光诱导金属纳腔的相干声学振动及应用 下载: 1715次特邀综述
Metal nanoparticles exhibit superior optical resonances, known as localized surface plasmon resonances, due to collective oscillations of free electrons during their interaction with incident light. These resonances enhance light absorption and scattering, making these nanoparticles highly efficient in interacting with electromagnetic waves. The tunability of plasmon resonances through nanoparticle size, shape, and composition further enhances their optical responses. As a result, plasmonic nanoparticles are valuable for applications such as sensing, imaging, and energy conversion.
In addition to their optical resonances, metal nanoparticles also serve as acoustic resonators, capable of converting electromagnetic energy to mechanical energy through photoacoustic and optoacoustic effects. Excitation of metal nanoparticles by short laser pulses leads to rapid increases in electron and lattice temperatures, which generates thermal expansions and particle vibrations. The mechanical vibrations in metallic nanoresonators are influenced by factors such as nanoparticle size, shape, and surrounding environment. Accurate measurements of the acoustic vibrations provide insights into the mechanical properties of nanoresonators and the surroundings, with potential applications in nano-optomechanical devices, sensor technology, and photoacoustic imaging.
The vibrational frequencies of metallic nanoresonators typically range from a few to hundreds of GHz. Ultrafast pump-probe spectroscopy has emerged as a powerful tool for investigating these high-frequency mechanical vibrations. Due to the large absorption cross-section of plasmonic nanoparticles, it is feasible to study the acoustic vibrations in metallic nanoresonators at a single-particle level. In such experiments, a pump laser excites mechanical vibrations in single particles, and a delayed probe laser monitors the dynamics of the vibrations with high temporal resolutions. The ability to perform single-particle studies of acoustic vibrations provides new opportunities for understanding the vibrational energy damping mechanisms and mode coupling effects.
A significant issue related to metallic nanoresonators is energy loss, where the acoustic energy dissipates through both intrinsic and extrinsic damping pathways. Extending the vibrational lifetimes of acoustic nanoresonators is beneficial for nanomechanical spectrometry and sensing, vibrational coupling, and quantum state preparations. Many experimental studies primarily focus on the energy dissipation mechanisms in nanoresonators. Mass sensing, high-frequency biomechanics and bioimaging, and nanofluid mechanics are at the forefront applications of acoustic resonators with large vibrational quality factors.
While metal nanoparticles have been extensively studied, exploring other materials platforms, such as 2D semiconductor materials and heterostructures, offers new avenues for studying and harnessing acoustic vibrations at the nanoscale. These materials possess unique mechanical and acoustic properties that can be tailored and engineered to present great opportunities for nanoscale acoustic research and device development.
We review the coherent acoustic vibrations of metallic nanoresonators and discuss their potential applications. First, we discuss the excitation mechanism of coherent acoustic vibrations in metallic nanoresonators, and the corresponding transient absorption microscopy measurements. Second, the acoustic vibrational modes and frequencies of several metallic nanoresonators (including nanospheres, nanorods, and nanoplates), and the correlations with particle sizes and shapes are described (Figs. 3-5). Then we give detailed discussions on vibrational strong coupling between metallic nanoresonators, from experimental measurements of various vibrational coupling systems to theoretical analysis of the coupling mechanisms and mode profiles (Figs. 6-9). Further investigations of strong phonon coupling between acoustic nanoresonators are essential for quantum phonon manipulations in plasmonics. Next, we provide a few examples of the potential applications of high-frequency acoustic nanoresonators, with special emphasis on nanofluidics (Fig. 10). The studies demonstrate that the standard continuum fluid mechanics assumptions are no longer applicable at the nanoscale, and viscoelastic effects and interfacial slip phenomena must be considered. The observed nanoscale fluid phenomena have broad significance for the description and understanding of nanofluidics. Finally, the discussions on future development and applications of high-frequency acoustic nanoresonators are presented.
