TW201409703A - 電子裝置、積層構造體及其製造方法 - Google Patents

電子裝置、積層構造體及其製造方法 Download PDF

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TW201409703A
TW201409703A TW102116375A TW102116375A TW201409703A TW 201409703 A TW201409703 A TW 201409703A TW 102116375 A TW102116375 A TW 102116375A TW 102116375 A TW102116375 A TW 102116375A TW 201409703 A TW201409703 A TW 201409703A
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graphene
layer
substrate
laminated structure
transition metal
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Junichi Yamaguchi
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Nat Inst Of Advanced Ind Scien
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Abstract

積層構造體包含：絕緣基板、形成於絕緣基板上之石墨烯層、及形成於石墨烯層上且由遷移金屬氧化物、例如Cr2O3所構成之保護膜。藉此，石墨烯之轉印時，光阻劑等之高分子材料不會直接接觸石墨烯，可抑制因光阻劑之高分子殘留物造成往石墨烯之非本質的載體摻雜。

Description

電子裝置、積層構造體及其製造方法 發明領域
本發明是有關於一種使用石墨烯之電子裝置、積層構造體及其製造方法。
發明背景
將藉由化學氣相沈積法(CVD法)、或者SiC基板之熱分解處理法而形成之石墨烯片利用於電晶體等之電子元件時，需要將石墨烯由成長基板轉印到絕緣體基板的製程。例如專利文獻1中，公開了如以下的轉印製程。採用了方法如下：在藉由CVD法形成於觸媒層上之石墨烯上，形成聚甲基丙烯酸酯(PMMA)、光阻劑、電子束光阻劑等之保護層後、形成由壓克力樹脂、環氧樹脂、熱剝離膠帶、黏著膠帶等構成之支持層。接著，在支持層/保護層/石墨烯層/觸媒層中，將觸媒層濕蝕刻，藉此由成長基板剝離支持層/保護層/石墨烯層，轉印到其他絕緣體基板後、除去支持層/保護層。另一方面，專利文獻2、3中，揭示了在電晶體之通道層將高介電體材料(high-k材料)利用到石墨烯、閘極絕緣層之電場效果電晶體之製造技術。
習知技術文獻 專利文獻
【專利文獻1】日本專利特開2011-105590號公報
【專利文獻2】日本專利特開2011-175996號公報
【專利文獻3】日本專利特開2011-114299號公報
發明概要
一般廣泛使用之石墨烯的轉印製程中，轉印時之石墨烯的保護層是使用以高分子材料構成之各種光阻劑劑。然而，會擔心高分子材料在除去處理後也會成為殘留物而殘留於石墨烯上，尤其是若高分子殘留物吸附於石墨烯之邊緣部分或局部缺陷部分時，被認為其除去是非常困難的。該等高分子殘留物會誘發往石墨烯之非本質的障壁摻雜。因此，例如將石墨烯使用於通道之石墨烯電晶體中，成為電傳導特性劣化及不安定動作的原因。
