TW201411870A - 接合基材之方法 - Google Patents

接合基材之方法 Download PDF

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Publication number
TW201411870A
TW201411870A TW102126157A TW102126157A TW201411870A TW 201411870 A TW201411870 A TW 201411870A TW 102126157 A TW102126157 A TW 102126157A TW 102126157 A TW102126157 A TW 102126157A TW 201411870 A TW201411870 A TW 201411870A
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Taiwan
Prior art keywords
layer
oxide
substrate
oxide layer
contact
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TW102126157A
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English (en)
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TWI590485B (zh
Inventor
Markus Wimplinger
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Ev Group E Thallner Gmbh
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
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    • H01L24/27—Manufacturing methods
    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B32B37/00—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding
    • B32B37/14—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by the properties of the layers
    • B32B37/24—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by the properties of the layers with at least one layer not being coherent before laminating, e.g. made up from granular material sprinkled onto a substrate
    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B32B38/00—Ancillary operations in connection with laminating processes
    • B32B38/0008—Electrical discharge treatment, e.g. corona, plasma treatment; wave energy or particle radiation
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Abstract

本發明係關於一種將第一至少大致透明基材(1)之第一接觸區(3)接合至第二至少大致透明基材(2)之第二接觸區(4)之方法，在該等接觸區之至少一者上使用氧化物來進行接合，於該第一及第二接觸區(3、4)上由該氧化物形成至少大致透明之互連層(14)，其具有：至少10e1 S/cm2之電導率(測量：四點法，相對於300K之溫度)及大於0.8之光透射率(針對400 nm至1500 nm之波長範圍)。

Description

接合基材之方法
本發明係關於一種如技術方案1之將至少對特定波長範圍大致透明之第一基材之第一接觸區接合至至少對特定波長範圍大致透明之第二基材之第二接觸區之方法、一種如技術方案2之用於製造第一基材之方法及一種如技術方案4之用於製造第二基材之方法。
該等一般方法尤其被用於製造多層半導體、玻璃或陶瓷複合體。一種尤其重要的應用係關於製造多層光伏打電池。
