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inorganic papers

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Yao and Ibers RbPbPS4 DOI: 10.1107/S1600536804018513 Acta Cryst.(2004). E60, i108±i110

Acta Crystallographica Section E Structure Reports Online

ISSN 1600-5368

RbPbPS

4

Jiyong Yao and James A. Ibers*

Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, IL 60208-3113, USA

Correspondence e-mail: [email protected]

Key indicators Single-crystal X-ray study T= 153 K

Mean(S±P) = 0.002 AÊ Rfactor = 0.020 wRfactor = 0.049

Data-to-parameter ratio = 27.8

For details of how these key indicators were automatically derived from the article, see http://journals.iucr.org/e.

#2004 International Union of Crystallography Printed in Great Britain ± all rights reserved

Rubidium lead phosphorus tetrasul®de, RbPbPS4, possesses

the CsSmGeS4 structure type, crystallizing in space group

P212121of the orthorhombic system. The structure consists of

two-dimensional [PbPS4] layers built from PbS7monocapped

trigonal prisms and PS4tetrahedra. The layers are separated

by Rb atoms.

Comment

In an effort to expand the range ofABiMS4(A= Rb and Cs,

andM = Si and Ge; Yao et al., 2002) compounds by substi-tution chemistry, the new compound RbPbPS4was obtained

by the simultaneous substitution of Pb2+for Bi3+and P5+for

M4+. The compound crystallizes in the non-centrosymmetric

space group P212121 and is isostructural with CsSmGeS4

(Bucher & Hwu, 1994), which was re®ned with a different cell setting. The two unit cells become similar by cyclic permuta-tion of the axes of the latter [aold=bnew;bold=cnew;cold=anew].

The structure of RbPbPS4 (Fig. 1) consists of

two-dimen-sional [PbPS4] layers separated by Rb atoms. Each Rb atom is

coordinated by a distorted bicapped trigonal prism of eight S atoms. The RbÐS bond lengths range from 3.368 (2) to 3.789 (1) AÊ, comparable with those of 3.323 (1)±3.577 (1) AÊ in RbBiSiS4(Yaoet al., 2002). Each P atom is coordinated by a

tetrahedron of four S atoms. The PÐS bond lengths range from 2.032 (2) to 2.064 (2) AÊ, consistent with those of 2.004 (2)±2.056 (2) AÊ in ScPS4 (Lee & Hilt, 1992). Each Pb

atom is coordinated by a monocapped trigonal prism of seven S atoms. The PbÐS distances range from 2.920 (1) to 3.282 (2) AÊ, comparable with those of 3.066 (3)±3.188 (3) AÊ in Li2PbGeS4(Aitkenet al., 2001). The largest difference in PbÐ

S bond lengths within the PbS7polyhedron is 0.362 (2) AÊ. The

Received 8 July 2004 Accepted 28 July 2004 Online 7 August 2004

Figure 1

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structure of the two-dimensional [PbPS4] layer is shown in

Fig. 2. The neighboring PbS7polyhedra share opposite edges

of the rectangular planes of the prisms to form zigzag chains along the b direction. Two parallel polyhedral chains are connected by the sharing of opposite edges of the PS4

tetra-hedra. Each PS4 tetrahedron is arranged in such a way that

one of the S atoms becomes the cap of an adjacent PbS7

polyhedron. The two [PbPS4] slabs in the unit cell of RbPbPS4

are related by a 21screw axis alonga.

Experimental

Yellow plates of RbPbPS4were obtained from a solid-state reaction of Rb2S3 (0.5 mmol), Pb (Alfa, 99.5%, 1.0 mmol), P2S5 (Aldrich, 99.5%, 0.5 mmol), and S (Aldrich, 99.5%, 1.0 mmol). The reactive ¯ux Rb2S3(Sunshineet al., 1987) was prepared by the stoichiometric reaction of Rb (Aldrich, 98+%) and S in liquid NH3. The reactants were loaded into a fused-silica tube under an Ar atmosphere in a glove box. The tube was sealed under a 10ÿ4Torr atmosphere (1 Torr = 133.322 Pa) and then placed in a computer-controlled furnace. The sample was heated to 1073 K over a period of 20 h, kept at 1073 K for 84 h, cooled at 6 K hÿ1to 373 K and then cooled rapidly to room temperature.

