Review
Quantum Science & Technology
Xiangyu Wang, Zidong Lin, Liangyu Che, Hanyu Chen, Dawei Lu
Summary: Machine learning has become a powerful tool with the advancement of computing power and algorithms, leading to the rapidly growing field of quantum-enhanced machine learning. The development of experimental quantum technologies has enabled many experimental demonstrations of quantum-enhanced machine learning in diverse physical systems.
ADVANCED QUANTUM TECHNOLOGIES
(2022)
Article
Physics, Multidisciplinary
Wentian Zheng, Ke Bian, Xiakun Chen, Yang Shen, Shichen Zhang, Rainer Stohr, Andrej Denisenko, Jorg Wrachtrup, Sen Yang, Ying Jiang
Summary: An efficient method was developed to engineer the electrostatic environment of near-surface nitrogen vacancy center qubits, increasing their coherence and sensitivity.
Article
Chemistry, Physical
James W. Whipham, Gamal A. I. Moustafa, Mohamed Sabba, Weidong Gong, Christian Bengs, Malcolm H. Levitt
Summary: In this study, the NMR spectra of spin-1/2 pairs in the near-equivalence regime were observed to have four peaks, with the two inner peaks stronger than the outer peaks. The strong inner peaks were found to have significantly different linewidths, potentially due to strong cross-correlation effects. The developed theory of cross-correlated relaxation in the case of near-equivalent homonuclear spin-1/2 pairs with strongly anisotropic rotational diffusion showed good agreement with experimental NMR lineshapes.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Multidisciplinary Sciences
Leonardo S. Lima
Summary: Transport in non-Hermitian quantum systems is investigated, specifically focusing on the Lieb lattice and the integrable Ising chain. The study aims to understand the influence of non-Hermitian parameters on spin conductivity and transport coefficients. The results show that the non-Hermitian parameters have minimal impact on conductivity in both the Ising model and noninteracting fermion models, with the opening of a gap in the spectrum also affecting longitudinal conductivity.
SCIENTIFIC REPORTS
(2023)
Article
Quantum Science & Technology
Paul C. Jerger, Yu-Xin Wang, Mykyta Onizhuk, Benjamin S. Soloway, Michael T. Solomon, Christopher Egerstrom, F. Joseph Heremans, Giulia Galli, Aashish A. Clerk, David D. Awschalom
Summary: Single-qubit sensing protocols can measure qubit-bath coupling parameters. However, the sensing protocol itself can perturb the bath, causing a quantum quench effect. This study observed the bath perturbation in a nitrogen-vacancy (NV) center by measuring the phase-resolved spin-echo of the nuclear spin bath. The relationship between the sensor phase and the Gaussian spin-bath polarization was derived to optimize the transfer efficiency of the dynamic nuclear polarization sequence.
Article
Chemistry, Physical
Matias Chavez, Matthias Ernst
Summary: We propose a framework that utilizes a continuous frequency space to describe and design solid-state nuclear magnetic resonance (NMR) experiments. This approach allows reverse engineering of experiments and is based on perturbation theory in a continuous Fourier space, resulting in time-independent effective Hamiltonians. The pulse scheme can be back-calculated from the desired effective Hamiltonian as a function of spin-system parameters. An example is provided to demonstrate how to back-calculate the rf irradiation in the MIRROR experiment from the desired chemical-shift offset behavior of the sequence.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Erik Rosendahl Kjellgren, Hans Jorgen Aagaard Jensen
Summary: The multi-configurational short-range (sr) density functional theory has been extended to calculate indirect spin-spin coupling constants (SSCCs) for nuclear magnetic resonance spectroscopy. The performance of the new method is compared to other density functional theories, showing that computationally cost-effective srLDA functionals are preferable. In organic compounds, HF-srDFT is the best choice for calculating SSCCs, while CAS-srDFT is needed for fluorine-metals SSCCs.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Laura A. Voelker, Konstantin Herb, Erika Janitz, Christian L. Degen, John M. Abendroth
Summary: In this study, a quantum sensing scheme is introduced to directly measure the hypothesized spin polarization in radical pairs using shallow nitrogen-vacancy (NV) centers in diamond. This method provides fresh insights into spin selectivity in electron transfer reactions.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
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.
