Modelling of Epitaxial Growth of Diamond Crystals in High-Carbon Fe—Al Alloys

Standard enthalpies of formation of different K-phase unit cells are calculated and compared with formation enthalpy of modified unit cell of K-phase. Spin-polarized calculations are performed to compare electronic structure of carbon atoms in K-phase substrate, diamond, and graphite. An assumpti...

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Veröffentlicht in:Наносистеми, наноматеріали, нанотехнології
Datum:2013
Hauptverfasser: Mekhed, A.A., Andryushchenko, V.A.
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Sprache:Englisch
Veröffentlicht: Інститут металофізики ім. Г.В. Курдюмова НАН України 2013
Online Zugang:https://nasplib.isofts.kiev.ua/handle/123456789/75896
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Zitieren:Modelling of Epitaxial Growth of Diamond Crystals in High-Carbon Fe—Al Alloys / A.A. Mekhed, V.A. Andryushchenko // Наносистеми, наноматеріали, нанотехнології: Зб. наук. пр. — К.: РВВ ІМФ, 2013. — Т. 11, № 1. — С. 33-38. — Бібліогр.: 4 назв. — анг.

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author Mekhed, A.A.
Andryushchenko, V.A.
author_facet Mekhed, A.A.
Andryushchenko, V.A.
citation_txt Modelling of Epitaxial Growth of Diamond Crystals in High-Carbon Fe—Al Alloys / A.A. Mekhed, V.A. Andryushchenko // Наносистеми, наноматеріали, нанотехнології: Зб. наук. пр. — К.: РВВ ІМФ, 2013. — Т. 11, № 1. — С. 33-38. — Бібліогр.: 4 назв. — анг.
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container_title Наносистеми, наноматеріали, нанотехнології
description Standard enthalpies of formation of different K-phase unit cells are calculated and compared with formation enthalpy of modified unit cell of K-phase. Spin-polarized calculations are performed to compare electronic structure of carbon atoms in K-phase substrate, diamond, and graphite. An assumption is made on the epitaxial growth of the diamond crystals during the thermobaric treatment of high-carbon Fe—Al alloys. Розраховано стандартні ентальпії утворення різних елементарних комірок K-фази, виконано порівняння їх з ентальпією утворення модифікованої елементарної комірки. Порівняно електронні структури атомів вуглецю в K-фазі, алмазу та графіту, яких одержано спін-поляризованими розрахунками у пакеті Wien2k. Припущено епітаксіальний ріст кристалів алмазу при термобаричному обробленні високовуглецевих стопів Fe—Al Рассчитаны стандартные энтальпии образования разных элементарных ячеек K-фазы, выполнено их сравнение с энтальпией образования модифицированной элементарной ячейки. Сравнены электронные структуры атомов углерода в K-фазе, алмаза и графита, полученные в результате спин-поляризованных расчётов в пакете Wien2k. Предположен эпитаксиальный рост кристаллов алмаза при термобарической обработке высокоуглеродистых сплавов Fe—Al.
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fulltext 33 PACS numbers: 71.15.Mb, 71.15.Nc,71.20.Be,81.05.uj,81.05.Zx,81.10.Aj, 82.60.Cx Modelling of Epitaxial Growth of Diamond Crystals in High-Carbon Fe—Al Alloys A. A. Mekhed and V. A. Andryushchenko G. V. Kurdyumov Institute for Metal Physics, N.A.S. of Ukraine, Acad. Vernadsky Blvd., 36, 03680 Kyyiv-142, Ukraine Standard enthalpies of formation of different K-phase unit cells are calculat- ed and compared with formation enthalpy of modified unit cell of K-phase. Spin-polarized calculations are performed to compare electronic structure of carbon atoms in K-phase substrate, diamond, and graphite. An assumption is made on the epitaxial growth of the diamond crystals during the thermobaric treatment of high-carbon Fe—Al alloys. Розраховано стандартні ентальпії утворення різних елементарних комі- рок K-фази, виконано порівняння їх з ентальпією утворення модифікова- ної елементарної комірки. Порівняно електронні структури атомів вугле- цю в K-фазі, алмазу та графіту, яких одержано спін-поляризованими роз- рахунками у пакеті Wien2k. Припущено епітаксіальний ріст кристалів алмазу при термобаричному обробленні високовуглецевих стопів Fe—Al. Рассчитаны стандартные энтальпии образования разных элементарных ячеек K-фазы, выполнено их сравнение с энтальпией образования моди- фицированной элементарной ячейки. Сравнены электронные структуры атомов углерода в K-фазе, алмаза и графита, полученные в результате спин-поляризованных расчётов в пакете Wien2k. Предположен эпитакси- альный рост кристаллов алмаза при термобарической обработке высоко- углеродистых сплавов Fe—Al. Key words: K-phase, diamond, graphite, epitaxy, substrate, Wien2k, elec- tron