原子级制造赋能非晶材料趋向性能极限

罗鹏; 赵睿; 沈来权; 孙永昊; 曹乘榕; 鲁振; 孙保安; 白海洋; 汪卫华

doi:10.7498/aps.74.20250862

摘要

非晶材料因其跨尺度结构均一性, 规避了传统晶体材料晶格缺陷敏感的固有特性, 在众多高技术领域具有不可替代的重要应用. 然而, 由于处于热力学非平衡态, 非晶材料会发生趋于平衡态的结构弛豫, 导致服役过程中的性能退化甚至失效. 此外, 非晶结构的无序性、复杂性伴随产生玻色峰与隧穿二能级系统等低能激发模式, 引发材料内耗与热噪声, 制约其在高端技术设备中的性能表现. 因此, 如何有效提升非晶材料的稳定性、抑制低能激发, 成为突破其性能极限的关键所在. 近年来研究发现, 基于材料表面动力学特性的原子级制造, 可成功制备超稳非晶材料, 实现对非晶材料微观结构、稳定性及低能激发进行常规方法难以企及的有效调控. 超稳非晶材料所具有的独特优势使其在引力波探测等尖端领域展现出巨大的应用潜力. 本文将深入探讨非晶材料中原子级制造的机理, 重点阐述超稳非晶材料相较于普通非晶材料的结构特征与性能优越性, 并展望原子级制造在非晶材料和物质领域未来的研究方向与发展趋势.

关键词:

Abstract

Amorphous materials avoid the inherent sensitivity to defects in traditional crystalline materials due to their cross-scale structural uniformity. Therefore, they have irreplaceable and important applications in many advanced technical fields. However, due to their thermodynamically non-equilibrium nature, amorphous materials experience structural relaxation towards equilibrium, leading to performance degradation or even failure during use. Additionally, the complex and disordered structure of amorphous materials results in low-energy excitation, such as boson peaks and tunneling two-level systems, which can cause internal friction and thermal noise in the materials. These factors significantly limit their performance in advanced technical applications. Therefore, effectively improving the stability of amorphous materials and suppressing low-energy excitation are key steps towards breaking through their performance limits. Recent studies have shown that atomic-level fabrication based on enhanced surface dynamics can successfully produce ultrastable amorphous materials, achieving unprecedented control over their microstructure, stability, and low-energy excitation, far exceeding the level achievable by traditional methods. The exceptional advantages of ultrastable amorphous materials endow them with significant application potential in advanced domains such as gravitational wave detection. This article delves into the underlying mechanisms of atomic-level fabrication for amorphous materials, highlighting their structural features and superior performances compared with traditional amorphous materials, and it also outlines future research directions and development trends of atomic-level fabrication in this field.

Keywords:

作者及机构信息

1.
中国科学院物理研究所, 极端条件物理重点实验室, 北京　100190

2.
中国科学院大学物理学院, 北京　100049

3.
松山湖材料实验室, 东莞　523808

4.
中国科学院大学材料科学与光电技术学院, 北京　100049

通信作者: 罗鹏, pengluo@iphy.ac.cn ; 白海洋, hybai@iphy.ac.cn ;

基金项目: 国家自然科学基金(批准号: 52192601, 52192602, 62488201)资助的课题.

Authors and contacts

1.
Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China

2.
School of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China

3.
Songshan Lake Materials Laboratory, Dongguan 523808, China

4.
College of Materials Science and Opto-Electronic Technology, University of Chinese Academy of Sciences, Beijing 100049, China

Corresponding author: LUO Peng, pengluo@iphy.ac.cn ; BAI Haiyang, hybai@iphy.ac.cn ;

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 52192601, 52192602, 62488201).

文章全文

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施引文献

图 1 非晶材料的表面动力学特性　(a)晶体表面可移动吸附原子和(b)非晶表面流动层示意图^[28], 可流动部分以红色标示; (c) IMC液态及玻璃态的表面与体相扩散系数^[29]; (d)非晶材料表面弛豫速率随温度的变化^[30]; (e)低能离子辐照作用下非晶和晶体合金表面形貌^[31]

Fig. 1. Surface dynamic characteristics of amorphous materials: Schematics of (a) mobile adatoms on a crystal surface and (b) the surface mobile layer of an amorphous material^[28] with movable parts marked in red; (c) surface and bulk diffusion coefficients of IMC liquid and glass^[29]; (d) surface relaxation rate of amorphous materials as a function of temperature^[30]; (e) surface morphology of amorphous and crystalline alloys under low-energy ion irradiation^[31].