Crystal data RbPbPS4

Mr= 451.87

Orthorhombic,P212121

a= 6.3987 (7) AÊ

b= 6.6899 (7) AÊ

c= 17.2975 (19) AÊ

V= 740.45 (14) AÊ3

Z= 4

Dx= 4.053 Mg mÿ3

MoKradiation Cell parameters from 7200

re¯ections = 2.4±28.8

= 30.54 mmÿ1

T= 153 (2) K Plate, yellow

0.180.160.016 mm

Data collection

Bruker SMART 1000 CCD diffractometer

!scans

Absorption correction: numerical face indexed (SHELXTL; Sheldrick, 2003)

Tmin= 0.047,Tmax= 0.603

8784 measured re¯ections

1807 independent re¯ections 1759 re¯ections withI> 2(I)

Rint= 0.032

max= 28.8

h=ÿ8!8

k=ÿ9!9

l=ÿ23!23

Re®nement Re®nement onF2

R[F2> 2(F2)] = 0.020

wR(F2) = 0.049

S= 1.39 1807 re¯ections 65 parameters

w= 1/[2(F

o2) + (0.02P)2]

whereP= (Fo2+ 2Fc2)/3

(/)max= 0.001

max= 2.11 e AÊÿ3

min=ÿ1.57 e AÊÿ3

Absolute structure: Flack (1983), 704 Friedel pairs

Flack parameter = 0.550 (7)

Table 1

Selected geometric parameters (AÊ,). RbÐS1 3.3680 (15) RbÐS2i 3.4075 (17)

RbÐS4ii 3.4345 (16)

RbÐS4 3.4412 (16) RbÐS3iii 3.4639 (17)

RbÐS2iv 3.4734 (17)

RbÐS3v 3.4898 (17)

RbÐS4iii 3.7887 (14)

PbÐS4 2.9204 (14) PbÐS1vi 2.9290 (14)

PbÐS2 2.9945 (16) PbÐS3 3.0430 (16) PbÐS1 3.0900 (14) PbÐS3vii 3.1116 (16)

PbÐS2vii 3.2823 (16)

PÐS4iv 2.0320 (18)

PÐS2 2.038 (2) PÐS3viii 2.0381 (19)

PÐS1 2.0644 (19)

S4ivÐPÐS2 111.36 (9)

S4ivÐPÐS3viii 109.75 (8)

S2ÐPÐS3viii 108.05 (8)

S4ivÐPÐS1 111.30 (8)

S2ÐPÐS1 106.65 (8) S3viiiÐPÐS1 109.62 (8)

Symmetry codes: (i) 1

2ÿx;ÿy;zÿ12; (ii) x;yÿ1;z; (iii) xÿ12;12ÿy;ÿz; (iv) ÿx;yÿ1

2;12ÿz; (v) xÿ1;y;z; (vi) ÿx;12‡y;12ÿz; (vii) 1ÿx;12‡y;12ÿz; (viii) 1ÿx;yÿ1

2;12ÿz.

The value of the Flack (1983) parameter suggests an enantiomeric twin. Examination of the resultant atomic coordinates with the programADDSYMin thePLATONsuite of programs (Spek, 2003) did not reveal additional symmetry. The structure was thus re®ned as a twin. The resultant twin ratio is 0.550 (7):0.450 (7). The displace-ment ellipsoids are reasonable (Fig. 3). The highest residual electron density is 0.06 AÊ from the Pb site. The deepest hole is 0.75 AÊ from this same site.

Data collection:SMART(Bruker, 2003); cell re®nement:SAINT

-Plus(Bruker, 2003); data reduction:SAINT-Plus; program(s) used to solve structure: SHELXTL (Sheldrick, 2003); program(s) used to re®ne structure:SHELXTL; molecular graphics:XPinSHELXTL; software used to prepare material for publication:SHELXTL.

This research was supported by the MRSEC program of the National Science Foundation (DMR00-76097) at the Materials Research Center of Northwestern University.

inorganic papers

Acta Cryst.(2004). E60, i108±i110 Yao and Ibers RbPbPS4

i109

Figure 2

The structure of the two-dimensional [PbPS4] layer in RbPbPS4.

