1. INTRODUCTION Crystals of the same mineral species can appear in different forms, i.e. habit types. Besides numerous rese- archers, KOSTOV (1966, 1969, 1970, 1975) has inves- tigated the changes of mineral habit during the crystal- lization of a particular mineral species. He pointed to the influence of crystalline structure (unit cell dimen- sions, nature of bonds in the structure) and external conditions during growth (chemical composition of solution, supersaturation degree of solution, type of ingredients) on the change of crystal habit of the same mineral species. BRAVAIS (1851) observed the evi- dent dependence between reticular density and proba- bility of appearance of a particular crystal form. Priority in crystal growth has the crystal form with maximal reticular density (BRAVAIS, 1851). In consideration of this fact, it is possible to determine the development sequence of barite crystal types by introduction of the term “average structural density of crystal” (KRIVO- VI»EV, 1971) which defines the total contribution of reticular density of all crystal form faces, and by calcu- lation of the values of average structural densities for different habit types of barite crystals. Barite is one of the mineral species, which could have extremely different habit types. BRAUN (1932) The Average Structural Density of Barite Crystals of Different Habit Types Biserka RADANOVI∆-GUÆVICA has determined seven different habit types of barite crystals on the basis of detailed investigation of rela- tionships between morphological characteristics and mineral association. Some specimens of barite from Westmorland and County Durham in the north of Eng- land, show up to six changes of habit during growth, from the crystals elongated in the [1 0 0] direction, thro- ugh the crystals tabular on the basal pinacoid {0 0 1}, to crystals elongated in the [0 1 0] direction (SEAGER & DAVIDSON, 1952). A similar sequence is described for barite crystals from the Tjuja-Mujun mine (SOLO- DOVNIKOVA, 1927). KRIVOVI»EV (1971) separat- ed three generations of different habit types of barite crystals from the BeloreËensko locality, and determined the development sequence from the prismatic crystals elongated in the [010] direction, through the thick-tabu- lar crystals elongated in the [0 1 0] direction, to crystals tabular on the basal pinacoid. This sequence is in accor- dance with decreasing average structural density of the crystals (KRIVOVI»EV, 1971). An inverse develop- ment sequence was determined on barite crystals from Krapinske Toplice (ZEBEC, 1976). A sequence from crystals tabular on the basal pinacoid, through crystals elongated in the [100] direction, to crystals elongated in the [0 1 0] direction, was accompanied with a change of genesis temperature and decrease of SrSO4 c o n t e n t (ZEBEC, 1976). Observations of phantoms and inclu- sions in crystals of barite from Muddy Creek, Colorado, suggest at least five episodes of crystal growth, with G EOL. CROAT. 52/1 59 - 65 1 Fig. 4 Tabs. ZAGREB 1999 Key words: Barite, Habit types, Reticular density, Average structural density of crystal. KljuËne rijeËi: barit, tipovi habitusa, retikularna gus- toÊa, srednja strukturna gustoÊa kristala. Department of Mineralogy and Petrography, Croatian Natural History Museum, Demetrova 1, HR-10000 Zagreb, Croatia. Abstract Eight different habit types of barite crystals which could be clas- sified into 4 essentially different groups were determined by morpho- logical analysis: Eb group - barite crystals elongated in the [0 1 0] direction; Ea group - barite crystals elongated in the [1 0 0] d i r e c t i o n ; Tc group - barite crystals tabular on the basal pinacoid {0 0 1}; Ec group - barite crystals elongated in the [001] direction. By determination and comparison of the average structural densi - ties of different habit types of barite crystals, it was possible to estab- lish the