TWI425559B - 以單晶氧化物作為基板成長纖鋅礦結構半導體非極性ｍ面磊晶層之方法 - Google Patents
以單晶氧化物作為基板成長纖鋅礦結構半導體非極性ｍ面磊晶層之方法 Download PDFInfo
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- 229910052984 zinc sulfide Inorganic materials 0.000 title claims description 10
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- 239000011777 magnesium Substances 0.000 claims description 4
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- JRPBQTZRNDNNOP-UHFFFAOYSA-N barium titanate Chemical compound [Ba+2].[Ba+2].[O-][Ti]([O-])([O-])[O-] JRPBQTZRNDNNOP-UHFFFAOYSA-N 0.000 claims description 3
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Description
本發明係關於一種單晶氧化物作為基板成長纖鋅礦結構半導體之非極性m面磊晶層之方法，尤指一種適用於具有低晶格不匹配度、在高溫時維持熱穩定性、並可用於成長m面氧化鋅或III族氮化物磊晶層之方法。本發明亦提供一種具有非極性m面之磊晶層。
近年來，氮化鎵(GaN)及其類似III族氮化物，因成功地應用在藍光到紫外光之固態發光元件及雷射二極體等領域中而逐漸受到重視。這些氮化物屬六方晶系中纖鋅礦(wurtzite)晶體結構，因此其晶體之生長以順著c軸[0001]為主。然而，根據過去之研究亦已發現，延c軸生長之GaN會因Ga與N原子排列產生內建電場而順著c軸衍生自發的極化效應(polarization effect)，而此會導致價電帶與導電帶之偏移，並使發光量子效率降低。
鑒於上述，發展出成長具有非極性面之晶面，如m面(m-plane)及a面(a-plane)之氮化鎵或其類似III族氮化物，以消除其極化效應來提生量子效率將刻不容緩。此外，氧化鋅(ZnO)材料因其具有高激子結合能(exciton binding energy，60meV)，故在雷射應用上與氮化鎵或其類似III族氮化物同樣具有極大潛力，亦需開發具有非極性面之晶面氧化鋅材料，以克服低發光量子效率之瓶頸。
習知中以異質成長具有非極性m面之氮化鎵或氧化鋅磊晶係於m面碳化矽基板、m面藍寶石基板、或γ-LiAlO2
(100)基板上成長。然而，上述m面碳化矽基板及m面藍寶石基板與所欲成長之氮化鎵或氧化鋅磊晶間具有相當大的晶格不匹配度(lattice mismatch)，而此往往會造成所成長出之磊晶層具有較高的缺陷密度，並影響其光電性質；另外，γ-LiAlO2
基板中之Li於高溫反應時的熱穩定性不佳，且其基板面積較小(約1吋)而導致影響其應用。
綜合上述，目前亟需一種不僅具有低晶格不匹配度、且需具備在高溫時維持熱穩定性、並可用於成長m面氧化鋅或III族氮化物磊晶層之基板及其方法。
本發明之主要目的係在提供一種以單晶氧化物作為基板成長非極性m面磊晶層之方法，俾能降低基板與磊晶層間晶格不匹配度，且該基板在高溫時仍能維持熱穩定性，作為適於成長m面氧化鋅或III族氮化物磊晶層。
本發明之另一目的係在提供一種具有非極性m面之磊晶層，藉以避免因磊晶層中原子排列產生極化效應導致價電帶與導電帶之偏移，而使發光量子效率降低之情形。
