CN101418438B - 通过来自乙硅烷前体的远程等离子体cvd的高质量氧化硅膜 - Google Patents

通过来自乙硅烷前体的远程等离子体cvd的高质量氧化硅膜 Download PDF

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CN101418438B
CN101418438B CN2008101711607A CN200810171160A CN101418438B CN 101418438 B CN101418438 B CN 101418438B CN 2008101711607 A CN2008101711607 A CN 2008101711607A CN 200810171160 A CN200810171160 A CN 200810171160A CN 101418438 B CN101418438 B CN 101418438B
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阿布海杰特·巴苏·马利克
斯里尼瓦斯·D·内曼尼
叶怡利
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Abstract

本发明提供了一种在基板上沉积含硅和氮的膜的方法。所述方法包括将含硅前体引入到包含基板的沉积室中，其中含硅前体包括至少两个硅原子。所述方法还包括通过远程等离子体系统产生至少一种自由基氮前体，所述远程等离子体系统设置在沉积室外部。而且，所述方法包括将自由基氮前体引入到沉积室中，在所述沉积室中自由基氮和含硅前体反应且在基板上沉积含硅和氮的膜。而且，所述方法包括在蒸汽气氛中退火含硅和氮的膜以形成氧化硅膜，其中蒸汽气氛包括水和酸性蒸汽。

Description

通过来自乙硅烷前体的远程等离子体CVD的高质量氧化硅膜
相关申请的交叉引用
本申请涉及到2006年5月30日提交的名称为“CHEMICAL VAPORDEPOSITION OF HIGH QUALITY FLOW-LIKE SILICON DIOXIDE USING ASILICON CONTANTING PRECURSOR AND ATOMIC OXYGEN”的、Ingle等人共同转让的美国专利申请第60/803,493号。所述申请还涉及到也是在2007年10月22日提交的名称为“METHOD AND SYSTEM FOR IMPROVINGDIELECTRIC FILM QUALITY FOR VOID FREE GAP FILL”的、Mallick等人共同转让的代理卷号为A11125/T79600的美国专利申请。在此引入两件相关申请的整体内容作为参考。
技术领域
本发明一般涉及用于制造半导体器件的形成氧化硅膜的方法，尤其涉及通过来自乙硅烷前体的远程等离子体CVD的高质量氧化硅膜。
背景技术
诸如浅沟槽隔离结构(STI)的间隙和沟槽通常被用于对半导体器件上的元件进行电隔离。STI可包括形成在半导体基板隔离区域中的沟槽或间隙，用介电材料对所述沟槽或间隙进行填充以防止附近器件结构(例如晶体管、二极管等)的电耦合。随着集成电路上的器件密度持续增加，在器件结构之间的尺寸和距离也持续降低。但是，STI沟槽的垂直高度通常不会与STI沟槽水平宽度一样快地降低，这导致间隙和沟槽具有较大的高宽比(即较高的纵横比)。
虽然使得器件结构具有增加的纵横比的能力允许更多结构(例如晶体管、电容器、二极管等)被封装到半导体芯片基板相同表面积上，但是这也产生了制造问题。这些问题中的一个是在填充工艺期间难以完全填充这些结构中的间隙和沟槽而不产生孔洞或缝隙(seam)。必须用介电材料诸如氧化硅填充间隙和沟槽从而对附近的器件结构进行相互电隔离以使电噪声和漏电流最小。随着纵横比的增加，更加难以填充深的狭窄沟槽而不在填充沟槽的介电材料中产生孔洞或缝隙。
在介电层中的孔洞和缝隙在半导体器件制造期间和完成的器件中都会引起问题。孔洞和缝隙在介电材料中随机形成且具有不可预知的尺寸、形状、位置和密度。这会导致不可预知的且不一致的层的后沉积处理，诸如不均匀的蚀刻、抛光、退火等。完成的器件中的孔洞和缝隙也在器件结构中的间隙和沟槽的介电质量方面产生变化。其他问题当中，这会导致由于电串扰、电荷泄漏以及一些情况下由于器件中的短路引起的错误的或劣质的器件性能。
