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851
19
20
LO
a
50 K 0 a 0.2 0.4 0.6 P0.8 1.0 1.2 GPa 1.4 40 I 30 l-5 20
60 P-
80
100kborl20
3 K
2 I l-z 1
IO 15 IO b 0 20 kbar 24
15
20
25 T-
30
35
40 K 45
Fig. 14. cc-U S.C. (a) Equilibrium pressure-low-temperature phase diagram for the three phase transitions: a,+~,, CI ,+cr, and a,+~,, as well as for the transition to the superconducting state (SC),proposed by [73 S I]. The heavy solid line represents the experimental data of the pressure dependence of the transition temperature T, between the u,fu, phases, measured on single crystalline cl-uranium by [73 C I]. (b) shows the temperature dependence of measured values (AT,,7 )- at p=O [73 C 11. AT,, is the temperature response to an ac heat input, being inversely proportional to the specific heat. The other data are from [70 F I, 67 G 1, and 70 P I].
b PFig. 15. U. (a) Superconducting temperature T, vs. pressure p up to 90 kbar for polycrystalline uranium metal [72 M I], (b) shows the superconducting transition temperature T, and transition temperatures TM for consecutive phases, CQ, u2 and us, as a function of pressure p up to 24 kbar. Note the maximum in T, is reached at = 12 kbar where only the u0 phase exists. See also [87 W I].
12
16
Tro6, Suski
20
45 K 40 I 35 <30 25 20 15 0
[Ref. p. 85
1
G
287
286
t
- 210 GPO -209 1 -4 1208
2 Pu -
of %
- 207 I.
100 801 0 I 20 I 40 II 60 I 80
0 b
2 Np,Pu-
ot%
IO0
Fig. 16. U-alloys. (a) Reduction of the a,,~~, transition temperature T, by alloying uranium with plutonium; derived from (solid circles) V vs. T and (open circles) n vs. T plots. (b) Reduction of the anomaly at 4.2 K in the unit cell volume. AK and lattice parameter, An, by alloying uranium with neptunium and plutonium. AV and An have been obtained by subtracting from the measured values of V and o the respective values for an alloy composition showing no anomaly in V and o, i.e., for instance, 5.5 at % Pu in the case of U-Pu alloys, after normalization of the different V(T) and n(T) curves at 77 K. See also Fig. 11 for V(T) of a-U [70 M 21.
Fig. 17. u-U S.C. Elastic constants cij as a function of temperature. Note the large variations in these values around the u ,,$u, transition at 43 K [61 F 21. See also [68Fl, 70Fl-j.
Tro6, Suski
Ref. p. 851
21
a,
II
\:
0.2 Ok
0.6
0.8
1.0
0.2
5-
-c
c-
I 0.8
Fig. 18. a-U S.C.(a) Phonon dispersion curves at room temperature by inelastic neutron scattering. The dashed line represents the Brillouin-zone boundary. For the meaning of the labels see the original paper [79 C 11.
(b) Room-temperature phonon dispersion curves along [IOO] direction. The temperature dependence of the lower Z, branch is indicated [SOS 3-j.
W-U
L+
a t / f I PJ
& ------ / 77
-----A7 r-----l
~1
j
,-L--L---&.
k, / r------l kL
,t
Fig. 19. a-U S.C. (a) Schematic illustration of sinusoidally modulated structure of a-uranium. Closed circles are atoms at (0, y, l/4) and open circles at (0, -y, -l/4). The directions of displacement are shown by arrows: the largest displacement is that along the a axis [82 M I]. (b) Shown is the sinusoidal modulation of charge density wave (CDW) for each direction - one independent atom with displacements in all directions [82M 11. It appeared that the magnitudes of the atomic displacement are too large by a factor of 2. See [87 V 21.
Land&BBmstein New Series III/19fl
g % 11 Q? k
a=0.285nm
b = 0.587nm
IO101
c = 0.486nm
I
Trot, Suski
[Ref. p. 85
_ TwUSond
Ud, dota
NIL
10
15
20
25 I-
30
35
40 K 45
0.1
0.2
0.4
0.5
0.6
Fig. 20. a-U S.C.Temperature dependence of the charge density modulation wavevector components: ql, qY,q, (see summary in [9OL 11). Circles are data from neutron [90 M 1J and crosses from X-ray [91 G l] experiments, respectively. Notice that the q, component is incommensurate below 43K in agreement with the theoretical prediction of [86 W 11. At 37.5 K qx/u* locks into l/2, while at 22K qJb* and q,/c* lock into l/6 and 2/l 1 (X-ray) or 5/27 (neutrons), respectively, though both should become l/6 [86 W 11. The difference between X-ray and neutron values is probably due to the surface and the bulk form of the experiments, respectively. The fact that q:/c* does not become l/6 is caused by faults in the c direction and explained by the so-called phase slip model, developed by [91 G 1J. Theoretically, the low-temperature transitions are from the orthorhombic Cmcm space group to a structure with superspace group CZ/mll(apy), a+OS, at 43 K followed by a lock-in transition at T=37 K to a structure with symmetry P2/ml1(1/2jYIy) [86 W 11. The latter is also suggested by the refinements [87 V 23 of neutron data [82 M 1) and electron microscopy observation [86 C 1-J.Below 30 K a squaring up of the CDW displacements takes place, being not completed even at the lowest temperatures [90 M 11. The total unit cell at low temperatures, below 22K, is about (2a, 2b, z6c). Finally, it should be noted that the discovery of the CDW features in a-U was made almost simultaneously by [SOS 33 and [80 M 11.