進而，為了有效率地控制石墨烯電晶體之載體濃度，需要更大的閘極容量，因此HfO2等之高介電體材料(high-k材料)使用作為閘極絕緣層。然而，high-k材料之薄膜難以直接形成於石墨烯上，需要將high-k材料之閘極絕緣層形成某種程度的厚度。由於愈增加閘極絕緣層之膜厚，閘極容量會愈減少，因此期望high-k材料之閘極絕緣層的薄膜化。又，從電晶體之低電壓動作的觀點來看，也需要high-k材料之閘極絕緣層之薄膜化。
本發明是有鑑於前述之課題而作成者，其目的在 於提供一種石墨烯轉印時，光阻劑等之高分子材料不會直接接觸到石墨烯，可抑制光阻劑之高分子殘留物造成往石墨烯之非本質的載體摻雜之積層構造體及其製造方法；及藉以前述之積層構造體構成電子裝置，可實現電特性之提升及安定動作，提供信賴性高之電子裝置。進而，其目的在於提供一種在前述之電子裝置中，形成於石墨烯膜上且由遷移金屬氧化物構成之保護層發揮high-k材料之閘極絕緣層之晶種層之效果，並且可使high-k材料之閘極絕緣層薄膜化，實現石墨烯膜之載體濃度之控制效率提升及低電壓動作的電子裝置。
本發明之電子裝置包含有：基板；石墨烯膜，形成於前述基板上；保護膜，形成於前述石墨烯膜上，且由遷移金屬氧化物構成；絕緣層，形成於前述保護膜上；及電極，形成於前述絕緣層上。
本發明之積層構造體之製造方法包含有下述步驟：於成長基板上形成觸媒；使用前述觸媒在前述成長基板上形成石墨烯膜；於前述石墨烯膜上形成由遷移金屬氧化物構成之保護膜；及將前述石墨烯膜及前述保護膜自前述成長基板剝離而轉印於基板上。
本發明之積層構造體包含有：基板；形成於前述基板上之石墨烯膜；及形成於前述石墨烯層上且由遷移金屬氧化物構成之保護膜。
根據本發明，可實現在石墨烯之轉印時，光阻劑等之高分子材料不會直接接觸於石墨烯，且可抑制光阻劑之高分子殘留物往石墨烯之非本質的載體摻雜的積層構造體。
根據本發明，藉以前述之積層構造體構成電子裝置，實現電氣特性之提升及安定動作，可得到信賴性高之電子裝置。進而，在前述之電子裝置中，由形成於石墨烯膜上之遷移金屬氧化物構成的保護層可發揮high-k材料之閘極絕緣層之晶種層之功能，可使high-k材料之閘極絕緣層之薄膜化，實現石墨烯膜之載體濃度之控制效率之提升及低電壓動作。
11‧‧‧成長基板
12‧‧‧觸媒層
13‧‧‧石墨烯層
14‧‧‧保護層
14a,14b‧‧‧電極形成部
15‧‧‧黏著層
16‧‧‧支持層
17‧‧‧絕緣基板
21‧‧‧源極電極
22‧‧‧汲極電極
23‧‧‧閘極絕緣層
24‧‧‧閘極電極
圖1A係顯示第1實施形態之積層構造體之製造方法的概略截面圖。
圖1B係接續圖1A，顯示第1實施形態之積層構造體之製造方法的概略截面圖。
圖1C係接續圖1B，顯示第1實施形態之積層構造體之製造方法的概略截面圖。
圖2A係接續圖1C，顯示第1實施形態之積層構造體之製造方法的概略截面圖。
圖2B係接續圖2A，顯示第1實施形態之積層構造體之製造方法的概略截面圖。
圖2C係接續圖2B，顯示第1實施形態之積層構造體之 製造方法的概略截面圖。
圖3A係第2實施形態之石墨烯電晶體之製造方法之主要製程的概略截面圖。
圖3B係接續圖3A，顯示第2實施形態之石墨烯電晶體之製造方法之主要製程的概略截面圖。
圖3C係接續圖3B，顯示第2實施形態之石墨烯電晶體之製造方法之主要製程的概略截面圖。
圖4A係接續圖3C，顯示第2實施形態之石墨烯電晶體之製造方法之主要製程的概略截面圖。
圖4B係接續圖4A，顯示第2實施形態之石墨烯電晶體之製造方法之主要製程的概略截面圖。
較佳實施例之詳細說明
以下，參照圖式詳細說明適用本發明之較佳各實施形態。
(第1實施形態)
本實施形態中，就使用了石墨烯之積層構造體一併說明其製造方法。圖1A~圖2C係依製程順序顯示第1實施形態之積層構造體之製造方法的概略截面圖。
首先，如圖1A所示，使用濺鍍法在成長基板11上堆積觸媒層12。
