Slow Relaxation Research Articles

A magnetic Ni-based metal-organic framework with interesting transformation dynamics

Herein, a flexible system composed of two Ni(II)-based coordination compounds: a 3D framework of {[Ni(μ-3isoani)2]·DMF}n (1) formula and a 0D monomeric [Ni(3isoani)2(H2O)4] (2) complex (where 3isoani = 3-aminoisonicotinato and DMF = dimethylformamide) which show mutual solvent-induced reversible transformations into each other is reported. The system shows reversible 1 ↔ 2 transformations upon the exposure of one compound to the solvent present in the other, that is, the MOF (1) in water and the monomer (2) in DMF. The process is easily followed by the naked eye because it involves a colour change from green (1)-to-brownish green (2), making the process traceable as previously observed for the Co(II)-based system. Moreover, these compounds present very different magnetic properties since 1 shows field-induced single-molecule magnet (SMM) behaviour, which corresponds to one of the few Ni(II)-based compounds showing single-ion behaviour (being Ni(II) the unique spin carrier), whereas 2 behaves as a regular paramagnet, all of which is explained according to a careful study of the magnetic properties by means of experimental direct-current (dc) and alternating-current (ac) measurements. Obtained experimental results are well supported by active space self-consistent field (CASSCF) calculations that allow understanding the slow relaxation occurring in the Ni(II) ion.

Slow magnetic relaxation of a {MnIIINaI}n zig-zag chain based single ion magnet

The synthesis using organic Schiff base ligands H2valen, and organic sulfonate ligands Na(4-HBS) in conjunction with Mn(Ac)3⋅2H2O, produces a one-dimensional coordination polymer with the formula {[Mn(valen)Na(4-HBS)2]⋅2CH3OH}n(1) [H2valen=6,6′-((1E,1′E)-(ethane-1,2-diylbis(azaneylylidene))bis(methaneylylidene))bis(2-methoxyphenol); Na(4-HBS)= Sodium 4-hydroxybenzenesulfonate]. Single crystal X-ray diffraction analysis reveals that complex 1 consist of neutral chains with one [Mn(valen)Na]2+ and two 4-HBS−moieties, in which the Mn(III) adopts an elongated octahedral geometry and Na(I) adopts a distorted pentagonal pyramid geometry, respectively. Magnetic investigations indicate the important magnetic anisotropy in the six-coordinated Mn(III) with the zero-field splitting parameter D = -3.2 cm−1. AC measurements suggest that complex 1 displays characteristics of slow magnetic relaxation under a 2000 Oe DC field, indicative of single ion magnet (SIM) behaviour. The effective energy barriers and the pre-exponential factor for complex 1 are determined to be 10.5 cm−1, and 1.36 × 10−7 s, respectively. This research reports not only a rare Mn(III) SIM molecular complex but also provide a potential approach to construct SIM chains.

From a Dy2 single-molecule magnet (SMM) to a 1D triangle-based Dy(III) chain SMM utilizing formate ions as bridging units

The reaction of Dy(NO3)2·6H2O with a Schiff base ligand N1,N3-bis(5-chlorosalicyladehyde)diethylenetriamine (H2bcsdt) afforded a dinuclear DyIII complex [Dy2(bcsdt)2(NO3)2] (1). The addition of HCOOH to the reaction system from which 1 was prepared generated a coordination polymer with the formula {[Dy3(bcsdt)3(HCOOH)(HCOO)(CO3)]·EtOH}n (2). Single-crystal X-ray diffraction analysis revealed that complex 2 possesses a one-dimensional chain structure based on a {[Dy3(bcsdt)3(HCOOH)(HCOO)(CO3)]·EtOH} repeating unit. In this unit, the three DyIII ions are connected by three oxygen atoms of one CO32– ion and display a nearly perfect triangle topology. The magnetic properties of 1 and 2 were investigated. They both exhibited slow relaxation of magnetization, indicative of single molecule magnet (SMM) behavior.

