Lanthanide‐Based Probes for Imaging Detection of Enzyme Activities by NIR Luminescence, T1‐ and ParaCEST MRI

Author:

Jouclas Rémy1,Laine Sophie2,Eliseeva Svetlana V.2,Mandel Jérémie1,Szeremeta Frédéric2,Retailleau Pascal1,He Jiefang1,Gallard Jean‐François1,Pallier Agnès2,Bonnet Célia S.2,Petoud Stéphane2,Durand Philippe1,Tóth Éva2ORCID

Affiliation:

1. Université Paris-Saclay CNRS Institut de Chimie des Substances Naturelles UPR 2301 91198 Gif-sur-Yvette France

2. Centre de Biophysique Moléculaire CNRS UPR 4301 Université d'Orléans rue Charles Sadron 45071 Orléans France

Abstract

AbstractApplying a single molecular probe to monitor enzymatic activities in multiple, complementary imaging modalities is highly desirable to ascertain detection and to avoid the complexity associated with the use of agents of different chemical entities. We demonstrate here the versatility of lanthanide (Ln3+) complexes with respect to their optical and magnetic properties and their potential for enzymatic detection in NIR luminescence, CEST and T1 MR imaging, controlled by the nature of the Ln3+ ion, while using a unique chelator. Based on X‐ray structural, photophysical, and solution NMR investigations of a family of Ln3+ DO3A‐pyridine model complexes, we could rationalize the luminescence (Eu3+, Yb3+), CEST (Yb3+) and relaxation (Gd3+) properties and their variations between carbamate and amine derivatives. This allowed the design of probes which undergo enzyme‐mediated changes detectable in NIR luminescence, CEST and T1‐weighted MRI, respectively governed by variations in their absorption energy, in their exchanging proton pool and in their size, thus relaxation efficacy. We demonstrate that these properties can be exploited for the visualization of β‐galactosidase activity in phantom samples by different imaging modalities: NIR optical imaging, CEST and T1‐weighted MRI.

Funder

Agence Nationale de la Recherche

Publisher

Wiley

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