已经开发出使在高纵横比结构上沉积介电材料期间形成的孔洞和缝隙最小化的技术。这些技术包括减慢介电材料的沉积速度以便介电材料在沟槽的侧壁和底部上保持得更加共形。更加共形的沉积能降低在沟槽顶部上的材料堆积和介电材料过早封堵沟槽顶部以形成孔洞的机会(这个问题有时被称作“breadloafing(面包块)”)。但是，不幸的是，减慢沉积速度也意味着增加沉积时间，这降低了处理效率以及产率。
控制孔洞形成的另一种技术是增加所沉积介电材料的可流动。具有更大可流动的材料能够更快速地填充孔洞或缝隙并防止所述孔洞或缝隙变成填充容积内的永久缺陷。例如，通常采用高度可流动的旋涂玻璃(SOG)前体诸如PSZ膜、SAM24、BTBAS等以良好的共形性填充沟槽。但是，通过这种常规SOG膜增加氧化硅介电材料的可流动性通常导致由于剩余碳和硅烷醇基团引起的所沉积的膜具有低的膜密度。增加膜密度的一种手段是当固化SOG膜成为氧化硅膜时使用高温退火。但是，用于去除剩余碳和OH基团的高温退火也会引起相当大程度的膜体积收缩。在用于STI应用的狭窄沟槽中，所沉积的膜受到限制且不稳定收缩，从而导致包含具有多孔或含孔洞结构的低密度膜。
由此，仍需要用于增加沟槽、间隙和具有高纵横比的其他器件结构中的介电膜密度以实现无孔间隙填充的改进工艺。仍需要对于能够以高速度和良好可流动特性沉积介电材料而不会不利地影响完成的间隙填充的质量的介电沉积工艺。本发明针对介电膜沉积的这些和其他方面。
发明内容
本发明涉及一种用于制造半导体器件的形成氧化硅膜的方法。实施例包括形成可流动介电膜的方法，所述方法包括化学气相沉积(CVD)由硅前体形成的Si-N(H)-Si键，所述硅前体具有一个或多个Si-Si键，所述硅前体与在远程等离子体中产生的自由基氮前体(例如-N、-NH、-NH2)反应。所沉积的膜被固化以将Si-N(H)-Si基团转换成氧化硅(例如Si-O-Si)，从而在后沉积退火(例如蒸汽退火)期间增加膜的致密度。所述方法能用于形成用于STI(浅沟槽隔离)结构的高质量氧化硅膜，但是将意识到，所述方法具有较宽的应用。
实施例还包括在基板上沉积含硅和氮的膜的方法。所述方法包括将含硅前体引入到含有基板的沉积室的步骤。含硅前体至少包括两个硅原子。所述方法还包括使用远程等离子体系统产生至少-个自由基氮前体，所述远程等离子体系统位于沉积室外部。此外，所述方法还包括将自由基氮前体引入到沉积室中，在所述沉积室中自由基氮和含硅前体反应且在基板上沉积含硅和氮的膜。
实施例还包括在基板上形成氧化硅膜的方法。所述方法包括在沉积室中提供基板和用远程等离子体系统产生激活的氮物种(例如氮氢自由基)，所述远程等离子体系统耦合到沉积室。此外，所述方法包括将含硅前体引入到沉积室中。含硅前体至少包括Si-Si键。所述方法还包括将激活的氮物种引入到沉积室中，这里，激活的氮物种与含硅前体反应且在基板上沉积第一层膜。所述第一层膜包括多个Si-N(H)-Si键。而且，所述方法包括在蒸汽气氛中退火第一层膜和在基板上形成第二层膜。所述第二层膜包括多个Si-O-Si键。
在以下的描述出列出了其他实施例和特征，且通过考察说明书本领域技术人员将明白部分所述描述或者通过实践本发明可学习到部分所述描述。可借助于说明书中描述的手段、组合和方法实现和获得本发明的特征和优点。
附图的简要描述
图1示意性示出了根据本发明实施例在硅前体中的Si-Si键与反应氮物种反应以形成含Si-N(H)-Si的组合物、和之后将所述组合物氧化成含Si-O-Si组合物的化学反应过程；
图2是示出根据本发明实施例在基板上形成氧化硅膜的方法的简化流程图；
图3示意性示出了根据本发明实施例用于由乙硅烷或聚硅烷前体以及通过在远程等离子体中分解氨产生的自由基氮前体形成碳氮化硅Si:C:N:H的化学反应步骤；
图4是根据本发明实施例沉积可流动性的含硅和氮的膜的方法的简化流程图；
图5示意性示出了根据本发明实施例用于酸催化去除沉积的介电膜中的碳基物种的化学反应机理；
图6A至图6B示出了根据本发明实施例用于碱催化去除在如此沉积的介电膜中的碳基物种的化学反应机理；和