Synthesis, structure, photoluminescence and magnetism of a series of cobalt‐lanthanide heterometallic complexes originated from 2,3‐dichlorobenzoate and 1,10‐phenanthroline

AbstractA series of 3d–4f heterometallic complexes, namely [Ln2Co2(2,3‐DCB)10(phen)2] [Ln=Nd (1), Sm (2), Eu (3), Gd (4), Tb (5), Dy (6), Er (7)], were obtained through the self‐assembly reactions of Ln(NO3)3 ⋅ nH2O, Co(NO3)2 ⋅ 6H2O, 2,3‐dichlorobenzoic acid (2,3‐HDCB), NaOH and 1,10‐phenanthroline (phen) under solvothermal conditions. Their crystal structures were determined by single‐crystal X‐ray diffraction. They were also characterized by elemental analysis, FT‐IR, powder X‐ray diffraction (PXRD) and thermogravimetric analysis (TGA) and differential thermoanalysis (DTA). These seven complexes have the same molecular formula but different crystal structures. Complexes 1–3, 4 and 5 as well as 6 and 7 are crystallographically isomorphous, respectively. They all exhibit zero‐dimensional (0D) linear tetranuclear cluster structures. These 0D linear tetranuclear clusters can be further connected into a two‐dimensional (2D) supramolecular network via the extensive intermolecular π–π interactions between 2,3‐DCB and phen. The photoluminescent properties of 3, 5 and 6 and the magnetic properties of 1–2 and 4–7 were investigated. Complex 6 shows a slow magnetic relaxation behavior.

Measuring the Contractile Kinetics of Isolated Myofibrils from Human-Induced Pluripotent Stem Cell Derived Cardiomyocyte (hiPSC-CM) Models of Cardiomyopathy.

Isolated myofibrils provide biomechanical data at the contractile organelle level that are independent of cellular calcium handling and signaling pathways. These myofibrils can be harvested from animal tissue, human muscle biopsies, or stem cell-derived striated muscle. Here we present our myofibril isolation and rapid solution switching protocols, which allow for precise measurements of activation (kinetics and tension generation) and a biphasic relaxation relationship (initial slow isometric relaxation followed by a fast exponential decay in tension). This experiment is generated on a custom-built myofibril apparatus utilizing a two-photodiode array to detect micron level deflection of our forged glass tip force transducers. A complete activation/relaxation curve can be produced from a single myofibril in under 30minutes.

Crystallization in blend of polycaprolactone and high molecular weight polyethylene oxide

The concentration distribution in blend of polyethylene oxide (PEO)/polycaprolactone (PCL) and subsequent crystallization were investigated with differential scanning calorimetry, in-situ small angle X-ray scattering and wide angle X-ray scattering. By using PEOs with a molecular weight of 1 × 106 g/mol (PEO1M) and 1 × 105 g/mol (PEO100k), respectively, it is revealed that in initial blend the concentration of PEO1M in PEO-rich region is higher than that determined by miscibility. This non-equilibrium distribution induced by crystallization is maintained after melting, since slow relaxation of PEO1M hinders the redistribution process. Crystallization behavior of blend with 25 % of PEO1M at different melting temperatures was further investigated. The crystallinity shows no dependence on melting temperature, while the long period of PEO1M decreases continuously when melting temperature exceeds 140 °C. This decrease indicates more PCL chains diffuse into PEO-rich regions with increasing temperature and molten PCL chains reduce the entanglement number of PEO1M as solvent. Moreover, the periodicity of PEO1M lamellae becomes worse when crystallization proceeds faster, which is related to slower exclusion of PCL chains.

Two Pairs of Homochiral Parallelogram-like Dy4 Cluster Complexes with Strong Magneto-Optical Properties.

