Plasma formation and temperature measurement during single-bubble cavitation

Single-bubble sonoluminescence (SBSL) results from the extreme temperatures and pressures achieved during bubble compression; calculations have predicted the existence of a hot, optically opaque plasma core with consequent bremsstrahlung radiation. Recent controversial reports claim the observation of neutrons from deuterium-deuterium fusion during acoustic cavitation. However, there has been previously no strong experimental evidence for the existence of a plasma during single- or multi-bubble sonoluminescence. SBSL typically produces featureless emission spectra that reveal little about the intra-cavity physical conditions or chemical processes. Here we report observations of atomic (Ar) emission and extensive molecular (SO) and ionic (O2+) progressions in SBSL spectra from concentrated aqueous H2SO4 solutions. Both the Ar and SO emission permit spectroscopic temperature determinations, as accomplished for multi-bubble sonoluminescence with other emitters. The emissive excited states observed from both Ar and O2+ are inconsistent with any thermal process. The Ar excited states involved are extremely high in energy (>13 eV) and cannot be thermally populated at the measured Ar emission temperatures (4,000-15,000 K); the ionization energy of O2 is more than twice its bond dissociation energy, so O2+ likewise cannot be thermally produced. We therefore conclude that these emitting species must originate from collisions with high-energy electrons, ions or particles from a hot plasma core.     

The energy efficiency of formation of photons, radicals and ions during single-bubble cavitation

It is extremely difficult to perform a quantitative analysis of the chemistry associated with multibubble cavitation: unknown parameters include the number of active bubbles, the acoustic pressure acting on each bubble and the bubble size distribution. Single-bubble sonoluminescence (characterized by the emission of picosecond flashes of light) results from nonlinear pulsations of an isolated vapour-gas bubble in an acoustic field. Although the latter offers a much simpler environment in which to study the chemical activity of cavitation, quantitative measurements have been hindered by the tiny amount of reacting gas within a single bubble (typically <10(-13) mol). Here we demonstrate the existence of chemical reactions within a single cavitating bubble, and quantify the sources of energy dissipation during bubble collapse. We measure the yields of nitrite ions, hydroxyl radicals and photons. The energy efficiency of hydroxyl radical formation is comparable to that in multibubble cavitation, but the energy efficiency of light emission is much higher. The observed rate of nitrite formation is in good agreement with the calculated diffusion rate of nitrogen into the bubble. We note that the temperatures attained in single-bubble cavitation in liquids with significant vapour pressures will be substantially limited by the endothermic chemical reactions of the polyatomic species inside the collapsing bubble.     

Parametric dependence of the line emissions in sonoluminescence

Based on a series of spectral measurements of sonoluminescence, this paper investigates parametric dependence of the line emissions in single bubble sonoluminescence (SBSL) and multi-bubble sonoluminescence (MBSL). The experiments show that the intensities of the OH* radical line, the sodium line and the noble gas lines in SBSL are relevant to the driving pressure of the acoustic field and the concentration of the noble gases dissolved in host liquids. The intensity of line emissions in total spectrum increases with the decreasing driving pressure and the increasing concentration of noble gases. Parametric dependence of line emissions in MBSL consists with that in SBSL. Line emissions in sonoluminescence should correspond to lower temperature inside the bubbles. SBSL and MBSL share the same spectral structure, and the difference between them found by previous experiments should result from the different temperatures inside bubbles.     

Snapping shrimp make flashing bubbles

Snapping shrimp produce a loud crackling noise that is intense enough to disturb underwater communication. This sound originates from the violent collapse of a large cavitation bubble generated under the tensile forces of a high-velocity water jet formed when the shrimp's snapper-claw snaps shut (Fig. 1). Here we show that a short, intense flash of light is emitted as the bubble collapses, indicating that extreme pressures and temperatures of at least 5,000 K (ref. 4) must exist inside the bubble at the point of collapse. We have dubbed this phenomenon 'shrimpoluminescence' - the first observation, to our knowledge, of this mode of light production in any animal - because of its apparent similarity to sonoluminescence, the light emission from a bubble periodically driven by ultrasound.     

空化气泡发光机理

介绍了单气泡声致发光现象的主要研究进展,总结了理论计算研究结果.通过求解流体力学方程组等比较完全的数值计算,发现空化气泡发光机理就是高温、高压和高密度的气体发光,因气泡达到的温度不同,有时原子或分子线谱贡献占优势,有时连续谱占主导.通过研究单气泡形状不稳定性,发现声压的非球对称微小偏离导致驱动声压上限.     

