分子动力学模拟方法研究铜团簇成膜及非晶化锗材料的辐照损伤
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摘要
本文第一部分内容是用分子动力学模拟方法模拟计算Cu团簇沉积在Si衬底上的成膜微观过程。改变入射团簇的大小、入射能量、衬底温度、衬底晶体取向,以及沉积率等初始条件来研究沉积成膜的物理机制。模拟中采用了两组描述体系中原子间相互作用势的方案。方案(一)：EAM势函数描述Cu-Cu原子间的相互作用；SW势函数描述Si-Si原子间的相互作用；LJ两体势函数描述Cu-Si原子间的相互作用。方案(二)：EAM势函数描述Cu-Cu原子间的相互租用；Tersoff势函数描述Si-Si原子间的相互作用：Morse两体势函数描述Cu-Si原子间的相互作用。这部分工作主要从三个方面模拟研究了沉积成膜过程：(1)单个铜团簇沉积演化过程；(2)单个铜原子连续沉积成膜过程；(3)单个铜团簇连续沉积成膜过程。通过模拟研究得到结果如下：
1、通过模拟计算单个Cu团簇沉积在Si衬底上的微观演化过程,研究得到：(1)两组势函数方案都能够比较准确地描述Cu-Si体系中原子间的相互作用,反映Cu团簇沉积在Si衬底上的动态演化过程；(2)在不同大小、形状团簇沉积过程中,原子间动能转化趋势基本相似。团簇越小,动能转化过程越短暂；(3)随着入射动能的增加,团簇原子的延展度增大,平均原子质心高度降低；(4)随着衬底温度的升高,团簇原子的延展度增大,较大团簇的平均原子质心高度明显下降；(5)在Si(001)衬底上,易形成Cu/Si(001)混合内界面；对于Cu13和Cu19团簇分别沉积在Si(111)衬底上,形成Cu/Si(111)混合内界面的入射动能阈值均为3.0eV/atom;对于Cu147团簇沉积在Si(111)衬底上,入射动能阈值为1.6eV/atom开始形成Cu/Si(111)混合内界面。
2、通过模拟计算单个Cu原子连续沉积在Si衬底上的成膜过程,研究得到：(1)随着入射动能的增加,沉积薄膜表面的粗糙度降低,这有利于生长高质量的薄膜；(2)随着衬底温度的升高,沉积薄膜表面的粗糙度降低；(3)当沉积率高于5atoms/ps时,沉积薄膜中会出现孔洞。当沉积率过小时,例如2atoms/ps,沉积薄膜表面比较平滑,但是计算时间大大增加。在本文的模拟计算中,选取5atoms/ps的沉积率研究Cu原子沉积在Si衬底上成膜；(4)在相同的沉积条件下,Si(111)衬底上形成薄膜的表面较Si(001)衬底上形成薄膜的表面平滑。另外,Cu/Si(001)和Cu/Si(111)的混合界面处存在不同程度的非晶化现象。(5)在不同的初始沉积条件下,形成薄膜的结构主要以FCC结构存在,并且薄膜形成起初是以“岛状”模式生长,随着沉积原子数的增多,转为“层状”模式生长。
3、通过模拟计算Cu团簇连续沉积在Si衬底上成膜过程,研究得到：(1)随着入射团簇动能的增加,成膜表面粗糙度减少；(2)随着衬底温度增加,成膜表面粗糙度减少,且Cu/Si混合内界面处原子的混合度增强；(3)随着入射团簇大小尺寸的增加,成膜表面粗糙度增加；(4)在相同衬底温度的条件下,在Si(111)表面上形成的薄膜表面较在Si(001)表面上形成的薄膜表面平滑；(5)团簇沉积成膜过程中,薄膜主要以“混合”模式生长。
本文第二部分内容是用分子动力学模拟方法研究Ge材料的辐照损伤过程,并探究孔洞形成的演化过程。研究得到：(1)能量的沉积导致孔洞形成；(2)“空位团”的形成与湮灭或孔洞的形成导致Ge材料在辐照方向上的肿胀；(3)采用Tersoff-ZBL势函数研究孔洞的演化过程,观察到第一个粒子辐照之后,一个清晰的孔洞出现,然后每隔120.0ps继续第二、三……个粒子辐照,发现模拟体系中有两个清晰孔洞共存的现象。由于模拟体系尺寸的选取,随着辐照次数的增多,形成孔洞的位置和形态总是发生变化,但是孔洞的数目没有增加；(4)采用SW-Yukawa势函数研究孔洞的形成问题。研究发现,孔洞的形成过程与使用Tersoff势函数的情况相似,但是形成的孔洞尺度较大；(5)通过拓扑分析方法分析非晶Ge材料中形成的孔洞边缘及其附近的原子分布情况。研究表明,孔洞边缘及边缘附近位置处,拓扑环所包含的原子数目减少且环的数目增多。这表明,孔洞边缘及其附近的原子排布致密。
Molecular dynamics simulation is employed to investigate the film formation of Cu cluster deposition on Si substrate at different deposition conditions of cluster size, incident energy, substrate temperature, crystallographic orientation and deposition rate in the Part I. We have set the two schenmes of potential functions to describe the atoms interaction in the simulation system, one is that the interaction of Cu-Cu is described by EAM many-body potentials, one of Si-Si using SW many-body potentials, and one of Cu-Si using LJ two-body potentials; another is that likewise interaction of Cu-Cu using EAM many-body potentials, Tersoff many-body potentials is selected to describe the interaction of Si-Si, and the Morse two-body potentials is chosen for the interation of Cu-Si. The following is the main content of the study and results:
1、As just one Cu cluster bombards on the Si surface in the microprocess, the results are:(1)The two kinds potentatial we chosed can be better to describe the interactation of atoms in the Cu-Si system and give some information about the dynamics process of Cu cluster deposition on Si substrate;(2) Under the same initial conditions, the trend of transformation of kinetic energy between cluster of different sizes, morphologies and substrate atoms is the similar. And as the number of cluster atoms is decreased, it takes long time to finish the kinetic energy transformation between atoms;(3) As the increasing of incident energy, the degree of epitaxy of cluster atoms increased, and the mean height of mass center of cluster debased. The smaller cluster prefers to diffuse toward the XY plane, while the larger cluster trends to move along the incident orientation;(4)As the substrate temperature goes up, the degree of epitaxy of cluster atom increased. And the MHMC decased apparently for larger cluster;(5)On the Si(001)surface, it is easier to appear the Cu/Si(001) interface,whereas on the Si(111)surface, as the incident energy is3.0eV/atom for Cu13and Cu19, Cu/Si(001) interface just occurences,1.6eV/atom threshold energy for Cu147, it appears Cu/Si(001)interface.