為達成上述目的，本發明以單晶氧化物作為基板成長非極性m面磊晶層之方法，包括：提供一具有鈣鈦礦結構之單晶氧化物；選擇單晶氧化物之一平面作為基板；
以及在基板上以氣相沉積法生長一具有纖鋅礦結構半導體之非極性m面磊晶層。
本發明亦提供一種具有非極性m面之磊晶層，其係以下列方法而得，包括：提供一具有鈣鈦礦結構之單晶氧化物；選擇單晶氧化物之一平面作為基板；以及在基板上以氣相沉積法生長一具有非極性m面之磊晶層。
根據本發明，且由於基板與非極性m面磊晶層間之晶格常數不匹配度較習知為小，故根據本發明之方法尤其適合用於生長具非極性m面磊晶層，其中，基板與非極性m面磊晶層間之晶格常數不匹配度較佳為小於10%。根據本發明之該平面係為單晶氧化物之晶面或截切面，並以此晶面或截切面作為基板生長具非極性m面磊晶層，其中該平面較佳係密勒指數(Miller Index)為{112}之平面。
根據本發明，可選擇地於前述單晶氧化物上另形成一氧化物層，並選擇該氧化物層之一平面作為該基板，其後再於該基板上以氣相沉積法生長一具有纖鋅礦結構半導體之非極性m面磊晶層；其中，該氧化物層之組成係與該單晶氧化物相同或不同。
再者，根據本發明，其中，具有鈣鈦礦結構之單晶氧化物或氧化物層之種類沒有限制，只要可具有優異熱穩定度並可抑制其他界面層生長之材料皆可屬之；較佳為鋁酸鑭(LaAlO3
)、鈦酸鍶(SrTiO3
)、鑭鍶鋁鉭氧(LaSrAlTaO3
)、或晶格常數相較鋁酸鑭在10%內之鋁酸鑭合金；最佳為鋁酸鑭。由於鋁酸鑭單晶氧化物之熔點高達2450K，除兼具熱穩定度佳及可抑制其他界面層生長之
優點外，鋁酸鑭單晶氧化物或氧化物層可使用2吋或以上之晶面或截切面作為基板來成長非極性m面磊晶層，其價格成本亦較傳統使用之基板便宜，增加其應用性。
根據本發明所形成之磊晶層可為氧化鋅、或III族氮化物；其中，該氧化鋅可依需要更包括摻雜有鎂、鈣、鍶、鋇、鎘、鋁、鎵、銦、或其組合之合金；至於該III族氮化物可為氮化鎵、氮化銦、氮化鋁、氮化銦鎵、氮化鋁鎵、氮化鋁銦、或氮化鋁銦鎵。
根據本發明之在基板上生長該具有非極性m面磊晶層之方法沒有限制，可使用物理氣相沉積法或化學氣相沉積法，較佳為脈衝雷射鍍膜法、有機金屬化學氣相沉積法、濺射法、或電子束(熱)蒸鍍法。
根據本發明之在基板上生長該具有非極性m面磊晶層之方法，在基板上以氣相沉積法生長一具有非極性m面之磊晶層之前，更包括有一使用有機溶劑清潔基板之步驟，使用之有機溶劑種類沒有限制，較佳為使用熱丙酮及異丙醇來清潔基板。
因此，本發明係藉前述以單晶氧化物作為基板成長非極性m面磊晶層之方法，其係藉由基板與磊晶層間極低晶格不匹配度，並使用在高溫時仍能維持熱穩定性之基板，作為適於成長m面氧化鋅或III族氮化物磊晶層。且根據前述方法所生成具有非極性m面之磊晶層，其並具有避免磊晶層中因原子排列而產生極化效應導致價電帶與導電帶之偏移，而產生發光量子效率降低之情形。
本發明係提供一種具有非極性m面之磊晶層及一種以單晶氧化物作為基板成長非極性m面磊晶層之方法，該方法包括：提供一具有鈣鈦礦結構之單晶氧化物；選擇單晶氧化物之一平面作為基板；以及在基板上以氣相沉積法生長一具有纖鋅礦結構半導體之非極性m面磊晶層。
以下，將詳述本發明以單晶氧化物作為基板成長非極性m面磊晶層之方法。
首先，提供一具有鈣鈦礦結構之單晶氧化物，該具有鈣鈦礦結構之單晶氧化物其種類沒有限制，只要可具有優異熱穩定度並可抑制其他界面層生長之材料皆可屬之；較佳為鋁酸鑭(LaAlO3
)、鈦酸鍶(SrTiO3
)、鑭鍶鋁鉭氧(LaSrAlTaO3
)、或晶格常數相較鋁酸鑭在10%內之鋁酸鑭合金。在本實施例中，係使用一2吋之鋁酸鑭單晶氧化物。接著，如圖1所示，其為本發明較佳實施例中成長非極性m面氧化鋅磊晶層示意圖，選擇該鋁酸鑭單晶氧化物之晶面或截切面作為基板，在本實施例中，係選擇密勒指數為{112}之平面作為基板，並置入真空腔中將該基板以熱丙酮及異丙醇清潔之，其後加熱至850℃持溫1小時以去除基板表面之雜質。