图7示出了根据本发明实施例用于在基板上形成氧化硅膜的示范性工艺系统的截面图。
具体实施方式
本发明涉及一种用于制造半导体器件的形成氧化硅膜的方法。实施例包括形成可流动介电膜的化学气相沉积方法，所述可流动介电膜包括Si-N(H)-Si键，所述Si-N(H)-Si键来自具有一个或多个Si-Si键的硅前体与在远程等离子体中形成的自由基氮前体(例如，-N、-NH，-NH2)的反应。所述方法还包括通过后沉积退火(例如蒸汽退火)固化可流动介电膜以将Si-N(H)-Si键转换成更加致密的Si-O-Si键。在其他应用当中，所述方法可用于形成高质量氧化硅间隙填充(例如形成STI结构)。
图1示意性示出了根据本发明实施例将硅前体中的Si-Si键转换成Si-N(H)-Si键之后膨胀地转换成Si-O-Si键的化学反应过程。这个图仅仅是实例，这不应过度地限制此处权利要求的范围。本领域技术人员会意识到其他变化、改进和替换方式。如所示出的，化学反应是CVD(化学气相沉积)工艺，在CVD工艺期间具有至少一个Si-Si键的含硅前体与自由基氮混合，所述自由基氮由远程等离子体(例如，与可流动Si-N(H)-Si膜的沉积分离地形成的等离子体)的分解产生。所述CVD工艺导致一个硅前体(或多个前体)中的Si-Si键转换成Si-N(H)-Si键。此时在随后的退火步骤中将Si-N(H)-Si键转换成Si-O-Si键，进行退火的环境是蒸汽(例如H2O蒸汽)环境。由于氧原子具有比氮原子更大的原子体积，因此在退火期间形成氧化硅会导致介电膜的膨胀。
上述CVD工艺包括将至少两种反应物单独引入到沉积室中，且使它们在预定条件下反应。在一个实施例中，第一反应物可以是选自由烷氧基乙硅烷、烷氧基-烷基乙硅烷、烷氧基-乙酰氧基乙硅烷和聚硅烷构成的组的一种前体。例如，烷氧基乙硅烷包括Si2(EtO)6乙氧基乙硅烷、Si2(MeO)6甲氧基乙硅烷、和Si6(MeO)12甲氧基环己硅烷，这里Et表示乙基(C2H6)以及Me表示甲基(CH3)。在另一实例中，烷氧基-烷基乙硅烷包括Si2(EtO)4(Me)2四乙氧基二甲基乙硅烷、Si2(EtO)4(Et)2四乙氧基二乙基乙硅烷、Si2(EtO)2(Me)4二乙氧基四甲基乙硅烷、Si2(MeO)4(Me)2四甲氧基二甲基乙硅烷、和Si4O2(Me)8甲基环己硅氧烷、Si6(MeO)6(Me)6甲氧基-甲基环己基硅烷、Si4O2(H2)4氢化-环己硅氧烷。在再一实例中，烷氧基-乙酰氧基乙硅烷包括Si2(AcO)6乙酰氧基乙硅烷、Si2(Me)4(AcO)2四甲基二乙酰氧基乙硅烷、和Si2(Me)2(AcO)4二甲基四乙酰氧基乙硅烷，这里，Ac表示乙酰氧基。和在再一实例中，聚硅烷包括环戊硅烷或其他替代物。在不遇到用于CVD工艺的任何其他反应物的情况下，上述这些前体中的任一种都可提供到沉积室中。
在另一实施例中，用于上述CVD工艺的其他反应物是第二反应物，所述第二反应物包括由远程氨等离子体产生的自由基氮物种。例如，自由基氮物种可包括氮离子、氮氢自由基NHx，这里x＝1或2。由于在这些以硅烷或聚硅烷基前体的分子结构中存在至少一个高度反应性的Si-Si键，因此，CVD工艺会导致含有多个Si-N(H)-Si键的产物，还含有氢氧基和碳基物种。例如，产物是沉积在基板上的碳氮化硅膜。由于存在这些氢氧基和碳基物种，因此CVD沉积的碳氮化硅膜是非晶的且是可流动的。
在再一实施例中，在水蒸汽环境中随后的热处理引起碳氮化硅膜和H2O蒸汽之间的另一化学反应。所述反应是氧化过程，在所述氧化过程中，在碳氮化硅膜中的Si-N(H)-Si键被转换成Si-O-Si键，导致形成氧化硅膜。一种副产物包括NH3氨，所述NH3氨能通过对于室建立的排气系统立即泵出。
图2是示出根据本发明实施例在基板上形成氧化硅膜的方法的简化流程图。如所示出的，所述方法200利用图1中所描述的化学反应过程以形成氧化硅膜。示范性方法200包括非排它性的一系列步骤，可向所述一系列步骤添加附加步骤(未示出)。本领域技术人员会意识到很多变化、改进和替换方式。在所示出的实施例中，方法200包括在沉积室中提供基板(210)。所述方法200还包括将一种或多种含硅前体引入到沉积室中(220)，所述含硅前体在分子结构中具有至少一个Si-Si键。所述方法还包括产生一种或多种自由基氮前体(230)。例如，一种或多种自由基氮前体在耦合到沉积室的远程氨等离子体系统中产生。