製造多層電池之其中一個主要限制係個別半導體材料之晶格結構在其尺寸及形狀方面之不相容性。在藉由於彼此上方直接生長層來製造個別層時，此不相容性導致於藉由其實施之半導體層中之缺陷。該等缺陷不利地影響所製得層之品質，及尤其係可達到之光能轉換成電能之效率)。關於以下參數之限制實際上係由此所導致：
a)結構中可獲得之活性層的數量。由於上述問題所致，目前此數量受限於2至最多三層。
b)個別層針對最佳波長範圍之最佳化。實際上，目前尚不可能完全自由地針對最佳波長範圍及光能轉換成電能之相關轉換特性將個別層最佳化，此乃因始終必需針對晶格結構之相容性達成折衷。
c)使用更有利的材料：就特定波長而言，將希望使用(例如)矽或鍺，因該等材料將容許在效率與成本之間之理想折衷。然而，通常不可能使用該等材料，因晶格結構無法適當地與用於電池中之其他結構相容。
因此，本發明之目標係設計一種能更有效率地製造前述多層複合體且可實現更多樣參數之方法。
藉由技術方案1、2及4之特徵達成此標的。於附屬請求項中給出本發明之有利發展。於本說明書、申請專利範圍及/或圖式中給出特徵中之至少兩者之所有組合亦落在本發明之架構內。於給定值範圍內，在所指示界限內之值亦將被視為經揭示作為邊界值且將以任何組合主張。
本發明係基於以接合兩基材來替代生長兩層及可藉由該接合來提供若干具有不同特性(尤其係光學特性)之層的概念。
本發明尤其基於一種在形成接觸之前於個別基板上製造位於電池結構中之個別層(尤其係意欲用於接合之互連層)，且隨後僅堆疊/接合其等之方法。因此，可在已針對此目的最佳化之生長基材上製得該等個別層。此製造尤其可藉由利用MOCVD生長來實現。
本發明之一尤其初始態樣係該等層可如何利用同時具經濟性之製程來以導電及光學透明形式堆疊。此外還描述一種為達此目的所需基材之製法。
所述方法較佳適於堆疊多層太陽能電池。然而，該方法亦可替代性地用於製造其中在任何(尤其係光學)材料(尤其係半導體材料、玻璃及陶瓷)之間需要光學透明及導電互連之任何其他結構及組件。於此產業中，由於在諸如照明、通訊、及材料加工之應用主體中諸如LED及雷射之固態光源之大大增加的重要性而產生愈來愈多的應用。於顯示器製造產業中，由於要將諸如接觸偵測(於觸控螢幕等之區域中之反饋)之額外功能整合於顯示器中，因而新穎創新的產品技術亦變得日益重要。
本發明之優點主要為以下各項：- 導電性、光學透明的接合界面(互連層)， - 一或多個在長時間內穩定之極薄耐用層，- 一或多個耐熱層及- 高效率(製造快速且經濟)。
本發明之一中心、尤其初始態樣係使用透明導電氧化物來製造介於基材間之導電及光學透明互連層。該互連尤其係藉由晶圓接合製得，較佳利用直接接合法，及甚至更佳係利用電漿活化的直接接合法。
尤其使用氧化銦錫(ITO)作為透明導電氧化物(TCO)。在下文將使用縮寫ITO來表示氧化銦錫。ITO被廣泛地用於製造LCD顯示器，其中其係用作光學透明電導體。或者，使用以下材料：- 摻雜氧化鋅，尤其係摻鋁氧化鋅(AZO)、摻鎵氧化鋅(GZO)，- [摻]氟氧化錫(FTO)，及- 氧化銻錫(ATO)。
可使用基本上任何可經氧化及尤其經適當摻雜時具有期望特性(尤其係導電性及光學透明度)之材料。
於此方面，如本發明所主張，當材料具有>10e1 S/cm2、較佳10e2 S/cm2、更佳10e3 S/cm2之電導率(利用半導體技術中習知之四點法，相對於300 K之溫度測量)時，滿足電導率。經定義為根據應用所設計層可通過之特定波長範圍光之百分比之光透射率(透射率)應為至少>80%、適宜地>87%、較佳>93%及甚至更佳>96%地通過具有根據該應用之厚度之膜。
如本發明所主張，就光伏打應用而言，自300 nm延伸至1800 nm之波長範圍為較佳。此意指在任一情況中相關波長範圍係大於人眼可見波長範圍。此意欲確保光中之UV部分及光中之IR部分亦可轉換成電能。由於多層太陽能電池中之最上層已處理一部分光譜且因此將其轉換成電能，故可接受接合互連具有稍微較小之其容許透射之波長範 圍之情況。因此，特定言之，前述透射率值將至少適用於波長>600 nm、適宜地>500 nm、更適宜地>400 nm、及最適宜地>350 nm。此外，透射率值尤其亦應適用於自最小波長範圍直至最大1300 nm、適宜地高達最大1500 nm、更適宜地高達最大1700 nm、及最適宜地高達最大1800 nm之整個波長範圍。
尤其藉由以下方法將氧化物施覆至欲如本發明所主張而互連之基材：- MO CVD、金屬有機分子束沉積，- 噴霧熱解、脈衝雷射沉積(PLD)或- 濺鍍。
為確保該等層之期望特性，如本發明所主張之關鍵在於確保正確的混合比。特定言之，氧比例可改良一些該等氧化物中之光學透明度，但須確保氧部份不過高，因否則將會降低電導率。
一般而言，接合互連(互連層，亦稱為接合界面)係由沉積於欲接合基材上之前驅體層狀結構所製得。接著使該等層電漿活化及尤其於室溫下結合，由此形成預接合(暫時接合)。於後續之熱處理製程(退火)期間，該前驅體層狀結構轉化成由透明導電氧化物組成之層，同時增強接合互連。