再提供一靶材，其中該靶材係為一經熱壓之氧化鋅塊狀材料，若有需要，可於該氧化鋅塊狀材料摻雜鎂、鈣、鍶、鋇、鎘、鋁、鎵、銦、或其組合之合金於其中。
使用雷射鍍膜法(DCA PLD-500脈衝雷射鍍膜系統，波長248nm及3Hz頻率之KrF準分子雷射)，控制其背景氣壓維持於20mtorr範圍以下之氧分壓環境中，持溫800℃，以沉積如圖1中之非極性m面()氧化鋅磊晶層。
如圖2(a)及圖2(b)，係為本實施例中非極性m面氧化鋅磊晶層之X-Ray繞射分析，其中圖2(a)可知本實施例中僅有m面氧化鋅磊晶在鋁酸鑭(112)平面之基板上成長。而圖2(b)依半高寬最大值為0.41°之結果可知所沉積之非極性m面氧化鋅磊晶層具有優異的結晶品質。
在本實施例中除靶材為III族氮化物如氮化鎵外，其餘與實施例1相同。在本例中，係沉積III族氮化物如氮化鎵磊晶層。根據本實施例所成長之非極性m面III族氮化物如氮化鎵磊晶層亦可達成如實施例1之目的及功效。
此外，在本實施例中雖僅舉例III族氮化物如氮化鎵，然而可依所需，亦可依實施例1之方法選擇使用其他靶材之III族氮化物，如氮化銦、氮化鋁、氮化銦鎵、氮化鋁鎵、氮化鋁銦、或氮化鋁銦鎵等，亦可達成如實施例1之目的及功效。
在本實施例中除於單晶氧化物上形成一氧化物層(圖中未示)，並選擇該氧化物層之一平面作為基板外，其餘與實施例1或2相同。
在本實施例中，係提供一具有鈣鈦礦結構之單晶氧化物，如鈦酸鍶(SrTiO3
)。接著，於前述鈦酸鍶單晶氧化物上另形成一鋁酸鑭(LaAlO3
)氧化物層，並選擇該鋁酸鑭氧化物層密勒指數為{112}之平面作為基板，其後與實施例1或2相同，再於該基板上以氣相沉積法生長一具有纖鋅礦結構半導體之非極性m面磊晶層。此外，在本實施例中雖僅舉例鈦酸鍶作為單晶氧化物及鋁酸鑭作為氧化物層，然而可依所需選擇該氧化物層之組成與該單晶氧化物為相同或不同。根據本實施例之方法亦可達成如實施例1或2之目的及功效。
在此測試例中，係將實施例1中所得到非極性m面氧化鋅磊晶層與作為基板之鋁酸鑭單晶氧化物(112)平面間的晶格不匹配度作一詳細說明。
圖3(a)及圖3(b)為鋁酸鑭單晶氧化物(112)平面及非極性m面()氧化鋅磊晶層之表層原子鍵結關係圖。由圖中可知，在鋁酸鑭單晶氧化物(112)平面表層之氧原子間距分別為5.360埃及6.566埃。非極性m面()氧化鋅磊晶層之氧原子間距分別為5.206埃及3.249埃。故而可以得知，非極性m面()氧化鋅磊晶層與鋁酸鑭單晶氧化物(112)平面其晶格不匹配度(%)在平行c軸方向為(5.206-5.360)/5.360=-2.9%，在垂直c軸方向則為(3.249x2-6.566)/6.566=-1.0%。與習知相較，本發明之基板與磊晶層間具有極低的晶格不匹配度，且該基板在高溫時仍能維持熱穩定性，作為適於成長m面氧化鋅或III族氮化物磊晶層。
綜合上述，本發明係藉前述以單晶氧化物作為基板成長非極性m面磊晶層之方法，由於基板與磊晶層間具有極低晶格不匹配度，並使用在高溫時仍能維持熱穩定性之基板，來作為適於成長m面氧化鋅或III族氮化物磊晶層。且根據前述方法所生成具有非極性m面之磊晶層，其並具有避免磊晶層中因原子排列而產生極化效應導致價電帶與導電帶之偏移，而使發光量子效率降低之情形。不僅可廣泛地應用在藍光到紫外光之固態發光元件及雷射二極體等領域中，亦可藉消除其極化效應來提生量子效率而大幅增加其發光量子效率。
上述實施例僅係為了方便說明而舉例而已，本發明所主張之權利範圍自應以申請專利範圍所述為準，而非僅限於上述實施例。
圖1為本發明較佳實施例中成長非極性m面氧化鋅磊晶層示意圖。
圖2(a)及圖2(b)為本發明較佳實施例中非極性m面氧化鋅磊晶層之X-Ray繞射分析。
