Article
Multidisciplinary Sciences
Linfei Li, Jeremy F. Schultz, Sayantan Mahapatra, Zhongyi Lu, Xu Zhang, Nan Jiang
Summary: By using ultrahigh vacuum tip-enhanced Raman spectroscopy (UHV-TERS), single oxygen adatoms on a boron monolayer (borophene) can be identified and mapped with a spatial resolution of approximately 4.8 angstrom and single bond sensitivity. This technique enables the atomically defined, chemically homogeneous, and thermally reversible oxidation of borophene via atomic oxygen in UHV. Additionally, it reveals the propensity of borophene towards molecular oxygen activation at room temperature and phase-dependent chemical properties. Overall, this work demonstrates the powerful utility of UHV-TERS in probing the local chemistry of surface adsorbates in the atomic regime and has important applications in heterogeneous catalysis, on-surface molecular engineering, and low-dimensional materials.
NATURE COMMUNICATIONS
(2022)
Review
Chemistry, Multidisciplinary
Chen Wang, Yin-Shan Meng, Shang-Da Jiang, Bing-Wu Wang, Song Gao
Summary: Single-molecule magnets (SMMs) with slow magnetization relaxation and purely molecular hysteresis are promising for information storage, spintronics, and quantum computing. Improving the blocking temperature (T-B) and effective relaxation barrier (U-eff) is crucial for their application. Multidisciplinary research has achieved SMMs with a U-eff up to 2,000 K and a T-B in the liquid nitrogen region. Enhancing the uniaxiality of magnetic anisotropy is critical for high-performance SMMs.
SCIENCE CHINA-CHEMISTRY
(2023)
Review
Chemistry, Multidisciplinary
Vijay S. Parmar, David P. Mills, Richard E. P. Winpenny
Summary: Recent studies have shown that mononuclear lanthanide (Ln) complexes can be high-performing single-molecule magnets (SMMs). The focus is on mononuclear Dy-III alkoxide and aryloxide SMMs with coordination numbers up to eight, covering synthesis, solid-state structures and magnetic attributes. Brief overviews are also provided of mononuclear Tb-III, Ho-III, Er-III and Yb-III alkoxide and aryloxide SMMs.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Yu-Xia Wang, Yinina Ma, Jie-Su Wang, Yue Yang, Yun-Nan Guo, Yi-Quan Zhang, Kui-Juan Jin, Young Sun, Peng Cheng
Summary: A new material, ferroelectric single-molecule magnets (FE SMMs), which exhibit single-molecule magnetic behaviors, toroidal magnetic moments, and room-temperature ferroelectricity, has been reported. The presence of toroidal moments and ferroelectricity, along with quantum magnetism, in these rare-earth single-molecule magnets, leads to a unique class of multiferroics.
Review
Chemistry, Inorganic & Nuclear
Zeng-Xi Yang, Feng Gong, Dunmin Lin, Yu Huo
Summary: Single-molecule magnets (SMMs) are attracting attention for their potential applications in high-density information storage and spintronic devices. Organic ligands and inorganic polyoxometalates (POMs) have been used to achieve high-performance SMMs. POMs offer advantages such as excluding dipole-dipole coupling and providing rigid frameworks for surface deposition and device applications. This review systematically summarizes the research progress and design strategies for POM-based SMMs, as well as the multifunctional properties for future application devices.
COORDINATION CHEMISTRY REVIEWS
(2023)
Article
Chemistry, Inorganic & Nuclear
Lidia Rosado Piquer, Jan Dreiser, E. Carolina Sanudo
Summary: The study deposited Heterometallic SMM onto iron oxide nanoparticles with an oleate SAM to separate the molecule from the magnetic substrate, ensuring the retention of the SMM's magnetic properties.
DALTON TRANSACTIONS
(2021)
Article
Chemistry, Multidisciplinary
Biao Hu, Jing Xi, Peipei Cen, Yan Guo, Yi Ding, Yuanyuan Qin, Yi-Quan Zhang, Xiangyu Liu
Summary: In this study, a new mononuclear Dy(III) complex was synthesized via self-assembly, and its structure and magnetic behavior were investigated. The complex exhibited field-induced slow magnetic relaxation.