2、As Cu atoms deposited on the Si substrate to form thin film, results are:(1) As the incident energy increases, the surface roughness decases and surface smoother.(2) As the substrate temperature goes up, deposition film becomes smoother;(3) As the deposition rate is increased, the film surface roughness increases, and above5atoms/ps, there are some voids inside or edge of deposition film. As the deposition rate is too lower (like2atoms/ps), even though the film surface is really smooth, but it will take much more time to finish film growth. So it is not the better choice in the real simulation. In our calculation, for Cu atom depositing on the Si surface, the5atoms/ps deposition rate is considered the best value to grow Cu film;(4) Under the same initial conditions, Si(111)surface is optimal; Moreover, there are some amorphous phenomenon in the interface mixing for Cu/Si(001) and Cu/Si(111);(5)The formation film maily is face-center-cubic structure, the most of them are growth Volmer-Weber model initially, then transform the FranK-vander Merwe growth model, so the main growth model is Stranski-Krastonov model.
3、As Cu clusters deposited on the Si substrate to form thin film, results are:(1) As the incident energy increases, the surface roughness of formation film decreases;(2)As the substrate temperature rises, the mixing mode of Cu/Si(001) becomes clear;(3)As the number of cluster atoms is increased, the surface roughness of formation film increases;(4) Under the same initial conditions, the film on the Si(111) become smooher than on the Si(001);(5) For the Cu cluster deposited on Si substrate, the main growth mode is the SK mode.
Molcular dynamics simulation studies the Ge irradiation-induced and the voids formation in the process in the Part II. We choose two schemes of potentials to investigate the void formation in a-Ge, seperarely. One is Tersoff-ZBL potentials, another is SW-Yukawa potentials. The following is the results:(1) The energy deposition leads to void formation;(2) The simulation results prove that the formation of the voids is mainly based on a shock wave mechanism and the swelling is determined by the competing processes of the formation and growth of voids on the one hand and the shrinking and annihilation of voids on the other hand;(3) In the case of Tersoff-ZBL potential, the void appears for the fisrt incident ion irradiation. Then continuing to irradiate substrate every other120.0ps, two voids coexist in simulation system at the different positions. The substrate happened swelling in the z direction. Because of the system size, even though the number of incident atoms increased, the positions and morphologies of forming voids always change, the number of voids does not increased;(4) In the case of the SW-Yukawa potential, there is a larger void formation.(5) By topological tool analysis, we come to conclustion that the density of atoms in our simulated system after irradiation is not uniformed, near the voids the rings sizes become smaller and the number of rings is increased. It is indicated that the density of atoms around the voids becomes bigger.
