Protein Diffusion and Stokes-Einstein Deviation in Supercooled Cryoprotectant Solutions
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2025
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| author | Bin, Maddalena Girelli, Anita Filianina, Mariia Reiser, Mario Berkowicz, Sharon Åhlfeldt, Milla Dargasz, Michelle Timmermann, Sonja Savelkouls, Jaqueline Kawasaki, Takeshi Saito, Shinji Zontone, Federico Chushkin, Yuriy Zhang, Fajun Schreiber, Frank Paulus, Michael Gutt, Christian Perakis, Fivos |
| author_facet | Bin, Maddalena Girelli, Anita Filianina, Mariia Reiser, Mario Berkowicz, Sharon Åhlfeldt, Milla Dargasz, Michelle Timmermann, Sonja Savelkouls, Jaqueline Kawasaki, Takeshi Saito, Shinji Zontone, Federico Chushkin, Yuriy Zhang, Fajun Schreiber, Frank Paulus, Michael Gutt, Christian Perakis, Fivos |
| contents | Vitrification during cryopreservation requires a detailed understanding of the dynamic behavior of biological solutions. We investigate ferritin diffusion in glycerol-water mixtures at supercooled temperatures using X-ray Photon Correlation Spectroscopy (XPCS). Diffusion coefficients were measured from ambient conditions to $T = 210$ K and analyzed using the Vogel-Fulcher-Tammann (VFT) relation, yielding an arrest temperature of $T_0 = 85 \pm 11$ K for ferritin ($R_{\rm h} = 7.3$ nm), markedly lower than $T_0 = 122 \pm 4$ K for larger nanoparticles ($R_{\rm h} = 50$ nm). Below $T \approx 230$ K, ferritin diffusion exceeds the Stokes-Einstein prediction by up to a factor of 2.7, revealing nanoscale deviations from bulk viscosity. A fluctuating-friction model quantitatively links this enhancement to local friction heterogeneity, with fluctuations increasing upon cooling and reaching $\sim 80\%$ of the mean friction at $T=210$ K. These results establish a molecular-scale connection between protein diffusion and solvent dynamical heterogeneity in cryoprotected solutions. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2512_02742 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Protein Diffusion and Stokes-Einstein Deviation in Supercooled Cryoprotectant Solutions Bin, Maddalena Girelli, Anita Filianina, Mariia Reiser, Mario Berkowicz, Sharon Åhlfeldt, Milla Dargasz, Michelle Timmermann, Sonja Savelkouls, Jaqueline Kawasaki, Takeshi Saito, Shinji Zontone, Federico Chushkin, Yuriy Zhang, Fajun Schreiber, Frank Paulus, Michael Gutt, Christian Perakis, Fivos Soft Condensed Matter Vitrification during cryopreservation requires a detailed understanding of the dynamic behavior of biological solutions. We investigate ferritin diffusion in glycerol-water mixtures at supercooled temperatures using X-ray Photon Correlation Spectroscopy (XPCS). Diffusion coefficients were measured from ambient conditions to $T = 210$ K and analyzed using the Vogel-Fulcher-Tammann (VFT) relation, yielding an arrest temperature of $T_0 = 85 \pm 11$ K for ferritin ($R_{\rm h} = 7.3$ nm), markedly lower than $T_0 = 122 \pm 4$ K for larger nanoparticles ($R_{\rm h} = 50$ nm). Below $T \approx 230$ K, ferritin diffusion exceeds the Stokes-Einstein prediction by up to a factor of 2.7, revealing nanoscale deviations from bulk viscosity. A fluctuating-friction model quantitatively links this enhancement to local friction heterogeneity, with fluctuations increasing upon cooling and reaching $\sim 80\%$ of the mean friction at $T=210$ K. These results establish a molecular-scale connection between protein diffusion and solvent dynamical heterogeneity in cryoprotected solutions. |
| title | Protein Diffusion and Stokes-Einstein Deviation in Supercooled Cryoprotectant Solutions |
| topic | Soft Condensed Matter |
| url | https://arxiv.org/abs/2512.02742 |