The study of acoustic vibrations in nanoresonators provides significant insights into the fundamental physics of nanoscale systems and opens up broad prospects for various applications, such as high-frequency biomechanics, nanofluid mechanics, and phonon frequency combs. Continuous research in this field has great potential for further discoveries and technological advancements.
1 引言
光子、电子、声子是凝聚态物理中几种基本的粒子,实现对这些基本粒子的操控也是人类科技创新的基础[1]。其中,声子是描述固体中晶格振动的简正模能量量子,它的存在决定了材料的热学、电学和力学等方面的性能。相较于光子和电子,人们对声子的研究和认识相对较少。鉴于人们在操控光子和电子方面的成功,实现对不同频率声子的控制也必将会带来巨大的应用价值,例如,对超高频声波(~THz)的调控将有利于发展高效新颖的热学器件;对低频声波(~MHz)的调控将实现医学声学成像的突破;对中频声波(~GHz)的调控是发展微纳机械振动系统的核心[1]。
微纳机械振动系统(MMS)是指微纳尺度下机械结构的振动。它是一门多学科交叉的前沿基础研究领域,涉及物理学、化学与材料科学等分支学科。由于其具有体积小、质量轻、灵敏度高、响应速度快等优点,在民用领域有着极其重要的应用。其核心是高品质因数的机械振动传感器,涉及不同的材料和器件原型,例如各种半导体声表面波器件、微纳悬臂梁、薄膜振动腔等等[2-5]。振动驱动的方式也多种多样,包括电磁驱动、压电驱动、光驱动和热驱动等。然而,传统微纳机械振动器件具有加工工艺复杂、振动频率相对较低(kHz~MHz)等缺点,限制了其系统的进一步发展。
声学纳腔作为光学纳腔的一种类比,是一种新型的机械振动传感器,也称声学振动传感器。涉及的材料包括金属纳米颗粒、半导体纳米颗粒和层状过渡金属化合物等等。这些声学纳腔振动频率高(GHz~THz)、振动模式相对简单;其次,相较于各种微纳机械振动器件,化学合成的声学纳腔具有制备简单、尺寸和形状可控、无需超净间等复杂制备工艺的特点[6-7];此外,飞秒脉冲激光可以有效激发声学纳腔的声学振动,并通过超快光学泵浦探测手段(PPS),在时域谱上对高频声学振动进行探测和研究。在过去的20年中,人们对声学纳腔进行了深入的研究,在纳腔声学振动的探测、振动模式和频谱分析、振动寿命和损耗机制研究、振动耦合和高频振动的应用等方面都取得了巨大的发展[8-9]。在此基础上,本文主要介绍了利用超快光谱技术研究金属纳腔的声学振动,主要原因是金属纳腔合成方法成熟、大小和尺寸可控。本文将重点讨论金属纳腔间的声学振动模式以及声学振动强耦合,最后讨论高频金属声学纳腔的应用,并展望该领域发展所面临的挑战和未来前景。
2 金属纳腔的超快动力学及其相干声学振动
金属纳米颗粒由于局域表面等离子体共振效应(LSPR),使其在可见光和近红外光谱范围内表现出非常强烈的吸收和散射现象,这也让金属纳米颗粒在各种光学传感、光学成像、光电子学和催化等领域具有广泛的应用。金属纳米颗粒也因此被认为是一种非常优异的光学谐振腔,很多优秀的研究工作都对其线性和非线性光学性能进行了深入的探讨和论述[8,10-13]。
金属纳米颗粒除了作为光学谐振腔,还具有非常优异的声学振动性能。超快光学可以有效激发和检测金属纳米颗粒的声学振动[8-9,14-15]。
图 1. 金属纳米颗粒声学振动示意图。(a)金属纳米颗粒的超快电子动力学过程;(b)金属纳米颗粒在超快光学测量中的时域声学振动曲线
Fig. 1. Schematic of acoustic vibrations in metal nanoparticles. (a) Ultrafast electron dynamics in metal nanoparticles; (b) time domain acoustic vibration curves of metal nanoparticles in ultrafast optical measurement
2.1 金属纳腔相干声学振动的泵浦探测
