fission i bbarrier i iis also l > 0 ffor
elements with Z �104.
some fission barriers have
complicated shapes, multiplyhumped
elements that exist only thanks
to shell effects:
superheavy elements
Deformation β2 after A. Sobiczewski / S. Hofmann
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
~114 –
126 (?)
82
50
20
Map of the Nuclear Landscape
Island of Stability
20 82 126
184
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Cross Sections in Hot / Cold / 48 Ca Induced Fusion Reactions
1 pb: ~1-2 Events per Week
Compilation: A. Yakushev, Habilitation thesis, TU Munich, 2009
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Cross Sections in Hot / Cold / 48 Ca Induced Fusion Reactions
Compilation: A. Yakushev, Habilitation thesis, TU Munich, 2009
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Unique Combination for SHE Studies
ECR +
Stable
UNILAC targets
Beam
TRIGA-
Actinide
targets g
-LASER LASER
Radiochem.
-TRAP labs
SHIP
TASCA
Chemistry
SHIPTRAP
TASISpec
Chemical
theory
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
HIM – The New Helmholtz Institute Mainz
HIM Director: Frank Maas
-
-J. Dvorak (IRiS)
(currently on leave of absence)
-
Chemistry Physics
CED N.N.
Toward a dedicated cw LINAC for SHE; ...
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Toward A New Accelerator for SHE Research
ps
sity / pp
m Intens
Beam
Pulsed
0 10 20 30 40
Time / ms
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Toward A New Accelerator for SHE Research
ps
sity / pp
m Intens
Beam
Pulsed �� �� cw Beams
0 10 20 30 40
Time / ms
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Toward A New Accelerator for SHE Research
ps
sity / pp
m Intens
Beam
Pulsed �� �� cw Beams
0 10 20 30 40
Time / ms
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Toward A New Accelerator for SHE Research
Beamm
Intenssity
/ ppps
Perspectives:
Pulsed �� �� cw Beams
New dedicated SHE cw cw-LINAC LINAC
In combination with new 28 GHz ECR ion source:
10x higher beam intensity
0 10 20 30 40
Time / ms
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Toward a Dedicated SHE LINAC
UNILAC not suited for simultaneous
FAIR (A>180 (A>180, �3 �3 Hz Hz, 100 �s �s pulses)
SHE operation (A
Toward a Dedicated SHE LINAC
UNILAC not suited for simultaneous
WW. Barth
S. Mickat
U. Ratzinger
FAIR (A>180 (A>180, �3 �3 Hz Hz, 100 �s �s pulses)
SHE operation (A
The Darmstadt/Mainz SHE Community
GSI Helmholtz Center for Heavy ion Research, Darmstadt:
SHE Chemistry (TASCA / X1) Department:
Scientific staff
Technical staff
Diploma / PhD students
Ch.E. Düllmann, A. Yakushev, V. Pershina (Theory) [3]
E. Jäger, J. Krier, J. Runke (@ JG Univ. Mainz), B. Schausten, M. Grimm [5]
SHE Physics y (SHIP/SHIPTRAP) ( ) Department: p
F.P. Hessberger, N.N. (NF Rudolph), D. Ackermann, M. Block, S. Heinz, S. Hofmann [5]
H.-G. Burkhard [1]
Target Laboratory Laboratory, Detector Laboratory Laboratory, Experimental Electronics Electronics....
Johannes Gutenberg-University Mainz (Institute for Nuclear Chemistry):
Ch.E. Düllmann (SHE Chemistry), N.N. (NF Rudolph, SHE Physics); J.V. Kratz,
NN. TTrautmann, t N. N Wi Wiehl hl [3]
J. Even, D. Hild, S. Klein, D. Renisch, A. Vascon [5]
Ch. Mokry, P. Thörle-Pospiech
TTransuranium i TTarget t Lab: L b K. Eberhardt et al.