1、通过模拟计算单个Cu团簇沉积在Si衬底上的微观演化过程,研究得到：(1)两组势函数方案都能够比较准确地描述Cu-Si体系中原子间的相互作用,反映Cu团簇沉积在Si衬底上的动态演化过程；(2)在不同大小、形状团簇沉积过程中,原子间动能转化趋势基本相似。团簇越小,动能转化过程越短暂；(3)随着入射动能的增加,团簇原子的延展度增大,平均原子质心高度降低；(4)随着衬底温度的升高,团簇原子的延展度增大,较大团簇的平均原子质心高度明显下降；(5)在Si(001)衬底上,易形成Cu/Si(001)混合内界面；对于Cu13和Cu19团簇分别沉积在Si(111)衬底上,形成Cu/Si(111)混合内界面的入射动能阈值均为3.0eV/atom;对于Cu147团簇沉积在Si(111)衬底上,入射动能阈值为1.6eV/atom开始形成Cu/Si(111)混合内界面。
2、通过模拟计算单个Cu原子连续沉积在Si衬底上的成膜过程,研究得到：(1)随着入射动能的增加,沉积薄膜表面的粗糙度降低,这有利于生长高质量的薄膜；(2)随着衬底温度的升高,沉积薄膜表面的粗糙度降低；(3)当沉积率高于5atoms/ps时,沉积薄膜中会出现孔洞。当沉积率过小时,例如2atoms/ps,沉积薄膜表面比较平滑,但是计算时间大大增加。在本文的模拟计算中,选取5atoms/ps的沉积率研究Cu原子沉积在Si衬底上成膜；(4)在相同的沉积条件下,Si(111)衬底上形成薄膜的表面较Si(001)衬底上形成薄膜的表面平滑。另外,Cu/Si(001)和Cu/Si(111)的混合界面处存在不同程度的非晶化现象。(5)在不同的初始沉积条件下,形成薄膜的结构主要以FCC结构存在,并且薄膜形成起初是以“岛状”模式生长,随着沉积原子数的增多,转为“层状”模式生长。
3、通过模拟计算Cu团簇连续沉积在Si衬底上成膜过程,研究得到：(1)随着入射团簇动能的增加,成膜表面粗糙度减少；(2)随着衬底温度增加,成膜表面粗糙度减少,且Cu/Si混合内界面处原子的混合度增强；(3)随着入射团簇大小尺寸的增加,成膜表面粗糙度增加；(4)在相同衬底温度的条件下,在Si(111)表面上形成的薄膜表面较在Si(001)表面上形成的薄膜表面平滑；(5)团簇沉积成膜过程中,薄膜主要以“混合”模式生长。
本文第二部分内容是用分子动力学模拟方法研究Ge材料的辐照损伤过程,并探究孔洞形成的演化过程。研究得到：(1)能量的沉积导致孔洞形成；(2)“空位团”的形成与湮灭或孔洞的形成导致Ge材料在辐照方向上的肿胀；(3)采用Tersoff-ZBL势函数研究孔洞的演化过程,观察到第一个粒子辐照之后,一个清晰的孔洞出现,然后每隔120.0ps继续第二、三……个粒子辐照,发现模拟体系中有两个清晰孔洞共存的现象。由于模拟体系尺寸的选取,随着辐照次数的增多,形成孔洞的位置和形态总是发生变化,但是孔洞的数目没有增加；(4)采用SW-Yukawa势函数研究孔洞的形成问题。研究发现,孔洞的形成过程与使用Tersoff势函数的情况相似,但是形成的孔洞尺度较大；(5)通过拓扑分析方法分析非晶Ge材料中形成的孔洞边缘及其附近的原子分布情况。研究表明,孔洞边缘及边缘附近位置处,拓扑环所包含的原子数目减少且环的数目增多。这表明,孔洞边缘及其附近的原子排布致密。
Molecular dynamics simulation is employed to investigate the film formation of Cu cluster deposition on Si substrate at different deposition conditions of cluster size, incident energy, substrate temperature, crystallographic orientation and deposition rate in the Part I. We have set the two schenmes of potential functions to describe the atoms interaction in the simulation system, one is that the interaction of Cu-Cu is described by EAM many-body potentials, one of Si-Si using SW many-body potentials, and one of Cu-Si using LJ two-body potentials; another is that likewise interaction of Cu-Cu using EAM many-body potentials, Tersoff many-body potentials is selected to describe the interaction of Si-Si, and the Morse two-body potentials is chosen for the interation of Cu-Si. The following is the main content of the study and results:
1、As just one Cu cluster bombards on the Si surface in the microprocess, the results are:(1)The two kinds potentatial we chosed can be better to describe the interactation of atoms in the Cu-Si system and give some information about the dynamics process of Cu cluster deposition on Si substrate;(2) Under the same initial conditions, the trend of transformation of kinetic energy between cluster of different sizes, morphologies and substrate atoms is the similar. And as the number of cluster atoms is decreased, it takes long time to finish the kinetic energy transformation between atoms;(3) As the increasing of incident energy, the degree of epitaxy of cluster atoms increased, and the mean height of mass center of cluster debased. The smaller cluster prefers to diffuse toward the XY plane, while the larger cluster trends to move along the incident orientation;(4)As the substrate temperature goes up, the degree of epitaxy of cluster atom increased. And the MHMC decased apparently for larger cluster;(5)On the Si(001)surface, it is easier to appear the Cu/Si(001) interface,whereas on the Si(111)surface, as the incident energy is3.0eV/atom for Cu13and Cu19, Cu/Si(001) interface just occurences,1.6eV/atom threshold energy for Cu147, it appears Cu/Si(001)interface.