研究纳米颗粒声学振动的方法多种多样。其中包括飞秒时间分辨的X射线衍射成像(UTXDI)[16-17]、飞秒时间分辨和纳米空间分辨的超快透射电子显微镜(UTTEM)[18-19]、非线性光学四波混频光谱(FWMS)[20-21]、非弹性散射的低频拉曼光谱(IUFRS)[22-23],以及瞬态吸收光谱(TAS)[24-25]等技术。随着电子科学技术的进步以及激光器稳定性的提高,瞬态吸收光学显微镜(TAM)取得了巨大的发展,进一步让研究单个纳米颗粒的声学振动成为可能[26-27]。2005年,Orrit课题组[26]利用瞬态光学显微镜研究了单个金属纳腔的声学振动,准确测量了振动的频率以及寿命。与溶液相研究纳米颗粒的集体振动行为相比,单个颗粒的声学振动测量更能准确地评估颗粒尺寸、形状对声学振动的影响,更好地理解纳米尺度下材料的力学性能,而且单个颗粒的测量让研究颗粒与颗粒、颗粒与环境之间的相互作用成为可能。相较于其他方法,TAM的独特优势也让它变得越来越普及。
图 2. TAM的原理[28]。(a)常用的高频调制实验装置;(b)输入和输出泵浦和探测脉冲序列的时间调制行为,其中探测光束的强度可能会经历增益或损失;(c)典型激光源的噪声谱(对数-对数图)随频率f的变化
Fig. 2. Principle of transient absorption microscopy (TAM)[28]. (a) Generic experimental setup with high-frequency modulation; (b) temporal modulation behavior of input and output pump and probe pulse trains, and intensity of detection beam may experience gain or loss; (c) noise spectrum (log-log plot) of a typical laser source as a function of frequency f
TAM不仅可以在“高频调制方案”下探测微弱的信号,也能在“低频调制方案”中通过增加泵浦和探测光束的强度(~nJ/pulse)或者样品浓度来提高信号强度,例如低重频的激光放大器中利用机械斩波器进行的低频率调制[29-32]。然而,在单个纳米颗粒测量的过程中,通常的低激光强度是必须的(~pJ/pulse),以避免高功率损害样品的完整性;另外,对于单个纳米颗粒的测量,信号强度非常弱。以单个直径为20 nm的 Au颗粒为例,800 nm光激发、530 nm光探测的条件下,信号大小正比于探测功率的相对变化
2.2 金属纳腔声学振动的模式
金属纳腔因为表面等离子体共振效应,具有非常优异的光声转换性能,在超短光脉冲激发下,能有效产生纳腔的声学振动[34]。瞬态吸收光谱也被广泛用来研究各种金属纳腔的声学振动,包括球形纳米颗粒[26,35-40]、纳米棒[37,41-48]、纳米线[49-55]、纳米盘[56-60]、纳米片[61-69]、纳米核壳结构[70-73]、三角形纳米颗粒[74-76]、双锥体[30,77-80]、立方体[81-83]、纳米孔[31]、纳米环[84],以及各种复杂结构的振动腔等[85-88]。下面将以三种简单的声学纳腔(Au纳米颗粒、纳米棒和纳米片)为例,重点讨论其声学振动模式,以及振动频率与尺寸的关系。
图 3. 球形Au纳米颗粒的声学振动。(a)计算得到的Au纳米颗粒的基频呼吸模式;(b)510 nm和550 nm探测波长下测量的直径为( )nm的Au纳米颗粒溶液的瞬态吸收曲线[8]。插图显示的是Au纳米颗粒溶液的吸收谱,箭头对应于探测波长相对于Au纳米颗粒的等离子体共振峰的位置;(c)Au纳米颗粒的声学振动频率与颗粒半径倒数(1/R)的关系[8]。实线是使用Au块体材料的弹性系数计算的球形纳米颗粒呼吸振动模式的频率
Fig. 3. Acoustic vibrations of spherical Au nanoparticles. (a) Calculated fundamental breathing mode of Au nanoparticles; (b) transient absorption traces for ensemble measurement of ( ) nm diameter Au nanoparticle solution recorded at 510 nm and 550 nm probe laser wavelengths[8]. Inset shows absorption spectrum of Au nanoparticle solution, and arrows correspond to positions of plasma formant of probe wavelengths relative to Au nanoparticles; (c) acoustic vibration frequency of Au nanoparticles as a function of reciprocal of particle radius (1/R)[8]. Solid line shows calculated frequency for breathing vibration mode of spherical nanoparticles using elastic constants of bulk gold