[2]
Helmholtz Institute Mainz:
Ch.E. Düllmann (SHE ( Chem.), ), F.P. Hessberger g ( (SHE Physics, y , interim), ), N.N. (NF ( Rudolph) p )
J. Dvorak (on leave), J. Khuyagbaatar, L.-L. Andersson, E. Rodriguez Minaya
J. Maurer, V. Yakusheva [6]
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Current International Collaboration Partners
(SHE Chemistry / TASCA)
LBNL/UCB Berkeley (USA) U Lund (Sweden)
LLNL Livermore (USA) U Jyväskylä (Finland)
Vanderbilt U (USA) UOslo(Norway)
U Oslo (Norway)
ORNL Oak Ridge (USA) Chalmers U Gothenburg (Sweden)
UNAL Bogota (Columbia) PSI Villigen (Switzerland)
U Liverpool (UK) ITE Warschau (Poland)
U Surrey (UK) SINP Kolkata (India)
IMP Lanzhou (China)
JAEA Tokai (Japan)
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
TransActinide Separator and Chemistry Apparatus
A Separator for Actinide Based Reactions
www.gsi.de/tasca
M. Schädel, Eur. Phys. J. D 45 (2007) 67
A. Semchenkov et al., NIMB 266 (2008) 4153
Timeline
2002 goals defined
2003 community formed
2004 decision: gas-filled sep sep.
2005 start building TASCA
define commissioning prog.
2006 first beam in cave (Jan.)
first EVR in focal plane det.(Apr.)
2006-2008
TASCA commissioning
2008 commissioning completed:
Transactinides reached! Z=104
2009 Heaviest Element at GSI: Z=114
2011 Hunting element 120
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
TransActinide Separator and Chemistry Apparatus
A Separator for Actinide Based Reactions
www.gsi.de/tasca
M. Schädel, Eur. Phys. J. D 45 (2007) 67
A. Semchenkov et al., NIMB 266 (2008) 4153
Timeline
2002 goals defined
2003 community formed
2004 decision: gas-filled sep sep.
2005 start building TASCA
define commissioning prog.
2006 first beam in cave (Jan.)
first EVR in focal plane det.(Apr.)
2006-2008
TASCA commissioning
2008 commissioning completed:
Transactinides reached! Z=104
2009 Heaviest Element at GSI: Z=114
2011 Hunting element 120
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Recoil Separators for SHE studies
Beam
Target
1) Synthesis of SHE; Decay studies
in Focal Plane Detectors
TASCA
TransActinide Separator
and Chemistry Apparatus
Particle Detector (�; e - ; SF)
Photon Detector (�; X)
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Recoil Separators for SHE studies
Beam
Target
1) Synthesis of SHE; Decay studies
in Focal Plane Detectors
TASCA
Inert gas TransActinide Separator
(He, ( , Ar,...) , ) and Chemistry Apparatus
2) Preseparated SHE for chemical studies under low-background
conditions (Important for volatile p-Elements Z=112, 114, ...)
To chemistry y setup p
(e.g., gas phase
chromatography in
COMPACT)
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
SHE physics
at TASCA
Briefly looking back: element 114 in 2009
Hot topic 2011: search for new element 120
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
2009: The Element 114 TASCA Experiment
13 Decay Chains in 22 Days � Highest SHE Detection Rate
48Ca+ 244Pu � 292114* � 288114+4n / 289114+3n 4n Evaporation Channel:
284 284CCn +31
97 ms
-19
SF
SF
�
288 114
DGFRS
288 114
+0.27
0.80 -0.16s
� 9.94�0.06
�
TASCA
288 114
+0.24
0.47 -0.12 s
� 9.95�0.03
3n Evaporation Channel:
DGFRS
289 114
+1.2
2.6 -0.7 s
� 9.82�0.05
284 284CCn 285 285CCn +50
101 -25
ms
SF �
+13
29 -7 s
� 9.15�0.05 �
SF
281Ds +5.0
11.1 -2.7 s
281Ds +20
20 -7 s
SF
SF (�)
SF 277Hs +15
3 -1 ms
SF
SF
�
�
SF
289 289114 114
285 285CCn +30
30 -10 s
� 9.21�0.03
�
TASCA
289 114
+0.97
0.97 s -0.32
� 9.87�0.03
TASCA data:
Ch.E.Düllmann et al.,
PRL 104 (2010) 252701
J.M. Gates et al.