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图 2 超稳非晶的均匀结构与去玻璃化转变特性　(a)普通非晶合金STEM照片^[62]; (b) 普通非晶整体协同弛豫方式去玻璃化转变示意图; (c) 超稳非晶合金STEM照片^[62]; (d) 超稳非晶前沿生长方式去玻璃化转变示意图; (e) TPD超稳非晶薄膜在T_g + 3 K等温退火过程中由表面开始形成的过冷液体厚度随时间的变化

Fig. 2. Homogeneous structure and devitrification behavior of ultrastable amorphous materials: (a) STEM image of a conventional amorphous alloy^[62]; (b) schematic illustration of the devitrification process via collective relaxation in a conventional amorphous material; (c) STEM image of an ultrastable amorphous alloy^[62]; (d) schematic illustration of the devitrification process via front growth in an ultrastable amorphous material; (e) temporal evolution of the thickness of supercooled liquid layer initiated from the surface in an ultrastable TPD amorphous film during isothermal annealing at T_g + 3 K.

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图 3 超稳非晶材料的SE和DSC表征　(a) 通过SE测量TPD薄膜的归一化厚度随温度变化曲线, 薄膜分别由298 K退火1周以及在T_dep = 298 K利用PVD制备^[32]; (b) 根据DSC测量计算得出的TNB和IMC薄膜的焓值随温度变化曲线, 薄膜分别由PVD、液相冷却以及退火方式制备^[52]

Fig. 3. SE and DSC characterization of ultrastable amorphous materials: (a) Normalized thickness vs. temperature for TPD films produced by annealing at 298 K for 1 week and by PVD at T_dep = 298 K, measured using SE^[32]; (b) enthalpy vs. temperature, calculated from DSC measurements, for TNB and IMC films, produced by PVD, liquid cooling, and annealing^[52].

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图 4 通过PVD制备的接近理想玻璃状态的乙苯超稳非晶^[87]

Fig. 4. Ultrastable amorphous ethylbenzene prepared by PVD that approaches the ideal glass state^[87].

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图 5 超稳非晶材料的低能激发　(a) 甲苯超稳非晶和普通非晶的介电弛豫谱^[93]; (b) IMC超稳非晶和普通非晶以及晶体的低温比热^[58]; (c) TPD超稳非晶和普通非晶与晶体比热的差值^[55]; (d) 1.1亿年前的琥珀的低温比热^[104]

Fig. 5. Low-energy excitation of ultrastable amorphous materials: (a) Dielectric relaxation spectra of ultrastable and ordinary amorphous toluene^[93]; (b) low-temperature specific heat of ultrastable, ordinary, and crystalline IMC^[58]; (c) specific heat of ultrastable and ordinary amorphous TPD after subtracting its value for the crystalline state^[55]; (d) low-temperature specific heat of a 110-million-year-old amber^[104].

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图 6 TPD超稳非晶的微观结构^[105]　(a) 不同衬底温度沉积的薄膜和液体冷却形成的薄膜的2D GIWAXS谱; (b) GIWAXS和SE测量的序参量随衬底温度的变化; (c) 层状结构衍射峰强度随衬底温度的变化

Fig. 6. Microstructure of ultrastable amorphous TPD^[105]: (a) 2D GIWAXS spectra of films deposited at different substrate temperatures and prepared by liquid cooling; (b) order parameters measured by GIWAXS and SE vs. substrate temperature; (c) intensity of layering structure vs. substrate temperature.