使用兩半導體晶圓(第一及第二基材)來描述本發明所主張方法之一尤其初始實施例。然而，該方法亦可類似地應用於材料之任何其他光學特定組合。
於第一模組(塗佈設備)中，使第一半導體層生長於尤其由基材自身(稍後經背部薄化)形成之第一載體上，此乃由於其晶體結構及其表面適於生長第一半導體層(第一基材)。藉此，在原位(亦即，未自已用於生長半導體層之塗佈設備移除基材)沉積一層(第一氧化物層)所選擇的TCO。該原位製程確保該TCO可直接附著至半導體，而不會形成將 影響電導率之氧化物。當原位基材係在設備(由其他模組組成)中在於氛圍中儘可能不含氧化元素之保護性氛圍中輸送時，尤其可確保此點。在大致上不含氧及水之氛圍中尤其可確保此點。較佳地，此係藉由具有高真空氛圍之設備之組態來確保，其中壓力小於1*e-5毫巴、較佳小於1*e-6毫巴、及最佳小於1*e-7毫巴。
使第二半導體層生長於其晶體結構及表面就第二半導體層(第二基材)之生長而言最佳化之第二載體上。視情況使在原位之由所選擇TCO材料組成之TCO層(第二氧化物層)沉積於該層上。
接著於該TCO層2"上沉積具有層厚度D3之前驅體層(第三氧化物層)。該前驅體層係經選擇，以致此處材料仍未完全氧化，但相較於已沉積的TCO層(第二氧化物層)缺乏氧。特定言之，缺乏將為完全氧化時所需的氧體積S最大之至少>30%、較佳至少>45%、更佳至少>60%、及最佳>75%。
接著視情況在該前驅體層上沉積由所選擇TCO材料組成具有厚度D4之TCO層(第四氧化物層)。
D3係經選擇為相當大，以致體積足以在後來確保反應期間之相對大體積生長，從而確保接合界面中缺陷之完全閉合。同時，將層厚度選為相當小，以致較佳所有包含於該層中之材料皆在製程期間完全氧化。自1至10 nm厚度之層厚度尤其可確保此點。較佳地，層厚度係介於1至7 nm之間。甚至更佳地，層厚度係介於1及5 nm之間。
D4係經選擇以致層厚度大到足以保護下層D3不在環境大氣中發生反應。特定言之，將大致防止前驅體層與來自環境大氣之氧或水分發生反應(尤其係氧化)。關於此點，大致意指當在室溫下使基材暴露於環境大氣持續最長2小時期間時，適宜地，前驅體層之小於20%將起反應。甚至更佳地，該前驅體層之小於10%起反應。最佳地，前驅體層之小於5%起反應。前驅體層至少0.5至1 nm之層厚度尤其可確保 此點。然而，同時地，該層將薄到足以在後來容許一或多種離析物自貯集槽(進一步參見下文)擴散。因此，該層之最大厚度宜為最大2至3 nm。甚至更適宜地，最大層厚度為至多1.5至2 nm。最適宜地，最大層厚度為最大1至1.5 nm。
接著使第一基材經歷電漿活化製程以產生貯集槽(進一步參見下文之貯集槽形成)。
接著於室溫下接合基材。在如此做時，凡得瓦力(van der Waals force)確保基材於室溫下彼此黏著。在後續之退火製程期間，於貯集槽中嵌入之第一離析物(尤其係H2O)擴散通過可選的第四氧化物層(尤其亦事先暴露於電漿)並氧化第三氧化物層。此增加經氧化材料之體積；此導致閉合表面(生長層)中之缺陷。
若存在，則可視需要移除一個或兩個載體。或者，該等載體中之一者亦可為在後來成為最終結構之一部分之半導體層。
本發明之另一尤其初始態樣係利用電容耦合電漿或感應耦合電漿或來自遠端電漿設備之電漿，以產生可使用其形成用於保存一基材中第一離析物之貯集槽之電漿，該離析物在使基材之間形成接觸或產生暫時接合之後與存於另一基材中之第二離析物反應，且因而形成基材間之不可逆或永久接合。於在第一接觸區上之氧化物層中形成貯集槽之前或之後，一般尤其藉由沖洗步驟進行一或多個基材之清潔。一般而言，此清潔應確保表面上不存在將會導致未接合部位之顆粒。貯集槽及容納於貯集槽中之離析物導致技術上可在以特定方式產生暫時或可逆接合之後直接於接觸區上引起反應，其尤其藉由以該反應使接觸區中之至少一者變形而增加接合速度及增強永久性接合(第一離析物或具有第二離析物之第一組或第二組)，較佳地，該接觸區係與該貯集槽相對。於本發明所主張之相對的第二接觸區上，存在其中發生如本發明所主張之變形且第一離析物(或第一組)與存於第二基材之反 應層中之第二離析物(或第二組)反應之生長層。為加速第一離析物(或第一組)與第二離析物(或第二組)間之反應，在一有利實施例中提供如本發明所主張之位於第二基材之反應層與在基材形成接觸前變薄之貯集槽之間之生長層，因為以此方式反應搭配物之間的距離以可調方式減小且同時促進本發明所主張生長層之變形/形成。藉由減薄至少部分地(尤其係大部分地，較佳係完全地)移除該生長層。即使已完全移除該生長層，生長層亦會再次於第一離析物與第二離析物之反應中生長。可如本發明所主張尤其藉由蝕刻(尤其係乾式蝕刻)、拋光、濺鍍或氧化物之還原進行該生長層之減薄。較佳地，亦可設想該等方法之組合(尤其係濺鍍及氧化物還原)。