PRC 83 (2011) 054618
DGFRS Data
YYu.Ts. T Oganessian O i et t al., l
JPG 34 (2007) R165
PRC 69 (2004) 054607
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
244 Pu+ 48 Ca: High cross sections for element 114 confirmed
RRun 1 RRun 2
4n
Energies g studied at
TASCA
DGFRS Data
Oganessian et al.,
J. Phys. G, 2008
3n TASCA Data
Ch.E.Düllmann et al.,
PRL 104 (2010) 252701
JM J.M. GGates t et t al. l
PRC 83 (2011) 054618
Error bars include statistical errors.
TASCA systematic error is estimated to 14%.
Theory
V. Zagrebaev,
NPA 734 (2004) 164
10 pb! Largest
�� for predicted
spherical SHE
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
244 Pu+ 48 Ca: High cross sections for element 114 confirmed
RRun 1 RRun 2
4n
Energies g studied at
TASCA
DGFRS Data
Oganessian et al.,
J. Phys. G, 2008
3n TASCA Data
Ch.E.Düllmann et al.,
PRL 104 (2010) 252701
JM J.M. GGates t et t al. l
PRC 83 (2011) 054618
Error bars include statistical errors.
TASCA systematic error is estimated to 14%.
Theory
V. Zagrebaev,
NPA 734 (2004) 164
10 pb! Largest
�� for predicted
spherical SHE
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Making Making new new elements
elements
E120 Z 0
Beam
22
Beam
50 Ti
Target
249 Cf
Asymmetry E*@BBass 31.7 31.7
23 51V 249Bk 35.9
24 54Cr 248Cm 33.0
25 55Mn 243Am 34.5
26 58Fe 244Pu 33.9
27 59 Co 237 Np 32 32.9 9
28 64Ni 238U 27.3
Similar arguments for E119 hint at
Ti+ 249 Bk as the preferred reaction
50 Ti+
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
crrosss
secctionn
/ fb
Choice of the optimum reaction: example E120
10 4
10 3
10 2
10
10 1
10 0
10 -1
10
10 -2
10 -3
Fe+Pu Zagrebaev Zagrebaev + et Greiner al. al
Ti+Cf Ti Cf Zagrebaev + Greiner
Cr+Cm Ni+U
Asymmetric
DGFRS
SHIP
Asymmetry
(More) symmetric
Adamian et al.
Liu et al.
Nasirov et al.
Siwek-Wilczynska et al.
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
crrosss
secctionn
/ fb
Choice of the optimum reaction: example E120
10 4
10 3
10 2
10
10 1
10 0
10 -1
10
10 -2
10 -3
Fe+Pu Zagrebaev Zagrebaev + et Greiner al. al
Ti+Cf Ti Cf Zagrebaev + Greiner
Cr+Cm Ni+U
Asymmetric
DGFRS
SHIP
Asymmetry
(More) symmetric
Adamian et al.
Liu et al.
Nasirov et al.
Siwek-Wilczynska et al.
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
crrosss
secctionn
/ fb
Choice of the optimum reaction: example E120
10 4
10 3
10 2
10
10 1
10 0
10 -1
10
10 -2
10 -3
Fe+Pu Zagrebaev Zagrebaev + et Greiner al. al
Ti+Cf Ti Cf Zagrebaev + Greiner
Cr+Cm Ni+U
TASCA
Asymmetric
DGFRS
SHIP
Asymmetry
(More) symmetric
Adamian et al.
Liu et al.
Nasirov et al.
Siwek-Wilczynska et al.
Conclusion:
� scales w/ asymmetry
Best reaction: 50 Ti+ 249 Cf
� predicted: 50 fb – 1 pb
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
50 Ti+ 249 Cf Excitation Function
05 0.5 mg/cm / 2 T t
2 Target
~ 4 MeV (lab)
V. Zagrebaev + W. Greiner, Phys. Rev. C 78 (2008) 034610
Maximum:
40 fb!