spans of their values from 276.1 to 495.8, and overlapping of values for Eb group with Ea group and Tc group with Ec group. The sequence of habit types, with regard to the decreasing average struc- tural density, i.e. the priority sequence of developing of barite crystal types, was determined: Eb group - Ea group - Tc group - Ec group. Saæetak Morfoloπkom analizom odreeno je 8 razliËitih tipova habitusa baritnih kristala koji se mogu svrstati u 4 bitno razliËite skupine: Eb skupina - kristali barita izduljeni smjerom [0 1 0]; Ea skupina - kristali barita izduljeni smjerom [100]; Tc skupina - kristali barita ploËasti po baznom pinakoidu {0 0 1}; Ec skupina - kristali barita izduljeni smjerom [001]. Odreivanjem i usporedbom srednjih srtukturnih gustoÊa razli- Ëitih tipova habitusa baritnih kristala utvreni su rasponi njihovih vri- jednosti od 276.1 do 495.8, te su uoËena preklapanja vrijednosti za Eb i Ea skupine, kao i za Tc i Ec skupine. Utvren je redosljed tipova habitusa s obzirom na smanjenje srednje strukturne gustoÊe kristala, tj. prioritetni slijed razvoja baritnih kristala: Eb skupina - Ea skupina - Tc skupina - Ec skupina. 60 Geologia Croatica 52/1 changes in morphology with respect to time (TRUEBE, 1981). Recently, researchers attempted to determine the dependence of barite morphology on different con- trolled conditions during experimental crystal growth (FERNANDEZ-DIAZ et al., 1990; PRIETO et al., 1992). Numerous barite specimens with different crystal habits are stored at the collection of Department of Mineralogy and Petrography of the Croatian Natural History Museum in Zagreb. Systematic researchs of barite morphology and the reticular density of the crys- tal form faces was undertaken in order to try to define the priority sequence of developing of barite crystals types, on the base of calculated values of average struc- tural density of crystal. This paper is the result of investigations performed as part of a Master’s Thesis (RADANOVI∆-GUÆVI- CA, 1995). 2. MATERIAL AND METHODS The crystals of barite from the Mrzle Vodice locali- ty in Gorski Kotar region, Sivac on mountain Petrova gora and RiËice in Lika region from Croatia, Æune in north-western Bosnia and Herzegovina, the valley of the river Krivaja, MaËkara district, VeovaËa and the environs of Kreπevo in the central part of Bosnia and Herzegovina, and PraËa in eastern Bosnia and Herze- govina, ©uplja Stena on Avala hill and Veliki Majdan in Serbia, Yugoslavia, and Stari Trg (TrepËa) in Koso- vo, Serbia, Yugoslavia, are elaborated in this paper. Under the research programme, the morphological, as well as relevant crystallographic analyses of the barite crystals, were performed. Morphological analysis included goniometric mea- surement of the crystals, performed for the most part (62 crystals) on a Goldschmidt type two-circle reflect- ing goniometer, and for a smaller number (5 crystals) on a contact goniometer. On the basis of faces determi- nation from a gnomon projection, and by the help of data for barite by GOLDSCHMIDT (1897) and PALA- CHE et al. (1951), construction of the parallel perspec- tive drawings of measured crystals was undertaken using the method described by TERPSTRA & CODD (1961), as well as the determination of the different ha- bit types of the barite crystals. Crystallographic research was performed by the X- ray powder method on the Philips vertical x-ray gonio- meter with Cu Kα radiation and graphite monochroma- tor. Standard conditions of recording were: 40 kV, 30 mA, 1° 2Θ/min for the counter, and 1 cm/min for the recording paper, in the angular region from 9° to 62° 2Θ. The barite X-ray diffraction pattern was indexed conformably to JCPDS card no. 24-1035. The unit cell dimensions are the result of refinement by the method of least squares performed by the GITTER computer program (HUMMEL, 1982) on the base of 28 to 32 indexed diffraction lines. The reticular