4.8 Article

Temperature response of 129Xe depolarization transfer and its application for ultrasensitive NMR detection

期刊

PHYSICAL REVIEW LETTERS
卷 100, 期 25, 页码 -

出版社

AMER PHYSICAL SOC
DOI: 10.1103/PhysRevLett.100.257603

关键词

-

向作者/读者索取更多资源

Trapping xenon in functionalized cryptophane cages makes the sensitivity of hyperpolarized (HP) (129)Xe available for specific NMR detection of biomolecules. Here, we study the signal transfer onto a reservoir of unbound HP xenon by gating the residence time of the nuclei in the cage through the temperature-dependant exchange rate. Temperature changes larger than similar to 0.6 K are detectable as an altered reservoir signal. The temperature response is adjustable with lower concentrations of caged xenon providing more sensitivity at higher temperatures. Ultrasensitive detection of functionalized cryptophane at 310 K is demonstrated with a concentration of 10 nM, corresponding to a similar to 4000-fold sensitivity enhancement compared to conventional detection. This makes HPNMR capable of detecting such constructs in concentrations far below the detection limit of benchtop uv-visible light absorbance.

作者

我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。

评论

主要评分

4.8
评分不足

次要评分

新颖性
-
重要性
-
科学严谨性
-
评价这篇论文

推荐

Review Biochemistry & Molecular Biology

Probing Reversible Guest Binding with Hyperpolarized 129Xe-NMR: Characteristics and Applications for Cucurbit[n]urils

Jabadurai Jayapaul, Leif Schroder

MOLECULES (2020)

Article Chemistry, Medicinal

Mapping of Absolute Host Concentration and Exchange Kinetics of Xenon Hyper-CEST MRI Agents

Martin Kunth, Christopher Witte, Leif Schroeder

Summary: Xenon magnetic resonance imaging (MRI) offers excellent sensitivity through the combination of spin hyperpolarization and chemical exchange saturation transfer (CEST), with molecular hosts like cryptophane-A or cucurbit[n]urils providing opportunities for switchable MRI reporters. Utilizing an internal reference host to resolve exchange kinetics information allows quantitative comparisons of different ultra-sensitive MRI reporters.

PHARMACEUTICALS (2021)

Article Chemistry, Multidisciplinary

M01 as a novel drug enhancer for specifically targeting the blood-brain barrier

Olga Breitkreuz-Korff, Christian Tscheik, Giovanna Del Vecchio, Sophie Dithmer, Wolfgang Walther, Andrea Orthmann, Hartwig Wolburg, Reiner F. Haseloff, Leif Schroeder, Ingolf E. Blasig, Lars Winkler

Summary: M01, identified as a claudin-5 interaction inhibitor, transiently increases BBB permeability and enables enhanced delivery of neuropharmaceuticals to the brain by weakening cell-cell interactions.

JOURNAL OF CONTROLLED RELEASE (2021)

Article Radiology, Nuclear Medicine & Medical Imaging

Microscopic multifrequency MR elastography for mapping viscoelasticity in zebrafish

Jakob Ernst Luis Jordan, Gergely Bertalan, Tom Meyer, Heiko Tzschaetzsch, Anton Gauert, Luca Brame, Helge Herthum, Yasmine Safraou, Leif Schroeder, Juergen Braun, Anja I. H. Hagemann, Ingolf Sack

Summary: The zebrafish has become an important model in biomedical research, and there is increasing interest in mapping its viscoelastic properties using elastography methods. A study using microscopic multifrequency MR elastography showed distinct differences in stiffness and viscosity of different tissue regions in zebrafish, providing valuable information for neuromechanical and oncological research.

MAGNETIC RESONANCE IN MEDICINE (2022)

Article Biophysics

Improving HyperCEST performance by favorable xenon exchange conditions in liposomal nanocarriers

Jan Oliver Jost, Leif Schroeder

Summary: This study introduces liposomes with a HyperCEST-active lipopeptide to enhance the efficiency of Xe host, CrA-ma. Using depolarization time as a comparative measure, the researchers found that incorporating CrA-lipopeptides into liposomal carriers allows for significant image contrast even with lower saturation power.