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
A new high-intensity transuranium target wheel for TASCA
Radiochemical labs at Mainz
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
A new high-intensity transuranium target wheel for TASCA
Radiochemical labs at Mainz
Making actinide targets
K. Eberhardt et al.
Used for E120 at
Ø Target g Wheel: 100 mm
Ø Beam Spot: 8 mm
Target g wheel tested up p to
2500 particle·nA
E. Jäger, T. Torres, J. Krier
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Z
50 Ti+ 249 Cf Very short-lived!
Mt
Hs
Bh
Sg
Db
Rf
266Mt
1.7ms
265Hs
Ds
266Hs
111
269Ds
Rg
270Ds
272Rg
1.6ms
271Ds
02ms 0.2ms 01ms 0.1ms 56 ms
268Mt
42 ms
267Hs
2 ms 2.3ms 49 ms
264Bh
0.97 s 0.94 s
263Sg
0.9 m
265Bh
264Sg
37 ms
262Db 263Db
34 s
261Rf
68 s
27 s
262Rf
2 s?
266Bh
1.1 s
265Sg
16 s
267Bh
17 s
266Sg
0.36 s
263Rf
8 s? 160 160
270Mt
0.57 s
269Hs
14 s
270Hs
~23 s
113
112
274Rg
15 ms
273Ds
02ms 0.2ms
113
Cn
278113
1.8ms
277Cn
0.6ms
275Ds
271Hs 272Hs 273Hs
~4 s
0.1 s
0.2 s
270Bh 271Bh 272Bh
61 s
267Sg 268Sg 269Sg
1.4 m
4 h
2 min
266Db 267Db 268Db
22min
265Rf
2 min
1.2 h
29 h
267Rf
?
162 164
1.3 h
276Ds
114
114
118
118
120
120
291118292118
0.5ms 0.3ms
117
295120296120
40 �s 7 �s
117
294118
1 ms
293117 294117
14 ms 78 ms
116
287116 287116288116
288116
116 0.4ms 2 ms
290116 290116 290116 290116 291116 291116292116
292116 293116 293116
29 7 ms
18 ms 18 ms 61ms
115
287115 288115289115
290115
115 32 ms 87 ms 0.22 s 16 ms
283114284114285114
286114 286114287114
287114288114
289114
0.3ms 0.5ms 0.1 s 0.13 0.36 s
0.48 5 ss
0.69 s 2.1 s
283113 284113 285113286113
0.10 s 0.48 s 5.5 s 20 s
176
279Cn 280Cn 281Cn 282Cn 283Cn 284Cn 285Cn
02 0.2ms 03 0.3ms
0.1 s
278Rg 279Rg 280Rg 281Rg 282Rg
4.2ms 0.17 s 3.6 s
277Ds
01ms 0.1ms 03ms 0.3ms 6ms 6 ms
274Mt 275Mt 276Mt
0.45 s 9.7ms 0.72 s
9.8 s
271Sg
1.9 m
270Db
23 h
166
275Hs
0.19 s
274Bh
0.9 m
279Ds 279Ds
03s 02s 0.3 0.2 s
278Mt
7.6 s
277Hs
3 ms
0.8ms 3.8 s
26 s
168 170
0.5 s
281Ds 279Ds
03s 0.3 13 s
99ms
172
29 s
174
SF
Ch.E. Düllmann – FIAS Colloquium – FIAS Frankfurt, Germany – October 20, 2011
�
� +
EC
E120 Chain Data: A. Sobiczewski et al. priv. comm.