density, thermobaric treatment, standard enthalpies of formation. (Received 8 January, 2013) 1. INTRODUCTION The most common designation for K-phase is Fe3AlC. Type of crystal Наносистеми, наноматеріали, нанотехнології Nanosystems, Nanomaterials, Nanotechnologies 2013, т. 11, № 1, сс. 33—38 © 2013 ІМФ (Інститут металофізики ім. Г. В. Курдюмова НАН України) Надруковано в Україні. Фотокопіювання дозволено тільки відповідно до ліцензії 34 structure bic face- mann—M eter is а ≈ are as fo 1/2 1/2 1 Howev [2], and r х = 0.08 chiometr temperat that com bulk of c diamond analysis the ratio Fig. 1. Sc a diamond a Fig. 3. Ca ration); (c A. A. e of the K-p centred cry Mauguin sym ≈ 3.75 Å. C ollows: 1Al 1/2 [1]. ver, actual real chemic to 0.66 [2, ric compos ture (up to mposition o compound, d crystals of has shown of 3 to 1. heme of epit d on the K-p alculated cry c) Fe3.125Al0.8 MEKHED an phase is des ystal lattic mbol of spac oordination l (Oh): 0 0 0 ly stoichio cal formula , 3]. Anoth ition unde 2.2 K). It w of obtained which con f 100—200 the presen taxial growt phase. b ystal cells: (a 825C0.5; (d) Fe nd V. A. AND scribed in r ce with Sch ace group Pm n number М 0, 3Fe (D4h ometric K-p a is Fe4−уAl her attempt r high pre was unsucc K-phase w sisted mos micrometr nce of Fe an th of Fig. 2 bon is treat a) Fe3.5Al0.5C e3.5Al0.5C0.5; ( DRYUSHCHE reference li hoenflies sy m3m. Aver М ≈ 5. Coor h): 1/2 0 0; phase has n уCх [2], wh t [4] was m essure (up t essful; exa was Fe3AlC tly of the K res in size w nd Al atoms 2. Octahedra s deposited d ment. c C, (b) Fe3.5Al (e) Fe3AlC0.6 NKO iterature as ymbol Oh 1 rage unit ce dinates of t ↓ 0.6—0.9 С never been ere у = 0.4— made to ach to 8 GPa) mination h C0.66. Beside K-phase, co were found. s in these cr al pore, in wh during therm l0.5C (distinc 6. s: L′12 cu- and Her- ell param- the atoms С (Oh) by observed —1.0, and hieve stoi- and high has shown es, in the olonies of . Spectral rystals in hich car- mobaric d ct configu- MODELLING OF GROWTH OF DIAMOND CRYSTALS IN HIGH-C Fe—Al ALLOYS 35 This and also the fact that the difference of lattice parameters of the K-phase (α ≈ 3.75 nm) and diamond (3.57 nm) is about 5%, allows to assume that epitaxial growth (or nucleation) of diamonds is possible on the surface (or inside the volume) of K-phase (Fig. 1). Increase of pres- sure during the thermobaric treatment will reduce the difference of parameters even more (α ≈ 3.69 nm at 7 GPa). The most suitable sub- strate crystal plane for epitaxial growth of diamonds on K-phase is [200]. It contains four atoms of carbon, and it has an octahedral pore in the middle. It is possible that undissolved carbon (K-phase can dissolve only up to 2/3 carbon atom per cell) is deposited in this pore during the process of thermobaric treatment (Fig. 2). As said earlier, K-phase composition varies in a broad range, so first we investigated different possible unit cells corresponding to different compositions of K-phase. Linearized augmented plane wave method as implemented in Wien2k package is used to perform spin-polarized calcu- lations of the following crystal cells (Fig. 3): Fe3AlC, Fe3.125Al0.825C0.5, Fe3.5Al0.5C0.5, Fe3.5Al0.5C (two configurations), Fe3Al0.66C0.66, Fe3AlC0.66. The last one corresponds to the real K-phase in terms of composition. Crystal cell parameter is chosen to be 0.375 nm, which corresponds to the optimal volume of stoichiometric K-phase according to our calculations. Generalized gradient approximation (Perdew—Burke—Ernzerhof’96) is used as exchange-correlation potential with cut-off energy equal to −7 Ry in all calculations. Atomic radii are chosen as follows: for Al, 2.34 a.u.; for Fe, 1.87 a.u.; for C, 1.66 a.u. Total energies of corresponding K-phase cells and their constituent elements are obtained from calculations and then used to compute en- thalpies of formation of these cells. Obtained values are listed in Table 1. Minimum of studied enthalpies of formation corresponds to the Fe3AlC0.5 cell. Fe3AlC0.6(6) cell also has low value of enthalpy and most probably forms when the melt is oversaturated with carbon. K-phase cell of stoichiometric composition Fe3AlC has higher formation en- TABLE 1. Standard enthalpies of formation of different compositions of K- phase. Unit cell Enthalpy of formation, eV/atom Fe3AlC −0.03 Fe3AlC0.6(6) −0.0328 Fe3AlC0.5 −0.033 Fe3.125Al0.825C0.5 −0.0308 Fe3.5Al0.5C0.5 −0.0244 Fe3.5Al0.5C −0.0286 Fe3.5Al0.5C * −0.0275 *Distinct atomic configuration. 