Molecular rotational correlation times and nanoviscosity determined by 111mCd perturbed angular correlation (PAC) of γ‐rays spectroscopy
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Molecular rotational correlation times and nanoviscosity determined by 111mCd perturbed angular correlation (PAC) of γ‐rays spectroscopy. / Fromsejer, Rasmus; Jensen, Marianne L.; Zacate, Matthew O.; Karner, Victoria; Pecoraro, Vincent L.; Hemmingsen, Lars.
In: Chemistry: A European Journal, Vol. 29, No. 9, e202203084, 2023.Research output: Contribution to journal › Journal article › Research › peer-review
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TY - JOUR
T1 - Molecular rotational correlation times and nanoviscosity determined by 111mCd perturbed angular correlation (PAC) of γ‐rays spectroscopy
AU - Fromsejer, Rasmus
AU - Jensen, Marianne L.
AU - Zacate, Matthew O.
AU - Karner, Victoria
AU - Pecoraro, Vincent L.
AU - Hemmingsen, Lars
PY - 2023
Y1 - 2023
N2 - The nanoviscosity experienced by molecules in solution may be determined through measurement of the molecular rotational correlation time, τc, for example, by fluorescence and NMR spectroscopy. With this work, we apply PAC spectroscopy to determine the rate of rotational diffusion, λ=1/τc, of a de novo designed protein, TRIL12AL16C, in solutions with viscosities, ξ, from 1.7 to 88 mPa⋅s. TRIL12AL16C was selected as molecular probe because it exhibits minimal effects due to intramolecular dynamics and static line broadening, allowing for exclusive elucidation of molecular rotational diffusion. Diffusion rates determined by PAC data agree well with literature data from fluorescence and NMR spectroscopy, and scales linearly with 1/ξ in agreement with the Stokes–Einstein–Debye model. PAC experiments require only trace amounts (∼1011) of probe nuclei and can be conducted over a broad range of sample temperatures and pressures. Moreover, most materials are relatively transparent to γ-rays. Thus, PAC spectroscopy could find applications under circumstances where conventional techniques cannot be applied, spanning from the physics of liquids to in-vivo biochemistry.
AB - The nanoviscosity experienced by molecules in solution may be determined through measurement of the molecular rotational correlation time, τc, for example, by fluorescence and NMR spectroscopy. With this work, we apply PAC spectroscopy to determine the rate of rotational diffusion, λ=1/τc, of a de novo designed protein, TRIL12AL16C, in solutions with viscosities, ξ, from 1.7 to 88 mPa⋅s. TRIL12AL16C was selected as molecular probe because it exhibits minimal effects due to intramolecular dynamics and static line broadening, allowing for exclusive elucidation of molecular rotational diffusion. Diffusion rates determined by PAC data agree well with literature data from fluorescence and NMR spectroscopy, and scales linearly with 1/ξ in agreement with the Stokes–Einstein–Debye model. PAC experiments require only trace amounts (∼1011) of probe nuclei and can be conducted over a broad range of sample temperatures and pressures. Moreover, most materials are relatively transparent to γ-rays. Thus, PAC spectroscopy could find applications under circumstances where conventional techniques cannot be applied, spanning from the physics of liquids to in-vivo biochemistry.
U2 - 10.1002/chem.202203084
DO - 10.1002/chem.202203084
M3 - Journal article
C2 - 36453728
VL - 29
JO - Chemistry: A European Journal
JF - Chemistry: A European Journal
SN - 0947-6539
IS - 9
M1 - e202203084
ER -
ID: 327938120