Two pairs of homochiral Dy(III) tetranuclear cluster complexes derived from (+)/(-)-3-trifluoroacetyl camphor (D-Htfc/L-Htfc), [Dy4(OH)2(L1)4(D-tfc)2(DMF)2]·4DMF (D-1) [H2L1 = (E)-2-(2-hydroxy-3-methoxybenzylideneamino)phenol)]/[Dy4(OH)2(L1)4(L-tfc)2(DMF)2]·4DMF (L-1) and [Dy4(OH)2(L2)4(D-tfc)2(DMF)2]·2H2O·3MeCN (D-2) [H2L2 = (E)-3-(2-hydroxy-3-methoxybenzylideneamino)naphthalen-2-ol]/[Dy4(OH)2(L2)4(L-tfc)2(DMF)2]·2H2O·3MeCN (L-2), were synthesized at room temperature, which have a Dy4 parallelogram-like core. The magnetic studies revealed that D-1 exhibits single-molecule magnet (SMM) behavior under zero dc magnetic field, and its magnetic relaxation has a distinct Raman process in addition to the Orbach process, with the Ueff/k value of 57.5 K and the C value of 28.27 s-1K-2.14; while D-2 displays dual magnetic relaxation behavior at 0 Oe field, with the Ueff/k value 114.8 K for the slow relaxation process (SR) and the C value of 10.656 s-1K-5.80 for the fast relaxation process (FR), respectively. Theoretical calculations indicated that the conjugated groups (phenyl vs naphthyl) of the Schiff base bridging ligands (H2L1 and H2L2) significantly affect the intramolecular magnetic interactions between the Dy3+ ions and ultimately lead to different relaxations. Furthermore, magnetic circular dichroism (MCD) measurements showed that these two pairs of Dy4 enantiomers exhibit strong room temperature magneto-optical Faraday effects; notably, increasing the conjugated group on the Schiff base bridging ligand is beneficial to enhancing the magneto-optical Faraday effects.

Magnetic Relaxations of Chromium Nitride Porphyrinato Complexes Driven by the Anisotropic g-Factor.

Molecule-based magnetic materials are useful candidates as the spin qubit due to their long coherence time and high designability. The anisotropy of the g-values of the metal complexes can be utilized to access the individual spin of the metal complexes, making it possible to achieve the scalable molecular spin qubit. For this goal, it is important to evaluate the effect of g-value anisotropy on the magnetic relaxation behaviour. This study reports the slow magnetic relaxation behaviour of chromium nitride (CrN2+ ) porphyrinato complex (1), which is structurally and magnetically similar with the vanadyl (VO2+ ) porphyrinato complex (2) which is known as the excellent spin qubit. Detailed analyses for vibrational and dynamical magnetism of 1 and 2 revealed that g-value anisotropy accelerates magnetic relaxations greater than the internal magnetic field from nuclear spin does. These results provide a design criterion for construction of multiple spin qubit based on g-tensor engineering.

Probing the strongly correlated magnetic state of Co2C nanoparticles at low temperatures using μSR