如本發明所主張，可有方法來抑制生長層在接觸區形成接觸之前之生長，尤其係藉由鈍化第二基材之反應層，較佳藉由暴露於N2、形成氣體或惰性氛圍或處於真空下或藉由非晶化。關於此點，已證實用包含形成氣體(尤其主要由形成氣體組成)之電漿處理係特別適宜。在此，形成氣體係定義為含有至少2%、更佳4%、理想上10%或15%氫氣之氣體。混合物之其餘部分係由惰性氣體(諸如(例如)氮氣或氬氣)組成。
在使用形成氣體時，尤其可藉由基於濺鍍及氧化物還原之製程使氧化物層變薄。
替代性地或除此措施之外，如本發明所主張宜縮短減薄與形成接觸之間之時間，尤其係<2小時，較佳<30分鐘，甚至更佳<15分鐘，理想地<5分鐘。因此，可使減薄後發生之氧化物生長最小化。
藉由已變薄且因而至少在開始形成永久性接合或反應開始時極薄之生長層來增加離析物通過生長層之擴散速率。此導致相同溫度下離析物之輸送時間更短。
關於預接合步驟，就在基材間產生暫時或可逆接合而言，關於 在基材之接觸區之間產生弱相互作用之目標存在各種可能性。預接合強度係低於永久性接合強度至少2至3倍，尤其5倍，較佳15倍，甚至更佳25倍。關於指導值，提及純的未活化親水化矽具有約100 mJ/m2及純的經電漿活化親水化矽具有約200-300 mJ/m2之預接合強度。分子潤濕基材間之預接合主要係由於不同晶圓側之分子間之凡得瓦相互作用所產生。因此，主要地，具有永久偶極矩之分子適於達成晶圓間之預接合。提及以下化合物作為互連劑，例如(但不限於)：- 水，- 硫醇，- AP3000，- 矽烷及/或- 矽醇。
適宜之如本發明所主張之基材為其材料可呈離析物形式與另一供給離析物反應形成具有較高莫耳體積之產物，因此導致於基材上形成生長層之該等基材。以下組合尤其有利(箭頭左側為指定離析物及箭頭右側為一或多種產物，不存在供給離析物或與特別指定離析物反應之副產物)：
-Si→SiO2、Si3N4、SiNxOy
-Ge→GeO2、Ge3N4
-α-Sn→SnO2
-B→B2O3、BN
-Se→SeO2
-Te→TeO2、TeO3
-Mg→MgO、Mg3N2
-Al→Al2O3、AlN
-Ti→TiO2、TiN
-V→V2O5
-Mn→MnO、MnO2、Mn2O3、Mn2O7、Mn3O4
-Fe→FeO、Fe2O3、Fe3O4
-Co→CoO、Co3O4
-Ni→NiO、Ni2O3
-Cu→CuO、Cu2O、Cu3N
-Zn→ZnO
-Cr→CrN、Cr23C6、Cr3C、Cr7C3、Cr3C2
-Mo→Mo3C2
-Ti→TiC
-Nb→Nb4C3
-Ta→Ta4C3
-Zr→ZrC
-Hf→HfC
-V→V4C3、VC
-W→W2C、WC
-Fe→Fe3C、Fe7C3、Fe2C
-In→In2O3
-Sn→Sn2O2
-Sn→SnO
-Zn→ZnO
-Al→Al2O3
此外，可設想以下述半導體之混合形式作為基材：
- III-V：GaP、GaAs、InP、InSb、InAs、GaSb、GaN、AlN、InN、AlxGa1-xAs、InxGa1-xN
- IV-IV：SiC、SiGe，
- III-VI：InAlP。
- 非線性光學器件：LiNbO3、LiTaO3、KDP(KH2PO4)
- 太陽能電池：CdS、CdSe、CdTe、CuInSe2、CuInGaSe2、CuInS2、CuInGaS2
- 導電氧化物：In2-xSnxO3-y
如本發明所主張，於該等晶圓中之至少一者上及直接於各別接觸區上存在一或多個其中可貯集特定量的用於體積膨脹反應之供給離析物中之至少一者之貯集槽。因此，離析物可為(例如)O2、O3、H2O、N2、NH3、H2O2等。因膨脹所致，尤其由氧化物生長所決定，基於反應搭配物減小系統能量之傾向，接觸區之間的可能間隙、孔隙、及腔經最小化及接合力因窄化該等區域中基材間之距離而相應地增加。於最佳的可能情況中，存在的間隙、孔隙及腔被完全閉合，以致整個接合區域增加且因而如本發明所主張之接合力相應地增加。
習知接觸區展示二次粗糙度(quadratic roughness(Rq))為0.2 nm之粗糙度。此對應於在1 nm範圍內之表面之峰-至-峰值。該等經驗值係利用原子力顯微鏡(AFM)測定。
如本發明所主張之反應適於容許直徑200至300 mm具有1單層(ML)水之圓形晶圓之習知晶圓表面之生長層生長0.1至0.3 nm。
因此，如本發明所主張，其限制條件特定言之為至少2 ML、較佳至少5 ML、甚至更佳至少10 ML流體(尤其係水)貯集於貯集槽中。
尤佳係藉由暴露於電漿來形成貯集槽，因為電漿暴露會進一步導致接觸區平滑化及親水化作為協同效應。表面主要係藉由氧化物層及視情況反應層之材料之黏性流進行電漿活化而平滑化。尤其藉由增加矽羥基化合物來發生親水性之增加，較佳藉由裂解存於表面上之Si-O化合物(諸如Si-O-Si)，尤其係根據以下反應：
就其他表面而言，一般可陳述發生單離OH化合物之密度增加；此導致改良的親水性。
尤其因前述效應所致之另一副作用在於預接合強度尤其經提升2至3倍。