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图 7 非晶材料表面动力学梯度　(a) T_g随薄膜厚度的变化^[33]; (b) 具有高运动能力的表面层厚度随温度的变化^[126]; (c) 不同厚度薄膜的表面扩散系数(左轴)和平均α弛豫时间(右轴)的Arrhenius图^[33]

Fig. 7. Dynamic gradient at the surface of amorphous materials: (a) Variation of T_g as a function of film thickness^[33]; (b) thickness of surface layer with high mobility vs. temperature^[126]; (c) Arrhenius plot of surface diffusion coefficient (left axis) and average α-relaxation time (right axis) of films with various thicknesses^[33].

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图 8 表面结构重排与速率-温度等效原理　(a) 沉积分子的取向序参量P₁(z)随距离表面深度的演化^[121]; (b) 在293 K下, 双折射率随基于平移因子为17 K/10倍频的速率-温度等效原理计算得到的有效沉积速率的变化^[111]

Fig. 8. Surface structure rearrangement and rate–temperature superposition principle: (a) Evolution of the orientation order parameter P₁(z) of the deposited molecules as a function of depth from the surface^[121]; (b) birefringence vs. an effective deposition rate at 293 K calculated by applying the rate–temperature superposition principle using a shift factor of 17 K/decade^[111].

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图 9 PVD过程中介电损耗的变化^[130], 沉积开始于t = 0 s, 终止于 t = 1158 s, 插图为沉积终止后, 随着时间的推移介电损耗的降低情况(以对数时间尺度表示), 变化情况以沉积初始阶段快速上升幅度的百分比来表示, 主图中的竖条对应数值为100%

Fig. 9. Evolution of dielectric dissipation during PVD process^[130], the deposition starts at t = 0 s and ends at t = 1158 s, the inset shows the reduction of dissipation after the deposition had stopped on a logarithmic time scale, here, the change is shown as percentage of the initial fast rise, with 100% being indicated by the vertical bar in the main frame.

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图 10 在T_dep < T_g (bulk)时, 表面介导的超稳非晶形成过程示意图, 棒状结构示意非球形分子的择优取向, 虚线表示T_g(local) = T_dep的位置, 薄膜可划分为从上至下的4个特征区域, 其主要的动力学行为分别为侧向表面扩散、平衡态弛豫、加速老化及动力学冻结的体相状态^[25]

Fig. 10. Schematic illustration of surface-mediated formation of ultrastable amorphous materials at T_dep < T_g (bulk), the rod-like shapes illustrate the preferred orientation of nonspheroidal molecules. The dashed line denotes the position where T_g(local) = T_dep, the film can be divided into four possible regions from top to bottom, with the dynamics dominated by: lateral surface diffusion, equilibrium relaxation, accelerated aging, and kinetically arrested bulk state^[25].

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图 11 不同衬底温度和沉积速率条件下表面介导形成超稳非晶的动力学过程示意图　(a) 在一定沉积速率(R_dep)下密度变化与T_dep的关系; (b)—(e) 表面区域内的动力学过程随着T_dep和 R_dep的演变, 虚线表示T_g(local) = T_dep的位置^[25]

Fig. 11. Schematic illustration of dynamical processes at play during surface-mediated formation of ultrastable amorphous materials at different T_dep and R_dep: (a) A representative sketch of the density change vs. T_dep at a constant deposition rate (R_dep); (b)–(e) evolution of the dynamic processes within surface region with T_dep and R_dep, dashed line denotes the position where T_g(local) = T_dep^[25].

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图 12 软衬底对超稳非晶的影响^[84]　(a) 在硅衬底和PDMS软衬底上沉积的薄膜相对密度随衬底温度和沉积速率的变化; (b) PVD薄膜相对密度随PDMS衬底弹性模量的变化; (c) 在硅衬底上沉积的薄膜的2D GIWAXS谱; (d) 在PDMS软衬底上沉积的薄膜的2D GIWAXS谱

Fig. 12. Effect of soft substrates on ultrastable amorphous materials^[84]: (a) Relative density as a function of substrate temperature and deposition rate for films deposited on silicon substrates and soft PDMS substrates; (b) relative density of PVD films vs. elastic modulus of PDMS substrates; (c) 2D GIWAXS spectrum of the film deposited on silicon substrate; (d) 2D GIWAXS spectrum of the film deposited on soft PDMS substrate.

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map

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