(arb. units)
Energy E
Getting ready for element 120 at TASCA
A new digital data acquisition system for �s-isotopes
�s isotopes
Test reaction: 176 Yb( 48 Ca,4n) 220 Th
E EVR ~21 MeV
�( 220 Th)=4.9 �s
E E��=9.35 935MMeV V
E ��=8.79 MeV
�( 216 Ra)=0.9 �s
Rn 212
23.9 m
� 6.26
�
Ra 216
0.18 �s
�� 935 9.35
Lifetimes down to about 100 ns
can be measured
Time (10 ns/ch)
Experimental Electronics Dept. (N. Kurz, ...); Dirk Rudolph (U Lund)
L.G. Sarmiento
��
Th 220
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
9.7 �s
� 8.79
�
SHE chemistry
Hottest topic: chemistry of element 114
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
The Periodic Table and Relativity
1 18
1 2
H 2 13 14 15 16 17 He
3 4 5 6 7 8 9 10
Li Be B C N O F Ne
11 12 13 14 15 16 17 18
NNa MMg 3 4 5 6 7 8 9 10 11 12 Al Si P S Cl AAr
19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36
K Ca Sc Ti V Cr Mn Fe Co Ni Cu Zn Ga Ge As Se Br Kr
37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54
Rb Sr Y Zr Nb Mo Tc Ru Rh Pd Ag Cd In Sn Sb Te I Xe
55 56 57+* 72 73 74 75 76 77 78 79 80 81 82 83 84 85 86
Cs
87
Ba
88
La
89+"
Hf
104
Ta
105
W
106
Re
107
Os
108
Ir Pt Au Hg
112
Tl Pb Bi Po At Rn
Fr Ra Ac Rf Db Sg Bh Hs 109 110 111 Cn 113 114 115 116 117 118
Mt Ds Rg --- --- --- --- --- ---
* 58 59 60 61 62 63 64 65 66 67 68 69 70 71
Ce Pr Nd Pm Sm Eu Gd Tb Dy Ho Er Tm Yb Lu
" 90 91 92 93 94 95 96 97 98 99 100 101 102 103
Th Pa U Np Pu Am Cm Bk Cf Es Fm Md No Lr
Examples of non-relativistic orbitals
s p d f
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
The Periodic Table and Relativity
1 18
1 2
H 2 13 14 15 16 17 He
3 4 5 6 7 8 9 10
Li Be B C N O F Ne
11 12 13 14 15 16 17 18
NNa MMg 3 4 5 6 7 8 9 10 11 12 Al Si P S Cl AAr
19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36
K Ca Sc Ti V Cr Mn Fe Co Ni Cu Zn Ga Ge As Se Br Kr
37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54
Rb Sr Y Zr Nb Mo Tc Ru Rh Pd Ag Cd In Sn Sb Te I Xe
55 56 57+* 72 73 74 75 76 77 78 79 80 81 82 83 84 85 86
Cs
87
Ba
88
La
89+"
Hf
104
Ta
105
W
106
Re
107
Os
108
Ir Pt Au Hg
112
Tl Pb Bi Po At Rn
Fr Ra Ac Rf Db Sg Bh Hs 109 110 111 Cn 113 114 115 116 117 118
Mt Ds Rg --- --- --- --- --- ---
Examples of relativistic orbitals
p1/2 p 3/2
s p d f
RRelativity l ti it in i Chemistry Ch i t
Electrons near nucleus:
v is a large g fraction of c
� relativistic mass increase
1) Direct relativistic effect:
*
"
58
Ce
90
Th
59
Pr
91
Pa
60
Nd
92
U
61
Pm
93
Np
62
Sm
94
Pu
63
Eu
95
Am
64
Gd
96
Cm
65
Tb
97
Bk
66
Dy
98
Cf
67
Ho
99
Es
68
Er
100
Fm
69
Tm
101
Md
70
Yb
102
No
71
Lu
103
Lr
s and d p1/2 orbitals bit l are
stabilized / contracted
Rel. effects ~Z
2) Indirect relativistic effect:
2 � Pronounced in heavy elements
-the color of Au:
Au: �E (5d conduct. band � Fermi): 2.4 eV (in vis)
Ag: g �E (4d ( conduct. band � Fermi): ) 3.5 eV (in ( UV) )
2) Indirect relativistic effect:
Other orbitals (p3/2, d, f) are
better shielded from nucleus
� ddestabilized t bili d / expanded d d
-the "inert pair" effect: stabilized 6s electron pair
reduces valency: Tl(I), not Tl(III); Pb(II), not Pb(IV),...