所述方法200还包括将一种或多种自由基氮前体引入到沉积室中以与一种或多种含硅前体反应(240)，引起具有Si-N(H)-Si键的可流动性介电膜在基板上的沉积。此外，方法200可包括蒸汽退火以将CVD沉积的可流动性介电膜氧化成氧化硅膜(250)。所述蒸汽氧化工艺(250)可包括由于将Si-N(H)-Si键转换成Si-O-Si键导致的膜膨胀，这与由于从CVD沉积的膜去除了一些氢氧基而导致的膜收缩相抵消。结果，平衡膜膨胀和收缩导致了致密的、无孔的氧化硅膜，所述致密的、无孔的氧化硅膜也降低了由于在沉积和退火期间引入了应力而导致破裂的可能性。
在一个实施例中，用于CVD工艺的一种或多种含硅前体包括在分子结构中的多个氢氧基。氢氧基保持在CVD沉积的膜中，提供与常规SOG(旋涂玻璃)膜相似的膜的流动特性。由于流动特性，基于方法200的CVD沉积膜在沉积期间易于聚集在基板间隙或沟槽底部部分中，由此减少了在间隙填充或STI沟槽中心附近产生的孔。在另一实施例中，在分子结构中具有至少一个Si-Si键的一种或多种含硅前体包括乙硅烷和/或聚硅烷前体。乙硅烷在分子结构中具有单个的Si-Si单元，而聚硅烷具有多个Si-Si键。例如，使用具有不同取代基的乙硅烷，所述乙硅烷包括烷氧基乙硅烷、烷氧基-烷基乙硅烷和烷氧基-醋酸基乙硅烷。在其他实例中，也可使用具有更高同系物的乙硅烷。当然，本领域技术人员会意识到在选择乙硅烷和聚硅烷前体时的很多替换方式、变化和改进。
上述的CVD沉积工艺与2006年5月30日提交的名称为“CHEMICALVAPOR DEPOSITION OF HIGH QUALITY FLOW-LIKE SILICON DIOXIDEUSING A SILICON CONTANTING PRECURSOR AND ATOMIC OXYGEN”的、Ingle等人共同转让的美国专利申请第60/803,493号中描述的工艺相似，在此引入所述美国专利申请整体内容作为参考。但是，在方法200中，使用由氨的等离子体分解产生的自由基氮代替原子氧，以与一种或多种含硅前体反应，从而由于存在氢氧基(例如硅烷醇基)而导致具有流动特性的含硅和氮的膜。
如上所述，在方法200中使用的反应物种(例如-N、-NH、-NH2)可通过在远程等离子体系统中引入氨(NH3)产生。远程等离子体系统可包括耦合到沉积室的分离的室。用于将氨分解成NH/N/H自由基的等离子体条件包括：使用3kW至15kW范围内的RF功率以在从1Torr(托)至10托范围内的室压下、在室温至约200℃范围内的温度室温度下产生等离子体。在远程等离子体系统中分解氨产生自由基氮前体，诸如氮氢自由基诸如NH或NH2。也可产生原子氢(H)自由基。例如，氮氢和氢自由基在方法200的步骤230中产生。自由基氮前体此时被传送到沉积室，所述室中已经单独引入了一种或多种含硅前体。例如，反应氮前体可通过喷头传送，而硅前体通过多个带槽的管子引入。
图3示意性示出了根据本发明实施例用于由乙硅烷和/或聚硅烷前体与通过氨远程等离子体产生的自由基氮前体的反应形成碳氮化硅(Si:C:N:H)膜的化学反应步骤。图3是一个示意性实例且不应过度限制此处权利要求的范围。本领域技术人员将意识到其他变化、改进和替换方式。
如所示出的，氮氢NH自由基和氢H自由基在工艺310中通过氨等离子体产生。当氮氢NH自由基和氢H自由基在沉积室中遇到乙硅烷或聚硅烷前体时，乙硅烷或聚硅烷前体中高度反应的Si-Si键通常会分裂以形成与-NH2重新键合的硅-氢氧自由基，如图3的反应过程320中所示的。可选地，乙硅烷或聚硅烷前体中的Si-Si键会破裂以形成直接与-H重新键合的硅-氢氧自由基，如图3中一侧的过程325中所示的。当然，本领域技术人员将意识到很多种替换方式、变化和改进。
在所示出的实例中，与-NH2自由基键合的硅-氢氧基可通过释放醇基分解成硅-氮氢自由基。例如，在最初的含硅前体中的氢氧基捕获键合到氮原子的H原子以形成甲醇(CH3OH)，如图3的过程330中所示的。所产生的所述甲醇能通过真空泵容易地去除从而促进形成另外的甲醇。反应物的剩余部分变成包含具有两个悬键(dangling bond)的Si-NH键的自由基。随后，两个悬键快速地重新键合以形成具有Si＝NH双键的二甲基硅烷亚胺自由基，如图3的过程340中所示的。当然，本领域技术人员将意识到很多替换方式、变化和改进。