1882年,Lamb[90]利用连续介质力学理论分析了球形颗粒的声学振动模式。对于半径为
式中:
式中:E是材料的杨氏模量;
图 4. Au纳米棒的声学振动。(a)计算得到的Au纳米棒的基频呼吸模式和伸展模式;(b)单根Au纳米棒的瞬态吸收曲线[41]。插图突出显示了在 200 ps 内的部分振动曲线。右侧是傅里叶变换后声学振动的功率谱密度。低频峰对应于纳米棒伸展模式,高频峰(插图)对应于纳米棒呼吸模式;(c)Au纳米棒直径依赖的声学振动呼吸模式[41];(d)具有不同生长方向的Au纳米棒声学振动伸展模式的平均振动周期与纳米棒平均长度的关系[8]
Fig. 4. Acoustic vibrations of Au nanorods. (a) Calculated fundamental breathing mode and extensional mode of Au nanorods; (b) transient absorption traces for a single Au nanorod[41]. Inset highlights partial vibration curves at early 200 ps. Right side is power spectral density of acoustic vibrations after Fourier transform. Low-frequency peak corresponds to extensional mode of nanorods, and high-frequency peak (inset) corresponds to breathing mode of nanorods; (c) acoustic vibration breathing mode dependent on diameter of Au nanorods[41]; (d) average vibrational period of extensional mode versus average length of Au nanorods with different growth directions[8]
式中:
图 5. Au纳米片的声学振动。(a)计算得到的Au纳米片的基频呼吸模式;(b)单个悬空 Au 纳米片的瞬态吸收曲线[95]。插图是振荡信号的相应快速傅里叶变换频谱;(c)Au纳米片声学振动周期与纳米片厚度的关系[61]
Fig. 5. Acoustic vibrations of Au nanoplates. (a) Calculated fundamental breathing mode of Au nanoplates; (b) transient absorption traces of a single suspended Au nanoplate[95]. Inset is corresponding fast Fourier transform spectrum of oscillation signal; (c) nanoplate thickness-dependent acoustic vibrational period of Au nanoplates[61]
通过对Au纳米颗粒、纳米棒和纳米片这三种简单声学纳腔的研究,讨论了它们的声学振动模式、振动频率与尺寸的关系。实验和理论都表明,声学纳腔的探测对于理解纳米尺度下材料的机械性能具有重要的作用。不仅对于简单声学纳腔,各种复杂声学纳腔结构也能通过TAM进行研究。从纳腔的振动模式、振动频率、振动寿命到纳腔与环境的相互作用都有充分的研究,也有大量的综述对这些方面进行了充分的论述[8-9,15,96]。然而,探索声学纳腔的能量损耗机制,尤其是复杂环境下的能量损耗,发展高频、长寿命的声学振动器件依然是一个研究难点;其次,扩展声学纳腔至多种多样的材料体系也是研究的一个热点,这有利于理解纳米尺度下材料的机械性能;另外,对于纳腔的高阶振动模式的激发、检测还没有一个有效的方法,对高阶模式的理解也需要更深入的研究;目前,对各种声学纳腔的研究都集中在室温环境下,低温环境下的声学纳腔动力学还有待发展。此外,对于纳腔间的耦合相互作用研究相对较少,本文接下来将对此进行论述。
3 金属纳腔声学振动之间的耦合
