Origins of suppressed self-diffusion of nanoscale constituents of a complex liquid
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2024
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| author | Tanner, Christian P. N. Wall, Vivian R. K. Gababa, Mumtaz Portner, Joshua Jeong, Ahhyun Hurley, Matthew J. Leonard, Nicholas Raybin, Jonathan G. Utterback, James K. Kim, Ahyoung Fluerasu, Andrei Sun, Yanwen Moeller, Johannes Zozulya, Alexey Jo, Wonhyuk Brausse, Felix Wrigley, James Boesenberg, Ulrike Pudell, Jan-Etienne Hallmann, Joerg Lu, Wei Shayduk, Roman Youssef, Mohamed Madsen, Anders Limmer, David T. Talapin, Dmitri V. Teitelbaum, Samuel W. Ginsberg, Naomi S. |
| author_facet | Tanner, Christian P. N. Wall, Vivian R. K. Gababa, Mumtaz Portner, Joshua Jeong, Ahhyun Hurley, Matthew J. Leonard, Nicholas Raybin, Jonathan G. Utterback, James K. Kim, Ahyoung Fluerasu, Andrei Sun, Yanwen Moeller, Johannes Zozulya, Alexey Jo, Wonhyuk Brausse, Felix Wrigley, James Boesenberg, Ulrike Pudell, Jan-Etienne Hallmann, Joerg Lu, Wei Shayduk, Roman Youssef, Mohamed Madsen, Anders Limmer, David T. Talapin, Dmitri V. Teitelbaum, Samuel W. Ginsberg, Naomi S. |
| contents | Understanding and ultimately controlling the transformations and properties of nanoscale systems, from proteins to synthetic nanomaterial assemblies, is limited by the inability to uncover their dynamics on their characteristic length and time scales. Here, we nevertheless demonstrate this ability using MHz X-ray photon correlation spectroscopy (XPCS) -- directly elucidating the characteristic microsecond-dynamics of density fluctuations of semiconductor nanocrystals (NCs), not only in a colloidal dispersion but also in a liquid phase consisting of densely packed, yet mobile, NCs with no long-range order. We find the wavevector-dependent fluctuation rates in the liquid phase are suppressed relative to those in the colloidal phase and relative to observations of densely packed repulsive particles. We show that the suppressed rates are due to a substantial decrease in the self-diffusion of NCs, which we attribute to explicit attractive interactions. Using coarse-grained simulations, we find that the extracted shape and strength of the interparticle potential explains the stability of the liquid phase, in contrast to the gelation observed via XPCS in many other charged colloidal systems. This work opens the door to elucidating fast, condensed phase dynamics in complex fluids and other nanoscale soft matter, such as densely packed proteins and non-equilibrium self-assembly processes, in addition to designing microscopic strategies to avert gelation. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2404_17756 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Origins of suppressed self-diffusion of nanoscale constituents of a complex liquid Tanner, Christian P. N. Wall, Vivian R. K. Gababa, Mumtaz Portner, Joshua Jeong, Ahhyun Hurley, Matthew J. Leonard, Nicholas Raybin, Jonathan G. Utterback, James K. Kim, Ahyoung Fluerasu, Andrei Sun, Yanwen Moeller, Johannes Zozulya, Alexey Jo, Wonhyuk Brausse, Felix Wrigley, James Boesenberg, Ulrike Pudell, Jan-Etienne Hallmann, Joerg Lu, Wei Shayduk, Roman Youssef, Mohamed Madsen, Anders Limmer, David T. Talapin, Dmitri V. Teitelbaum, Samuel W. Ginsberg, Naomi S. Soft Condensed Matter Mesoscale and Nanoscale Physics Materials Science Statistical Mechanics Chemical Physics Understanding and ultimately controlling the transformations and properties of nanoscale systems, from proteins to synthetic nanomaterial assemblies, is limited by the inability to uncover their dynamics on their characteristic length and time scales. Here, we nevertheless demonstrate this ability using MHz X-ray photon correlation spectroscopy (XPCS) -- directly elucidating the characteristic microsecond-dynamics of density fluctuations of semiconductor nanocrystals (NCs), not only in a colloidal dispersion but also in a liquid phase consisting of densely packed, yet mobile, NCs with no long-range order. We find the wavevector-dependent fluctuation rates in the liquid phase are suppressed relative to those in the colloidal phase and relative to observations of densely packed repulsive particles. We show that the suppressed rates are due to a substantial decrease in the self-diffusion of NCs, which we attribute to explicit attractive interactions. Using coarse-grained simulations, we find that the extracted shape and strength of the interparticle potential explains the stability of the liquid phase, in contrast to the gelation observed via XPCS in many other charged colloidal systems. This work opens the door to elucidating fast, condensed phase dynamics in complex fluids and other nanoscale soft matter, such as densely packed proteins and non-equilibrium self-assembly processes, in addition to designing microscopic strategies to avert gelation. |
| title | Origins of suppressed self-diffusion of nanoscale constituents of a complex liquid |
| topic | Soft Condensed Matter Mesoscale and Nanoscale Physics Materials Science Statistical Mechanics Chemical Physics |
| url | https://arxiv.org/abs/2404.17756 |