Coherent X-ray Scattering Reveals Nanoscale Fluctuations in Hydrated Proteins

Bin, Maddalena; Reiser, M.; Filianina, Mariia; Berkowicz, Sharon; Das, Sudipta; Timmermann, Sonja; Roseker, Wojciech; Bauer, Robert; Öström, Jonatan; Karina, Aigerim; Amann‐Winkel, Katrin; Ladd-Parada, Marjorie; Westermeier, Fabian; Sprung, Michael; Möller, Johannes; Lehmkühler, Felix; Gutt, Christian; Perakis, Fivos

doi:10.1021/acs.jpcb.3c02492

Cited by 5 publications

(2 citation statements)

References 67 publications

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“…( 3 )). The plot also includes data from Chushkin et al 30 on protein glasses (yellow), Ruta et al 26 on oxide glasses (grey) and Bin et al 79 who investigated hydrated lysozyme (pink, see SI material for details). …”

Section: Methodsmentioning

confidence: 99%

X-ray driven and intrinsic dynamics in protein gels

Timmermann,

Anthuparambil,

Girelli

et al. 2023

Sci Rep

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We use X-ray photon correlation spectroscopy to investigate how structure and dynamics of egg white protein gels are affected by X-ray dose and dose rate. We find that both, changes in structure and beam-induced dynamics, depend on the viscoelastic properties of the gels with soft gels prepared at low temperatures being more sensitive to beam-induced effects. Soft gels can be fluidized by X-ray doses of a few kGy with a crossover from stress relaxation dynamics (Kohlrausch–Williams–Watts exponents $$k \approx 1.5$$ k ≈ 1.5 to 2) to typical dynamical heterogeneous behavior ($$k<$$ k < 1) while the high temperature egg white gels are radiation-stable up to doses of 15 kGy with $$k\ge 1.5$$ k ≥ 1.5 . For all gel samples we observe a crossover from equilibrium dynamics to beam induced motion upon increasing X-ray fluence and determine the resulting fluence threshold values $$\Phi _D$$ Φ D . Surprisingly small threshold values of $$\Phi _D=(3 \pm 2)\times 10^{-3} \,\textrm{ph}\,$$ Φ D = ( 3 ± 2 ) × 10 - 3 ph s$$^{-1}$$ - 1 nm$$^{-2}$$ - 2 can drive the dynamics in the soft gels while for stronger gels this threshold is increased to $$\Phi _D=(0.9 \pm 0.3) \,\textrm{ph}$$ Φ D = ( 0.9 ± 0.3 ) ph s$$^{-1}$$ - 1 nm$$^{-2}$$ - 2 . We explain our observations with the viscoelastic properties of the materials and can connect the threshold dose for structural beam damage with the dynamic properties of beam-induced motion. Our results suggest that soft viscoelastic materials can display pronounced X-ray driven motion even for low X-ray fluences. This induced motion is not detectable by static scattering as it appears at dose values well below the static damage threshold. We show that intrinsic sample dynamics can be separated from X-ray driven motion by measuring the fluence dependence of the dynamical properties.

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Section: Methodsmentioning

confidence: 99%

X-ray driven and intrinsic dynamics in protein gels

Timmermann,

Anthuparambil,

Girelli

et al. 2023

Sci Rep

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“…Recently, XPCS has proven to be a powerful tool for studies of protein dynamics. [31][32][33][34][35] For instance, Reiser et al monitored antibody protein dynamics at sub-μs temporal resolution on molecular length scales using megahertz XPCS measurements at the European X-ray free-electron laser (XFEL). [32] Typically, NPs can be used as tracers in XPCS studies or be the subject under study itself.…”

Section: Introductionmentioning

confidence: 99%

The dynamics of PEG‐coated nanoparticles in concentrated protein solutions up to the molecular crowding range

Otto,

Dallari,

Westermeier

et al. 2024

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Polymer‐coated nanoparticles are widely studied in the context of nanomedicine and it is therefore of utmost importance to understand not only how their structure but also how their colloidal dynamics are affected by physiologically relevant conditions. A characteristic feature of the cytosol of cells is the very high concentration of proteins among other matrix components, often termed macromolecular crowding. Here, the structure and colloidal dynamics of poly(ethylene glycol) (PEG)‐coated gold nanoparticles in the presence of bovine serum albumin (BSA) concentrations ranging from 0 to 265 mg/mL are studied with X‐ray photon correlation spectroscopy. For protein–nanoparticle mixtures with high BSA concentrations, comparable to intracellular levels, a significant deviation of the apparent viscosity from expectations for pure BSA solutions is found. The findings strongly indicate that the nanoscopic viscous properties of the dense protein solutions are significantly affected by the nanoparticles. At these high concentrations, the colloidal stability of the samples depends on the molecular weight of the coating PEG–ligand, whereas at lower concentrations no differences are observed.

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Distinguishing Protein Corona from Nanoparticle Aggregate Formation in Complex Biological Media Using X-ray Photon Correlation Spectroscopy

Silva,

Picco,

Galdino

et al. 2024

Nano Lett.

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In biological systems, nanoparticles interact with biomolecules, which may undergo protein corona formation that can result in noncontrolled aggregation. Therefore, comprehending the behavior and evolution of nanoparticles in the presence of biological fluids is paramount in nanomedicine. However, traditional lab-based colloid methods characterize diluted suspensions in low-complexity media, which hinders in-depth studies in complex biological environments. Here, we apply X-ray photon correlation spectroscopy (XPCS) to investigate silica nanoparticles (SiO 2 ) in various environments, ranging from low to high complex biological media. Interestingly, SiO 2 revealed Brownian motion behavior, irrespective of the complexity of the chosen media. Moreover, the SiO 2 surface and media composition were tailored to underline the differences between a corona-free system from protein corona and aggregates formation. Our results highlighted XPCS potential for real-time nanoparticle analysis in biological media, surpassing the limitations of conventional techniques and offering deeper insights into colloidal behavior in complex environments.

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Coherent X-ray Scattering Reveals Nanoscale Fluctuations in Hydrated Proteins

Cited by 5 publications

References 67 publications

X-ray driven and intrinsic dynamics in protein gels

X-ray driven and intrinsic dynamics in protein gels

The dynamics of PEG‐coated nanoparticles in concentrated protein solutions up to the molecular crowding range

Distinguishing Protein Corona from Nanoparticle Aggregate Formation in Complex Biological Media Using X-ray Photon Correlation Spectroscopy

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