Figure 3

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References

Aitken, J. A., Larson, P., Mahanti, S. D. & Kanatzidis, M. G. (2001).Chem. Mater.13, 4714±4721.

Bruker (2003). SMART (Version 5.054) and SAINT-Plus (Version 6.45). Bruker AXS Inc., Madison, Wisconsin, USA.

Bucher, C. K. & Hwu, S.-J. (1994).Inorg. Chem.33, 5831±5835.

Flack, H. D. (1983).Acta Cryst.A39, 876±881.

Lee, S. & Hilt, R. J. (1992).J. Alloys Compd.189, 269±271.

Sheldrick, G. M. (2003). SHELXTL for DOS/Windows/NT. Version 6.14. Bruker AXS Inc., Madison, Wisconsin, USA.

Spek, A. L. (2003).J. Appl. Cryst.36, 7±13.

Sunshine, S. A., Kang, D. & Ibers, J. A. (1987).J. Am. Chem. Soc.109, 6202± 6204.

Yao, J., Deng, B., Ellis, D. E. & Ibers, J. A. (2002).Inorg. Chem.41, 7094±7099.

inorganic papers

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supporting information

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Acta Cryst. (2004). E60, i108–i110

supporting information

Acta Cryst. (2004). E60, i108–i110 [https://doi.org/10.1107/S1600536804018513]

RbPbPS

4

Jiyong Yao and James A. Ibers

Rubidium lead phosphorus tetrasulfide

Crystal data

RbPbPS4

Mr = 451.87

Orthorhombic, P212121

Hall symbol: P 2ac 2ab

a = 6.3987 (7) Å

b = 6.6899 (7) Å

c = 17.2975 (19) Å

V = 740.45 (14) Å3

Z = 4

F(000) = 792

Dx = 4.053 Mg m−3

Mo radiation, λ = 0.71073 Å Cell parameters from 7200 reflections

θ = 2.4–28.8°

µ = 30.54 mm−1

T = 153 K Plate, yellow

0.18 × 0.16 × 0.02 mm

Data collection

Bruker SMART 1000 CCD diffractometer

Radiation source: fine-focus sealed tube Graphite monochromator

ω scans

Absorption correction: numerical

face indexed (SHELXTL; Sheldrick, 2003)

Tmin = 0.047, Tmax = 0.603

8784 measured reflections 1807 independent reflections 1759 reflections with I > 2σ(I)

Rint = 0.032

θmax = 28.8°, θmin = 2.4°

h = −8→8

k = −9→9

l = −23→23

Refinement

Refinement on F2

Least-squares matrix: full

R[F2 > 2σ(F2)] = 0.020

wR(F2) = 0.049

S = 1.39 1807 reflections 65 parameters 0 restraints

Primary atom site location: structure-invariant direct methods

Secondary atom site location: difference Fourier map

w = 1/[σ2(F

o2) + (0.02P)2]

where P = (Fo2 + 2Fc2)/3

(Δ/σ)max = 0.001

Δρmax = 2.11 e Å−3

Δρmin = −1.57 e Å−3

Absolute structure: Flack (1983): 704 Friedel pairs

Absolute structure parameter: 0.550 (7)

Special details

Geometry. All e.s.d.'s (except the e.s.d. in the dihedral angle between two l.s. planes) are estimated using the full covariance matrix. The cell e.s.d.'s are taken into account individually in the estimation of e.s.d.'s in distances, angles and torsion angles; correlations between e.s.d.'s in cell parameters are only used when they are defined by crystal symmetry. An approximate (isotropic) treatment of cell e.s.d.'s is used for estimating e.s.d.'s involving l.s. planes.