NMR IN BIOMEDICINE (2023)

Article Multidisciplinary Sciences

An NMR relaxometry approach for quantitative investigation of the transchelation of gadolinium ions from GBCAs to a competing macromolecular chelator

Patrick Werner, Matthias Taupitz, Leif Schroeder, Patrick Schuenke

Summary: Gadolinium-based contrast agents have been used in clinical MRI for over 30 years, but evidence suggests their dissociation in vivo can lead to long-term deposition of gadolinium ions. In vitro experiments provide insight into the kinetics and thermodynamics of these processes. A new MRI relaxometry-based approach is developed to study the interactions of GBCAs with competing chelators, showing potential for identifying potent Gd-complexing macromolecular species.

SCIENTIFIC REPORTS (2021)

Article Chemistry, Medicinal

Investigating the Role of Sulfate Groups for the Binding of Gd3+ Ions to Glycosaminoglycans with NMR Relaxometry

Patrick Werner, Patrick Schuenke, Oxana Krylova, Heike Nikolenko, Matthias Taupitz, Leif Schroeder

Summary: This study investigates the interaction between glycosaminoglycans and gadolinium ions and its impact on clinical MR imaging contrast agents. The results highlight the crucial role of sulfate groups in the chelation process and suggest that GAGs with higher degrees of sulfation are more likely to engage in this mechanism.

CHEMMEDCHEM (2022)

Article Multidisciplinary Sciences

Hyper-CEST NMR of metal organic polyhedral cages reveals hidden diastereomers with diverse guest exchange kinetics

Jabadurai Jayapaul, Sanna Komulainen, Vladimir V. Zhivonitko, Jiri Mares, Chandan Giri, Kari Rissanen, Perttu Lantto, Ville-Veikko Telkki, Leif Schroeder

Summary: Guest capture and release are essential properties of self-assembling nanostructures, with guests potentially transitioning between different environments to escape common spectroscopy techniques. This study uses spin-hyperpolarized Xe-129 hyper-CEST NMR to investigate an iron-based metal organic polyhedron's cavity, revealing unknown signals persisting under various perturbations, likely originating from Xe bound to three Fe-MOP diastereomers inducing steric effects. These findings have implications for selective spin manipulation in CEST MRI agents and processes occurring on a millisecond time scale.

NATURE COMMUNICATIONS (2022)

Article Engineering, Biomedical

Mechanical behavior of the hippocampus and corpus callosum: An attempt to reconcile ex vivo with in vivo and micro with macro properties

Gergerly Bertalan, Julia Becker, Heiko Tzschaetzsch, Anna Morr, Helge Herthum, Mehrgan Shahryari, Ryan D. Greenhalgh, Jing Guo, Leif Schroeder, Christian Alzheimer, Silvia Budday, Kristian Franze, Juergen Braun, Ingolf Sack

Summary: The mechanical properties of brain tissue are complex and vary depending on species, region, measurement method, and in vivo or ex vivo conditions. Through various methods, we found that brain stiffness shows remarkable consistency across species, in vivo and ex vivo states, and different measurement techniques when considering viscoelastic dispersion properties combining equilibrium and non-equilibrium mechanical elements.

JOURNAL OF THE MECHANICAL BEHAVIOR OF BIOMEDICAL MATERIALS (2023)

Article Chemistry, Multidisciplinary

Automated optimization of spatial resolution for single-sided NMR

Lyndi Kiple, John Ballenger, Kristina Keating, Anagi M. M. Balachandra, Tyler Meldrum

Summary: Single-sided NMR instruments use inhomogeneous magnetic fields to probe physical properties of materials. We developed an algorithmic approach to position flat samples coplanar with the magnet's sensitive region. This positioning process improves the spatial resolution of single-sided NMR measurements for planar samples in research and industrial settings.