36 thalpy a sponds t found ye crease of caused b form new rounds c stronger Fe—Fe an (Fig. 4). ture as a As for Fig. 4. Sp (left) and Fig. A. A. and thus pr to experime et. Fe3.5Al0.5 f formation by the fact w bonds w carbon) an r than prev nd Fe—C bo As a result whole. r the carbo patial distri Fe3.125Al0.875 5. Total elec MEKHED an robability ental data: 5C has even n enthalpie that iron ith iron at nd, despite vious bonds onds of ato t, this leads on non-stoi bution of el 5C0.5 (right). ctron densit nd V. A. AND of its form : stoichiom n lower prob s with decr atoms em toms from this newl s with alum oms from o s to decreas ichiometry lectron dens ties of Fe3AlC DRYUSHCHE mation is l metric K-ph bability of rease of alu mbedded ins octahedra ly formed minium ato ctahedral c se of stabili y, one can sities in pla C (left) and F NKO lower, whi hase has ne formation. uminium co stead of al al carcass ( bonds are ms, the str carcass is d ty of K-pha see that st ane [200] of Fe3AlC0.5 (ri ich corre- ever been . Such in- ontents is luminium (that sur- e slightly rength of decreased ase struc- tructures f Fe3AlC0.5 ight). MODEL with carb of states thermod Despit and Fe3A our furth computa can be a mond an pressure calculati phase (an ties of ca in diamo Fig. 6. Co densities atom of K lines stan pressure o LING OF GRO bon non-sto s compared ynamically te the expe AlC0.66 are m her calcula ationally ex substrate nd modified of 7 GPa) ion shows t nd thus, gr arbon atom nds. С1 omparison o of correspon K-phase; C2 nd for K-ph of 7 GPa. OWTH OF DIA oichiometr d to stoich y stable (Fig eriment an more therm ations we u xpensive. I for a diam d K-phase c were calcu that with g radual decr s in K-phas of electron d nding carbo is on the rig ase under n AMOND CRYS ry have mor hiometric o g. 5). nd calculati modynamica used the las n order to mond, electr cell (Fig. 2 ulated. The radual incr rease of latt se become m densities of on atoms of m ght (see Fig no pressure, STALS IN HIG re evident m one, which ions had sh ally prefera st one, bec understan ron densiti ) (with no ey are comp rease in pre tice parame more and m graphite/d modified K- . 2 for atom , dashed lin GH-C Fe—Al A minimum o h makes th hown that able than F ause it is m nd whether ies of grap pressure a pared in Fi essure appl eter) electr more similar С2 iamond with -phase. On t m designation es for K-ph ALLOYS 37 of density hem more Fe3AlC0.5 Fe3AlC, in much less r K-phase hite, dia- and under ig. 6. The lied to K- ron densi- r to those h electron the left, C1 n). Dotted hase under 38 A. A. MEKHED and V. A. ANDRYUSHCHENKO Several cells with different number of layers of ordinary (varying from 1 to 4) and modified K-phase were also calculated. Additional layers of K-phase create additional splitting, but the picture mostly remains the same. Enthalpies of formation of such unit cells are close to 0 (varying from −0.008 to −0.01 eV/atom) and are bigger than that of ordinary K-phase, so, these cells require special conditions to form, e.g., abundance of the carbon. 2. CONCLUSION We have made an assumption that K-phase, because its lattice parame- ter (0.375 nm) is close to that of diamond (0.357 nm), can be a sub- strate for a diamond with the substrate plane [200]. We have per- formed electron densities calculations of K-phase unit cells with addi- tional carbon atom in the octahedral pore of [200] plane. Calculations have shown that with gradual increase of pressure electron densities of carbon atoms from the substrate plane of the modified K-phase become more and more similar to the electron densities of carbon in diamond. We also have performed calculations of standard enthalpies of for- mation that have shown that Fe3AlC0.5 and Fe3AlC2/3 have the lowest enthalpies and thus have the highest probability of formation. The rea- sons for this are provided in the article. It is worth mentioning that we have used Fe3AlC unit cell as a basis for modified K-phase because it has lower computational costs. Formation enthalpies of all calculated modified K-phase unit cells are slightly higher than that of Fe3AlC, which means that they need special conditions to form, e.g., abundance of the carbon. REFERENCES 1. K. J. Smittels, Metals: Handbook (Moscow: Metallurgiya: 1980) [Russian translation]. 2. V. A. Andrushenko, V. G. Gavrilyuk, and V. M. Nadutov, Fiz. Met. Metalloved., 60, No. 4: 683 (1985) (in Russian). 3. H. G. Goldshmidt, Interstitial Alloys (London: Butterworths: 1967). 4. V. A. Andryushchenko et al., Metallofiz. Noveishie Tekhnol., 31, No. 9: 1257 (2009) (in Russian).