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supporting information

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Acta Cryst. (2004). E60, i108–i110

Fractional atomic coordinates and isotropic or equivalent isotropic displacement parameters (Å2)

x y z Uiso*/Ueq

Rb 0.02119 (9) 0.00342 (8) 0.04319 (3) 0.02110 (13)

Pb 0.28891 (3) 0.47494 (3) 0.230842 (12) 0.01418 (7)

P 0.2189 (2) 0.01031 (19) 0.34791 (8) 0.0100 (3)

S1 0.1533 (2) 0.0316 (2) 0.23134 (8) 0.0131 (3)

S2 0.3990 (2) 0.25142 (19) 0.37520 (10) 0.0142 (3)

S3 0.6101 (3) 0.25876 (19) 0.13163 (10) 0.0134 (3)

S4 0.0472 (2) 0.5039 (2) 0.08806 (8) 0.0135 (3)

Atomic displacement parameters (Å2)

U11 U22 U33 U12 U13 U23

Rb 0.0374 (3) 0.0118 (3) 0.0142 (3) −0.0009 (2) 0.0062 (2) −0.0007 (2) Pb 0.01344 (10) 0.01498 (11) 0.01413 (11) 0.00007 (8) −0.00011 (8) 0.00066 (9)

P 0.0121 (6) 0.0077 (6) 0.0103 (6) −0.0002 (6) 0.0001 (5) 0.0003 (5)

S1 0.0152 (6) 0.0152 (6) 0.0089 (6) −0.0015 (5) 0.0010 (5) 0.0003 (7) S2 0.0181 (8) 0.0069 (6) 0.0178 (8) −0.0015 (5) −0.0035 (7) 0.0000 (5) S3 0.0176 (7) 0.0070 (6) 0.0155 (8) −0.0013 (5) 0.0000 (6) 0.0004 (5)

S4 0.0158 (6) 0.0130 (7) 0.0116 (6) 0.0004 (6) 0.0045 (5) 0.0004 (6)

Geometric parameters (Å, º)

Rb—S1 3.3680 (15) Pb—Pbviii 4.3504 (4)

Rb—S2i 3.4075 (17) Pb—Pbix 4.3504 (4)

Rb—S4ii 3.4345 (16) Pb—Rbvii 4.3877 (7)

Rb—S4 3.4412 (16) P—S4iv 2.0320 (18)

Rb—S3iii 3.4639 (17) P—S2 2.038 (2)

Rb—S2iv 3.4734 (17) P—S3ix 2.0381 (19)

Rb—S3v 3.4898 (17) P—S1 2.0644 (19)

Rb—Pi 3.7660 (15) P—Pbix 3.4392 (14)

Rb—S4iii 3.7887 (14) P—Pbiv 3.5315 (14)

Rb—Pbiv 4.3877 (7) P—Rbx 3.7660 (15)

Rb—Rbvi 4.8324 (9) S1—Pbiv 2.9290 (13)

Rb—Rbiii 4.8324 (9) S2—Pbix 3.2823 (16)

Pb—S4 2.9204 (14) S2—Rbx 3.4075 (17)

Pb—S1vii 2.9290 (14) S2—Rbvii 3.4733 (17)

Pb—S2 2.9945 (16) S3—Pviii 2.0381 (19)

Pb—S3 3.0430 (16) S3—Pbix 3.1116 (16)

Pb—S1 3.0900 (14) S3—Rbvi 3.4640 (17)

Pb—S3viii 3.1116 (16) S3—Rbxi 3.4898 (17)

Pb—S2viii 3.2823 (16) S4—Pvii 2.0320 (18)

Pb—Pviii 3.4392 (14) S4—Rbxii 3.4345 (16)

Pb—Pvii 3.5315 (14) S4—Rbvi 3.7888 (14)

S1—Rb—S2i 144.54 (4) S1vii—Pb—Pvii 35.75 (4)

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Acta Cryst. (2004). E60, i108–i110

S2i—Rb—S4ii 72.46 (3) S3—Pb—Pvii 115.83 (4)

S1—Rb—S4 73.46 (3) S1—Pb—Pvii 78.87 (3)

S2i—Rb—S4 132.22 (4) S3viii—Pb—Pvii 116.43 (4)

S4ii—Rb—S4 153.30 (5) S2viii—Pb—Pvii 107.85 (4)

S1—Rb—S3iii 140.96 (4) Pviii—Pb—Pvii 133.25 (4)

S2i—Rb—S3iii 57.37 (3) S4—Pb—Pbviii 113.99 (3)

S4ii—Rb—S3iii 129.51 (4) S1vii—Pb—Pbviii 117.80 (3)

S4—Rb—S3iii 75.05 (3) S2—Pb—Pbviii 96.36 (3)

S1—Rb—S2iv 80.14 (4) S3—Pb—Pbviii 91.83 (3)