MAGNETIC RESONANCE IN CHEMISTRY (2023)

Review Nanoscience & Nanotechnology

Nanomaterials for hyperpolarized nuclear magnetic resonance and magnetic resonance imaging

Philip Saul, Leif Schroder, Andreas B. B. Schmidt, Jan-Bernd Hovener

Summary: Nanomaterials are crucial in the development and application of hyperpolarized materials for MRI. They can function as both directly imaged hyperpolarized materials, carriers for hyperpolarized gases, and catalysts for generating hyperpolarized substrates. This article provides an overview of recent developments in these three application possibilities, highlighting carbon-based materials for direct imaging. The importance of nanomaterials in MRI is discussed, including their biocompatibility and imaging experiments.

WILEY INTERDISCIPLINARY REVIEWS-NANOMEDICINE AND NANOBIOTECHNOLOGY (2023)

Article Chemistry, Applied

Characterization of molecular environments and chemical exchange in acrylic paints via single-sided NMR

Lyndi Kiple, Tyler Lee, Gillian Zavaglia, Tyler Meldrum

Summary: In this study, single-sided 1H NMR relaxometry was used to characterize the molecular environments in both dry and wet acrylic paints by their molecular mobilities. Two different relaxation behaviors were identified in dry paint, indicating regions of greater and lesser mobility, attributed to amorphous and crystalline domains of the semi-crystalline acrylic polymer. In wet paint, two different relaxation behaviors were characterized, hypothesized to come from unique molecular environments in the acrylic binding medium, along with two simultaneous exchange processes involving aqueous solvent.

PROGRESS IN ORGANIC COATINGS (2023)

Article Chemistry, Physical

Rapid analytical CEST spectroscopy of competitive host-guest interactions using spatial parallelization with a combined approach of variable flip angle, keyhole and averaging (CAVKA)

Hen-Amit Morik, Patrick Schuenke, Leif Schroeder

Summary: A serious limitation of high resolution Xe-129 chemical exchange saturation transfer (CEST) NMR spectroscopy is the long acquisition time due to step-wise encoding of the chemical shift dimension. This study presents a method of optimized use of Xe-129 spin magnetization to enable the accelerated and simultaneous acquisition of CEST spectra from multiple samples or regions. The method is applied to investigate the host-guest system of CB7 and xenon with competing guests, revealing that the observed CEST signal is from a CB6 impurity and that CB7 itself does not produce a CEST signal.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2022)

Article Chemistry, Multidisciplinary

Identification of extracellular nanoparticle subsets by nuclear magnetic resonance

Md Sharif Ullah, Vladimir V. Zhivonitko, Anatoliy Samoylenko, Artem Zhyvolozhnyi, Sirja Viitala, Santeri Kankaanpaa, Sanna Komulainen, Leif Schroeder, Seppo J. Vainio, Ville-Veikko Telkki

Summary: Exosomes are a subset of lipid envelope-encapsulated extracellular vesicles of 50-150 nm diameter, with many smaller and larger nanoparticles co-isolated during purification processes. Diffusion ordered spectroscopy (DOSY) nuclear magnetic resonance (NMR) method enables the determination of a broad distribution of extracellular nanoparticles, ranging from 1 to 500 nm, showing the presence of smaller particles not visible in traditional analysis methods. Hyperpolarized chemical exchange saturation transfer (Hyper-CEST) with Xe-129 NMR also indicates the existence of smaller and larger nanoparticles in the EV samples, suggesting faster exchange rates in the EV pool compared to other nanoparticle pools.

CHEMICAL SCIENCE (2021)

Article Chemistry, Multidisciplinary

Binding site exchange kinetics revealed through efficient spin-spin dephasing of hyperpolarized 129Xe

Martin Kunth, Leif Schroeder

Summary: The study simplifies the behavior of spin-spin relaxation rates in different chemical environments using hyperpolarized Xe-129 as a reporter ligand. It was found that even in a diamagnetic system, detection of analyte concentrations can be achieved through large Larmor frequency jumps. This approach provides a way to measure exchange rates even in systems where direct measurements are challenging.

CHEMICAL SCIENCE (2021)

暂无数据