Co2C nanoparticles (NPs) are amongst transition metal carbides whose magnetic properties have not been well explored. An earlier study (Roy et al 2021 J. Phys.: Condens. Matter 33 375804) showed that a pellet made from Co2C NPs exhibits exchange bias (EB) effect below a temperature, T EB = 50 K and a spin glass (SG) feature emerges below T SG = 5 K. In the current study we use magnetic, electrical transport, specific heat, and muon spin rotation (μSR) measurements to explore further the magnetic properties of a pellet made with 40 nm diameter pure Co2C NPs. We uncover the onset of Kondo localization at Kondo temperature T K (= 40.1 K), which is close to the onset temperature (T EB) of the EB effect. A crossover from the Kondo-screened scenario to the Ruderman–Kittel–Kasuya–Yosida interaction-dominated regime is also observed for T < T K. Temperature-dependent specific heat measurement further supports the Kondo localization scenario in the pellet and shows the heavy fermionic nature of the strongly correlated electronic state in Co2C. The zero field μSR asymmetry spectra in the low-temperature regime are characterized by two distinct fast and slow relaxation rates. The spectra show the absence of long-range magnetic order in the sample. However, our analysis suggests the NPs-pellet shows the presence of a dominant magnetically disordered fraction and a smaller fraction with short-range order. Muons in the disordered fraction exhibit a slower relaxation rate, while muons in the smaller fraction with short-range order exhibit a faster relaxation rate. We observe an increase in this fast relaxation rate between T EB and T SG. This increase below T EB ∼ 50 K suggests a slowing down of the fluctuating local magnetic environment around muons. Transverse field-μSR asymmetry spectra show the emergence of a stable, multi-peaked local magnetic field distribution in the pellet below T EB. Longitudinal field μSR spectra shows distinct changes in the dynamics of fluctuations suggesting the presence of a frozen glassy like state below 6 K. Based on our results, we suggest that below T EB, the pellet of Co2C NPs develops a magnetic interface that separates the two magnetic fractions; one is a disordered fraction, and the other is a fraction with short-range order. The exchange interaction that sets in below T EB at the interface couples the two fractions, leading to a suppression of the fluctuations. With the suppression of magnetic fluctuations below T EB, strong correlation effects in the electronic state of Co2C lead to Kondo localization.

Honey-like Odor Meets Single-Ion Magnet: Synthesis, Crystal Structure, and Magnetism of Cobalt(II) Complex with Aromatic Trans-Cinnamic Acid

The hexacoordinate Co(II) complex [Co(neo)2(cin)][BPh4]·½Me2CO (1·½Me2CO) containing trans-cinnamic acid (Hcin) and neocuproine (neo) was prepared. The compound 1·½Me2CO was characterized via single-crystal X-ray analysis, FT-IR spectroscopy, and magnetic measurements. The coordination polyhedron of the complex cation adopts a deformed octahedron shape, and cinnamate exhibits a bidentate mode of coordination, which is unusual for mononuclear Co(II) cinnamate complexes. The analysis of DC magnetic measurements with zero-field splitting (ZFS) spin Hamiltonian revealed large magnetic anisotropy defined by the axial ZFS parameter D = +53.2 cm−1. AC susceptibility measurements revealed the slow relaxation of magnetization under the applied field; thus, 1·½Me2CO behaves as a field-induced single-molecule magnet. The analysis of magnetic properties was also supported by CASSCF/NEVPT2 calculations.

Understanding heterogeneous mechanisms of heart failure with preserved ejection fraction through cardiorenal mathematical modeling.

In contrast to heart failure (HF) with reduced ejection fraction (HFrEF), effective interventions for HF with preserved ejection fraction (HFpEF) have proven elusive, in part because it is a heterogeneous syndrome with incompletely understood pathophysiology. This study utilized mathematical modeling to evaluate mechanisms distinguishing HFpEF and HFrEF. HF was defined as a state of chronically elevated left ventricle end diastolic pressure (LVEDP > 20mmHg). First, using a previously developed cardiorenal model, sensitivities of LVEDP to potential contributing mechanisms of HFpEF, including increased myocardial, arterial, or venous stiffness, slowed ventricular relaxation, reduced LV contractility, hypertension, or reduced venous capacitance, were evaluated. Elevated LV stiffness was identified as the most sensitive factor. Large LV stiffness increases alone, or milder increases combined with either decreased LV contractility, increased arterial stiffness, or hypertension, could increase LVEDP into the HF range without reducing EF. We then evaluated effects of these mechanisms on mechanical signals of cardiac outward remodeling, and tested the ability to maintain stable EF (as opposed to progressive EF decline) under two remodeling assumptions: LV passive stress-driven vs. strain-driven remodeling. While elevated LV stiffness increased LVEDP and LV wall stress, it mitigated wall strain rise for a given LVEDP. This suggests that if LV strain drives outward remodeling, a stiffer myocardium will experience less strain and less outward dilatation when additional factors such as impaired contractility, hypertension, or arterial stiffening exacerbate LVEDP, allowing EF to remain normal even at high filling pressures. Thus, HFpEF heterogeneity may result from a range of different pathologic mechanisms occurring in an already stiffened myocardium. Together, these simulations further support LV stiffening as a critical mechanism contributing to elevated cardiac filling pressures; support LV passive strain as the outward dilatation signal; offer an explanation for HFpEF heterogeneity; and provide a mechanistic explanation distinguishing between HFpEF and HFrEF.