-high ox.states of light actinides: expanded 5f orbitals
available for chemical bonding: U(VI) [but no Nd(VI)]
3) Spin-orbit splitting:
Heavy atoms: two states per l
� p1/2/p3/2; d3/2/d5/2; f5/2/f7/2 Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
The Periodic Table and Relativity
1 18
1 2
H 2 13 14 15 16 17 He
3 4 5 6 7 8 9 10
Li Be B C N O F Ne
11 12 13 14 15 16 17 18
NNa MMg 3 4 5 6 7 8 9 10 11 12 Al Si P S Cl AAr
19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36
K Ca Sc Ti V Cr Mn Fe Co Ni Cu Zn Ga Ge As Se Br Kr
37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54
Rb Sr Y Zr Nb Mo Tc Ru Rh Pd Ag Cd In Sn Sb Te I Xe
55 56 57+* 72 73 74 75 76 77 78 79 80 81 82 83 84 85 86
Cs
87
Ba
88
La
89+"
Hf
104
Ta
105
W
106
Re
107
Os
108
Ir Pt Au Hg
112
Tl Pb Bi Po At Rn
Fr Ra Ac Rf Db Sg Bh Hs 109 110 111 Cn 113 114 115 116 117 118
Mt Ds Rg --- --- --- --- --- ---
* 58 59 60 61 62 63 64 65 66 67 68 69 70 71
Ce Pr Nd Pm Sm Eu Gd Tb Dy Ho Er Tm Yb Lu
" 90 91 92 93 94 95 96 97 98 99 100 101 102 103
Th Pa U Np Pu Am Cm Bk Cf Es Fm Md No Lr
Rel. effects ~Z2 Element 114, � member Pronounced in group in heavy 14: elements
-the -Electronic color of Au: conf.: [Rn] 7s
Au: �E (5d conduct. band � Fermi): 2.4 eV (in vis)
Ag: �E (4d conduct. band � Fermi): 3.5 eV (in UV)
2 6d10 5f14 7p 2
1/2
-"Quasi-closed g ( shell" configuration g ) due ( to )
relativistic p
-the "inert pair" 1/2 subshell closure
effect: stabilized 6s electron pair
reduces Evident valency: question: Tl(I), not Tl(III); Pb(II), not Pb(IV),...
-high metallic t ox.states lli (Pb (Pb-like) lik of light )bbehavior, actinides: h i or expanded 5f orbitals
available noble-gas for (Rn-like) chemical bonding: behavior? U(VI) [but no Nd(VI)]
Examples of relativistic orbitals
p1/2 p 3/2
s p d f
RRelativity l ti it in i Chemistry Ch i t
Electrons near nucleus:
v is a large g fraction of c
� relativistic mass increase
1) Direct relativistic effect:
s and d p1/2 orbitals bit l are
stabilized / contracted
2) Indirect relativistic effect:
Other orbitals (p3/2, d, f) are
better shielded from nucleus
� ddestabilized t bili d / expanded d d
3) Spin-orbit splitting:
Heavy atoms: two states per l
� p1/2/p3/2; d3/2/d5/2; f5/2/f7/2 Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Chemical Theory on Element 114
(a small selection)
1975: Pitzer: "Are elements 112, 114, and 118 relatively inert gases?" [1]
Recent fully relativistic quantum chemical calculations:
Solid-state calculations [2]: Cn resembles group 12 metals more closely
than the noble gases
Solid-state calculations [3]: E114 more weakly bound than Pb and Hg;
spin-oirbit effects lead to chemical inertness (along the lines of Pitzer)
Calculations on MM-M M' interactions (M=Cn; E114; M'=metal M=metal, ee.g., g Au) [4 [4-6]: 6]:
M-M' NOT of VAN DER WAALS type, should reveal a metallic character:
For Cn due to the 7s and 6d 5/2 AOs
For E114 due to 7p 1/2 and 7p 3/2 AOs
�Element 114 expected to be a rather inert, volatile metal
[1] K.S. Pitzer, J. Chem. Phys. 63, 1032 (1975).
[2] N. Gaston et al., Angew. Chem. Int. Ed. 46, 1663 (2007).
[3] A. Hermann et al., Phy. Rev. B 82, 155116 (2010).