density of a particular crystal form is the ratio of the number of all atoms in the section of a crystal structure, defined by the elementary parallelo- gram Shkl and interplanar spacing dhkl. The number of all atoms in a certain section was performed by the ATO- MS computer program (DOWTY, 1991), which gave us the display of structure based on the data (coordinate system, unit cell parameters, space-group symmetry, atom coordinates). The data according to HILL (1977) are used for the display of barite structure. The surface of the elementary parallelogram was calculated accord- ing to the formula: S2 hkl = h2S2 100 + k2S2 010 + l2S2 001 + 2(hkS100S010cosν + klS010S001cosλ + lhS001S100cosµ) where: Shkl - surface of the elementary parallelogram of the face (hkl) in [Å2]; S1 0 0 = b0c0s i nα, S0 1 0 = c0a0s i nβ, S001 = a0b0sinγ (a0, b0, c0 - unit cell dimension in [Å]; α, β, γ - angles between crystal axes); ν = (100) ∧ ( ( 0 1 0 ) ; λ = (010) ∧ (001); µ = (001) ∧ (100)) (PHILLIPS, 1946). This formula can be simplified since barite is orthorhombic: S2 hkl = h2b2 0c 2 0 + k2c2 0a 2 0 + l2a2 0b 2 0 According to KRIVOVI»EV (1971) the average structural density of crystal “ECR” was calculated accor- ding to the formula: ECR = ∑(M x Ehkl) where: M is the morphological persistence of a particu- lar crystal form (FRANK-KAMENECKII, 1951), Ehkl is the reticular density of a crystal form in number of atoms in Å3, and the product “M x Ehkl” defines the con- tribution of reticular density of a given crystal form in the total structural density of crystal. Morphological persistence is the ratio of the total surface of all faces of a certain crystal form and the surface of the whole crys- tal, and was expressed in percent. “M” is calculated thus: face surfaces of emphasized crystal forms were measured on several crystals of a certain habit type, and the average value of these surfaces for a respective crystal form was calculated. The studied barite specimens are stored in the col- lection of the Department of Mineralogy and Petrogra- phy of the Croatian Natural History Museum in Zagreb, and are marked by the inventory numbers: 600:ZAG ;3310:MP1, 600:ZAG;3602:MP1, 600:ZAG;3641:MP1, 600:ZAG;5183:MP1, 600:ZAG;5677:MP1, 600:ZAG; 5689:MP1, 600:ZAG;5718:MP1, 600:ZAG;5780:MP1, 600:ZAG;6688:MP1, 600:ZAG;6691:MP1, 600:ZAG; 6703:MP1, 600:ZAG;8541:MP1, 600:ZAG;8542:MP1, 600:ZAG;8546:MP1, 600:ZAG;9013:MP1, 600:ZAG; 9014:MP1, 600:ZAG;9016:MP1, 600:ZAG;9017:MP1, 600:ZAG;9018:MP1, 600:ZAG;9021:MP1, 600:ZAG; 9022:MP1, 600:ZAG;9023:MP1, 600:ZAG;9025:MP1, 600:ZAG;9026:MP1, 600:ZAG;9027:MP1, 600:ZAG; 9029:MP1, 600:ZAG;9030:MP1, 600:ZAG;9031:MP1 and 600:ZAG;9039:MP1. 3. RESULTS 3.1. MORPHOLOGICAL ANALYSIS From morphological analysis of barite crystals from 12 localities, 8 different habit types were determined. These habit types could be classified into 4 essentially different groups: The Eb group of barite crystals (Table 1) is repre- sented by 2 habit types elongated in the [010] direction. One habit type was observed only in ©uplja Stena, and had been described before (BARI∆, 1949). These colu- mnar crystals have prominent {1 0 1} and somewhat smaller {0 1 1} faces. According to Braun’s classifica- tion, this habit type is intermediate between ore - IIIb type - Pb 0 0 1[0 1 0] and carbonate - IVa type - Ab ( B R A- UN, 1932). Another habit type was observed in Veliki Majdan. These columnar crystals have well-developed {0 0 1} and {1 0 1} faces, and somewhat smaller {0 1 1} and {210} faces, and correspond to the carbonate - IVa type - Ab (BRAUN, 1932). The Ea group of barite crystals (Table 2) is repre- sented by 2 habit types elongated in the [100] direction. One habit type was noticed in RiËice and Kreπevo (Raπtelica, Dubrave, Dusina). These thick-tabular crys- tals have prominent {001}, {011} and {101} faces, and correspond to the rectangularly-tabular - I type - 61RadanoviÊ-Guævica: The Average Structural Density of Barite Crystals of Different Habit Types Table 1 The average structural density of barite crystals elongated in the [010] direction (Eb group). Table 2 The average structural density of barite crystals elongated in the [100] direction (Ea group). 