Slow Magnetic Relaxation in Silver(II) Macrocyclic Systems.

The spin-lattice relaxation time has been studied trough alternating-current susceptometry and ultralow-frequency Raman spectroscopy in a family of silver(II)-derived molecular systems with spin 1/2 and formulas [AgII(m-CTH)(NO3)2] (1) and [AgII(m-CTH)(ClO4)2] (2), where CTH = meso-5,5,7,12,12,14-hexamethyl-1,4,8,11-tetraazacyclotetradecane. The combination of both techniques demonstrates the occurrence of slow spin magnetic relaxation induced by spin-phonon interaction. The magnetic behavior of these silver(II)-derived systems opens the door to a new cation in the scarce family of S = 1/2 systems with slow relaxation of magnetization.

Nd─Nd Bond in Ih and D5h Cage Isomers of Nd2 @C80 Stabilized by Electrophilic CF3 Addition.

Synthesis of molecular compounds with metal-metal bonds between 4f elements is recognized as one of the fascinating milestones in lanthanide metallochemistry. The main focus of such studies is on heavy lanthanides due to the interest in their magnetism, while bonding between light lanthanides remains unexplored. In this work, the Nd─Nd bonding in Nd-dimetallofullerenes as a case study of metal-metal bonding between early lanthanides is demonstrated. Combined experimental and computational study proves that pristine Nd2 @C80 has an open shell structure with a single electron occupying the Nd─Nd bonding orbital. Nd2 @C80 is stabilized by a one-electron reduction and further by the electrophilic CF3 addition to [Nd2 @C80 ]- . Single-crystal X-ray diffraction reveals the formation of two Nd2 @C80 (CF3 ) isomers with D5h -C80 and Ih -C80 carbon cages, both featuring a single-electron Nd─Nd bond with the length of 3.78-3.79 Å. The mutual influence of the exohedral CF3 group and endohedral metal dimer in determining the molecular structure of the adducts is analyzed. Unlike Tb or Dy analogs, which are strong single-molecule magnets with high blocking temperature of magnetization, the slow relaxation of magnetization in Nd2 @Ih -C80 (CF3 ) is detectable via out-of-phase magnetic susceptibility only below 3 K and in the presence of magnetic field.

Abstract 18327: Influence of Microtubule Detyrosination on Left Atrial Myopathy in a Rat Model of Heart Failure With Preserved Ejection Fraction

Introduction: Heart failure with preserved ejection fraction (HFpEF) is characterized in part by increased left ventricular (LV) stiffness and left atrial (LA) remodeling. LA myopathy in HFpEF is associated with poor clinical outcomes. In the LV, the magnitude of post-translational detyrosination of α-tubulin, regulated by vasohibins (VASH1/2), contributes to LV stiffness. However, the role of tubulin detyrosination in the LA is currently unknown. To this end, we assessed the extent of LA myopathy in the ZSF rat model of HFpEF, and assessed the effect of acute VASH inhibition on LA remodeling. Methods: ZSF obese rats with diastolic dysfunction were compared alongside ZSF lean hypertensive-only rats and Wistar Kyoto rats (WKY). Rats were aged to 30 weeks, then received a tail vein injection of VASH inhibitor or vehicle, followed by echocardiography. Following a second injection, hearts were excised, and LA and LV were separated for downstream protein analysis. Results : ZSF obese rats develop hallmark features of HFpEF including preserved systolic function, left ventricular hypertrophy, and slowed relaxation compared to lean and WKY. ZSF obese animals demonstrated significant LA myopathy, including increased LA area, reduced LA emptying fraction, and reduced LA strain. Acute VASH inhibition led to trends towards normalization of LA kinetics. There were no significant differences in levels of detyrosinated tubulin between vehicle and VASH inhibition groups in the LA, though there was a significant reduction of detyrosinated tubulin in the LV by Western Blot (detyrosinated tubulin / GAPDH relative quantity Vehicle: 1.5±0.2 vs. VASH inhibitor 0.5±0.1; p&lt;0.05). Conclusions: Acute VASH inhibition improves LA kinetics in ZSF obese rats secondary to reductions in detyrosinated tubulin in the LV. Future studies employing sustained reductions of detyrosinated tubulin may lead to better understanding of LA-LV interactions in the pathogenesis of LA myopathy in HFpEF.