[4] V. Pershina, Radiochim. Acta, 99, 459 ( (2011). )
[5] V. Pershina et al., J. Chem. Phys. 131, 084713 (2009).
[6] A. Zaitsevkii et al., Russ. Chem. Rev. 78, 1173 (2009).
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
(Relativistic) Energy of Valence Orbitals
E , eV
-5
-77
-9
-11
-13
-15
-17 17
-19
s s1/2 1/2
Hg
112
Tl
p p1/2 1/2
113
Pb
114
115
Bi
116
p p3/2 3/2
117
7p3/2
118
6p3/2
6p1/2
7p1/2
-21
11 12 13 14 15 16 17 18 Group 19
V. Pershina et al., J. Chem. Phys. 132 (2010) 194314
s 2 p 1 p 2 p 1 p 2 p 3 p 4
s 2
1/2 p1/2
1
p1/2
2
p3/2
1
p3/2
2
p3/2
3
p3/2
4
Vl Valence El Electrons t
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
12
13
14
6s
-7 eV
6p 1/2
-3.0 eV
6p 1/2
-4.2 eV
M-Au Bonding (Dimer)
��
�
HgAu 112Au D e (eV)
D e (eV)
��
�
��
6s
-66 eV
0.67
7s
-9.7 eV
TlAu 113Au
6s
-6 eV
2.72
7p 1/2
-4.0 eV
PbAu 114Au
6s
2.15
��
�
��
�
��
6s
-6 eV
6s
-6 eV
� -6 eV
-5.3 eV � -6 eV
6s
0.51
1.83
7p 1/2 0.73
155 BiAu 2.62
115Au 2.52
E114-Au bond is stronger than E112-Au!!
V. Pershina et al.,
J. Chem. Phys. 133 (2010) 104304
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Simulation of M Adsorbed on Au(100)
Clusters MAu
top hollow
n=14 n=9
bridge
Embedded cluster MAu MAunAu Aum
ad-atom
cluster l t
environment
n = 16 n = 34-36 m = 156
Increase cluster size until convergence g is reached � M-M' dimer trends preserved! p
Interaction E114 – Aun is stronger than Cn – Aun V. Pershina, "Electronic Structure and Chemistry of the Heaviest Elements" in Relativistic Methods for Chemists; Eds: Leszczynski/Ishikawa; Springer (2010) 451
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Production of elements 112 and 114
238 U( 48 Ca,3n)
Z
112
112
110 110 Ds
confirmed at TASCA!
244Pu( 48Ca,3-4n) 242Pu( ( 48Ca,3n) , )
112
279Ds 279Ds
0.2 s
N
114
114 114
286114 286114 286114 286114 286114 287114 287114 288114 288114 289114 289114
0.36 0.13 0.36 0.13 0.36 0.13 0.36 0.13 s
s 0.5 s 0.8 s 2.7 s
282112 282112 283112 283112 284112 284112 285112 285112
0.8ms 3.8 s 0.1 s 34 s
281Ds 281Ds
9.6 s
170 170 172
172
174
174
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
��
SF
Experimental approach:
Testing interaction "E114 E114 �� Au" Au
Isothermal Gas Chromatography
Temperat T ure [°C]
Temmperaturee
[°C]
Gas flow
Column lengths [cm]
Rel. Yieeld
[%]
T 50%
Thermochromatography g p y
Gas flow
Column length [cm]
Rel. Yieldd
[%]
t Ret.=T 1/2
low Temperature [°C] high
T a
high Temperature [°C] low
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Previous study: Volatility and reactivity of Hg, Rn, Cn, and E114
R. Eichler et al., Radiochim. Acta 98 (2010) 133
Element -�H �Hads d
Hg ≥50 kJ/mol
Rn 19 kJ/mol
Cn (Z=112) 52 kJ/mol
287 114 34 kJ/mol
288 114 34 kJ/ kJ/mol l
+20
E114 (68%): 34 -3 kJ/mol
+54 54
(95%): 34 -11 kJ/mol
Theory Experiment
Pb > 114 �� Hg > 112 Hg > 112 > 114
The TASCA Element 114 Chemistry Collaboration
TU MMunich nich (D) AA. Yak Yakushev she (collaboration spokesperson)
J.M. Gates, A. Gorshkov, R. Graeger, A. Türler
GSI Darmstadt (D) D. Ackermann, M. Block, W. Brüchle, Ch.E. Düllmann, H.