金属纳腔由于存在局域表面等离子体共振效应,导致纳腔周围电场增强。当两个或者多个金属纳腔相互接近时,它们的表面等离子体共振模式会产生耦合作用,导致共振模式的频率和强度发生变化,这种现象可以用来制备高度灵敏的生物传感器、纳米光学元件、光电转换器件等。表面等离子体共振耦合效应是纳米光学和纳米光子学中一个非常重要的现象[97]。与金属纳腔光学模式间的耦合相似,金属纳腔的声学振动也能发生耦合效应[22,50,65,68-69,74,82,98-103]。然而,声学振动耦合的物理机制与光学模式的耦合具有本质的不同,研究声学纳腔间的耦合对于理解及发展声学振动耦合体系具有重要作用。
物理光刻法制备的微纳结构在样品的尺寸、大小和结构上都具有非常好的调控性,是研究微纳结构中声学振动耦合的重要体系[44,74,82,99,104]。
图 6. 等离子体团簇中表面介导的声学振动耦合的距离依赖性[99,103]。(a)瞬态吸收曲线和(b)具有不同间隙尺寸的单个纳米团簇的声学振动的快速傅里叶变换频谱。纳米团簇的相应 SEM 图像显示在图的顶部;(c)测量的声学振动频率与间隙大小的函数关系;(d)瞬态吸收曲线和(e)具有不同中心纳米盘直径的单个纳米团簇的声学振动的快速傅里叶变换频谱。纳米团簇的相应 SEM 图像显示在图的顶部;(f)测量的声学振动频率与中心纳米盘声学振动频率的关系
Fig. 6. Distance dependence of surface-mediated acoustic vibrational coupling in plasmonic nanoclusters[99, 103]. (a) Transient absorption traces and (b) fast Fourier transform spectra of acoustic vibrations of individual nanoclusters with different gap sizes. Corresponding SEM images for nanoclusters are shown on top of figures; (c) measured acoustic vibrational frequencies as a function of gap size; (d) transient absorption traces and (e) fast Fourier transform spectra of acoustic vibrations of individual nanoclusters with different central disk diameters. Corresponding SEM images for nanoclusters are shown on top of figures; (f) measured acoustic vibration frequencies as a function of acoustic vibrational frequencies of central disk
为了能够定量地描述体系中的耦合效应,可以采用耦合的谐振子模型对其进行分析,并假设纳米团簇中颗粒声学振动的耦合是通过基底中传导的声子。中心纳米盘在飞秒激光激发下产生相干声学振动,纳米盘自身的振动以声波的方式传递到周围的基底中,声波的传播引起基底发生形变,其晶格形变的强度I为
式中:
因此,在耦合情况下,外环纳米盘的频移取决于到中心纳米盘的距离和中心纳米盘的声学振动频率。
尽管光刻法在制备和加工微纳结构上具有巨大的优势,但是结构表面和内部的缺陷极大地降低了声学振动的寿命[59],也影响了声学振动的耦合强度。相反,化学合成法制备的纳米颗粒具有较高的晶体质量,声学振动的寿命有了极大的提高,然而对结构上的调控相对困难,尤其是在研究颗粒与颗粒之间的耦合方面。
图 7. 两根Cu纳米线中的声学振动耦合[50]。(a)Cu纳米线声学振动耦合的瞬态吸收曲线,具有明显的拍频现象。插图是 SEM 图像,显示两条直径相同、中间被MAKROFOL聚合物相连的纳米线;(b)相应的快速傅里叶变换频谱。由于耦合效应,在 15 GHz和 16 GHz 频率处具有明显的分裂效应
Fig. 7. Acoustic vibrational coupling in two Cu nanowires[50]. (a) Transient absorption trace of acoustic vibrational coupling of Cu nanowires with a clear beating phenomenon. Inset is SEM image showing two nanowires with same diameter connected by MAKROFOL polymer; (b) corresponding fast Fourier transform spectrum with obvious splitting effect at frequencies of 15 GHz and 16 GHz due to coupling effect