在另一实施例中，化学反应进一步包括在存在于含硅前体中的Si-C键和二甲基硅烷亚胺自由基之间的反应。如图3的过程350中所示，反应是键插入过程，在所述键插入过程中二甲基硅烷亚胺自由基直接插入到Si原子和C原子之间以产生碳氮化硅产物。当然，本领域技术人员将意识到很多替换方式、变化和改进。
图4是示出根据本发明实施例沉积可流动的含硅和氮的膜的方法的简化流程图。所述图仅仅是实例且不应当过度限制此处的权利要求的范围。本领域技术人员将意识到其他变化、改进和替换方式。如所示出的，方法400是CVD工艺，用于在基板上沉积具有流动特性的非晶碳氮化硅膜。方法400包括在沉积室中提供基板(410)。沉积室耦合到远程等离子体系统。所述方法400也可包括将氨引入到远程等离子体系统中以由远程等离子体中氨的分解产生自由基氮前体。所产生的自由基氮前体可包括氮氢NH自由基和氢H自由基。当然，存在其他的替换方式、变化和改进。
此外，方法400包括将氮氢NH自由基和氢H自由基传送到沉积室中(420)。在一个实施例中，氮氢NH自由基和氢H自由基通过喷头被传送，所述喷头流体地耦合沉积室和远程等离子体系统。例如，反应氮自由基(和伴随载气)可通过挡板或喷头进入到沉积室，所述挡板或喷头诸如在2007年5月29日提交的名称为“PROCESS CHAMBER FOR DIELECTRIC GAPFILL”的、Lubomirsky等人共同转让的美国专利申请序列号11/754,924中示出的那种，在此引入所述美国专利申请全部内容作为参考。
方法400还包括将具有至少一个Si-Si键的一种或多种含硅前体引入到沉积室中(430)。在一个实施例中，含硅前体被单独导向到沉积室中。例如，这些前体来自一个或多个分离的CVD气体源，且在被引入到沉积室之前不会遇到任何的氨等离子体。在另一实施例中，含硅前体包括在分子结构中具有单个Si-Si单元的乙硅烷和/或具有多个Si-Si单元的聚硅烷。例如，含硅前体是具有如图3中所示的乙基羟基的乙硅烷。
方法400还包括实施CVD工艺以在沉积室中的基板上沉积可流动碳氮化硅膜(440)。由于含硅前体在沉积室中遇到氮氢NH自由基和氢H自由基，因此在前体中的Si-Si键高度反应以使得具有Si-Si键的乙硅烷或聚硅烷前体破裂成硅-氮氢自由基。而且，在甲醇分解和重新键合反应过程中，硅-氮氢自由基会转变成二甲基硅烷亚胺自由基。二甲基硅烷亚胺自由基此时通过键插入过程与前体中的Si-C键反应以形成碳氮化硅分子。
例如在沉积室中在以下处理条件下进行CVD工艺440：1)前体流速被设置为1mgm/分钟至15gm/分钟；2)将沉积室保持在约1m托至约600托范围内的压力下；3)室温被控制在约0℃至约400℃之间。形成硅-氮氢自由基在图3的过程320期间发生。包括在上述CVD工艺440中的其他化学反应过程可包括图3中示出的反应步骤330、340或350。获得的碳氮化硅分子此时沉积在基板上以形成固体膜。所述膜实质上是非晶的且通过在分子结构中的氢氧基而具有流动特性。
可流动的沉积膜形成了具有很低密度的无孔间隙填充，用于器件的介电隔离。方法400还包括在氧化环境中退火可流动碳氮化硅膜以形成致密度氧化硅膜(450)。与其他可流动介电膜相似，诸如常规的SOG膜，高温退火引起氢氧基和剩余的碳分解成被立即泵出的水和/或甲醇蒸气，导致明显的膜收缩和致密化。在特定实施例中，退火工艺450是在蒸汽(水蒸汽)气氛内在氧化环境中的热退火。例如，在从约200℃至高达约1050℃的基板温度下进行蒸汽退火。在退火期间的水蒸气压力约在从1托至1atm(即约760托)的范围内。
在替换实施例中，退火工艺450是将基板保持在室温至高达约600℃下的臭氧处理。臭氧处理可进一步与UV光照射结合。在另一替换实施例中，退火工艺450是包括从室温至约900℃的分子氧处理或从室温至高达约600℃的原子氧处理的膜固化处理。当然，本领域技术人员将意识到很多替换方式、变化和改进。