2、As Cu atoms deposited on the Si substrate to form thin film, results are:(1) As the incident energy increases, the surface roughness decases and surface smoother.(2) As the substrate temperature goes up, deposition film becomes smoother;(3) As the deposition rate is increased, the film surface roughness increases, and above5atoms/ps, there are some voids inside or edge of deposition film. As the deposition rate is too lower (like2atoms/ps), even though the film surface is really smooth, but it will take much more time to finish film growth. So it is not the better choice in the real simulation. In our calculation, for Cu atom depositing on the Si surface, the5atoms/ps deposition rate is considered the best value to grow Cu film;(4) Under the same initial conditions, Si(111)surface is optimal; Moreover, there are some amorphous phenomenon in the interface mixing for Cu/Si(001) and Cu/Si(111);(5)The formation film maily is face-center-cubic structure, the most of them are growth Volmer-Weber model initially, then transform the FranK-vander Merwe growth model, so the main growth model is Stranski-Krastonov model.
3、As Cu clusters deposited on the Si substrate to form thin film, results are:(1) As the incident energy increases, the surface roughness of formation film decreases;(2)As the substrate temperature rises, the mixing mode of Cu/Si(001) becomes clear;(3)As the number of cluster atoms is increased, the surface roughness of formation film increases;(4) Under the same initial conditions, the film on the Si(111) become smooher than on the Si(001);(5) For the Cu cluster deposited on Si substrate, the main growth mode is the SK mode.
Molcular dynamics simulation studies the Ge irradiation-induced and the voids formation in the process in the Part II. We choose two schemes of potentials to investigate the void formation in a-Ge, seperarely. One is Tersoff-ZBL potentials, another is SW-Yukawa potentials. The following is the results:(1) The energy deposition leads to void formation;(2) The simulation results prove that the formation of the voids is mainly based on a shock wave mechanism and the swelling is determined by the competing processes of the formation and growth of voids on the one hand and the shrinking and annihilation of voids on the other hand;(3) In the case of Tersoff-ZBL potential, the void appears for the fisrt incident ion irradiation. Then continuing to irradiate substrate every other120.0ps, two voids coexist in simulation system at the different positions. The substrate happened swelling in the z direction. Because of the system size, even though the number of incident atoms increased, the positions and morphologies of forming voids always change, the number of voids does not increased;(4) In the case of the SW-Yukawa potential, there is a larger void formation.(5) By topological tool analysis, we come to conclustion that the density of atoms in our simulated system after irradiation is not uniformed, near the voids the rings sizes become smaller and the number of rings is increased. It is indicated that the density of atoms around the voids becomes bigger.
引文
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