化学合成的Au纳米片晶体质量好、面积大、声学振动的品质因数高,是研究声学振动间耦合效应的理想体系[65,68-69]。
图 8. 重叠Au纳米片中声学振动的强耦合[65,68-69]。(a)重叠Au 纳米片的 SEM图像[68];(b)由聚合物层PVP-40K隔开的两个重叠 Au 纳米片示意图;(c)重叠Au纳米片的声学振动频谱,第一个Au纳米片的振动频率为 ,第二个Au纳米片的振动频率为 。Au纳米片声学振动耦合后产生新的频率 和 ;(d)不同耦合强度下所计算的声学纳腔之间的振动耦合频率谱。插图显示了耦合谐振子的理论模型[65];(e)重叠Au纳米片体系中聚合物依赖的声学振动耦合强度[69];(f)耦合模式 和 相对于非耦合纳米片频率的频移与非耦合模式的频率失谐图。实验数据(点)可以利用耦合谐振子模型进行拟合(线),其中图形显示强耦合的反交叉行为特征
Fig. 8. Strong acoustic vibrational coupling in stacked Au nanoplates[65, 68-69]. (a) SEM image of stacked Au nanoplates[68]; (b) diagram of two stacked Au nanoplates separated by a PVP-40K polymer layer; (c) acoustic vibrational spectra of first plate , second plate , and overlapping area. Acoustic vibrational coupling between plates creates new frequencies and ; (d) calculated vibrational coupling spectra between acoustic resonators with different coupling rates[65]. Inset shows schematic model of coupled resonators; (e) polymer dependent acoustic vibrational coupling strength of stacked Au nanoplates[69]; (f) frequency shift of coupled modes and relative to uncoupled nanoplate frequency versus frequency detuning of uncoupled modes. Experimental data (dots) are fitted to coupled oscillator model (lines), showing anticrossing behavior characteristic of strong coupling
在Au纳米片的重叠结构中,每个Au纳米片
式中:
式中:耦合强度
为了更好地理解中间层的性质对声学振动耦合效应的影响,接下来通过连续介质力学模型对Au纳米片声学振动进行分析[102]。对于弹性各向同性的材料,它们的机械性能仅取决于三个参数:密度
对于重叠的Au纳米片结构,假设不同介质之间的所有界面都存在完美的机械接触(即位移和应力的连续性)。
式中:
反对称模式的频率满足以下方程:
图 9. 重叠Au纳米片声学振动耦合的理论研究[102]。(a)基于连续介质力学模型计算重叠Au纳米片的振动频率。点划线是对称模式的结果,实线是反对称模式的结果;(b)前三种振动模式(从左到右)对应于图(a)中 的虚线框标记(从低到高)。这三种模式分别为重叠Au纳米片的相对模式、 和 [如图8(c)所示];(c)三个Au纳米片重叠结构的前五种振动特征频率的有限元计算;(d)五种振动模式(从左到右)对应于图(c)中 的虚线框标记(从低到高)