在另一特定实施例中，由于存在形成于如此沉积的碳氮化硅膜中的Si-N(H)-Si键，氧化工艺450将引起这些Si-N(H)-Si键向Si-O-Si键的转换。由于氧比氮大的原子体积，所述转换固有地膨胀了所述膜。例如，键转换过程与图1中描述的化学反应过程相同。所述膜膨胀抵消了由于未反应的碳和OH物种的损失导致的膜收缩。平衡膜膨胀和收缩的净效果导致较高质量的氧化硅膜，所述氧化硅膜具有较少整体收缩，但是具有增加的膜密度，同时保持无孔间隙填充。
在另一实施例中，退火可流动碳氮化硅膜在包括水蒸气和酸性蒸汽的气氛中进行。由于CVD沉积膜包括烷氧基取代的乙硅烷，因此酸性环境在沉积期间有助于催化未反应有机部分的反应。图5示意性示出了根据本发明实施例酸性催化剂处理沉积的介电膜的化学绘图(chemical drawing)。所述图仅是实例且不应当过度限制此处权利要求的范围。本领域技术人员将意识到其他变化、改进和替换方式。如所示出的，通过在退火期间添加的酸性蒸汽，未反应的氢氧基经历酸的亲电子攻击，即通过从氧原子取一个电子到氢原子，来自酸的H+离子会将未反应的CH3O基团转换成反应性的CH3OH基团。这在图5的过程510中示出。
此时水蒸气与反应性的CH3OH基团反应，如过程520中所示。反应导致形成硅烷醇Si-OH基团且从膜中释放了甲醇CH3OH分子。所形成的硅烷醇Si-OH基团的缩合(即，两个硅烷醇Si-OH基团结合而释放出水)导致在膜中形成氧化硅结构。在一个实施例中，用酸处理退火有助于通过去除碳物种而增加膜密度且经由其他方式通过氢氧基的损失有助于降低孔洞形成的可能性。当然，存在其他替换方式、变形和改进。
在其他实施例中，退火可流动碳氮化硅膜在包括水蒸气和碱蒸汽诸如氨(NH3)的气氛中进行。由于CVD沉积膜包括烷氧基取代的乙硅烷，因此碱性环境有助于在沉积期间催化未反应有机部分的反应。
图6A至图6B示意性示出了用于所沉积介电膜碱性催化处理的两个化学反应机理。于图6A中示出的第一个机理包括通过包括氨的碱性蒸汽进行的烷基的亲核攻击。这种机理中，硅烷氧基的烷基部分传送给氨，在传送期间所述烷基部分也释放质子(H+)。由于烷基的传送也包括水分子，因此水分子贡献出质子以取代离开的所述烷基，并且形成硅烷醇(-Si-OH)基。在随后的反应中，会发生硅烷醇缩合反应以在固化的介电氧化膜中将-Si-OH基转换成-Si-O-Si-基。
在图6B中示出的第二个反应机理包括通过包括氨的碱性蒸汽在硅烷氧中的硅原子的亲核攻击。反应包括用氨分子取代贴附到硅的烷氧基以形成硅烷基胺。烷氧基与从水分子贡献出的质子反应以形成醇类。在随后的反应中，硅烷基胺可被水解以形成硅烷醇并重新产生氨。此时，与图6A中描述的机理相似，硅烷醇基团进行缩合反应，在固化的介电氧化膜中将-Si-OH基转换成-Si-O-Si基。
应当理解，在图6A至图6B中描述的碱性催化反应原理仅是可能的反应机理中的两个实例，且不应过度地限制此处权利要求的范围。本领域技术人员将意识到其他变化、改进和替换方式，用于如此沉积的硅烷氧物种的碱性催化处理。
用于从可流动有机硅膜碱性催化去除碳(诸如烷基和烷氧基)示范性处理条件可包括在包括水和碱性蒸汽的环境中膜的后沉积固化。例如，如果碱性蒸汽包括氨作为碱性催化剂，则所沉积的膜可被加热至约300℃同时被暴露到压力为约1托至约40托的潮湿氨气氛中达约2至约5分钟。在另外的实施例中，氨气氛也可包括氧(O2)气和/或由氮前体(例如NH3)的远程等离子体离解产生的原子氮(N)。
现在参考图7，示出了根据本发明实施例的示范性处理系统700的截面图。系统700包括沉积室701，在在所述沉积室701中前体化学反应且在基板晶片702上沉积可流动介电膜。晶片702(例如200mm、300mm、400mm等直径的半导体基板晶片)可耦合到可旋转基板底座704上，所述底座可被垂直传送以将基板702定位成更接近或更远离上方的前体分配系统706。基座可以以约1rpm至约2000rpm(例如约10rpm至约120rpm)的旋转速度旋转基板晶片。基座可以以例如从约0.5mm至约100mm的距离从前体分配系统的侧面管子708垂直传送基板。
前体分配系统706包括多个径向分布侧面管子708，所述多个径向分布侧面管子708每一个都具有两个不同长度中的一个。在另外的实施例(未示出)中，可去掉侧面管子以留下在沉积室的壁附近分布的开口环。前体通过这些开口流入到室中。
