Light-Induced Pulsed EPR Dipolar Spectroscopy on a Paradigmatic Hemeprotein

Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry
Maria Giulia Dal FarraMarilena Di Valentin

Abstract

Light-induced pulsed EPR dipolar spectroscopic methods allow the determination of nanometer distances between paramagnetic sites. Here we employ orthogonal spin labels, a chromophore triplet state and a stable radical, to carry out distance measurements in singly nitroxide-labeled human neuroglobin. We demonstrate that Zn-substitution of neuroglobin, to populate the Zn(II) protoporphyrin IX triplet state, makes it possible to perform light-induced pulsed dipolar experiments on hemeproteins, extending the use of light-induced dipolar spectroscopy to this large class of metalloproteins. The versatility of the method is ensured by the employment of different techniques: relaxation-induced dipolar modulation enhancement (RIDME) is applied for the first time to the photoexcited triplet state. In addition, an alternative pulse scheme for laser-induced magnetic dipole (LaserIMD) spectroscopy, based on the refocused-echo detection sequence, is proposed for accurate zero-time determination and reliable distance analysis.

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Citations

Sep 2, 2020·Physical Chemistry Chemical Physics : PCCP·Maria Giulia Dal FarraMarilena Di Valentin
Jun 13, 2020·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Natalya SannikovaOlesya Krumkacheva
Nov 8, 2020·Chemical Communications : Chem Comm·Lara WilliamsMalte Drescher
Dec 9, 2020·Physical Chemistry Chemical Physics : PCCP·Matthew W DaleChristopher J Wedge
Dec 12, 2020·The Journal of Physical Chemistry Letters·Arnau BertranAlice M Bowen
Apr 16, 2021·The Journal of Physical Chemistry Letters·Alice M BowenMarilena Di Valentin
Sep 11, 2019·The Journal of Physical Chemistry. B·Alessandro AgostiniDonatella Carbonera
Feb 4, 2022·Physical Chemistry Chemical Physics : PCCP·Ivan O TimofeevMatvey V Fedin

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Methods Mentioned

BETA
dipolar
electron double resonance

Software Mentioned

MMM ( Multiscale Modelling of Macromolecules )
LiDEER
LaserIMD
MMM
RIDME
DEER
DeerAnalysis
OvertoneAnalysis
ReLaserIMD

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