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Control of Oxygen Impurities in a Continuous-Feeding Czochralski-Silicon Crystal Growth by the Double-Crucible Method

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Control of Oxygen Impurities in a Continuous-Feeding Czochralski-Silicon Crystal Growth by the Double-Crucible Method crystals Article Control of Oxygen Impurities in a Continuous-Feeding Czochralski-Silicon Crystal Growth by the Double-Crucible Method Wenhan Zhao, Jiancheng Li and Lijun Liu * Key Laboratory of Thermo-Fluid Science and Engineering, Ministry of Education, School of Energy and Power Engineering, Xi’an Jiaotong University, Xi’an 710049, China; [email protected] (W.Z.); [email protected] (J.L.) * Correspondence: [email protected]; Tel.: +86-29-82663443 Abstract: The continuous-feeding Czochralski method is a cost-effective method to grow single silicon crystals. An inner crucible is used to prevent the un-melted silicon feedstock from transferring to the melt-crystal interface in this method. A series of global simulations were carried out to investigate the impact of the inner crucible on the oxygen impurity distributions at the melt-crystal interface. The results indicate that, the inner crucible plays a more important role in affecting the O concentration at the melt-crystal interface than the outer crucible. It can prevent the oxygen impurities from being transported from the outer crucible wall effectively. Meanwhile, it also introduces as a new source of oxygen impurity in the melt, likely resulting in a high oxygen concentration zone under the melt-crystal interface. We proposed to enlarge the inner crucible diameter so that the oxygen concentration at the melt-crystal interface can be controlled at low levels. Citation: Zhao, W.; Li, J.; Liu, L. Keywords: computer simulation; impurities; continuous-feeding Czochralski method; heat transfer; Control of Oxygen Impurities in a double crucible technique Continuous-Feeding Czochralski- Silicon Crystal Growth by the Double-Crucible Method. Crystals 2021, 11, 264. https://doi.org/ 1. Introduction 10.3390/cryst11030264 The continuous-feeding Czochralski method (CCZ) is an effective method to produce Academic Editor: Evgeniy single crystals, especially for crystalline silicon (Si) [1,2]. Compared with the standard N. Mokhov Czochralski (CZ) method, it has many advantages. For example, since silicon melt can be replenished continuously during a CCZ crystal growth process, the melt volume can Received: 29 January 2021 remain limited and unchanged in the crucible so that the melt flow becomes stable and Accepted: 24 February 2021 the unsteady kinetics of the melt will be suppressed. In addition, continuous recharging Published: 8 March 2021 of the melt allows for stable control of dopant [3], impurities, and resistivity distribution in a growing crystal, which helps to improve the crystal quality [4,5]. Therefore, it is Publisher’s Note: MDPI stays neutral a very promising technology to produce high-quality crystals at a low cost. However, with regard to jurisdictional claims in the CCZ grown crystal exhibits special defects, which are considered to be related to the published maps and institutional affil- relatively high hydrogen content of the recharged Si granules [6]. These defects lead to iations. serious challenges in the application of CCZ single crystals of silicon in electronic devices. Fortunately, with respect to the solar application, they are considered unlikely to have an adverse effect on solar cell performance [7]. In recent years, with a strong demand for producing n-type crystals for high-efficiency solar cells, the CCZ method has become very Copyright: © 2021 by the authors. promising [8–10]. It is predicted that the CCZ method will make significant gains in the Licensee MDPI, Basel, Switzerland. market share over conventional CZ in the next 3–5 years [11]. This article is an open access article The growth of crystalline silicon is invariably accompanied by impurities transport, distributed under the terms and such as oxygen (O), carbon (C), and other related products, from reactions [12]. Special conditions of the Creative Commons attention has been paid to, and, therefore, many researches [13–22] have been contributed, Attribution (CC BY) license (https:// the control O concentration in the melt and growing crystals. In the growth process of creativecommons.org/licenses/by/ some conventional methods, it affects the formation of micro-defects in the growing crystal 4.0/). Crystals 2021, 11, 264. https://doi.org/10.3390/cryst11030264 https://www.mdpi.com/journal/crystals Crystals 2021, 11, x FOR PEER REVIEW 2 of 10 some conventional methods, it affects the formation of micro-defects in the growing crys- tal in a complex manner [13]. In the CCZ process, to prevent the unmelted silicon feed- stock from transferring to the melt-crystal (m-c) interface, an inner quartz crucible is usu- ally placed on the bottom of the outer quartz crucible [23]. Since O impurities are dis- Crystals 2021, 11, 264 solved from the quartz crucible wall, a new source of O impurity is thus introduced.2 of 9 Therefore, it is important to investigate the impact of the inner crucible on the O distribu- tions in the melt, especially at the