Hair relaxation after shaping - A kinetic approach.

Hair fibres have been shaped via either a thermal route or via a chemical route. The time-relaxation transients of the shaped hairs in air, and in water, respectively, were evaluated. The collected data were kinetically modelled in order to reveal information about the rate controlling mechanism of the recovery process. Hair fibres were thermally shaped at different temperatures between heated plates and left to relax in an environment of controlled humidity and temperature. Different hair fibres were chemically shaped and left to relax in water of different controlled temperatures. Relaxation data were used for modelling the kinetics of the recovery processes by using exponential and logarithmic kinetic laws. The fitting of the models to the two sets of data has been checked by using the residual sum of squares for matching the proper model to each set of data. The processes of shaping and recovery were assimilated with a sequence of two successive quasi-chemical reactions, occurring at the used temperatures. Based on chemical and physical assumptions, the two groups of experiments were modelled by two different laws: an exponential law, suggesting a first-order process as the rate-determining step of the relaxation of thermally shaped fibres, and a logarithmic law, suggesting a slow relaxation, based on percolation theory, for the chemically shaped fibres. This allowed use of chemical kinetics tools for calculating the values of the activation energy in each case. The evaluated values of activation energy of the relaxation processes for both thermal and chemical shaping were found to be close to each other, in spite of the different methods of shaping. The kinetic analysis suggests that despite different reaction sequences occurring during the different shaping-relaxation processes, the rate-controlling mechanism that manages the recovery process is the same in all cases; and this process is proposed to be the thiol-disulphide reformation of intra-protein bonds inside hair.

Formation of a single-ion magnet in the lanthanum calcium silicate apatite structure by the cobalt oxide doping

A small amount of cobalt was incorporated into the lanthanum calcium silicate apatite structure by annealing at 1500 °C in argon. The compound exhibits easy-axis magnetic anisotropy with a zero-field splitting parameter 2D of −60 cm−1 and field- induced slow relaxation of magnetization with a remagnetization energy barrier of 58–63 cm−1. Thereby, for the first time, a cobalt-based single-ion magnet was created in silicate.

The Effect of Slow Deep Breathing and Progressive Muscle Relaxation on Blood Pressure in Hypertensive Patients in Kedaung Wetan Health Center Tangerang

Slow and deep breathing and progressive muscle relaxation are non-pharmacological therapies that are easy to do. This therapy can make the body more relaxed so that it can lower blood pressure. This study aims to determine the effectiveness of slow deep breathing therapy and progressive muscle relaxation in reducing blood pressure in hypertensive patients. This research uses a quasi-experimental design with a one-group research design using a pre-test and post-test approach without a control group. Respondents in this study consisted of 16 hypertensive patients selected by purposive sampling, with one intervention group. The intervention was carried out by the respondent, who performed slow and deep breathing techniques and progressive muscle relaxation through the media provided. The results showed a significant difference in blood pressure before and after instruction in deep breathing techniques and progressive muscle relaxation, using the paired t-test. The results of the analysis using the t-test showed that there was a significant influence between slow deep breathing techniques and progressive muscle relaxation on blood pressure in hypertensive patients (p-value &lt; 0.05). Therefore, it is hoped that nurses can optimize slow and deep breathing techniques and progressive muscle relaxation as non-pharmacological therapies for managing patient hypertension.