例如，於第一基材之第一接觸區上之氧化物層(及視情況，於第二基材之第二接觸區上之氧化物層)中之貯集槽係藉由已塗覆有熱氧化物之第一基材之電漿活化形成。為了可設定電漿所需之條件，於真空室中進行該電漿活化。如本發明所主張，就電漿放電而言，使用離子能量在自0至2000 eV(振幅)範圍內之N2氣、O2氣或氬氣，結果製得具有經處理之表面(於此情況中為第一接觸區)深度高達20 nm、較佳高達15 nm、更佳高達10 nm、最佳高達5 nm之貯集槽。
藉由於真空室中設定特定壓力，可設想影響或如本發明所主張設定電漿離子之平均自由徑長度。
依本發明於相對電極上使用兩不同頻率來產生電漿可在於接觸區/表面上製造貯集槽中產生可再現的結果，該等電極尤其藉由施加交流電流或交流電壓、及/或藉由使用感應耦合電漿源及/或遠端電漿來加速電漿離子。
就電容耦合而言，若電極位於電漿室中將有利。
在此，可藉由設定參數電極之(不同)頻率(尤其係振幅，較佳(排他地)係施加於第二電極上之偏壓及室壓)來達成接觸區之最佳暴露且因而製得尤其就體積及/或深度而言經準確界定之貯集槽。
作為電容耦合雙頻電漿設備之電漿活化設備可有利地分開設定離子密度及離子到達晶圓表面上之加速度來執行。因此，可於寬廣窗中設定可獲得的製程結果且與應用需求最佳地匹配。
尤其呈第二(尤其係下部)電極之基準電壓形式之偏壓係用於影響電極對固定在該第二電極上之基材的接觸區之衝擊(速度)，尤其係減 慢或加速該衝擊。
特定言之，貯集槽中之孔隙密度分佈變得可藉由前述參數(尤其係下文所述之有利實施例)來調整。
於感應耦合電漿源中，可對用於產生磁場之交流電流採用關於電容耦合之交流電壓之對應類似考量。如本發明所主張可設想藉由不同強度及/或頻率之交流電流或交流磁場來控制感應耦合電漿源之電漿，以致電漿具有本發明所主張之對應特性。
於遠端電漿中，實際使用之電漿係於外部源中產生且經引入至樣本空間中。特定言之，將該電漿之組分(尤其係離子)輸送至樣本空間中。可藉由不同元件(諸如鎖扣、加速器、磁及/或電透鏡、光欄等)確保電漿自源空間進入至基材空間中。在電及/或磁場之頻率及/或強度方面適用於電容及/或感應耦合電漿之所有考量將適用於確保電漿自源空間產生及/或進入至基材空間中之所有元件。例如，將可設想依照本發明所主張參數藉由電容或感應耦合在源空間中產生電漿且隨後藉由前述元件穿入至基材空間中。
如本發明所主張，可使用適於產生貯集槽之任何顆粒類型(原子及/或分子)。較佳地，使用產生具有所需特性之貯集槽的該等原子及/或分子。相關特性主要為孔徑、孔隙分佈及孔隙密度。或者，如本發明所主張，可使用氣體混合物，諸如(例如)空氣或由95% Ar及5% H2組成之形成氣體。取決於所使用之氣體，於電漿處理期間，於貯集槽中尤其存在以下離子：N+、N2+、O+、O2+、Ar+。第一離析物可容納於一或多個貯集槽之未佔用自由空間中。氧化物層及因此貯集槽可延伸至反應層中。
有利地，存在可與反應層反應且至少部分(較佳主要)由第一離析物組成之不同類型的電漿物質。在第二離析物為Si/Si之情況，Ox電漿物質將有利。
基於以下考量來形成貯集槽：孔徑小於10 nm、較佳小於5 nm、更佳小於1 nm、甚至更佳小於0.5 nm、最佳小於0.2 nm。
孔隙密度較佳與藉由撞擊作用產生孔隙之顆粒之密度成正比，最佳甚至可隨撞擊物質之分壓改變，且取決於處理時間及參數，尤其係所使用電漿系統之處理時間及參數。
孔隙分佈較佳具有藉由改變經疊加形成較佳平線狀區域(參見圖8)之若干該等區域之參數之至少一個在表面下方具最大孔隙濃度之區域。孔隙分佈隨厚度之增加朝零減小。於轟擊期間，接近表面之區域具有幾乎等於接近該表面之孔隙密度的孔隙密度。於電漿處理結束之後，由於應力鬆弛機制的結果，於表面上之孔隙密度可能會減小。於相對於表面之厚度方向上之孔隙分佈具有一陡側翼及相對於整體而言相當平坦但連續減小之側翼(參見圖8)。
就孔徑、孔隙分佈及孔隙密度而言，類似的考量適用於不利用電漿來產生之所有方法。
可藉由製程參數之受控使用及組合來設計貯集槽。圖8顯示由電漿注射之氮原子之濃度成穿透至氧化矽層中之深度之函數關係之圖示。可藉由改變物理參數產生兩曲線。第一曲線11係因氧化矽中較深處之更高度加速原子所產生，反之，曲線12係在改變製程參數之後以較低密度產生。兩曲線之疊加獲得表徵貯集槽之總和曲線13。明顯可見注射原子及/或分子物質之濃度之間的關係。較高濃度指示具有較高缺陷結構之區域，因此更多空間可容納隨後的離析物。尤其於電漿活化期間以特定方式控制之連續改變的製程參數使得可獲得具有添加離子隨深度分佈之貯集槽，該分佈係儘可能地均勻。類似地，該等考量同樣適用於除氧化矽外之層，其中貯集槽可在其他材料組合之情況下形成。特定言之，該等考量亦可適用於TCO層。
作為已藉由電漿製得之貯集槽之另一選擇，可設想在基材中之 至少一者(至少第一基材)上使用TEOS(正矽酸四乙酯)氧化物層作為貯集槽。一般而言，該氧化物不如熱氧化物緻密，因此，如本發明所主張，宜進行壓縮。基於設定貯集槽之一定孔隙度之目標藉由熱處理進行壓縮。