62 Geologia Croatica 52/1 Pa 0 0 1[1 0 0], [0 1 0] (BRAUN, 1932). Another habit type was observed only in the MaËkara district. These columnar crystals have well-developed {0 0 1}, {0 1 1}, {101} and {210} faces, and correspond to the carbonate - IVb type - Aa (BRAUN, 1932). The Tc group of barite crystals (Table 3) is repre- sented by 2 habit types tabular on the basal pinacoid {001}. One habit type was noticed only in Æune. These tabular crystals have well-developed faces from the [1 0 0] and [0 1 0] crystallographic axe’s zones, specially Table 3 The average structural density of barite crystals tabular on the basal pinacoid {001} (Tc group). HAB~rTYtPe LQCAI..JTY FORM M ,~ E'~ Mi)l e"", ~. (1ftrIm ~ A.~~ I "hE~ 001 1i3G.9 3L~1 237''''; ,0111 1:1.5 ~,.,3:J 8 oo.G- 101 1 ~.6 5.S741 75.2 G_ ZUM O ~ Qo 2,5 2:726 M 394..1 - : 2 0. HI 3,. ... 1'12 1iJ._~ 100 1.8 4~8 S..i8 201 1.'1 ,3: , n 4,1 001 ,57..3 3..534 2D5..-4, 210 .32'.3 3.440' '11U ~=----j 'dI01' 6.7 5.515 ,37.4, Ei 'VodI C>!! 2;" 2.4 :U01 7A, ::iIiJS.3 010 1..0 2.724 2.7 O'U 0'.3- 4.337 1..3 00 M .ll 9.571 228-9 210 '2<1 _7 3 . .j,3.q, 134 (i,11i) 60.,1 U,25 '7..3 C5JIt:~ au :12: ·U~ 13.!.!i v:~~ 2C1 ~ 0..8 3.763 3") 34(1 ,:3 10D 0...7 41 .4129 ,U 101 0_7 5,500 3,~ :291] M 1,678 (iI .I I1Jt1D 0..3 2. ;H QJ!: 001 55_'2 :1.515 18'1.3 :1l'10 SOiG 3. 'a1 105.2 ~3 101 1 jj1 5,JiM 61.2 1I(JEt§~,j) ('IU ~ '1.~32 12,1 977'.2: ~aD 0..3 ~ , oi!\B ~ " f) 6 10 0. 1-4 213 0.1 00,1 5,'1,4 ;J..507~ 184l.Q :2:10 39.9 ~4412 1:37.9 10-2 5.1 3..319 15.9 Pr.ao!;a 103 2.7 2'.304 !;i,:2 849..1 101 0..7 5..571 9,9 :2&i 1112 3L171 0.8 f.01 ~9, 1 3.,5;76 1:JS.9 ~10 2'd.7 3.A36 7>11 .,6 211 , 41.9 3;.007 44,3 201 13.0 3..1liiB 49,0 'It MsrpBr'l i 111 1!.7 3.1J:W 33B 364,5 101 '3.1 5.$0 6..1 W 1.1 3 .:316 3..6 010 0.6 ,2.720 1..(1. 100 0, 41 4..433 1.S 001 !;)7 . .6, 3 ,811(1, 2£62 210 ~Ji; SMl ,~ 211 8.a 3.101 :27J) Stan Trg 1 0 ~ 15.9, 5.!;i71 29 . .15- 361.41 (li~~ an 1-3 ~.m M om 0.6 2.727 1..6 100 OJl oji ,43'!i 1...~ 63RadanoviÊ-Guævica: The Average Structural Density of Barite Crystals of Different Habit Types {0 1 1} and {1 0 1} faces. Another habit type was the most frequent type, and discovered at the following localities: Mrzle Vodice, Æune, VeovaËa, Kreπevo, PraËa, Veliki Majdan and Stari Trg (TrepËa). These tab- ular crystals have marked {2 1 0} faces, and correspond to the silicate - VI type - Pb 001[010] (BRAUN, 1932). The Ec group of barite crystals (Table 4) is repre- sented by 2 habit types elongated in the [001] direction. One habit type was observed only in Sivac. These crys- tals have well-developed {4 1 0} and {1 0 0} faces and somewhat smaller {0 0 1} and {2 1 0} faces, and corre- spond to the Wolnyn - VII type - Ac (BRAUN, 1932). Another habit type was noticed only in Krivaja. These isometric to elongated crystals have prominent {2 1 0} faces and well-developed {0 0 1}, {1 0 1} and {2 1 1} faces, and correspond to the cubic-pyramidal - V type - I001,210[120] (BRAUN, 1932). A detailed review of the results of morphological analysis is given in RADANOVI∆-GUÆVICA et al. (in press). 