Article
Physics, Multidisciplinary
Martin Koppenhoefer, Carl Padgett, Jeffrey Cady, Viraj Dharod, Hyunseok Oh, Ania C. Bleszynski Jayich, A. A. Clerk
Summary: Solid-state spin defects can be used as quantum sensors for various sensing targets, with some defects coupling to strain in the host material. This strain coupling can be utilized for mechanically mediated dispersive single-shot spin readout using optomechanically induced transparency measurement. Surprisingly, the estimated measurement times for negatively charged silicon-vacancy defects in diamond are much shorter than those for single-shot optical fluorescence readout. This scheme can also be applied for general parameter-estimation metrology and offers higher sensitivity than conventional schemes using continuous position detection.
PHYSICAL REVIEW LETTERS
(2023)
Article
Optics
Jacob R. Lindale, Shannon L. Eriksson, Warren S. Warren
Summary: The theoretical description of the interplay between coherent evolution and chemical exchange, which was originally developed for magnetic resonance and later applied to other spectroscopic regimes, was derived under incorrect statistical assumptions. Correcting these assumptions allows access to the exact form of the chemical exchange interaction, derived within the Lindblad master equation formalism for generality. The exact form of the interaction differs from the traditional equation only by a scalar correction factor derived from higher-order interactions, and it regularly improves the convergence radius of the solution (thus increasing the allowable step size in calculations) by up to an order of magnitude, without any additional computational cost.
Article
Engineering, Electrical & Electronic
Daniel Krueger, Aoyang Zhang, Behdad Aghelnejad, Henry Hinton, Victor Marrugat Arnal, Yi-Qiao Song, Yiqiao Tang, Ka-Meng Lei, Jens Anders, Donhee Ham
Summary: Nuclear magnetic resonance (NMR) is an important analytical tool in various fields, and efforts have been made to miniaturize NMR systems using permanent magnets and CMOS RF-integrated circuits. This study presents a small NMR system, which combines a digitally assisted CMOS RF transceiver IC and a 0.51-T permanent magnet, achieving high spectral resolution and imaging resolution.
IEEE JOURNAL OF SOLID-STATE CIRCUITS
(2023)
Review
Chemistry, Multidisciplinary
Florence Franconi, Laurent Lemaire, Jean-Christophe Gimel, Samuel Bonnet, Patrick Saulnier
Summary: NMR-based diffusion methods are valuable tools for nanomedicine characterization and understanding interactions with the biological environment. They provide insights into diffusion phenomena and measurement of self-diffusion and mutual diffusion coefficients. NMR diffusometry spectroscopic and imaging methods have broad applications in nanomedicine, aiding in elucidating important issues.
JOURNAL OF CONTROLLED RELEASE
(2021)
Article
Physics, Multidisciplinary
T. G. H. Blank, K. A. Grishunin, B. A. Ivanov, E. A. Mashkovich, D. Afanasiev, A. V. Kimel
Summary: This study demonstrates a new approach to control antiferromagnetism by utilizing the magnetization emerging from a state of coherent spin precession in antiferromagnetic iron borate FeBO3, enabling the nonlinear coupling of light to another mode of spin precession.
PHYSICAL REVIEW LETTERS
(2023)
Article
Physics, Multidisciplinary
Fahimeh Naghdi, Mohammad Ali Jafarizadeh, Mohammad Reza Bazrafkan
Summary: In this letter, we investigate the problem of time-optimal control for a system of quadrupole nucleus with spin I = 1 under nuclear magnetic resonance conditions with unbounded control using Pontryagin's minimum principle. For spin I = 1, we calculate the minimal duration for steering the system from any given initial pure state to any final pure state, and derive an explicit analytical formula for the minimum duration.