单泡声致发光研究

介绍了作者在研究单泡声致发光SBSL动力学特性和发光特征方面的进展情况。用气泡振子模型，研究了在不可压缩、粘滞流体中气泡近球对称运动的动力学行为；运用Mie散射理论和Dave倒推算法，系统地计算了适用于单泡声致发光的Mie射测量参数；实验给出单泡发光强度的衰减特性、SBSL光强与频率的关系、SBSL与激励电压的关系等结果。     

Sonoluminescence from non-aqueous liquids

Our understanding of the chemical effects of high-intensity ultrasonic irradiation of liquids is still quite limited. It is generally accepted that sonochemistry results from acoustic cavitation: the creation, growth, and implosive collapse of bubbles in ultrasonically irradiated liquids. The mechanism of sonoluminescence in aqueous systems has been a matter of some dispute; recent discussions have suggested at least three possible origins: black-body emission, chemiluminescence from radical recombination, and electric discharge. Few studies of non-aqueous sonoluminescence, however, have been conducted. We present here the first spectrally resolved sonoluminescence spectra from hydrocarbon and halocarbon liquids. These spectra originate unambiguously from excited-state molecules created during acoustic cavitation. These high-energy species probably result from the recombination of radical and atomic species generated during the high temperatures and pressures of cavitation.     

乙二醇溶液中圆锥泡声致发光的发光光谱

利用一种改进后的U型管圆锥泡声致发光装置,研究了乙二醇溶液中圆锥泡声致发光的发光光谱.实验结果表明,光谱为从紫外到可见光波长范围的连续谱,在589 nm附近叠加有钠的3p-3s原子发射谱线.在钠的原子发射谱线左侧测量得到了Na-Ar分子激发态跃迁形成的蓝卫星带,并首次在声致发光实验中测得了Na-Ar的红卫星带以及钠的3d-3p原子发射谱线.最后,讨论了钠的原子发射谱线以及卫星带的形成机理.     

气体性质对单泡声致发光平衡参数空间的影响

构造了一个描述气泡宏观运动的均匀非绝热模型,结合气泡的平衡机制,分析了空气和惰性气体的各种特性对单泡声致发光的平衡参数空间的影响．发现气体性质通过对平衡参数空间的影响对单泡声致发光起着重要作用．其中热传导系数起着主要作用,它的减小将导致气泡的平衡半径与压缩比增大,并导致发光亮度的增强．     

若丹明6G圆锥泡光致发光的实验研究

利用一种改进后的U型管圆锥泡声致发光装置,研究了若丹明6G在1,2-丙二醇溶液中的光致发光现象.测量得到了若丹明6G在不同浓度时的圆锥泡声致发光光谱,结果表明利用圆锥泡声致发光可以激发若丹明6G使其发出荧光,从而证明了在溶液中加入荧光物质的声致发光实验中存在光致发光现象.在较高浓度时,由于若丹明6G存在强烈的自吸收,圆锥泡光致发光的荧光峰值与利用普通激光激发得到的荧光峰值相比向长波方向发生了红移.圆锥泡光致发光能否在光谱测量中被探测到在一定程度上取决于荧光与圆锥泡声致发光的光发射强度的比值.     

自发辐射的全量子解释

产生激光的过程是受激辐射的光放大过程。然而,最初的辐射场必须至少有一个光子来引发处于受激态的工作物质。因此从理论上弄清自发辐射过程,了解这些最初由自发辐射过程所产生的光子及其特性是具有一定意义的。本文拟就大多数量子力学教材未能处理好的自发辐射现象,用全量子理论作较详细的处理,从而得出符合实际的全面解释。     

利用声致发光原理检测水质装置的设计

设计了一种利用声致发光原理检测水质的装置,该装置由反应室、超声驱动电源、换能器及光电转换装置等组成。检测时,将水样放在样品容器中,用管路与水泵连接,抽取水样并经进样口进入反应室,超声功率放大器驱动换能器,带动变幅杆与水样作用产生超声空化区域并伴随发光。通过探测窗口由光电倍增管接收并转换,输出给电脑进行处理。该装置可以快速获取水体样品中声致发光强度的大小,以及随着声功率的不同产生的发光强度的变化规律,并根据发光规律判断水体中不同物质的组成。     

对声致发光单气泡半径计算

从Keller-Miksis方程出发,推导出声致发光气泡半径微分方程,通过数值计算,计算出不同驱动声压,不同驱动声压频率下的气泡半径,讨论了驱动声压,驱动声压频率与声致发光气泡半径的关系,得到理论计算结果与实验数据很好的吻合.     