Fig. 9. Theoretical studies of acoustic vibrational coupling in stacked Au nanoplates[102]. (a) Calculated vibrational frequencies in stacked Au nanoplates based on continuum mechanics model. Dot-dash lines are results of symmetric modes and solid lines are results of antisymmetric modes; (b) vibrational profiles (from left to right) that correspond to first three modes at marked with dashed box in (a) (from low to high). Modes are relative mode, , and for stacked Au nanoplates as shown in Fig. 8(c); (c) finite element calculations of first five vibrational eigenfrequencies in three Au-polymer-Au-polymer-Au stacking structures; (d) vibrational profiles (from left to right) that correspond to first five modes at marked with dashed box in (c) (from low to high)
4 金属纳腔声学振动的应用
相比于传统的微纳机械振动器件,高频声学纳腔的应用相对较少,随着研究的深入,高频声学纳腔在一些领域也表现出重要的应用价值。其中最基础的一个应用领域是通过声学振动研究纳米尺度下物质的性质,包括材料科学和生物学等[105-107]。此外,声学振动还可以应用于声学感应和测量,如声学振动质量传感。声学振动质量传感是一种利用声学振动对质量变化的敏感度来实现物质检测和分析的方法。通过其超高的振动频率,金属声学纳腔在质量传感方面表现出了较高的灵敏度[67,77]。单个Au纳米棒声学振动的质量探测灵敏度可以达到
金属声学纳腔的另外一个重要应用是皮秒超声波成像,其目的是将传统声学技术扩展到千兆赫兹和太赫兹频率范围[108]。金属纳腔在与飞秒脉冲激光相互作用后,除了产生自身的晶格振动,还会向外界环境中以声波的形式辐射能量(如
金属声学纳腔也被用于探测高频振动下简单液体的流体学性质[125]。研究发现,在考虑纳米尺度的液体流动时,通常用于描述简单液体的流体学标准连续介质假设有可能被打破。其中的两个常见假设是:1)简单液体表现出牛顿响应(外加应力和产生应变速率之间的线性关系,流体的黏度提供了线性关系的比例常数);2)简单液体的无滑移条件(在任何固-液界面,液体与固体界面一起移动)。然而,即使是简单的分子液体也会在皮秒时间尺度上表现出非牛顿的黏弹性响应,这是许多纳米量级物体振动的特征,出现这种黏弹性是因为这些时间尺度可以与液体中分子弛豫的时间尺度相媲美。另外,即使是在润湿固体表面,液体也会表现出纳米级的滑动。最近人们开始利用金属纳腔的声学振动来研究简单液体的黏弹性响应和相关的纳米级滑移,对纳米尺度下液体的流动进行深入的理解[40,53,55,78,80,95,126]。
瞬态吸收光谱测量能得到声学纳腔的振动频率和阻尼率(声学振动寿命),提供有关声学纳腔与其周围液体之间的机械耦合和能量损耗的定量信息。反过来,通过这些信息阐明简单液体在纳米尺度上的流体性能,包括流体的剪切黏弹性和压缩黏弹性响应,以及固-液界面处的纳米级滑移。
式中:E是Au颗粒的杨氏模量;
图 10. 金属声学纳腔用于研究固-液界面处的纳米量级滑移和液体黏弹性[40,78,80,95]。(a)高度球形 Au 纳米颗粒在甘油-水混合液中的声学振动[40];(b)Au 纳米颗粒的声学振动品质因数。图中点对应实验数据,实线对应液体黏弹性理论,虚线对应牛顿流体理论;双锥体Au颗粒在甘油-水混合液中的(c)品质因数和(d)声学振动频率[78];(e)Au 纳米片在甘油-水混合液中的基频声学振动品质因数 与振动频率的关系[95]。虚线和实线分别对应于无黏性和黏弹性流体模型的计算结果。标记点为实验数据;(f)实验确定的液体弛豫时间 (点),以及文献报道的弛豫时间(实线)
Fig. 10. Metal acoustic nanocavity used for studies on nanometer slip at solid-liquid interface and liquid viscoelastic properties[40, 78, 80, 95]. (a) Acoustic vibrations of highly spherical Au nanoparticles in glycerol-water mixtures[40]; (b) corresponding quality factors for acoustic vibrations of Au nanosparticles. Points correspond to experimental data, solid lines correspond to viscoelastic