Fig. 21. a-U. Experimental magnetic form factor compared to the radial integral Go) (see Fig. 3) (solid line) and to those of uranium compounds (hatched area). The difference suggests that the orbital angular momentum is quenched in the metallic state: thus the zero-order radial integral is related to the radial extent of the 5f electrons [78 M 1-J.
9/
100
200
300 I-
400
500
600 C
Fig. 22. Pu. Length change, AI/l, vs. temperature [70G 11.
Trot, Suski
Ref. p. 851
I
23
a-ru
0.484 nm 0.482 I 0.480 21 0.478 OA7E 101.98" A
0.616 1 0 0.614
1.096 nm 1.094
I 1.092 u .- 316
318
101.74O0 T-
320
Fig. 23. a-Pu. Lattice parameters vs. temperature for high-purity a-Pu. Note anomalous changes in expansion coefficient at zz 60 K [67 L 21.
Fig. 24. cl-Pu. Unit cell volume Yvs. temperature [67 L 21.
0.51 nm 0.50
1.0
3.6
0.46
0.45 0
IO
15 P-
20
25
30 GPO :
Fig. 25. Th. Pressure dependence of the lattice parameter a (open circles) and the relative volume Y(p)/V(O) (solid line) of thorium fee phase at room temperature. The solid line through experimental points represents a fit to the second-order Birch equation [81 B I].
Land&BBmstein New Series IW19fl
Trod, Suski
24
properties
[Ref. p. 85
603 NP
c, 400 CL
I 203 203800 800 C liquid
Pu
600
I
2 6 P8
10 GPO 12
l z
0.7 b
0 IO
20
P-
30
LO
50 GPa 60
Fig. 26. U, Np, Pu. Pressure-temperature phase diagrams for uranium. neptunium and plutonium of diffcrcnt investigations. taken from [84 B 11.
Fig. 27. u-U. (a) Pressure dependence of the unit cell ratios: alar,, b/b, and c/c,, [85A 11. Note that the crystal is least compressible in the c direction. (b) Relative volume V(p)/V(O) vs. pressure. The solid line through experimental points, I [SS A l] and 2 [79 M 23, is a fit to the Birch-Murnaghan equation [SS A 11. No indication of a phase transition up to 50GPa.
Trot, Suski
Land&-Bhstein
Nca Series 111 1911
Ref. p. 851
25
0.95
IO
20
PFig. 28. cl-Np. Relative volume V(p)/V(O) vs. pressure forneptunium metal [87 D 11. No indication of a phase transition up to 52 GPa. The solid curve represents both the Birch and Murnaghan tits.
30 P-
40
50
60 GPa70
Fig. 29. Light An. Relative volume V(p)/V(O) for the ambient pressure phases of the light actinide metals, taken from [87 B 11.
175 GPa 150 125 I 100 ap 75 50 25 7.5 I 5.0 = 2.5 12.5 10.0
OTT
Pu
Fig. 30. Light An. Bulk moduli B, (solid line) and pressure derivative Bb (dashed line) for the light actinides taken from [87D I] experimental values. For the calculated values see [84 B 41.
TroC, Suski
26
[Ref. p. 85 Cm
dhco
RT
1750 K
0.6 0
10
20
30 P-
LO
50 GPO 60
Fig. 32. Cm. (a) Unit-cell volume Vat room temperature vs. pressure [89B 11. (b) shows the volume ratio, V(p)/V(O), up to 40GPa [85 H 11.
250
Fig. 31. Am. (a) Relative volume, k (p)/V(O), vs. pressure for americium metal taken from [SS B 23. The observed phase transitions, dhcp (double hexagonal close packed)jccp (cubic close packed)/trigonal (distorted ccpphase)lorthorhombic (u-U-type phase), occur due to volume decrease caused by increasing delocalization of the 5f elements with pressure. (b) Possible T-p diagram for americium metal, taken from [87 B 1) and constructed on the basis of experiments marked by shaded zones. There are two versions of the diagram: the first (marked by thicker dashed line) is based on [85 B 23 and [68 S 11, and the second (marked by thinner line) on [80 A 11.
25
10
20
30 P-
LO
50 GPO 60
Fig. 33. Bk, Cf. Unit-cell volume V vs. pressure for Bk [84 B2] and Cf [83P 1, 84 B2] metals at room temperature.
TroC, Suski
Ref. p. 851
27
GPO I
m m
AC
Th
Pa
Np
Pu
Am Cm Bk
Cf
Es
Fm Md
No
Lr
Fig. 34. An. Generalized presentation of the phase relations of the actinide metals under pressure [S9 B 21.
ann
G6Ol
P cq 25
50
150;
G
1.
localized 5f
10 --3 2 1 4
I
5
I I 01 I
j^
01
Am
Cm
Bk
Cf
AC
Th
Pa
tl
Np
Pu
Am
Cm
Bk
Cf
Es
Fig. 35. Heavy An. Bulk moduli B, and their pressure derivative EO for the heavy actinides, compared with those of Pr and Nd, taken from [87B I]. The values for the Am-Cm and Bk-Cf alloys are from [87 H2] and [SS I I], respectively. There is a relatively large uncertainty on these bulk moduli, and therefore only a range of values indicated as a shaded area can be considered.
Land&Blimstein New Series III/19fl
Fig. 36. An. Calculated (see f [82 J I] and 2 [84 B 43) and experimental (3 [86 W 21 and [86 W 3],4 [81 B 21) values for cohesive energies of actinide metals, being in general correlation with compressibilities (see [84 B 41 and [87 B I]).
Trot?, Suski