S2i—Rb—S2iv 102.70 (4) S1—Pb—Pbviii 155.77 (3)

S4ii—Rb—S2iv 58.23 (3) S3viii—Pb—Pbviii 44.38 (3)

S4—Rb—S2iv 114.71 (3) S2viii—Pb—Pbviii 43.45 (3)

S3iii—Rb—S2iv 134.82 (4) Pviii—Pb—Pbviii 55.87 (2)

S1—Rb—S3v 74.82 (4) Pvii—Pb—Pbviii 125.36 (2)

S2i—Rb—S3v 137.03 (4) S4—Pb—Pbix 120.58 (3)

S4ii—Rb—S3v 114.44 (3) S1vii—Pb—Pbix 131.72 (3)

S4—Rb—S3v 57.41 (3) S2—Pb—Pbix 48.92 (3)

S3iii—Rb—S3v 106.36 (4) S3—Pb—Pbix 45.66 (3)

S2iv—Rb—S3v 58.39 (3) S1—Pb—Pbix 55.66 (3)

S1—Rb—Pi 139.22 (4) S3viii—Pb—Pbix 102.93 (3)

S2i—Rb—Pi 32.52 (3) S2viii—Pb—Pbix 98.08 (3)

S4ii—Rb—Pi 99.07 (3) Pviii—Pb—Pbix 62.91 (2)

S4—Rb—Pi 101.81 (3) Pvii—Pb—Pbix 132.98 (2)

S3iii—Rb—Pi 32.40 (3) Pbviii—Pb—Pbix 100.508 (12)

S2iv—Rb—Pi 133.99 (4) S4—Pb—Rbvii 120.73 (3)

S3v—Rb—Pi 137.56 (4) S1vii—Pb—Rbvii 50.10 (3)

S1—Rb—S4iii 141.33 (3) S2—Pb—Rbvii 52.07 (3)

S2i—Rb—S4iii 66.58 (4) S3—Pb—Rbvii 145.94 (3)

S4ii—Rb—S4iii 99.30 (3) S1—Pb—Rbvii 84.96 (3)

S4—Rb—S4iii 100.75 (3) S3viii—Pb—Rbvii 52.15 (3)

S3iii—Rb—S4iii 67.31 (4) S2viii—Pb—Rbvii 138.46 (3)

S2iv—Rb—S4iii 67.52 (4) Pviii—Pb—Rbvii 139.81 (2)

S3v—Rb—S4iii 70.47 (4) Pvii—Pb—Rbvii 85.67 (2)

Pi—Rb—S4iii 79.38 (3) Pbviii—Pb—Rbvii 96.413 (11)

S1—Rb—Pbiv 41.85 (2) Pbix—Pb—Rbvii 100.282 (11)

S2i—Rb—Pbiv 143.68 (3) S4iv—P—S2 111.36 (9)

S4ii—Rb—Pbiv 77.19 (2) S4iv—P—S3ix 109.75 (8)

S4—Rb—Pbiv 82.14 (2) S2—P—S3ix 108.05 (8)

S3iii—Rb—Pbiv 150.68 (3) S4iv—P—S1 111.30 (8)

S2iv—Rb—Pbiv 42.84 (3) S2—P—S1 106.65 (8)

S3v—Rb—Pbiv 44.75 (3) S3ix—P—S1 109.62 (8)

Pi—Rb—Pbiv 176.05 (3) S4iv—P—Pbix 169.07 (7)

S4iii—Rb—Pbiv 99.86 (3) S2—P—Pbix 68.19 (6)

S1—Rb—Rbvi 95.41 (3) S3ix—P—Pbix 61.34 (6)

S2i—Rb—Rbvi 88.78 (3) S1—P—Pbix 78.71 (5)

S4ii—Rb—Rbvi 134.59 (3) S4iv—P—Pbiv 55.78 (5)

S4—Rb—Rbvi 51.20 (3) S2—P—Pbiv 131.50 (7)

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Acta Cryst. (2004). E60, i108–i110

S2iv—Rb—Rbvi 165.82 (3) S1—P—Pbiv 56.00 (5)

S3v—Rb—Rbvi 107.48 (3) Pbix—P—Pbiv 133.25 (4)

Pi—Rb—Rbvi 56.43 (2) S4iv—P—Rbx 83.15 (6)

