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Computing distance distributions from dipolar evolution data with overtones: RIDME spectroscopy with Gd(iii)-based

Katharina Keller1, Valerie Mertens1, Mian Qi2

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This study improves distance measurements using relaxation induced dipolar modulation enhancement (RIDME) by accounting for harmonic overtones. This method offers more accurate distance distributions than DEER for high-spin labels in structural biology.

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Area of Science:

  • Biophysics
  • Structural Biology
  • Magnetic Resonance Spectroscopy

Background:

  • Accurate distance measurements are crucial for understanding molecular structures.
  • Relaxation Induced Dipolar Modulation Enhancement (RIDME) is a technique for determining distances between paramagnetic centers.
  • Overtones of dipolar frequencies can complicate RIDME data analysis.

Purpose of the Study:

  • To analyze the performance of a modified kernel function in Tikhonov regularization for RIDME data analysis.
  • To account for harmonic overtones in RIDME measurements.
  • To compare the accuracy of RIDME with harmonic overtones to Double Electron-Electron Resonance (DEER).

Main Methods:

  • Utilized a modified kernel function within Tikhonov regularization analysis.
  • Employed Gd(iii)-PyMTA complexes as paramagnetic high-spin labels in model compounds.
  • Calibrated overtone coefficients for the RIDME kernel.

Main Results:

  • Demonstrated accurate distance distribution extraction from RIDME data by including harmonic overtones.
  • Showed that RIDME with overtone analysis provides more accurate distances than Gd(iii)-Gd(iii) DEER for the studied Gd-rulers.
  • Developed and utilized the open-source MATLAB program OvertoneAnalysis.

Conclusions:

  • The developed approach accurately extracts distance distributions from RIDME data, even with harmonic overtones.
  • RIDME, when analyzed with harmonic overtones, offers superior accuracy compared to DEER for high-spin labels.
  • This method facilitates the routine application of RIDME in structural biology and soft matter studies.