成長基板11使用表面形成有膜厚100nm~300nm左右之熱氧化膜之Si基板。觸媒層12使用膜厚為500nm~1μm左右之Cu。除了Cu之外，包含Fe、Co、Ni、Ru、Pt中任1種之 金屬材料也可利用作為觸媒層。
接著，如圖1B所示，使用觸媒層12形成石墨烯層13。
使用CVD法，在以Ar稀釋之氫(H2)環境中，以約800℃對觸媒層12/成長基板11進行加熱處理，並在保持同溫度之狀態下，導入CH4作為源氣體。藉此，形成石墨烯層13。在此，石墨烯層13形成為單層、或者2層。源氣體除了CH4之外，可利用包含C之C2H2、C2H4、CO等。
接著，如圖1C所示，在石墨烯層13上形成由遷移金屬氧化物構成之保護層14。
使用電子線蒸鍍法，在石墨烯層13上將遷移金屬堆積到1nm~5nm左右之厚度，形成遷移金屬膜。石墨烯層13上之遷移金屬薄膜會因為曝露於大氣中造成之自然氧化、或者在氧環境中施行低溫熱處理(200℃~300℃左右)而氧化，形成保護層14。
其他，在石墨烯層13上直接形成遷移金屬氧化物之保護層14的方法亦可使用原子層堆積法(ALD法)、濺鍍法、脈衝雷射堆積法(PLD法)等。遷移金屬材料必須具有容易氧化之物性、及進而難以與構成石墨烯之C化學結合、即難以碳化之物性二者。遷移金屬(氧化物)材料可使用例如、Sc(Sc2O3)、Cr(Cr2O3)、Mn(MnO2)、Co(CoO)、Zn(ZnO)、Y(Y2O3)、Zr(ZrO2)、Mo(MoO3)、Ru(RuO2)。
本實施形態中，在石墨烯層13上以電子線蒸鍍法堆積Cr後，將自然氧化之Cr2O3使用於保護層14。Ti容易氧 化而成為TiO2是廣為人知，但若將Ti堆積於石墨烯上時，在Ti/石墨烯界面會形成TiCx而破壞石墨烯之結晶性。因此，TiO2作為保護層之材料並不有用。
接著，如圖2A所示，依序在保護層14上形成黏著層15及支持層16。
在保護層14上依序將1μm~2μm左右之厚度之光阻劑劑及100μm~500μm左右之厚度之壓克力樹脂旋轉塗覆。藉此，在保護層14上形成黏著層15及支持層16。黏著層15除了光阻劑劑之外，亦可使用PMMA、電子束光阻劑等。又，支持層16除了壓克力樹脂之外，亦可使用環氧樹脂、熱剝離膠帶、黏著膠帶等。
接著，使用BHF將成長基板11之熱氧化膜進行濕蝕刻，並以觸媒層12、石墨烯層13、保護層14、黏著層15及支持層16為一體自成長基板11剝離。
接著，由成長基板11剝離之觸媒層12、石墨烯層13、保護層14、黏著層15及支持層16之中，對觸媒層12進行濕蝕刻並除去。蝕刻劑時使用FeCl3水溶液或稀釋HCl。要除去觸媒層12，除了濕蝕刻之外，亦可利用反應性離子蝕刻、離子銑等之乾蝕刻。在經除去觸媒層12之石墨烯層13、保護層14、黏著層15及支持層16，使用純水施行沖洗洗淨處理。
接著，如圖2B所示，將石墨烯層13、保護層14、黏著層15及支持層16轉印於絕緣基板17上。
將業經沖洗洗淨處理之石墨烯層13、保護層14、黏著 層15及支持層16，以石墨烯層13與轉印目的地之絕緣基板17接觸之方向，轉印於絕緣基板17之表面。然後、藉由支持層16之上面朝向絕緣基板17施加一樣的應力，提高石墨烯層13與絕緣基板17之黏著性。轉印目的地之絕緣基板17，使用表面形成有90nm左右之厚度之熱氧化膜的Si基板。該熱氧化膜具有絕緣機能。絕緣基板17除了需要表面之平坦性之外，對於材質等沒有特別限制，亦可利用例如藍寶石基板、石英基板、MgO基板、PET基板等。
接著，如圖2C所示，於絕緣基板17上形成具有石 墨烯層13及保護層14之積層構造體。
在轉印到絕緣基板17後，在石墨烯層13、保護層14、黏著層15及支持層16中，除去黏著層15及支持層16。若於支持層16使用壓克力樹脂、於黏著層15使用光阻劑時，則將該等浸漬於約70℃之丙酮後除去，並使用異丙醇、或者乙醇施行沖洗洗淨處理。藉由上述，於絕緣基板17上形成具有石墨烯層13及保護層14之積層構造體。