m-c interface, because O impurities will enter the crystal throughin a complex the m manner-c interface. [13]. If In the the initial CCZ O process, concentration to prevent of n the-type unmelted CCZ wafers silicon is feedstocktoo high, thefrom solar transferring cell efficiency to the will melt-crystal be reduced (m-c) [24] interface,. Previous an research inner quartz indicates crucible that isthe usually inner crucibleplaced onis the main bottom reason of the for outer this quartzphenomenon, crucible and [23 ].the Since O concentration O impurities at are the dissolved m-c in- terfacefrom the will quartz increase crucible in the wall, double a new-crucible source ofCCZ O impuritymethod [25] is thus. Providin introduced.g an electromag- Therefore, it neticis important stirring toof investigatethe melt is thean effective impact of way the to inner decrease crucible the on O theconcentration O distributions at the in m the-c interfacemelt, especially [26]. However, at the m-c theinterface, complexity because of the Ocrystal impurities growth will systems enter and the crystalthe cost through will be increasedthe m-c interface. by this method. If the initial O concentration of n-type CCZ wafers is too high, the solar cell efficiencyThis study will aim bes to reduced find an effective [24]. Previous way to research reduce the indicates O concentration that the inner by the crucible double is- cruciblethe main CCZ reason method. for this The phenomenon, impact of the and inner the crucible O concentration was investigated at the m-c by interfaceglobal simu- will lationsincrease, including in the double-crucible coupled O and CCZ C transport, method [which25]. Providing have been an widely electromagnetic used to study stirring the Oof distributions the melt is an in effectivea crystal waygrowth to decreaseprocess [16,20,27 the O concentration–33]. The influence at the mechanism m-c interface of [the26]. innerHowever, crucible the on complexity the O concentration of the crystal in the growth melt systemswas analyzed. and the Based cost willon this be increasedresearch, an by effectivethis method. method to decrease the O distribution in the double-crucible CCZ method was proposed.This study aims to find an effective way to reduce the O concentration by the double- crucible CCZ method. The impact of the inner crucible was investigated by global simu- 2.lations, Problem including Description coupled and O M andathematical C transport, Models which have been widely used to study the 2.1.O distributions Furnace Configuration in a crystal growth process [16,20,27–33]. The influence mechanism of the inner crucible on the O concentration in the melt was analyzed. Based on this research, an effectiveA schematic method diagram to decrease of the CCZ the Ofurnace distribution for industrial in the double-cruciblemanufacture is given CCZ methodin Figurewas proposed. 1. The diameter of the crystal was 200 mm. The crystal length was 600 mm. The inner and outer crucible diameters were 300 mm and 540 mm, respectively. To prevent the2.Problem un-melted Description silicon feedstock and Mathematical from transferring Models to the m-c interface, an inner quartz cru- cible2.1. Furnacewas placed Configuration on the bottom of the outer quartz crucible. The main dimensions of the CCZ furnaceA schematic are listed diagram in Table of the1. CCZ furnace for industrial manufacture is given in FigureIn 1our. The investigation, diameter of we the compare crystal wasd the 200 case mm. of Thethe conventional crystal length CZ was method 600 mm. with The a singleinner andcrucible outer (the crucible single diameters-crucible case) were and 300 the mm proposed and 540 mm,CCZ respectively.method with To two prevent crucibles the (theun-melted double silicon-crucible feedstock case). For from the transferring single-crucible to the case, m-c interface,the crystal an and inner crucible quartz rotation crucible rateswas placedwere set on as the 12bottom rpm and of − the6 rpm, outer respectively. quartz crucible. For the The double main- dimensionscrucible case, of the the rota- CCZ tionfurnace rates are of listedcrystal in and Table crucible1. were set as 12 rpm and −4 rpm, respectively. 1：Crystal 2：Melt 3：Inner crucible 4：Outer crucible 5：Heat shields 1 5 3 2 Windows of the inner crucible 4 FigureFigure 1. 1. SchematicSchematic diagram diagram of of the the continuous continuous-feeding-feeding Czochralski Czochralski method method (CCZ (CCZ)) furnace furnace with with doubledouble crucibles. crucibles. Table 1. The dimensions of the continuous-feeding Czochralski method (CCZ) furnace. Diameter of Inner Diameter of Outer Crystal Diameter (mm) Crystal Length (mm) Crucible (mm) Crucible (mm) 200 600 300 540 Crystals 2021, 11, x FOR PEER REVIEW 3 of 10 Crystals 2021, 11, 264 Table 1. The dimensions of the continuous-feeding Czochralski method (CCZ) furnace. 3 of 9 Crystal Diameter Crystal Length Diameter of Inner Crucible Diameter of Outer Crucible (mm) (mm) (mm) (mm) In200 our investigation,600 we compared the case300 of the conventional CZ540 method with a single crucible (the single-crucible case) and the proposed CCZ method with two crucibles 2.2.(the Numerical double-crucible Modeling case).
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