分配系统706也包括圆锥形顶部挡板710，所述圆锥形顶部挡板710与基板底座704中心共轴。流体通路712可通过挡板710中心延伸以提供前体或载气，所述前体或载气具有与向下流到挡板导向表面外部的前体不同的成分。
挡板710外部表面可被管道714包围，所述管道714从被反应物种产生系统(未示出)导向反应前体，所述反应物种产生系统设置在沉积室701上方。导管714可以是直线圆形管，所述直线圆形管具有在挡板710外部表面上打开的一端和耦合到反应物种产生系统的相对一端。
反应物种产生系统可以是远程等离子体产生系统(RPS)，所述远程等离子体产生系统(RPS)通过将更稳定的起始材料暴露到等离子体产生反应物种。例如，起始材料可以是包括分子氧(或臭氧)的混合物。所述起始材料从RPS暴露到等离子体引起一部分分子氧分离成原子氧、将在较低温度下(例如低于100℃)与有机硅前体(例如四甲基原硅酸酯(TMOS)，八甲基环四硅氧烷(OMCTS))化学反应的高度反应自由基物种，以在基板表面上形成可流动介电膜。由于在反应物种产生系统中产生的反应物种通常即使在室温下也可与其他沉积前体高度反应，因此在隔离的气体混合物中向下游导管714传输并在与其他沉积前体混合之前通过挡板710将所述反应物种分配到反应室701中。
系统700也可包括RF线圈(未示出)，所述RF线圈缠绕在沉积室701的圆顶716周围。这些线圈能在沉积室701中产生电感耦合等离子体以进一步增强反应物种前体和其他前体的反应性从而在基板上沉积流体介电膜。例如，含有通过挡板710分配到室中的反应原子氧和自通路712和/或一个或多个侧面管子708的有机硅前体的气流可通过RF线圈导向到形成在基板702上方的等离子体中。原子氧和有机硅前体甚至在低温下也能在等离子体中快速反应以在基板表面上形成高度可流动的介电膜。
基板表面自身也可通过底座704旋转以增强所沉积膜的均匀性。旋转平面与晶片沉积表面平行，或者两个平面部分地不对准。当平面不对准时，基板704的旋转会产生摇摆，这会产生沉积表面上方空间内的流体扰动。在一些情况下，这种扰动也会增强沉积在基板表面上的介电膜的均匀性。基座704也包括产生真空吸附的凹槽和/或其他结构，从而当晶片移动时将晶片保持在底座上适当位置处。典型的室内沉积压力是从约0.05托至约200托范围内的总室压(例如1托)，这使得真空吸附以保持晶片在适当位置是可行的。
底座旋转可通过设置在沉积室701下方的发动机718激励且所述发动机718可旋转耦合到轴720，所述轴720支撑底座704。轴720也包括内部通路(未示出)，所述内部通路运载自沉积室(未示出)下方的冷却/加热系统的冷却流体和/或电线至底座704。这些通路可从底座中心向外围延伸以提供对上方基板晶片702的均匀冷却和/或加热。这些通路也被设计成当轴720和基板底座704旋转和/或传送时进行操作。例如，可操作冷却系统以当底座旋转时在沉积可流动氧化膜期间保持基板晶片702的温度低于100℃。
系统700还包括设置在圆顶716上方的照射系统722。自照明系统722的灯(未示出)可照射下方的基板702以烘焙或退火基板上的所沉积膜。在沉积期间灯也可被激励以增强膜前体或所沉积膜中的反应。至少圆顶716的顶部部分由能传输从灯发出的一部分光的半透明材料制成。
这里，提供了值的范围，应当明白，对于下限单位的十分之一，除了上下文清楚说明，也特别公开了上限和下限范围之间的每一个插入值。所述范围内的任何所述值或者插入值和在所述范围内的任何其他所述的或插入的值之间的每个较小范围都包括在本发明中。这些较小范围的上限和下限在所述范围内是单独地包括或排除的，且其中两个极限中的任一个、任一个都不、或两个都包括在较小范围内的每个范围也包括在本发明内，以所述范围内任何特别排除范围为依据。这里所述的范围包括一个或两个极限，排除了这些所包括极限中的任一个或两个的范围也包括在本发明中。
如在此以及在所附的权利要求中所使用的，单数形式的“一个”和“那个”包括复数参考，除非上下文清楚另外说明。由此，例如，参考“一个工艺”包括多个这种工艺且参考“那个管子”包括参考一种或多种管子以及本领域技术人员熟知的管子的等价物，等等。