如以上所說明，根據本實施形態，在石墨烯膜13 之轉印時，光阻劑等之高分子材料不會直接接觸到石墨烯膜13，可抑制因為光阻劑之高分子殘留物造成對石墨烯膜13之非本質的載體摻雜，可實現具有石墨烯膜13之信賴性高的積層構造體。
(第2實施形態)
本實施形態中，就使用第1實施形態之積層構造體的電子裝置，例示石墨烯電晶體，並且一併說明其構成及製造 方法。圖3A~圖4B係依序顯示第2實施形態之石墨烯電晶體之製造方法之主要製程的概略截面圖。
準備第1實施形態之在絕緣基板17上具有石墨烯 層13及保護層14之積層構造體。如圖3A所示，在積層構造體之中，將石墨烯層13及保護層14加工成電晶體之所期望之通道尺寸。
具體而言，使用電子束微影術，於所期望之通道尺寸將電子束光阻劑圖案化，將電子束光阻劑作為光遮罩，對石墨烯層13及保護層14進行蝕刻。對Cr2O3之保護層14，進行將硝酸第二鈰銨、或加熱到約50℃左右之HNO3及HCl之混合水溶液作為蝕刻劑之濕蝕刻。然後，對石墨烯層13，進行O2電漿之乾蝕刻。通道尺寸寬度為100nm~1μm左右、長度為1μm~5μm左右。
接著，如圖3B所示，將保護層14蝕刻形成電極形 成部14a,14b。
將保護層14之兩端部位進行濕蝕刻，形成電極形成部14a,14b。由電極形成部14a,14b露出石墨烯層13，後述之源極電極及汲極電極電接觸於該石墨烯層13之露出部位，降低導電電阻。
接著，如圖3C所示，形成源極電極21及汲極電極 22。
藉由電子束微影術，在保護層14上形成包含電極形成部14a,14b之區域開口之光遮罩，將電極金屬、例如Pd蒸鍍成50nm左右之厚度。藉由剝離，除去光遮罩及其上之Pd。 藉由上述，形成與在石墨烯層13之電極形成部14a,14b露出之部位電連接之源極電極21及汲極電極22。電極材料亦可使用於其他Cr、Ni、Pt之單層電極、或者Au/Ti等之二層電極。又，電極之成膜方法沒有特別限制，除了蒸鍍法以外，可使用PLD法、測鍍等。
接著，如圖4A所示，在保護層14上形成由高介 電體材料(high-k材料)構成之閘極絕緣層23。
使用ALD法，在保護層14上堆積high-k材料、在此將HfO2堆積成5nm~50nm左右、宜為5nm~10nm左右，藉此堆積成5nm左右之厚度。藉此，於保護層14上形成閘極絕緣層23。
據說high-k材料之薄膜難以直接形成於石墨烯上。本實施形態中，於石墨烯層13上形成由遷移金屬氧化物構成之保護層14，於保護層14上形成閘極絕緣層23。因此，閘極絕緣層23可薄膜化。即、保護層14不僅具有保護轉印製程時之石墨烯層13的機能，也作為用以形成由high-k材料構成之較薄的閘極絕緣層23之晶種層之機能。high-k材料亦可使用於其他Al2O3、Si3N4、HfSiO、HfAlON、Y2O3、SrTiO3、PbZrTiO3、BaTiO3等。又，成膜方法也可因應於high-k材料之種類而適當選擇CVD法、蒸鍍法、ALD法、PLD法、濺鍍等。
接著，如圖4B所示，於閘極絕緣層23上形成閘極 電極24。
藉由與源極電極21及汲極電極22之形成相同的方法， 在閘極絕緣層23上形成50nm左右之厚度之由Pd構成之閘極電極24。藉由上述，可得到上閘極型之石墨烯電晶體。
根據本實施形態，使用在第1實施形態得到之積 層構造體構成石墨烯電晶體，實現電特性的提升及安定動作，可得到信賴性高之石墨烯電晶體。進而，石墨烯電晶體中，形成於石墨烯膜13上且由遷移金屬氧化物構成之保護層14發揮high-k材料之閘極絕緣層23之晶種層之效果，可使閘極絕緣層23薄膜化，並可實現石墨烯膜13之載體濃度之控制效率之提升及低電壓動作。
再者，本實施形態中，使用第1實施形態之積層 構造體的電子裝置係例示石墨烯電晶體，但本發明不限定於此。例如、可將積層構造體適用於使用於顯示電極之顯示器等。