根據本發明之一實施例，尤其有利地，可在藉由將貯集槽以塗層形式施加至第一基材來形成貯集槽的同時發生貯集槽之填充，該塗層已包含第一離析物。
可將貯集槽設想為具有在奈米範圍內之孔隙度之多孔層或具有通道厚度小於10 nm、更佳小於5 nm、甚至更佳小於2 nm、最佳小於1 nm，其等中最佳小於0.5 nm之通道之層。
關於將貯集槽填充第一離析物或第一組離析物之步驟，如本發明所主張，可設想以下實施例及其組合：- 將貯集槽暴露於環境大氣，- 尤其以去離子水沖洗，- 以含有離析物或由離析物組成之流體(尤其係H2O、H2O2、NH4OH)沖洗，- 將該貯集槽暴露於任一氣體氛圍，尤其係原子氣體、分子氣體、氣體混合物，- 將該貯集槽暴露於含水蒸氣或含過氧化氫蒸氣之氛圍，及- 使作為氧化物層之已填充離析物之貯集槽沉積於第一基材上。
以下化合物可作為離析物：Ox +、O2、O3、N2、NH3、H2O、H2O2、及/或NH4OH。
除了使用水之外，使用上述過氧化氫蒸氣被認為是較佳方式。此外，過氧化氫的優點係具有較大的氧對氫比。另外，過氧化氫於高於特定溫度下及/或透過使用MHz範圍內之高頻場解離為氫及氧。
另一方面，H2O的優點係具有小分子尺寸。H2O分子之尺寸甚至 比O2分子之尺寸更小，因此，H2O提供可更容易地嵌入孔隙中及可更容易地擴散通過生長層的優勢。
大體上，當使用具有不同熱膨脹係數之材料時，宜採用不會導致任何顯著溫度增加、或至多局部/特定溫度增加之用於解離前述物質之方法。特定言之，微波照射可至少促進、較佳導致解離。
根據本發明之一有利實施例，提供藉由使第一離析物擴散至反應層中來發生生長層之形成及不可逆接合之強化。
根據本發明之另一有利實施例，提供不可逆接合之形成係在通常小於300℃、適宜小於200℃、更佳小於150℃、甚至更佳小於100℃之溫度，最佳在室溫下，尤其於最長12天、更佳最長1天、甚至更佳最長1小時、最佳最長15分鐘之期間內發生。另一有利的熱處理法係藉由微波之介質加熱。
此處尤其有利的係不可逆接合具有大於1.5 J/m2、尤其大於2 J/m2、較佳大於2.5 J/m2之接合強度。
可尤其有利地增加接合強度，其中，於反應期間，如本發明所主張，在反應層中形成具有比第二離析物之莫耳體積更大莫耳體積之產物。依此方式實現於第二基材上之生長，結果，接觸區之間之間隙可如本發明所主張藉由化學反應閉合。結果，接觸區之間的距離(因此，平均距離)減小，及無效空間(dead space)經最小化。
在藉由電漿活化進行貯集槽形成之情況，尤其係利用介於10 kHz及20000 kHz之間、較佳介於10 kHz及5000 kHz之間、甚至更佳介於10 kHz及1000 kHz之間、最佳介於10 kHz及600 kHz之間之活化頻率及/或介於0.075及0.2瓦/cm2之間之功率密度及/或利用介於0.1及0.6毫巴之間之壓力加壓，導致此種接觸區平滑化以及接觸區之親水性顯著增加之額外效應。
或者，如本發明所主張，可藉由使用已尤其以受控方式壓縮成 作為氧化物層之特定孔隙度之四乙氧基矽烷氧化物層來進行貯集槽之形成。
根據本發明之另一有利實施例，提供氧化物層尤其主要(尤其係基本上完全)由非晶型二氧化矽(尤其係已藉由熱氧化製得之二氧化矽)組成，及反應層係由可氧化材料，尤其主要(較佳基本上完全)由Si、Ge、InP、GaP或GaN(或選擇性地於上文提及之另一材料)組成。尤其有效地閉合所存在間隙之尤其穩定的反應可藉由氧化實現。
如本發明所主張，在此提供在第二接觸區與反應層之間存在生長層，尤其主要為原生二氧化矽(或選擇性地於上文提及之另一材料)。該生長層經受由本發明所主張之反應導致之生長。該生長係自Si-SiO2轉變區(7)開始經由非晶型SiO2之再形成及藉此引起之生長層之變形(尤其係隆起)，尤其於界面上至反應層(及尤其於第一及第二接觸區間之間隙區中)進行。此導致兩接觸區之間的距離縮短或無效空間減小，結果，兩基材之間之接合強度增加。介於200及400℃之間之溫度尤其有利，較佳為約200℃及150℃，更佳係介於150℃及100℃之間之溫度，最佳係介於100℃及室溫之間之溫度。該生長層可分為若干生長區。該生長層可同時為其中形成另一加速反應之貯集槽之第二基材的氧化物層。
此處尤其有利的係在形成不可逆接合之前，生長層具有介於0.1 nm及5 nm之間之平均厚度A。生長層越薄，則通過該生長層(尤其係藉由使第一離析物擴散通過生長層至該反應層)在第一及第二離析物間之反應可更快速及容易地發生。藉由已變薄且因而至少在開始形成永久性接合或反應開始時極薄之生長層來增加離析物通過生長層之擴散速率。此導致離析物在相同溫度下之更短的輸送時間。
