近幾年來，如何改善塊狀金屬玻璃(bulk metallic glass)的脆性是一個很重要的議題。本研究中，藉由熱力學的計算，我們成功地製備出具有液態相分離結構的鋯鎳銅鋁(Zr63.8Ni16.2Cu15Al5)塊狀金屬玻璃。基於在均質的非晶結構中分佈著液態相分離，相分離鋯基塊狀金屬玻璃的壓縮塑性可以被改善至高達15%。透過研究不同壓縮應變量的相分離鋯基塊狀金屬玻璃，其結果顯示塊狀金屬玻璃變形方式為，先約2%的彈性變形，接著混亂眾多的剪切帶(shear band)會在變形初期形成，然後逐漸地發展成一個主要的剪切帶，並且此剪切帶幾乎支配整個塑性變形直到破壞之前。同時，沿著剪切平面上之主要剪切帶的局部應變會隨著越遠離剪切帶起始形成位置越遠而降低。為了更進一步地去分析此主要的剪切帶，影像紀錄器被應用來紀錄完整的試片變形的過程，根據影像結果發現，應力應變圖塑性區間中的鋸齒狀現象(Serration phenomenon)與影像中每次的剪切滑移有著一對一相符合的結果，說明這些鋸齒狀現象是由在變形的過程中試片間歇性的滑移所引起。

隨後，高取樣速度的應變量測計被使用來研究鈀基塊狀金屬玻璃(Pd40Ni40P20)之應力應變圖中的鋸齒狀現象與剪切帶傳播(shear band propagation)。由於兩片應變量測計是直接地黏貼在測試試片的兩側，故一旦剪切帶形成開始傳播時，兩側的應變量測計會立即補抓到一突然性的位移變化量。基於位移時間曲線，剪切帶傳播速度可以被量測並且發現此速度對外加應變速率並不敏感。在高應變速率下，鋸齒狀現象消失的原因並非是缺乏剪切帶的形成也並非是剪切帶速度改變，而只是因為突然性的位移變化量之訊號被運行中的外加應變速率所淹蓋過去。同時，利用此剪切帶傳播的速度可以計算出剪切帶傳播期間的剪切帶黏度，而此黏度值與一般在高溫過冷液體區間均勻變形下所得到的黏度值相似。比較五種不同的塊狀金屬玻璃，如脆性的鎂基、金基、銅基、延性的鈀基以及具有相分離的鋯基塊狀金屬玻璃，我們發現金屬玻璃的塑性與剪切帶傳播間的動態有著密切的關係，在本質上延展性越好的金屬玻璃其剪切帶傳播的速度會比較慢。

藉由添加二十五體積百分比的具孔隙性鉬顆粒來強化鎂基塊狀金屬玻璃，此鎂基塊狀金屬玻璃複材的塑性可以被改善至高達約10%，與一般文獻上沒有塑性能力的鎂基塊狀金屬玻璃有著很大的區別。然而，在應力應變圖的塑性區間中卻缺乏鋸齒狀的現象。使用應變量測計來研究此鎂基塊狀金屬玻璃複材的剪切帶傳播，結果亦顯示沒有補抓到任何突然性的位移變化量。基於此塊狀金屬玻璃複材微結構的形貌，鋸齒狀現象的消失與缺乏長程的剪切帶傳播有關。透過將一均質玻璃基地區分成許多的分隔區塊，在目前的鎂基塊狀金屬玻璃複材中，只有短程的剪切帶傳播在運行著。考慮強化相顆粒之間的間距以及強化相顆粒的尺寸大小，我們提出一個模型可以成功地解釋塊狀金屬玻璃複材裡剪切帶傳播的發展，同時，此模型對於在設計具延展性的金屬玻璃複材來說將會是個有助益的指標。

On the toughening of bulk metallic glasses (BMGs), successful results in the phase-separated Zr63.8Ni16.2Cu15Al5 BMG have achieved compressive ductility over 15% through the computational-thermodynamic approach. In this study, the phase-separated Zr63.8Ni16.2Cu15Al5 BMG was compressed to nominal strains of 3%, 7%, and 10% at low strain rates (~10-4 s-1) and the results demonstrated that the BMG exhibited apparent uniform deformation initially, followed by visible local shear bands development. Afterwards, a single shear along the principal shear plane was soon developed and mainly dominated the whole deformation process. The principal shear contributed more than 2/3 of the overall plastic strain until failure. It was also found that the local shear strain varied along the principal shear plane and decreased monotonically from the shear band initiation site. Subsequently, in-situ compression experiments were conducted to monitor the change of sample shape during deformation in order to properly correlate with the stress-strain curve. The observed images showed that there was a one-to-one correspondence between the intermittent sample sliding and flow serration in the plastic region of stress-strain curve.