3.2. AVERAGE STRUCTURAL DENSITY OF BARITE CRYSTALS The average structural density of crystal was calcu- lated according to aforesaid procedure for 14 barite samples, e.g. 8 different habit types of crystals (Tables 1-4). Values of the average structural density of a crystal are greatest in the case of barite crystals elongated in the [0 1 0] direction, and amounts vary from 419.5 to 495.8 (Table 1). Barite crystals elongated in the [1 0 0] direction have values of average structural density in a relatively small range from 415.8 to 431.3 (Table 2). Values of the average structural density of barite crys- tals tabular on the basal pinacoid {0 0 1} are 346.3 to 394.1 (Table 3). Values of the average structural densi- ty of a crystal are smallest in the case of barite crystals elongated in the [0 0 1] direction, and range from 276.1 to 349.4 (Table 4). The ranges of values of the average structural densi- ties of the four main groups of barite crystal habit types are shown in Fig. 1. Overlapping of the Eb group (barite crystals elongated in the [0 1 0] direction) with the Ea group (barite crystals elongated in the [1 0 0] d i r e c t i o n ) was observed, as well as the Tc group (barite crystals tabular on the basal pinacoid {0 0 1}) with the Ec g r o u p (barite crystals elongated in the [0 0 1] d i r e c t i o n ) . Besides, it is necessary to highlight that the value of the average structural density of columnar barite crystals, Fig. 1 The ranges of values of average structural densities of four main groups of barite crystal habit types: Eb group - barite crys- tals elongated in the [0 1 0] direction; Ea group - barite crystals elongated in the [100] direction; Tc group - barite crystals tabular on the basal pinacoid {0 0 1}; Ec group - barite crystals elongated in the [001] direction. Table 4 The average structural density of barite crystals elongated in the [001] direction (Ec group). 64 Geologia Croatica 52/1 elongated in the [0 1 0] direction, with well-formed {1 0 1} and {0 0 1} faces, as well as with somewhat smaller {2 1 0}, {2 0 1} and {0 1 1} form faces, which were noticed in Veliki Majdan mine is very close to the value of average structural density of columnar crystals elongated in the [1 0 0] direction, with well-formed {0 1 1} and {0 0 1}, as well as with somewhat smaller {1 0 1} and {2 1 0} form faces, from MaËkara district. According to Braun’s classification, both habit types correspond to the carbonate type, i.e. crystals elongated in the [010] direction are carbonate - IVa type - Ab, and the crystals elongated in the [100] direction are carbon- ate - IVb type - Aa (BRAUN, 1932). 4. DISCUSSION AND CONCLUSIONS By comparison of the values of average structural densities of different habit types of barite crystals, the development sequence of barite crystal types in consid- eration to a decrease of average structural density, was determined. In general, the priority sequence was: bari- te crystals elongated in the [0 1 0] direction (Eb group) - barite crystals elongated in the [1 0 0] direction (Ea group) - barite crystals tabular on the basal pinacoid {001} (Tc group) - barite crystals elongated in the [001] direction (Ec group) (Fig. 1). From similar previous researches (SOLODOVNI- KOVA, 1927; SEAGER & DAVIDSON, 1952; KRI- VOVI»EV, 1971; ZEBEC, 1976), together with the one performed here, it is possible to conclude that the sequence of developing of barite crystal types is not strictly defined, and is changeable (alternate) from case to case. Besides the density of the atomic arrangement, which defined the development sequence of crystal habit types, there are many other factors, which are able to cause a change in the sequence, or a change of direc- tion. It would be of great interest to know something about the mineral associations in which particular habit types of barite crystals occur, since the morphology of barite crystals together with information on mineral association, can help identify conditions under which some mineral assemblages were formed. However, research on mineral associations, as well as comparison with Braun’s group was beyond the scope of this paper and is left for future investigation. Acknowledgements I would like to thank academician Stjepan ©∆A- VNI»AR for his helpful and expert advise during the elaboration of the Master’s Thesis, and comments on the manuscript. 5. REFERENCES BARI∆, Lj. 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