时辨光子计数法测量单泡声致发光光谱

利用单泡声致发光光脉冲间期短以及与声场精确同步的特点,首次把高时辨的光子计数器用于单泡声致发光光谱的测量,极大程度地提高了信噪比,在较高的灵敏度下亦可达到较高的分辨率.利用该方法得到了稳态单泡声致发光的光谱曲线,并且对原始光谱曲线进行了校准.     

Structural basis for the spectral difference in luciferase bioluminescence

Fireflies communicate with each other by emitting yellow-green to yellow-orange brilliant light. The bioluminescence reaction, which uses luciferin, Mg-ATP and molecular oxygen to yield an electronically excited oxyluciferin species, is carried out by the enzyme luciferase. Visible light is emitted during relaxation of excited oxyluciferin to its ground state. The high quantum yield of the luciferin/luciferase reaction and the change in bioluminescence colour caused by subtle structural differences in luciferase have attracted much research interest. In fact, a single amino acid substitution in luciferase changes the emission colour from yellow-green to red. Although the crystal structure of luciferase from the North American firefly (Photinus pyralis) has been described, the detailed mechanism for the bioluminescence colour change is still unclear. Here we report the crystal structures of wild-type and red mutant (S286N) luciferases from the Japanese Genji-botaru (Luciola cruciata) in complex with a high-energy intermediate analogue, 5'-O-[N-(dehydroluciferyl)-sulfamoyl]adenosine (DLSA). Comparing these structures to those of the wild-type luciferase complexed with AMP plus oxyluciferin (products) reveals a significant conformational change in the wild-type enzyme but not in the red mutant. This conformational change involves movement of the hydrophobic side chain of Ile 288 towards the benzothiazole ring of DLSA. Our results indicate that the degree of molecular rigidity of the excited state of oxyluciferin, which is controlled by a transient movement of Ile 288, determines the colour of bioluminescence during the emission reaction.     

全失重环境下液体的受迫振动

研究全失重环境下带核液体和腔内多层液体的受迫振动问题．采用球函数和Ｇａｌｅｒｋｉｎ方法给出了问题的解析解．研究结果表明，对于理想不可压缩流体在线性理论范围内，刚体的激励运动不激发液体自由面或多层液体交界面的波动响应，从而使问题转化为液泡的运动．     

高电荷态离子N~(q+)(q=3,6)与原子、分子碰撞中发射光谱

本实验对N6+—He，N3+—He和N3+—H2碰撞中的发射光谱进行了测量.从测量到的发射光谱分析证明：上述碰撞中存在着三种或四种激发通道：（1）单电子俘获激发通道：（2）双电子俘获激发通道：（3）入射离子直接激发通道；（4）靶直接激发通道。本文还给出了发射截面数据。     

用分子相互作用模型预测纯液体的均匀核化过热极限

采用液滴上升法测定纯液体的气泡均匀核化过热极值值，并用分子相互作用模型计算了９种纯液体的过热极限值；计算结果与实验，文献值均符合良好。     

液体表面张力对气泡声散射的影响

气泡在液体中受液体的表面张力和液体静态压力相当的情况下,研究了表面张力对气泡声散射的影响.建立球形气泡表面的速度和压力连续性方程,并在方程中引入气泡受液体表面张力的影响,求出了气泡在对称振动模式下的散射系数及散射声功率,并进一步推导了在多气泡的情况下的等效入射声场.通过数值分析发现,当球形气泡在液体中受液体的表面张力和液体静态压力相当时,球形气泡的半径约为10^-6m,在此情况下,液体表面张力对气泡声散射的影响只在驱动声场的角频率小于10^5rad/s时才能表现出来,并且在多气泡的情况下对等效入射声场的等效声压振幅会产生较大影响.而在驱动声场的角频率大于10^5rad/s的情况下,液体表面张力对气泡的散射系数、散射声功率及等效入射声场声压振幅的影响不明显.对于气泡的声散射问题,气泡受液体表面张力的影响需根据所研究的具体问题进行取舍.     

7-羟基黄酮分子在水中分子内电荷转移及分子间多重质子的转移

基于密度泛函和含时密度泛函理论的B3LYP方法, 在TZVP基组水平上模拟7-羟基黄酮(7HF)的水复合物--7HF-(H₂O)4激发态的动力学机制. 结果表明： 复合物中7HF在第一电子激发态的前线分子轨道出现分子内电荷转移过程; 复合物中7HF在基态和第一电子激发态发生了分子结构扭转, 复合物中5个分子间的氢键在第一电子激发态均出现加强机制, 该机制可以驱动激发态的多重质子转移反应.