Further investigations on flow serration were conducted on the Pd40Ni40P20 BMG through the compression experiments equipped with high-sensitivity strain gauges directly attached to two opposite sides of the test sample. There was an accompanied displacement burst when a shear band starts to propagate during deformation and this displacement burst would be accurately captured by the high-sensitivity strain gauges. Based on the displacement-time profile for one serration, shear-band propagating speed can be estimated and found to be insensitive to the applied strain rates (or the applied crosshead speeds). The disappearance of flow serration at high strain rates should be a result that the signal of displacement burst was overwhelmed by the applied strain rate. Using the shear strain rate data, the measured viscosity within a propagating shear band was found to be relatively low, which is in similar to the viscosity values reported in the supercooled liquid region during homogeneous deformation. In comparison with shear band propagation in the brittle Mg58Cu31Y6Nd5 and Au49Ag5.5Pd2.3Cu26.9Si16.3, moderately ductile Cu50Zr43Al7 and Pd40Ni40P20, and highly ductile phased-separated Zr63.8Ni16.2Cu15Al5 systems, the ductility of BMGs appears to be closely related to the dynamics during shear band propagation. The more ductile in nature the metallic glass is, the slower the shear band propagating speed would become.

We also made attempts to investigate the shear band propagation in the porous Mo particles reinforced Mg58Cu28.5Gd11Ag2.5 bulk metallic glass composites (BMGCs) with up to 10% compressive failure strain. It was found that flow serration was absent in the stress-strain curve. Using high-sensitivity strain gauges, no distinct displacement burst was detected in the displacement-time profile. The diappearance of flow serration for the current porous Mo particles reinforced Mg58Cu28.5Gd11Ag2.5 BMGC is apparently associated with the lack of long-range shear band propagagtion. By employing the approach of separating the homogeneous amorphous matrix into many individual compartments, only short-range shear band propgagation is possible in the current Mg-based BMGC. An effective free spacing considering the spacing between two porous Mo particles and porous Mo particle size was applied to interpret the development of shear band propagation and is a useful indicator for the design of BMGC with high ductility.

Content i
List of Tables iv
List of Figures vi
中文摘要 xvi
Abstract xviii
Chapter 1 Introduction 1
1.1 Amorphous alloys 1
1.2 Early developments of metallic glasses 2
1.3 Birth of bulk metallic glasses 3
1.4 Status of bulk metallic glasses 4
1.5 Motivation 6
Chapter 2 Background 9
2.1 Evolution of fabrication methods 9
2.2 Systems of bulk metallic glasses 11
2.3 Indexes of glass forming ability 12
2.4 Empirical rules for the formation of amorphous alloys 16
2.5 Characterization of amorphous alloys 19
2.5.1 Mechanical properties 19
2.5.2 Magnetic properties 21
2.5.3 Chemical properties 22
2.5.4 Other properties 22
2.6 Mechanical behaviors of metallic glasses 23
2.6.1 Stress-strain curves and fracture morphologies 23
2.6.2 Temperature effect 25
2.6.3 Strain rate effect 27
2.6.4 Sample size effect 28
2.6.5 Geometric constraint effect 30
2.6.6 Reinforcement effect on BMG composites 31
2.7 Deformation mechanisms of metallic glasses 33
2.8 Fracture mechanisms of metallic glasses 36
Chapter 3 Experimental procedures 42
3.1 Raw materials 42
3.2 Computational thermodynamic approach 43
3.3 Sample preparations 44
3.3.1 Arc melting 45
3.3.2 Suction and injection casting 46
3.4 Identifications of amorphous nature 47
3.4.1 X-ray diffraction analyses 47
3.4.2 Qualitative and quantitative analyses 47
3.4.3 Thermal analyses 48
3.5 Mechanical tests 48
3.5.1 Micro-indentation tests 48
3.5.2 Compression tests 49
3.5.3 Compression tests using high-sensitivity strain gauges 50
3.6 Microstructure observations 51
Chapter 4 Results 53
4.1 Sample observations 53
4.2 Amorphous nature 53
4.2.1 SEM/EDS observations 53
4.2.2 XRD analyses 54
4.2.3 Thermal analyses 55
4.2.4 TEM microstructure observations 56
4.3 Mechanical tests in phase-separated Zr-based BMGs 57
4.3.1 Mechanical properties 57
4.3.2 Fracture characteristics 58
4.3.3 Compressed samples with various strains 60
4.3.4 Continuously strained sample 63
4.4 Mechanical tests in Pd-based BMGs 63
4.4.1 In-situ compression tests 63
4.4.2 Compression tests equipped with high-sensitivity strain gauges 65
4.5 Mechanical tests in the Mg-based BMGC 69
Chapter 5 Discussion 72
5.1 Plastic strain and deformation mode of BMGs 72
5.2 Local shear strain 76
5.3 Intermittent sample sliding 78
5.4 Local heating 81
5.6 Flow serration and shear band viscosity 86
5.7 Flow serration and shear band propagation 90
5.8 Flow serration in porous Mo particles reinforced Mg-based BMGC 94
Chapter 6 Conclusions 100
References 104
Tables 119
Figures 134

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