-
复杂受限环境中的扩散的研究在凝聚态物理领域中备受关注。胶体体系的出现,为定量研究微观粒子的受限扩散提供了卓越的实验模型系统。当胶体粒子的形状由球形变为椭球形时,体系展现出各向异性的扩散动力学特性。近年来,研究者们发现粗糙表面能够诱发球形胶体体系异常的旋转动力学。然而,由于实验体系的局限性,粗糙表面对椭球形胶体粒子的受限扩散的影响依然知之甚少。本文建立了胶体受限扩散的模型体系,由粗糙圆球胶体构成受限环境,研究了粗糙和光滑椭球在其中的受限扩散。当圆球的堆积分数较低时,粗糙表面未发挥作用,因此光滑和粗糙椭球的平动和转动扩散相近。随着圆球堆积分数的增高,粗糙表面之间发生互锁,导致粗糙椭球的平动扩散明显慢于光滑椭球;随着堆积分数的进一步增高,由于粗糙表面产生的空间位阻效应,粗糙椭球的转动扩散也显著慢于光滑椭球。该工作表明粗糙表面会改变椭球的受限扩散,为揭示复杂环境中具有粗糙表面的物质的扩散规律提供了实验依据。The study of diffusion in complex confined environments has received great attention in the field of condensed matter physics. The emergence of colloidal systems provides an excellent experimental model system for the quantitative study of the confined diffusion of microscopic particles. When the shape of colloidal particles changes from spherical to ellipsoidal, the system exhibits anisotropic diffusion dynamics. Recent studies have found that rough surfaces, another important physical parameter of colloids, can lead to unusual rotational dynamics in spherical colloidal systems. However, due to the lack of a suitable experimental system, little is known about the effect of rough surfaces on the confined diffusion of ellipsoidal colloidal particles. In this paper, rough colloidal sphere, rough colloidal ellipsoid and smooth colloidal ellipsoid are prepared, and then monolayer colloidal samples are prepared to study the confined diffusion of these two types of ellipsoids in a dense packing of the rough sphere colloids. By calculating the mean square displacement, intermediate self-scattering function, and orientation correlation function of the ellipsoids, we quantitatively characterized the diffusion dynamics of rough and smooth ellipsoids in varying concentrations of rough spheres. The results indicate that the translational and rotational diffusion of both rough and smooth ellipsoids slow down as the concentration of rough spheres increases. This is due to the confinement of the ellipsoid by the surrounding spheres. At low stacking fractions of spheres, smooth and rough ellipsoids show similar translational and rotational diffusion. However, as the stacking fraction of spheres increases, the advection diffusion of rough and smooth ellipsoids differs significantly. The advection diffusion of rough ellipsoids is significantly slower than that of smooth ellipsoids. This is because the rough surface strongly inhibits rotation, meaning that the rotational diffusion of the rough ellipsoid is significantly slower than that of the smooth ellipsoid. By extracting the diffusion coefficients for translation and rotation from the ellipsoid's long-time mean-square displacements, we found that at Φ = 0.60 and 0.65, the diffusion coefficients of rough ellipsoids are smaller than those of smooth ellipsoids. The translational diffusion coefficient of the rough ellipsoid is notably smaller than that of the smooth ellipsoid. However, the rotation diffusion coefficient of the rough ellipsoid does not significantly differ from that of the smooth ellipsoid. This suggests that rough surfaces primarily impact translational diffusion, strongly suppressing the translational diffusion of the ellipsoid. By calculating the displacement probability distribution for ellipsoidal motion, we found that at Φ = 0.65, the rough ellipsoid's translational displacements have a relatively narrow distribution. This suggests that the particles' translational motion is suppressed by the rough surface. However, the distributions of rotation displacement for both are very similar, indicating that the rough surface has less impact on particle rotation. At Φ = 0.74, the rough surface suppresses both the translation and rotation of the ellipsoid, resulting in a narrower displacement distribution compared to the smooth ellipsoid.