theory, and dashed lines correspond to Newtonian theory; (c) quality factor and (d) frequency of acoustic vibrations of Au bipyramids in glycerol-water mixtures[78]; (e) quality factors of fundamental acoustic vibrations versus vibrational frequency for Au nanoplates in glycerol-water mixtures[95]; Dashed and solid lines correspond to calculation results of inviscid and viscoelastic fluid models, respectively. Symbols show experimental data; (f) liquid relaxation time determined from experiments (spots). Solid line shows relaxation time from reference
下面通过Au纳米双锥体的声学振动讨论液体的滑移边界条件。图
溶液法测量纳米颗粒的集体声学振动会因为纳米颗粒的不均匀性分布引入较大的实验误差,对单个纳米颗粒声学振动的测量能更准确地研究颗粒与液体的相互作用。一维Au纳米线和二维Au纳米片都被用来研究高频振动下简单液体的流体学性能[53,55,95,126]。相比于Au纳米线(通常具有不规则的横截面),化学合成的Au纳米片结构更均匀,声学振动频率更高,振动寿命和品质因数更大,振动模式更清晰,能更准确地研究振动与液体的相互作用。根据连续介质力学模型,可以得到Au纳米片在黏性液体中声学振动频率特征值方程[95,126]:
式中:
当液体表现出黏弹性效应时,其中的剪切黏度和体积黏度则表示为
式中,
此外高频声学振动与液体的黏弹性相互作用提供了一种新方法来分析液体分子的弛豫时间。
5 总结与展望
本文主要简述了金属声学纳腔的超快光谱探测,讨论了单颗粒测量的优势和特点;对三种简单的金属声学纳腔(球形纳米颗粒、纳米棒以及纳米片)的声学振动模式、振动频率进行了总结;重点讨论了金属声学纳腔间的耦合和强耦合现象,理论分析了其耦合模式和耦合物理机制;最后对高频声学纳腔的应用进行了举例,详细讨论了高频声学振动在纳米流体学方面的应用。
尽管本文主要讨论了金属声学纳腔,但是发展高频、高品质因数的各类声学纳腔一直是一个重要的目标。对声学纳腔的研究也可以拓展到其他多种多样的材料体系和结构,其中包括过渡金属层状化合物或半导体异质结等[29,128-133]。目前对这类声学纳腔的研究相对较少,其中丰富的激子和声子特性将有利于研究纳腔中激子-声子相互作用[134-137];另外,更高的时间分辨和空间分辨能力将帮助人们深入理解各类声学纳腔中的局域声学模式[18,138-140]。
声学纳腔间的强耦合相互作用是另外一个重要的研究方向。追求新型的耦合物理体系,实现强耦合以及超强耦合一直是凝聚态物理的一个目标[141-142]。目前在金属纳腔、二维层状半导体纳腔中实现的声学强耦合相互作用[65,143],将激发人们继续探索新型的声学强耦合体系,理解其中的耦合物理机制,尤其是低温声子耦合物理。除了简单结构中声学纳腔间的耦合,多体结构中的声学模式耦合也是一个未知的方向[144]。
继续拓展声学纳腔的应用领域,开发新型的高频声子学器件也是研究重点。声学纳腔在纳米流体学方面的探索还处在起步阶段,虽然人们已对简单液体的黏弹性理论有了基本的认识,但是对于其中的滑移边界条件还需要更多的实验支持和理论指导;另外,推动声学纳腔-流体相互作用至更高的频率区间,以便探测各种流体的黏弹性质[145],这将对发展医学声子学器件具有重要意义。总之,相比于传统的MMS,高频声学振动具有其独有的特点和优势,对高频声子学器件的开发也将带来其全新的应用。
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Article Outline
余快, 陈云高, 汪国平. 光诱导金属纳腔的相干声学振动及应用[J]. 光学学报, 2023, 43(16): 1623015. Kuai Yu, Yungao Chen, Guoping Wang. Laser Excitation of Coherent Acoustic Vibrations of Metallic Nanoresonators and Their Applications[J]. Acta Optica Sinica, 2023, 43(16): 1623015.