而且，词语“包括”、“包括有”、“含有”、“具有”和“包含”，当用在该说明书以及下面的权利要求中时旨在指定存在所述特征、整体、部件或步骤，但是不排除存在或附加一个或多个其他部件、整体、部件、步骤、动作或组合。

Claims (26)

1.一种在基板上沉积含硅和氮的膜的方法，所述方法包括：
引入含硅前体到沉积室中，所述沉积室含有所述基板，其中所述含硅前体包括至少两个硅原子；
通过远程等离子体系统产生至少一种自由基氮前体，所述远程等离子体系统设置在所述沉积室的外部；和
引入所述自由基氮前体到所述沉积室中，其中所述自由基氮和所述含硅前体反应且在所述基板上沉积所述含硅和氮的膜，并且其中所述含硅和氮的膜是通过化学气相沉积工艺而沉积的，并且化学气相沉积所沉积的所述含硅和氮的膜是可流动的。
2.如权利要求1所述的方法，其中产生原子氮包括将氨暴露到在所述远程等离子体系统中的等离子体，其中至少一部分所述氨分解为所述自由基氮前体。
3.如权利要求1所述的方法，其中所述自由基氮前体具有化学式NHx，这里x是0、1或2。
4.如权利要求1所述的方法，其中所述含硅前体包括乙硅烷前体或聚硅烷前体。
5.如权利要求1所述的方法，其中所述含硅前体选自由烷氧基乙硅烷、烷氧基-烷基乙硅烷和聚硅烷构成的组。
6.如权利要求1所述的方法，其中所述含硅和氮的膜包括碳氮化硅膜。
7.如权利要求1所述的方法，其中所述含硅和氮的膜包括含Si-N(H)-Si键的膜。
8.如权利要求1所述的方法，其中所述方法还包括对所述含硅和氮的膜进行退火以形成氧化硅膜。
9.如权利要求8所述的方法，其中在包括蒸汽的气氛中执行所述退火。
10.如权利要求8所述的方法，其中在包括酸性蒸汽的气氛中执行所述退火。
11.如权利要求8所述的方法，其中在从20℃至900℃范围内的温度下执行所述退火。
12.如权利要求8所述的方法，其中在包括臭氧的气氛中执行所述退火。
13.如权利要求12所述的方法，其中所述退火还包括在从20℃至600℃范围内的温度下将所述基板暴露到紫外光。
14.如权利要求8所述的方法，其中在包括分子氧的气氛中执行所述退火。
15.如权利要求8所述的方法，其中在包括原子氧的气氛中在从20℃至600℃范围内的温度下执行所述退火。
16.如权利要求8所述的方法，其中在从200℃到1050℃范围的温度下执行所述退火。
17.一种在基板上形成氧化硅膜的方法，所述方法包括：
在沉积室中提供基板；
通过远程等离子体系统产生多个氢氮自由基，所述远程等离子体系统耦合到所述沉积室；
将含硅前体引入到沉积室，所述含硅前体包括至少Si-Si键；
将多种氮氢自由基引入到所述沉积室，其中所述氮氢自由基和含硅前体反应且在所述基板上沉积第一层膜，所述第一层膜包括多个Si-N(H)-Si键，并且其中所述第一层膜是通过化学气相沉积工艺而沉积的，并且化学气相沉积所沉积的所述第一层膜是可流动的；
在蒸汽气氛中对所述第一层膜进行退火；和
在所述基板上形成第二层膜，所述第二层膜包括多个Si-O-Si键。
18.如权利要求17所述的方法，其中产生多个氮氢自由基包括将氨暴露到所述远程等离子体系统中的等离子体，其中至少一部分氨分解成所述多个氢氮自由基。
19.如权利要求17所述的方法，其中所述含硅前体包括乙硅烷前体或聚硅烷前体。
20.如权利要求17所述的方法，其中所述第一层膜还包括具有可流动特性的氢氧基。
21.如权利要求17所述的方法，其中对所述第一层膜进行退火在从20℃至900℃范围内的温度下执行。
22.如权利要求17所述的方法，其中所述蒸汽气氛包括水蒸汽和酸性蒸汽。
23.如权利要求22所述的方法，其中所述形成第二层膜包括使用所述水蒸汽以将所述第一层膜中所述多个Si-N(H)-Si键的至少一部分转换成多个Si-O-Si键的至少第一部分。
24.如权利要求22所述的方法，其中所述形成第二层膜还包括使用所述酸性蒸汽以催化未反应氢氧基与所述水蒸气的反应以形成反应的OH基，导致所述多个Si-O-Si键的至少第二部分。
25.如权利要求22所述的方法，其中所述酸性蒸汽包括氢氯酸或醋酸。
26.如权利要求17所述的方法，其中所述第二层膜具有比所述第一层膜高的密度。
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