These findings suggest that rough surfaces significantly impede ellipsoidal diffusion, with effects on translational and rotational motions not occurring simultaneously. This study marks a significant advancement in understanding the role of rough surfaces of colloidal particles in confined diffusion and provides an experimental basis for explaining the diffusion laws of rough materials.-
Keywords:
- Colloidal ellipsoids /
- rough particles /
- confined diffusion /
- dynamics
-
[1] Weeks E R, Crocker J C, Levitt A C, Schofield A, Weitz D A 2000 Science 287 627
[2] Mitragotri S, Lahann J 2009 Nat. Mater. 8 15
[3] Anderson V J, Lekkerkerker H N W 2002 Nature 416 811
[4] Carrasco-Fadanelli V, Mao Y S, Nakakomi T, Xu H A, Yamamoto J, Yanagishima T, Buttinoni I 2024 Soft Matter 20 2024
[5] Doan D, Kulikowski J, Gu X W 2024 Nat. Commun. 15 1954
[6] Han Y, Alsayed A M, Nobili M, Zhang J, Lubensky T C, Yodh A G 2006 Science 314 626
[7] Chakrabarty A, Konya A, Wang F, Selinger J V, Sun K, Wei Q H 2013 Phys. Rev. Lett. 111 160603
[8] Zhou F, Wang H G, Zhang Z X 2020 Langmuir 36 11866
[9] Zhou H X, Rivas G N, Minton A P 2008 Annu. Rev. Biophys. 37 375
[10] Liu X Z, Wang H G 2020 Acta Phys. Sin. 69 293 (in Chinese) [刘心卓, 王华光 2020 物理学报 69 293]
[11] Carbajal-Tinoco M D, Lopez-Fernandez R, Arauz-Lara J L 2007 Phys. Rev. Lett. 99 138303
[12] Boniello G, Blanc C, Fedorenko D, Medfai M, Ben Mbarek N, In M, Gross M, Stocco A, Nobili M 2015 Nat. Mater. 14 908
[13] Edmond K V, Elsesser M T, Hunter G L, Pine D J, Weeks E R 2012 P. Natl. Acad. Sci. U.S.A. 109 17891
[14] Peng Y, Lai L, Tai Y S, Zhang K, Xu X, Cheng X 2016 Phys. Rev. Lett. 116 068303
[15] Kim J, Sung B J 2015 Phys. Rev. Lett. 115 158302
[16] Cervantes-Martínez A E, Ramírez-Saito A, Armenta-Calderón R, Ojeda-López M A, Arauz-Lara J L 2011 Phys. Rev. E 83 030402
[17] He K, Khorasani F B, Retterer S T, Thomas D K, Conrad J C, Krishnamoorti R 2013 ACS Nano 7 5122
[18] Hsu C P, Mandal J, Ramakrishna S N, Spencer N D, Isa L 2021 Nat. Commun. 12 1477
[19] Moinuddin M, Biswas P, Tripathy M 2020 J. Chem. Phys. 152 044902
[20] Ilhan B, Mugele F, Duits M H G 2022 J. Colloid Interface Sci. 607 1709
[21] Zhang H, Pham P, Metzger B, Kopelevich D I, Butler J E 2023 Phys. Rev. Fluids 8 064303
[22] Zhang Z X, Yunker P J, Habdas P, Yodh A G 2011 Phys. Rev. Lett. 107 208303
[23] Wang H G, Zhang Z X 2016 Acta Phys. Sin. 65 226 (in Chinese) [王华光, 张泽新 2016 物理学报 65 226]
[24] Xu Z Y, Gao L J, Chen P Y, Yan L T 2020 Soft Matter 16 3869
[25] Mishra C K, Rangarajan A, Ganapathy R 2013 Phys. Rev. Lett. 110 188301
计量
- 文章访问数: 142
- PDF下载量: 1
- 被引次数: 0