在此，本發明所主張之減薄發揮決定性作用，因為藉此可進一步加速反應及/或進一步減低溫度。減薄可尤其藉由蝕刻(較佳於潮濕 氛圍中，又更佳在原位)來完成。或者，該減薄尤其係藉由乾式蝕刻(較佳在原位)進行。此處，在原位意指在進行至少一先前及/或一後續步驟之同一室中進行。屬於此處所用在原位概念之另一設備配置為其中基材在個別製程室之間之輸送係發生在可以受控方式(例如，使用惰性氣體)調整之氛圍中(但尤其係在真空環境中)之設備。濕式蝕刻係利用呈氣相之化學品發生，而乾式蝕刻係利用呈液態之化學品發生。在生長層係由二氧化矽組成之情況，可利用氫氟酸或稀氫氟酸進行蝕刻。在生長層係由純Si組成之情況，可利用KOH進行蝕刻。
根據本發明之一實施例，有利地提供於真空中進行貯集槽之形成。因此，可避免貯集槽受不期望的材料或化合物污染。
於本發明之另一實施例中，有利地提供藉由一或多個下述步驟進行貯集槽之填充：- 將第一接觸區暴露於大氣，以利用大氣濕度及/或空氣中所含之氧氣填充貯集槽，- 將該第一接觸區暴露於尤其主要(較佳幾乎完全)由(尤其係)去離子H2O及/或H2O2組成之流體，- 將該第一接觸區暴露於尤其具有在自0至2000 eV範圍內之離子能量之N2氣及/或O2氣及/或Ar氣、及/或形成氣體(尤其係由95% Ar及5% H2組成)，- 利用任何已指定之離析物氣相沉積以填充貯集槽。
在貯集槽較佳以介於0.1 nm及25 nm之間、更佳介於0.1 nm及15 nm之間、甚至更佳介於0.1 nm及10 nm之間、最佳介於0.1 nm及5 nm之間之厚度R形成之情況，製程順序尤其有效。此外，根據本發明之一實施例，有利的係緊接於形成不可逆接合之前貯集槽與反應層間之平均距離B介於0.1 nm及15 nm之間、尤其介於0.5 nm及5 nm之間、較佳介於0.5 nm及3 nm之間之情況。距離B會受減薄影響或係如本發明 所主張藉由減薄產生。
如本發明所主張製造用於執行該方法之裝置，該裝置配備用於形成貯集槽之室、尤其與該室分開設置用於填充貯集槽之室、及尤其分開設置用於形成預接合之室，該等室均透過真空系統彼此直接連接。
於另一實施例中，貯集槽之填充亦可直接透過大氣進行，因此係在可對大氣敞開之室中，或簡單地在不具有夾套但可半自動及/或完全自動處理晶圓之結構上進行。
由於石化燃料在中期將變得稀少，且除此之外在回收及使用上會構成重大環境問題(尤其係促成溫室效應)，故藉由光伏打系統來利用太陽能之重要性日益增加。由純粹經濟觀點來看，為加強光伏打器件之競爭性，必需提高在相同成本或至多適度成本增加下將光轉化成電能之效率。但可能的效率具有限度。該等限度主要起因於單一半導體材料僅可處理有限波長範圍之光及將其轉化成電能之限制。
因此，尤其有利的係用於製造多層太陽能電池或英文稱為「多接面太陽能電池(multi-junction solar cell)」之本發明的一應用。
於其等中，在太陽能電池中將個別層垂直堆疊於彼此之上。入射光首先撞擊經最佳化以將特定第一波長範圍之光轉化成電能之最上層。具有大致無法在該層中處理之波長範圍之光穿透該第一層且入射於經最佳化以處理第二波長範圍之下方第二層上，且因而產生電能。於該等多層電池中，視情況可行的係，具有大致亦無法在該第二層中處理之波長範圍之光入射於經最佳化以處理第三波長範圍之光之下方第三層上，且因而產生電能。可設想複數個(n)該等層在純理論上來說係可行的。實際上，該等電池係經結構化，以致入射光首先穿透之最上層係處理具最短波長之波長範圍。第二層處理第二短波長範圍等等。在此，如本發明所主張，不僅可設想雙層結構，而且可實施三層 或更多層。在此提供該等層係以導電方式(亦即，電阻儘可能地小)及以光學透明方式垂直互連。尤其藉由所謂的「金屬有機化學氣相沉積」(簡寫為「MO CVD」)製程來沉積該等層，多個電池中兩活性層之沉積尤其係「在原位」發生，亦即，在沉積製程之間未將基材暴露於正常環境大氣。較佳地，亦在該等活性層之間放置阻隔層(第二或第四氧化物層)及/或緩衝層(第二或第四氧化物層)以改良所得電池之品質。
自以下較佳例示性實施例之說明及利用附圖當可明瞭本發明之其他優點、特徵及詳細內容。
1‧‧‧第一基材
2‧‧‧第二基材
3‧‧‧第一接觸區
4‧‧‧第二接觸區
5‧‧‧貯集槽
6‧‧‧第一氧化物層
7‧‧‧第一半導體
8‧‧‧第一載體
9‧‧‧第四氧化物層
10‧‧‧第三氧化物層
11‧‧‧第二氧化物層
12‧‧‧第二半導體
13‧‧‧第二載體
14‧‧‧互連層
圖1顯示緊接於第一基材與第二基材形成接觸之前之本發明一實施例之示意圖。
以相同參考數字指示相同或等效特徵。
圖1中之情況僅顯示第一基材1之第一接觸區3與第二基材2之第二接觸區4之一個橫截面片段。該等接觸區3、4之表面具有極性OH基末端且因此具親水性。該第一基材1及該第二基材2係藉由存於表面上的OH基與H2O分子間以及單單H2O分子間之氫橋之引力，尤其係藉由凡得瓦力及/或氫橋固定。已藉由於前一步驟中之電漿處理來增加至少該第一基材1之親水性。
電漿處理係在可暴露於電漿及真空及/或一定氣體氛圍及可設置於其自身對應設備模組中之電漿室中進行。暴露於真空及/或一定氣體氛圍意指可設定並控制低於1毫巴之壓力。於此處所述之例示性實施例中，氣體為0.3毫巴壓力下之N2。