以下，整理電子裝置、積層構造體及其製造方法 之各態樣且記載為附記。
(附記1)一種電子裝置，其特徵在於包含有： 基板；石墨烯膜，形成於前述基板上；保護膜，形成於前述石墨烯膜上，且由遷移金屬氧化物構成；絕緣層，形成於前述保護膜上；及電極，形成於前述絕緣層上。
(附記2)如附記1所記載之電子裝置，其中前述 絕緣層由高介電體材料構成。
(附記3)如附記2所記載之電子裝置，其中前述 絕緣層之厚度為5nm~10nm之範圍內之值。
(附記4)如附記1~3之任一項所記載之電子裝 置，其中構成前述保護膜之遷移金屬氧化物之遷移金屬係選自於Sc、Cr、Mn、Co、Zn、Y、Zr、Mo、Ru之1種。
(附記5)一種積層構造體之製造方法，其特徵 在於包含有下述步驟：於成長基板上形成觸媒；使用前述觸媒在前述成長基板上形成石墨烯膜；於前述石墨烯膜上形成由遷移金屬氧化物構成之保護膜；及將前述石墨烯膜及前述保護膜自前述成長基板剝離而轉印於基板上。
(附記6)如附記5所記載之積層構造體之製造方 法，其中構成前述保護膜之遷移金屬氧化物之遷移金屬係選自於Sc、Cr、Mn、Co、Zn、Y、Zr、Mo、Ru之1種。
(附記7)一種積層構造體，其特徵在於包含有： 基板；形成於前述基板上之石墨烯膜；及形成於前述石墨烯層上且由遷移金屬氧化物構成之保護膜。
(附記8)如附記7所記載之積層構造體，其中構 成前述保護膜之遷移金屬氧化物之遷移金屬選自於Sc、Cr、Mn、Co、Zn、Y、Zr、Mo、Ru之1種。
產業上之可利用性
根據本發明，在石墨烯轉印時，光阻劑等之高分子材料不會直接接觸於石墨烯，可實現抑制因光阻劑之高分子殘留物往石墨烯之非本質的載體摻雜的積層構造體。
根據本發明，藉以前述之積層構造體構成電子裝置，實現電特性之提升及安定動作，可得到信賴性高之電子裝置。進而，在前述之電子裝置中，形成於石墨烯膜上且由遷移金屬氧化物構成之保護層發揮high-k材料之閘極 絕緣層之晶種層的效果，可使high-k材料之閘極絕緣層薄膜化，並實現提昇石墨烯膜之載體濃度之控制效率及低電壓動作。
11‧‧‧成長基板
12‧‧‧觸媒層
13‧‧‧石墨烯層
14‧‧‧保護層
15‧‧‧黏著層
16‧‧‧支持層
17‧‧‧絕緣基板

Claims (8)

  1. 一種電子裝置，其特徵在於包含有：基板；石墨烯膜，形成於前述基板上；保護膜，形成於前述石墨烯膜上，且由遷移金屬氧化物構成；絕緣層，形成於前述保護膜上；及電極，形成於前述絕緣層上。
  2. 如請求項1之電子裝置，其中前述絕緣層由高誘電體材料構成。
  3. 如請求項2之電子裝置，其中前述絕緣層之厚度為5nm~10nm之範圍內之值。
  4. 如請求項1之電子裝置，其中構成前述保護膜之遷移金屬氧化物之遷移金屬係選自於Sc，Cr，Mn，Co，Zn，Y，Zr，Mo，Ru之1種。
  5. 一種積層構造體之製造方法，其特徵在於包含有下述步驟：於成長基板上形成觸媒；使用前述觸媒在前述成長基板上形成石墨烯膜；於前述石墨烯膜上形成由遷移金屬氧化物構成之保護膜；及將前述石墨烯膜及前述保護膜自前述成長基板剝離而轉寫於基板上。
  6. 如請求項5之積層構造體之製造方法，其中構成前述保護膜之遷移金屬氧化物之遷移金屬係選自於Sc，Cr，Mn，Co，Zn，Y，Zr，Mo，Ru之1種。
  7. 一種積層構造體，其特徵在於包含有：基板；石墨烯膜，形成於前述基板上；及保護膜，形成於前述石墨烯層上且由遷移金屬氧化物構成。
  8. 如請求項7之積層構造體，其中構成前述保護膜之遷移金屬氧化物之遷移金屬係選自於Sc、Cr、Mn、Co、Zn、Y、Zr、Mo、Ru之1種。
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