Article
Chemistry, Multidisciplinary
Aditya Mishra, Michael A. Hope, Masaud Almalki, Lukas Pfeifer, Shaik Mohammed Zakeeruddin, Michael Graetzel, Lyndon Emsley
Summary: By studying layered hybrid perovskite analogues, we identified the factors that limit the efficiency of DNP NMR for perovskite samples. We found that the fast-relaxing dynamic cation is the major impediment, but this can be mitigated by deuteration, leading to significant DNP enhancement.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Manuel Cordova, Pinelopi Moutzouri, Bruno Simoes de Almeida, Daria Torodii, Lyndon Emsley
Summary: A deep learning approach is introduced to determine pure isotropic proton spectra from a two-dimensional set of magic-angle spinning spectra acquired at different spinning rates. The model is applied to 8 organic solids, yielding high-resolution H-1 solid-state NMR spectra with isotropic linewidths in the 50-400 Hz range.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Biao Li, Gwenaelle Rousse, Leiting Zhang, Maxim Avdeev, Michael Deschamps, Artem M. Abakumov, Jean-Marie Tarascon
Summary: The current exploration of high-energy-density cathode materials for Li-ion batteries is mainly focused on Li-rich or Ni-rich oxides, which both have practical challenges. This study combines these two concepts to obtain Li-rich Ni-rich oxides for more practical high-energy-density cathodes.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Pinelopi Moutzouri, Manuel Cordova, Bruno Simoes de Almeida, Daria Torodii, Lyndon Emsley
Summary: One key bottleneck of solid-state NMR spectroscopy is the broadness of H-1 NMR spectra of organic solids due to dipolar couplings. A new approach called PIP was suggested to address this problem by mapping errors leading to dipolar broadening and removing them in a correlation experiment. By extending the PIP approach to a second dimension using deep learning, high resolution H-1-H-1 double-quantum/single-quantum dipolar correlation and spin-diffusion spectra were obtained with significantly higher resolution than the corresponding spectra at 100 kHz MAS, allowing the identification of previously overlapped isotropic correlation peaks.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Ridvan Ince, Abdelatif Doudouh, Nicolas Claiser, Eric Furet, Thierry Guizouarn, Laurent Le Polle, Gwendal Kervern
Summary: Exploring magnetic properties at the molecular level is a challenge that has been met by developing many experimental and theoretical solutions. In order to complement the possibilities offered by these methods, a new tool combining simulation and fitting for high-resolution solid-state NMR spectra of lanthanide-based paramagnetic species is proposed. This method relies on a rigorous acquisition of high-resolution solid-state NMR isotropic and anisotropic data on a powdered magnetic material and an efficient modeling of this data based on a parametrization of the local magnetism and the crystal structure provided by diffraction methods.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Physical
Aditya Mishra, Michael A. Hope, Gabriele Stevanato, Dominik J. Kubicki, Lyndon Emsley
Summary: Researchers studied cesium lead chloride and found that metal-ion DNP provides the highest bulk sensitivity in this case, while highly surface-selective NMR spectra can be acquired using impregnation DNP. The performance of both methods is explained in terms of the relaxation times, particle size, dopant concentration, and surface wettability.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Florian Brette, Dani Kourati, Michael Paris, Lola Loupias, Stephane Celerier, Thierry Cabioc'h, Michael Deschamps, Florent Boucher, Vincent Mauchamp
Summary: The functionalization of MXenes, a class of 2D materials, can significantly modify their physicochemical properties. Through experiments and theoretical calculations, we found that the carbon NMR signal in MXenes is highly sensitive to functionalization, even though carbon atoms are not directly bonded to the surface groups. We developed a theoretical model to quantitatively relate the 13C NMR shift to different surface compositions and the number of surface chemistry variants induced by different etching agents.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Pierrick Berruyer, Cynthia Cibaka-Ndaya, Arthur Pinon, Clement Sanchez, Glenna L. Drisko, Lyndon Emsley
Summary: The physical properties of modern multi-component materials are determined by their internal microstructure, making tools for characterizing complex nanoscale architectures essential. This study introduces a method to obtain radial images of the internal structure of multi-component particles from NMR measurements, demonstrating its accuracy in imaging core-shell structures with nanometer resolution.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Damien Degoulange, Raj Pandya, Michael Deschamps, Dhyllan A. Skiba, Betar M. Gallant, Sylvain Gigan, Hilton B. de Aguiar, Alexis Grimaud
Summary: High-resolution Raman imaging is used to investigate the interface of salt-salt aqueous biphasic systems (ABSs) at a molecular level, revealing a gradual change of environment instead of a sharp molecular interface. This knowledge is of great importance in understanding aqueous interfaces and has significant implications in various biological and technological settings, including novel battery technologies.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2023)
Article
Chemistry, Physical
Kunal Datta, Alessandro Caiazzo, Michael A. Hope, Junyu Li, Aditya Mishra, Manuel Cordova, Zehua Chen, Lyndon Emsley, Martijn M. Wienk, Rene A. J. Janssen
Summary: Photoinduced halide segregation limits the widespread application of three-dimensional mixed-halide perovskites. In this study, we investigate the phenomenon of photoinduced halide segregation in lower-dimensional mixed iodide-bromide perovskites. We find that layered two-dimensional structures exhibit additional stability against halide demixing due to reduced halide mobility, which is supported by solid-state NMR analysis.