根據該替代性實施例，尤其宜另使該第二基材2或該第二接觸區4經歷電漿處理，尤其係與該第一基材1之電漿處理同時進行。
已如本發明所主張藉由電漿處理在由所選擇TCO組成之氧化物層6中形成貯集槽5。於該氧化物層6下方直接鄰接半導體7及其尤其亦可視情況使用作為包含第二離析物或第二組離析物之反應層。以具有前述離子能量之N2離子進行電漿處理獲得平均厚度R約15 nm之貯集槽5，該等電漿離子在該氧化物層6中形成通道或孔隙。該貯集槽填充有與第二離析物反應之第一離析物。
於所說明實施例中該半導體7係暫時由載體8支撐。
位於第二接觸區4上之第二基材2係由第四氧化物層9組成，該第四氧化物層9直接鄰接第三氧化物層10(前驅體層)，後者又直接鄰接第二氧化物層11。
該氧化物層10(前驅體層)尤其係由含有不完全氧化組分之TCO所組成，以致該層具有小於最大氧體積S最大之氧體積S1，若整體體積被完全氧化，則該層中將包含該最大氧體積S最大。特定言之，氧體積S1最大為S最大之70%。該百分比宜為55%，更適宜為40%，及最適宜為25%。
第二氧化物層11係緊密接合至第二基材2之半導體12，繼而暫時固定於載體13上。
尤其使用該半導體12作為包含第二離析物或第二組離析物之反應層。
生長層係在該等氧化物層6、9、10、11及視情況該等反應層(半導體7、12)之間由第一離析物與第二離析物反應形成。
於一較佳實施例中，已嵌入於氧化物層6中所形成貯集槽5中之第一離析物與前驅體層10反應。由於該第一離析物與該前驅體層之反應產物具有較高莫耳體積，因此該反應導致體積增加。
藉由增加莫耳體積及H2O分子之擴散，尤其在介於氧化物層9及10之間之界面上，體積以生長層形式生長，歸因於使吉布斯自由焓 (free Gibb's enthalpy)減至最低之目標，在於接觸區3、4之間存在間隙之區域中發生增強生長。藉由生長層體積之增加來閉合該等間隙。
該等氧化物層6、9、10、及11於接合之後共同形成互連層14。
在一個較佳實施例中，於反應後之該互連層宜由基本上對應於包含初始時所沉積氧化物層9、11及6之相同TCO之均質材料所組成。
1‧‧‧第一基材
2‧‧‧第二基材
3‧‧‧第一接觸區
4‧‧‧第二接觸區
5‧‧‧貯集槽
6‧‧‧第一氧化物層
7‧‧‧第一半導體
8‧‧‧第一載體
9‧‧‧第四氧化物層
10‧‧‧第三氧化物層
11‧‧‧第二氧化物層
12‧‧‧第二半導體
13‧‧‧第二載體
14‧‧‧互連層

Claims (8)

  1. 一種將第一至少大致透明基材(1)之第一接觸區(3)接合至第二至少大致透明基材(2)之第二接觸區(4)之方法，在該等接觸區(3、4)之至少一者上使用氧化物來進行接合，於該第一及第二接觸區(3、4)上由該氧化物形成至少大致透明之互連層(14)，其具有：至少10e1 S/cm2之電導率(測量：四點法，相對於300K之溫度)及大於0.8之光透射率(針對自400 nm至1500 nm之波長範圍)。
  2. 一種製造具有用於接合至第二基材(2)之第二接觸區(4)之第一接觸區(3)的第一基材(1)之方法，其中對該第一基材(1)施覆具有以下特性之第一氧化物層(6)：至少10e1 S/cm2之電導率(測量：四點法，相對於300K之溫度)及大於0.8之光透射率(針對自400 nm至1500 nm之波長範圍)。
  3. 如請求項1或2之方法，其中該第一接觸區(3)尤其在形成接觸之前經電漿活化。
  4. 一種利用以下步驟(尤其係以下順序)製造具有用於接合至第一基材(1)之第一接觸區(3)之第二接觸區(4)的第二基材(2)之方法：對第二基材(2)施覆第二氧化物層(11)，對該第二氧化物層(11)施覆第三氧化物層(10)，該第三氧化物層(10)具有小於該第三氧化物層(10)最大氧體積S最大之70%的氧體積S1，及對該第三氧化物層(10)施覆第四氧化物層(9)。
  5. 如請求項1或2之方法，其中該氧化物或該等氧化物層(6、9、10、11)中之一或多層尤其以摻雜形式包含以下組分中之至少一 者：銦，錫，鋁，鋅，鎵，氟或銻。
  6. 如請求項1或2之方法，其中該氧化物或該等氧化物層(6、9、10、11)中之一或多層係藉由以下方法中之一者施覆：金屬有機化學氣相沉積，金屬有機分子束沉積，噴霧熱解，脈衝雷射沉積或濺鍍。
  7. 如請求項4之方法，其中該氧化物或該等氧化物層(6、9、10、11)中之一或多層尤其以摻雜形式包含以下組分中之至少一者：銦，錫，鋁，鋅，鎵，氟或銻。
  8. 如請求項4之方法，其中該氧化物或該等氧化物層(6、9、10、11)中之一或多層係藉由以下方法中之一者施覆： 金屬有機化學氣相沉積，金屬有機分子束沉積，噴霧熱解，脈衝雷射沉積或濺鍍。
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