id nasplib_isofts_kiev_ua-123456789-75896
institution Digital Library of Periodicals of National Academy of Sciences of Ukraine
issn 1816-5230
language English
last_indexed 2025-11-29T14:11:29Z
publishDate 2013
publisher Інститут металофізики ім. Г.В. Курдюмова НАН України
record_format dspace
spelling Mekhed, A.A.
Andryushchenko, V.A.
2015-02-05T17:37:26Z
2015-02-05T17:37:26Z
2013
Modelling of Epitaxial Growth of Diamond Crystals in High-Carbon Fe—Al Alloys / A.A. Mekhed, V.A. Andryushchenko // Наносистеми, наноматеріали, нанотехнології: Зб. наук. пр. — К.: РВВ ІМФ, 2013. — Т. 11, № 1. — С. 33-38. — Бібліогр.: 4 назв. — анг.
1816-5230
PACSnumbers:71.15.Mb,71.15.Nc,71.20.Be,81.05.uj,81.05.Zx,81.10.Aj,82.60.Cx
https://nasplib.isofts.kiev.ua/handle/123456789/75896
Standard enthalpies of formation of different K-phase unit cells are calculated and compared with formation enthalpy of modified unit cell of K-phase. Spin-polarized calculations are performed to compare electronic structure of carbon atoms in K-phase substrate, diamond, and graphite. An assumption is made on the epitaxial growth of the diamond crystals during the thermobaric treatment of high-carbon Fe—Al alloys.
Розраховано стандартні ентальпії утворення різних елементарних комірок K-фази, виконано порівняння їх з ентальпією утворення модифікованої елементарної комірки. Порівняно електронні структури атомів вуглецю в K-фазі, алмазу та графіту, яких одержано спін-поляризованими розрахунками у пакеті Wien2k. Припущено епітаксіальний ріст кристалів алмазу при термобаричному обробленні високовуглецевих стопів Fe—Al
Рассчитаны стандартные энтальпии образования разных элементарных ячеек K-фазы, выполнено их сравнение с энтальпией образования модифицированной элементарной ячейки. Сравнены электронные структуры атомов углерода в K-фазе, алмаза и графита, полученные в результате спин-поляризованных расчётов в пакете Wien2k. Предположен эпитаксиальный рост кристаллов алмаза при термобарической обработке высокоуглеродистых сплавов Fe—Al.
en
Інститут металофізики ім. Г.В. Курдюмова НАН України
Наносистеми, наноматеріали, нанотехнології
Modelling of Epitaxial Growth of Diamond Crystals in High-Carbon Fe—Al Alloys
Article
published earlier
spellingShingle Modelling of Epitaxial Growth of Diamond Crystals in High-Carbon Fe—Al Alloys
Mekhed, A.A.
Andryushchenko, V.A.
title Modelling of Epitaxial Growth of Diamond Crystals in High-Carbon Fe—Al Alloys
title_full Modelling of Epitaxial Growth of Diamond Crystals in High-Carbon Fe—Al Alloys
title_fullStr Modelling of Epitaxial Growth of Diamond Crystals in High-Carbon Fe—Al Alloys
title_full_unstemmed Modelling of Epitaxial Growth of Diamond Crystals in High-Carbon Fe—Al Alloys
title_short Modelling of Epitaxial Growth of Diamond Crystals in High-Carbon Fe—Al Alloys
title_sort modelling of epitaxial growth of diamond crystals in high-carbon fe—al alloys
url https://nasplib.isofts.kiev.ua/handle/123456789/75896
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AT andryushchenkova modellingofepitaxialgrowthofdiamondcrystalsinhighcarbonfealalloys