ACS ENERGY LETTERS
(2023)
Article
Biochemical Research Methods
Bruno Simoes de Almeida, Daria Torodii, Pinelopi Moutzouri, Lyndon Emsley
Summary: The role of 1H solid-state NMR in structure elucidation of solids is becoming more important, especially with the availability of faster magic-angle spinning rates (MAS) which improve 1H detected assignment strategies. However, the current 1H spectral resolution is still relatively low. This study investigates the factors limiting proton linewidths and line shapes in MAS experiments with five different samples and identifies the different contributions through one-and two-dimensional experiments.
JOURNAL OF MAGNETIC RESONANCE
(2023)
Article
Biochemical Research Methods
Michael A. Hope, Yuxuan Zhang, Amrit Venkatesh, Lyndon Emsley
Summary: Dynamic nuclear polarisation (DNP) using high-spin metal ions, such as Gd3+, can enhance nuclear magnetic resonance (NMR) sensitivity. Spin diffusion and metal site symmetry are factors affecting DNP efficiency. In this study, cubic In(OH)3 was investigated as a high-symmetry proton-containing material for DNP using endogenous Gd3+. A 1H enhancement of up to 9 was achieved, and the clustering of Gd3+ dopants and the local reduction in symmetry of the metal site induced by proton disorder were identified as the reasons for the enhancement. This is the first example of 1H DNP using Gd3+ dopants in an inorganic solid.
JOURNAL OF MAGNETIC RESONANCE
(2023)
Article
Chemistry, Physical
Zlanseu Ruth Tan, Cecile Pagnoux, Vincent Sarou-Kanian, Michae''l Deschamps
Summary: The adsorption of small ions on the surface of inorganic material has been extensively studied using nuclear magnetic resonance relaxation enhancements. In this study, the adsorption of various ions onto TiO2 was investigated using NMR analysis and relaxation curve analysis. The results showed that NH4+ ions preferred to adsorb onto TiO2, as evidenced by the broadening of the N-14 peak and higher longitudinal relaxation rates. The adsorption properties of alkali ions were also compared, with Cs+ showing the highest surface affinity, followed by Rb+, Na+, and Li+.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Manuel Cordova, Lyndon Emsley
Summary: The determination of the molecular solid structure using NMR crystallography relies on generating a comprehensive set of candidate crystal structures and comparing computed chemical shifts with experimental values. However, exploring the polymorph landscape of molecular solids requires a significant computational power, leading to a bottleneck in candidate crystal generation. This study constructs three-dimensional interaction maps using a crystal structure database with associated chemical shifts to identify structural constraints for accelerating crystal structure prediction protocols, without requiring DFT-level chemical shift computations.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Medicine, Research & Experimental
Pierrick Berruyer, Maria Lindkvist, Sandra Gracin, Tatiana Starciuc, Andrea Bertarello, Baptiste Busi, Staffan Schantz, Lyndon Emsley
Summary: Protein-based drug formulations pose challenges in terms of stability and morphology. This study used DNP NMR spectroscopy to determine the hierarchy of components within spray-dried particles containing protein, trehalose, leucine, and trileucine. The findings provide insights for rationalizing the performance of these formulations.
MOLECULAR PHARMACEUTICS
(2023)