Essel, J.M. Gates, W. Hartmann, F.P. Heßberger, A. Hübner,
E. Jäger, J. Khuyagbaatar, B. Kindler, J. Krier, N. Kurz, B.
Lommel, J. Runke, M. Schädel, B. Schausten, E. Schimpf,
JJ. Steiner
Univ. Mainz (D) Ch.E. Düllmann, K. Eberhardt, M. Eibach, J. Even, D. Hild,
J.V. Kratz, L.J. Niewisch, P. Thörle-Pospiech, N. Wiehl
HIM Mainz (D) Ch.E. Düllmann, F.P. Heßberger
Univ. Liverpool (UK) L.-L. Andersson, R.-D. Herzberg, E. Parr
LBNL/UC Berkeley (USA) J. Dvorak, H. Nitsche
Univ. Lund (S) U. Forsberg, D. Rudolph
Univ. Oslo (N) J.P. Omtvedt, A. Semchenkov
IMP Lanzhou (PRC) Z. Qin
U Jyväskylä J. Uusitalo
ITE Warsaw (PL) M. Wegrzecki
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
TransActinide Separator and Chemistry Apparatus
TASCA
Preseparator: clean samples available for transport
TASCA – COMPACT 2 configuration for the study of element 114 chemistry
Element 114
Trajectory
TASCA: M. Schädel, EPJD 45 (2007) 67; A. Semchenkov et al., NIMB 266 (2008) 4153, J. Gates et al., PRC 83 (2011) 054618
TASCA Preseparator: Ch.E. Düllmann, Radiochim. Acta 99 (2011) 515; J. Even et al., NIMA 638 (2011) 157; J.P. Omtvedt et al. (to be publ.)
COMPACT J. Dvorak et al., PRL 97 (2006) 242501; PRL 100 (2008) 132503
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
TransActinide Separator and Chemistry Apparatus
TASCA
Preseparator: clean samples available for transport
TASCA – COMPACT 2 configuration for the study of element 114 chemistry
Element 114
Trajectory
COMPACT I
Isothermal Chromatography (IC)
Metals
(e.g., Pb; Hg)
+21°C 21 C
COMPACT II
Thermochromatography (TC)
Cn
Rn...
+21°C
-162°C
TASCA: M. Schädel, EPJD 45 (2007) 67; A. Semchenkov et al., NIMB 266 (2008) 4153, J. Gates et al., PRC 83 (2011) 054618
TASCA Preseparator: Ch.E. Düllmann, Radiochim. Acta 99 (2011) 515; J. Even et al., NIMA 638 (2011) 157; J.P. Omtvedt et al. (to be publ.)
COMPACT J. Dvorak et al., PRL 97 (2006) 242501; PRL 100 (2008) 132503
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Experimental setup: IC + TC
COMPACT2 COMPACT @ TASCA
RTC
COMPACT CO COMPACT AC I ( (@ room temp) )
COMPACT
COMPACT II
(+21 to ‐160 160°C) C)
A. Yakushev, 2010
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
Summary
Superheavy elements:
Elements up p to Z=118 reported; p up p to 112 and 114/116 approved pp
Location of next spherical shell closure still unclear
Research at GSI/U Mainz: Unique combination of facilities
HIM: A new SHE condensation nucleus
Toward a dedicated SHE Linac (together with IAP Frankfurt)
TASCA TASCA: TASCA TASCA: highest efficiency for hot fusion reactions: 60%
Physics @ TASCA TASCA: 50Ti+ 249Cf � element 120 ended last week
Chemistry @ TASCA TASCA: TASCA TASCA: E114!
Ch.E. Düllmann – Superheavy element research – FIAS Colloquium – Frankfurt Institute for Advanced Studies, Frankfurt – October 20, 2011
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