Magneto-Chiral Dichroism in a One-Dimensional Assembly of Helical Dysprosium(III) Single-Molecule Magnets.

Here we report magneto-chiral dichroism (MChD) detected through visible and near-infrared light absorption of a chiral dysprosium(III) coordination polymer. The two enantiomers of [DyIII(H6(py)2)(hfac)3]n [H6(py)2 = 2,15-bis(4-pyridyl)ethynylcarbo[6]helicene; hfac- = 1,1,1,5,5,5-hexafluoroacetylacetonate], where the chirality is provided by a functionalized helicene ligand, were structurally, spectroscopically, and magnetically investigated. Magnetic measurements reveal a slow relaxation of the magnetization, with differences between enantiopure and racemic systems rationalized on the basis of theoretical calculations. When the enantiopure complexes are irradiated with unpolarized light in a magnetic field, they exhibit multiple MChD signals associated with the f-f electronic transitions of DyIII, thus providing the coexistence of MChD-active absorptions and single-molecule-magnet (SMM) behavior. These findings clearly show the potential that rationally designed chiral SMMs have in enabling the optical readout of magnetic memory through MChD.

Identification of Favorable Silica Surface Sites for Single‐Molecule Magnets

AbstractIndustrial data storage application based on single‐molecule magnets (SMMs) necessitates not only strong magnetic remanence at high temperatures but also requires the implementation of SMMs into a solid material to increase their durability and addressability. While the understanding of the relationship between the local structure of the metal and the resulting magnetic behavior is well understood in molecular systems, it remains challenging to establish a similar understanding for magnetic materials, especially for isolated lanthanide sites on surfaces. For instance, dispersed Dy(III) ions on silica prepared via surface organometallic chemistry exhibit slow magnetic relaxation at low temperatures, but the origin of these properties remains unclear. In this work, we modelled ten neutral complexes with coordination numbers (CN) between three and six ([Dy(OSiF3)3(O(SiF3)2)CN‐3]) representing possible surface sites for dispersed Dy(III) ions and investigated their SMM potential via ab initio CASSCF/RASSI‐SO calculations. Detailed analysis of the data shows the strong influence of the spatial position of the anionic ligands while the neutral ligands only play a minor role for the magnetic properties. In particular, a T‐shape like orientation of the anionic ligands is predicted to exhibit good SMM properties making it a promising targeted coordination environment for molecular and surface‐based SMMs.

Spin Qubit in a 2D GdIII NaI -Based Oxamato Supramolecular Coordination Framework.

Qubits are the basic unit of quantum information and computation. To realize quantum computing and information processing, the decoherence times of qubits must be long enough. Among the studies of molecule-based electron spin qubits, most of the work focused on the ions with the spin S=1/2, where only single-bit gates can be constructed. However, quantum operations require the qubits to interact with each other, so people gradually carry out relevant research in ions or systems with S>1/2 and multilevel states. In this work, a two-dimensional (2D) oxygen-coordinated GdIII NaI -based oxamato supramolecular coordination framework, Na[Gd(4-HOpa)4 (H2 O)] ⋅ 2H2 O (1, 4-HOpa=N-4-hydroxyphenyloxamate), was selected as a possible carrier of qubit. The field-induced slow magnetic relaxation shows this system has phonon bottleneck (PB) effect at low temperatures with a very weak magnetic anisotropy. The pulse electron paramagnetic resonance studies show the spin-lattice and spin-spin relaxation times are T1 =1.66 ms at 4 K and Tm =4.25 μs at 8 K for its diamagnetically diluted sample (1Gd0.12 %). It suggested that the relatively long decoherence time is mainly ascribed to its near isotropic and the PB effect from resonance phonon trapped for pure sample, while the dilution further improves its qubit performance.