Coherent X-rays reveal anomalous molecular diffusion and cage effects in crowded protein solutions
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| Format: | Preprint |
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2024
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| author | Girelli, Anita Bin, Maddalena Filianina, Mariia Dargasz, Michelle Anthuparambil, Nimmi Das Möller, Johannes Zozulya, Alexey Andronis, Iason Timmermann, Sonja Berkowicz, Sharon Retzbach, Sebastian Reiser, Mario Raza, Agha Mohammad Kowalski, Marvin Akhundzadeh, Mohammad Sayed Schrage, Jenny Woo, Chang Hee Senft, Maximilian D. Reichart, Lara Franziska Leonau, Aliaksandr Rajaiah, Prince Prabhu Chèvremont, William Seydel, Tilo Hallmann, Jörg Rodriguez-Fernandez, Angel Pudell, Jan-Etienne Brausse, Felix Boesenberg, Ulrike Wrigley, James Youssef, Mohamed Lu, Wei Jo, Wonhyuk Shayduk, Roman Guest, Trey Madsen, Anders Lehmkühler, Felix Paulus, Michael Zhang, Fajun Schreiber, Frank Gutt, Christian Perakis, Fivos |
| author_facet | Girelli, Anita Bin, Maddalena Filianina, Mariia Dargasz, Michelle Anthuparambil, Nimmi Das Möller, Johannes Zozulya, Alexey Andronis, Iason Timmermann, Sonja Berkowicz, Sharon Retzbach, Sebastian Reiser, Mario Raza, Agha Mohammad Kowalski, Marvin Akhundzadeh, Mohammad Sayed Schrage, Jenny Woo, Chang Hee Senft, Maximilian D. Reichart, Lara Franziska Leonau, Aliaksandr Rajaiah, Prince Prabhu Chèvremont, William Seydel, Tilo Hallmann, Jörg Rodriguez-Fernandez, Angel Pudell, Jan-Etienne Brausse, Felix Boesenberg, Ulrike Wrigley, James Youssef, Mohamed Lu, Wei Jo, Wonhyuk Shayduk, Roman Guest, Trey Madsen, Anders Lehmkühler, Felix Paulus, Michael Zhang, Fajun Schreiber, Frank Gutt, Christian Perakis, Fivos |
| contents | Understanding protein motion within the cell is crucial for predicting reaction rates and macromolecular transport in the cytoplasm. A key question is how crowded environments affect protein dynamics through hydrodynamic and direct interactions at molecular length scales. Using megahertz X-ray Photon Correlation Spectroscopy (MHz-XPCS) at the European X-ray Free Electron Laser (EuXFEL), we investigate ferritin diffusion at microsecond time scales. Our results reveal anomalous diffusion, indicated by the non-exponential decay of the intensity autocorrelation function $g_2(q,t)$ at high concentrations. This behavior is consistent with the presence of cage-trapping in between the short- and long-time protein diffusion regimes. Modeling with the $δγ$-theory of hydrodynamically interacting colloidal spheres successfully reproduces the experimental data by including a scaling factor linked to the protein direct interactions. These findings offer new insights into the complex molecular motion in crowded protein solutions, with potential applications for optimizing ferritin-based drug delivery, where protein diffusion is the rate-limiting step. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2410_08873 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Coherent X-rays reveal anomalous molecular diffusion and cage effects in crowded protein solutions Girelli, Anita Bin, Maddalena Filianina, Mariia Dargasz, Michelle Anthuparambil, Nimmi Das Möller, Johannes Zozulya, Alexey Andronis, Iason Timmermann, Sonja Berkowicz, Sharon Retzbach, Sebastian Reiser, Mario Raza, Agha Mohammad Kowalski, Marvin Akhundzadeh, Mohammad Sayed Schrage, Jenny Woo, Chang Hee Senft, Maximilian D. Reichart, Lara Franziska Leonau, Aliaksandr Rajaiah, Prince Prabhu Chèvremont, William Seydel, Tilo Hallmann, Jörg Rodriguez-Fernandez, Angel Pudell, Jan-Etienne Brausse, Felix Boesenberg, Ulrike Wrigley, James Youssef, Mohamed Lu, Wei Jo, Wonhyuk Shayduk, Roman Guest, Trey Madsen, Anders Lehmkühler, Felix Paulus, Michael Zhang, Fajun Schreiber, Frank Gutt, Christian Perakis, Fivos Soft Condensed Matter Chemical Physics Understanding protein motion within the cell is crucial for predicting reaction rates and macromolecular transport in the cytoplasm. A key question is how crowded environments affect protein dynamics through hydrodynamic and direct interactions at molecular length scales. Using megahertz X-ray Photon Correlation Spectroscopy (MHz-XPCS) at the European X-ray Free Electron Laser (EuXFEL), we investigate ferritin diffusion at microsecond time scales. Our results reveal anomalous diffusion, indicated by the non-exponential decay of the intensity autocorrelation function $g_2(q,t)$ at high concentrations. This behavior is consistent with the presence of cage-trapping in between the short- and long-time protein diffusion regimes. Modeling with the $δγ$-theory of hydrodynamically interacting colloidal spheres successfully reproduces the experimental data by including a scaling factor linked to the protein direct interactions. These findings offer new insights into the complex molecular motion in crowded protein solutions, with potential applications for optimizing ferritin-based drug delivery, where protein diffusion is the rate-limiting step. |
| title | Coherent X-rays reveal anomalous molecular diffusion and cage effects in crowded protein solutions |
| topic | Soft Condensed Matter Chemical Physics |
| url | https://arxiv.org/abs/2410.08873 |