S4iii—Rb—Rbvi 110.71 (3) S2—P—Rbx 64.02 (6)

Pbiv—Rb—Rbvi 127.191 (19) S3ix—P—Rbx 65.62 (6)

S1—Rb—Rbiii 115.26 (3) S1—P—Rbx 165.34 (7)

S2i—Rb—Rbiii 100.20 (3) Pbix—P—Rbx 87.09 (3)

S4ii—Rb—Rbiii 140.01 (3) Pbiv—P—Rbx 138.64 (4)

S4—Rb—Rbiii 55.77 (3) P—S1—Pbiv 88.25 (6)

S3iii—Rb—Rbiii 61.66 (3) P—S1—Pb 90.69 (6)

S2iv—Rb—Rbiii 86.82 (3) Pbiv—S1—Pb 113.34 (4)

S3v—Rb—Rbiii 45.76 (3) P—S1—Rb 172.30 (7)

Pi—Rb—Rbiii 91.82 (3) Pbiv—S1—Rb 88.05 (4)

S4iii—Rb—Rbiii 45.06 (2) Pb—S1—Rb 96.98 (4)

Pbiv—Rb—Rbiii 90.325 (13) P—S2—Pb 93.96 (7)

Rbvi—Rb—Rbiii 82.914 (19) P—S2—Pbix 76.61 (6)

S4—Pb—S1vii 70.65 (4) Pb—S2—Pbix 87.63 (4)

S4—Pb—S2 149.64 (4) P—S2—Rbx 83.47 (6)

S1vii—Pb—S2 96.07 (4) Pb—S2—Rbx 174.99 (6)

S4—Pb—S3 84.97 (4) Pbix—S2—Rbx 95.93 (4)

S1vii—Pb—S3 147.13 (4) P—S2—Rbvii 92.33 (7)

S2—Pb—S3 94.25 (4) Pb—S2—Rbvii 85.09 (4)

S4—Pb—S1 85.27 (4) Pbix—S2—Rbvii 166.32 (5)

S1vii—Pb—S1 81.51 (3) Rbx—S2—Rbvii 90.70 (4)

S2—Pb—S1 65.45 (4) Pviii—S3—Pb 82.66 (6)

S3—Pb—S1 74.64 (4) Pviii—S3—Pbix 105.04 (7)

S4—Pb—S3viii 135.72 (4) Pb—S3—Pbix 89.95 (4)

S1vii—Pb—S3viii 87.19 (4) Pviii—S3—Rbvi 81.98 (6)

S2—Pb—S3viii 67.56 (4) Pb—S3—Rbvi 99.39 (4)

S3—Pb—S3viii 125.51 (2) Pbix—S3—Rbvi 169.05 (5)

S1—Pb—S3viii 129.93 (4) Pviii—S3—Rbxi 94.34 (7)

S4—Pb—S2viii 79.17 (4) Pb—S3—Rbxi 171.47 (6)

S1vii—Pb—S2viii 129.76 (4) Pbix—S3—Rbxi 83.10 (4)

S2—Pb—S2viii 127.17 (2) Rbvi—S3—Rbxi 88.04 (4)

S3—Pb—S2viii 62.73 (3) Pvii—S4—Pb 89.10 (6)

S1—Pb—S2viii 135.50 (4) Pvii—S4—Rbxii 93.56 (6)

S3viii—Pb—S2viii 87.53 (4) Pb—S4—Rbxii 106.35 (4)

S4—Pb—Pviii 98.36 (3) Pvii—S4—Rb 95.90 (6)

S1vii—Pb—Pviii 164.61 (4) Pb—S4—Rb 98.73 (4)

S2—Pb—Pviii 98.58 (4) Rbxii—S4—Rb 153.29 (5)

S3—Pb—Pviii 36.00 (4) Pvii—S4—Rbvi 176.19 (7)

S1—Pb—Pviii 108.92 (3) Pb—S4—Rbvi 94.70 (4)

S3viii—Pb—Pviii 94.05 (4) Rbxii—S4—Rbvi 85.18 (3)

S2viii—Pb—Pviii 35.20 (3) Rb—S4—Rbvi 83.74 (3)

S4—Pb—Pvii 35.12 (3)

References

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