圖3(a)及圖3(b)為鋁酸鑭單晶氧化物(112)平面及非極性m面()氧化鋅磊晶層之表層原子鍵結關係圖。
Claims (18)
- 一種以單晶氧化物作為基板成長非極性m面磊晶層之方法，包括：提供一具有鈣鈦礦結構之單晶氧化物；選擇該單晶氧化物之密勒指數為{112}之平面作為一基板；以及在該基板上以氣相沉積法生長一具有纖鋅礦結構半導體之非極性m面磊晶層。
- 如申請專利範圍第1項所述之方法，更包括於該單晶氧化物上形成一氧化物層，並選擇該氧化物層之密勒指數為{112}之平面作為該基板，在該基板上以氣相沉積法生長一具有纖鋅礦結構半導體之非極性m面磊晶層；其中，該氧化物層之組成係與該單晶氧化物相同或不同。
- 如申請專利範圍第1或2項所述之方法，其中，該基板與該非極性m面磊晶層間之晶格常數不匹配度係小於10%。
- 如申請專利範圍第1或2項所述之方法，其中，該單晶氧化物係為鋁酸鑭(LaAlO3 )、鈦酸鍶(SrTiO3 )、鑭鍶鋁鉭氧(LaSrAlTaO3 )、或晶格常數相較鋁酸鑭在10%內之鋁酸鑭合金。
- 如申請專利範圍第1或2項所述之方法，其中，該非極性m面磊晶層係為氧化鋅、或III族氮化物。
- 如申請專利範圍第5項所述之方法，其中，該氧化鋅更包括摻雜有鎂、鈣、鍶、鋇、鎘、鋁、鎵、銦、或其組合之合金。
- 如申請專利範圍第5項所述之方法，其中，該III族氮化物係為氮化鎵、氮化銦、氮化鋁、氮化銦鎵、氮化鋁鎵、氮化鋁銦、或氮化鋁銦鎵。
- 如申請專利範圍第1或2項所述之方法，其中，該氣相沉積法係為物理氣相沉積法或化學氣相沉積法，包括脈衝雷射鍍膜法、濺射法、電子束(熱)蒸鍍法、或有機金屬化學氣相沉積法。
- 如申請專利範圍第1或2項所述之方法，其中，在該基板上以氣相沉積法生長該非極性m面磊晶層之前，更包括有一使用熱丙酮及異丙醇清潔該基板之步驟。
- 一種具有非極性m面之磊晶層，其係以下列方法而得，包括：提供一具有鈣鈦礦結構之單晶氧化物；選擇該單晶氧化物之密勒指數為{112}之平面作為一基板；以及在該基板上以氣相沉積法生長一具有纖鋅礦結構半導體之非極性m面磊晶層。
- 如申請專利範圍第10項所述之方法，更包括於該單晶氧化物上形成一氧化物層，並選擇該氧化物層之密勒指數為{112}之平面作為該基板，在該基板上以氣相沉積法生長一具有纖鋅礦結構半導體之非極性m面磊晶層； 其中，該氧化物層之組成係與該單晶氧化物相同或不同。
- 如申請專利範圍第10或11項所述具有非極性m面之磊晶層，其中，該基板與該非極性m面磊晶層間之晶格常數不匹配度係小於10%。
- 如申請專利範圍第10或11項所述具有非極性m面之磊晶層，其中，該單晶氧化物係為鋁酸鑭(LaAlO3 )、鈦酸鍶(SrTiO3 )、鑭鍶鋁鉭氧(LaSrAlTaO3 )、或晶格常數相較鋁酸鑭在10%內之鋁酸鑭合金。
- 如申請專利範圍第10或11項所述具有非極性m面之磊晶層，其中，該非極性m面磊晶層係為氧化鋅、或III族氮化物。
- 如申請專利範圍第14項所述具有非極性m面之磊晶層，其中，該氧化鋅更包括摻雜有鎂、鈣、鍶、鋇、鎘、鋁、鎵、銦、或其組合之合金。
- 如申請專利範圍第14項所述具有非極性m面之磊晶層，其中，該III族氮化物係為氮化鎵、氮化銦、氮化鋁、氮化銦鎵、氮化鋁鎵、氮化鋁銦、或氮化鋁銦鎵。
- 如申請專利範圍第10或11項所述具有非極性m面之磊晶層，其中，該氣相沉積法係為物理氣相沉積法或化學氣相沉積法，包括脈衝雷射鍍膜法、濺射法、電子束(熱)蒸鍍法、或有機金屬化學氣相沉積法。
- 如申請專利範圍第10或11項所述具有非極性m面之磊晶層，其中，在該基板上以氣相沉積法生長一具有 非極性m面之磊晶層之前，更包括有一使用熱丙酮及異丙醇清潔該基板之步驟。
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