Article
Chemistry, Multidisciplinary
Qian-Cheng Luo, Ning Ge, Yuan-Qi Zhai, Tengbo Wang, Lin Sun, Qi Sun, Fanni Li, Zhendong Fu, Yan-Zhen Zheng
Summary: Two erbium(III) complexes, [ErCl(OArAd)3][Na(THF)6] (1) and Er(OArAd)3 (2), were prepared using a hard base ligand with large steric hindrance. The change in coordination geometry around the Er(III) site from distorted tetrahedral to flat trigonal pyramid geometry in different solvent environments enhanced the single-molecule magnet (SMM) behavior, with a field-induced effective energy barrier (Ueff) of 43(1) cm -1 for the latter. The study demonstrates the importance of a strong equatorial ligand field and high local symmetry in suppressing quantum tunneling of the magnetization (QTM) to achieve high-performance erbium(III)-based SMMs.
CHINESE CHEMICAL LETTERS
(2023)
Article
Chemistry, Multidisciplinary
James P. Durrant, Benjamin M. Day, Jinkui Tang, Akseli Mansikkamaki, Richard A. Layfield
Summary: Replacing the ligands in dysprosium single-molecule magnets with a different type leads to larger energy barriers to magnetization reversal. The distances between the ligands in the new complexes suggest a different crystal field splitting. Theoretical analysis shows that the magnetic axes in the ground Kramers doublets are oriented towards the new ligands. Introducing new parameters allows for comparisons between different single-molecule magnets, indicating the potential for improved performance in the new system.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Chia-Hsiang Chen, Lukas Spree, Emmanouil Koutsouflakis, Denis S. Krylov, Fupin Liu, Ariane Brandenburg, Georgios Velkos, Sebastian Schimmel, Stanislav M. Avdoshenko, Alexander Fedorov, Eugen Weschke, Fadi Choueikani, Philippe Ohresser, Jan Dreiser, Bernd Buchner, Alexey A. Popov
Summary: This study demonstrates a facile solution-based procedure for preparing functional magnetic sub-monolayers by self-assembling fullerene-SMM derivatives on metal substrates, with DySc2N@C-80 grafted on gold showing magnetic bistability up to 10 K.
Article
Chemistry, Multidisciplinary
Lukas Spree, Fupin Liu, Volker Neu, Marco Rosenkranz, Georgios Velkos, Yaofeng Wang, Sandra Schiemenz, Jan Dreiser, Pierluigi Gargiani, Manuel Valvidares, Chia-Hsiang Chen, Bernd Buchner, Stanislav M. Avdoshenko, Alexey A. Popov, H. Chen
Summary: Chemical functionalization of fullerene single molecule magnet enables the facile preparation of robust monolayers on graphene and highly oriented pyrolytic graphite without impairing their magnetic properties. Monolayers of endohedral fullerene functionalized with pyrene exhibit magnetic bistability up to a temperature of 28 K, showing potential for integration of spin carrying units encapsulated by fullerene cages on graphitic substrates.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Chemistry, Physical
Hao Sun, Ying Guo, Yanfeng Cui, Dawei Li, Gaocheng Yang, Yeye She, Qian Zhang, Yahong Li, Yi-Quan Zhang, Jinlei Yao
Summary: Two trinuclear complexes, [Dy3(mu 3-H2O)(hmp)3(CH3COO)3] (1) and [Gd3(mu 3-H2O)(hmp)3(CH3COO)3] (2), were synthesized and their crystal structures and magnetic properties were investigated. Complex 1 exhibits field-induced single-molecule magnet behavior, while complex 2 shows weak antiferromagnetic interactions.
JOURNAL OF MOLECULAR STRUCTURE
(2023)
Article
Chemistry, Physical
Yang Zhou, Run-Zhuo Yao, Xingwei Cai, Zhenxing Wang, Peipei Cen, Yong Yang, Aihua Yuan, Yisong Tang, Xiaoyun Chen, Shuanhong Zhang, Zhong-Wen Ouyang, Lei Chen
Summary: Soft donor ligands play a critical role in the construction of 3d transition-metal complexes with large magnetic anisotropy. In this study, a soft tripodal ligand was used to construct a high-spin mononuclear complex, which exhibited single-molecule magnet behavior.
JOURNAL OF MOLECULAR STRUCTURE
(2023)
Review
Chemistry, Multidisciplinary
Liu Kang, Guo Yan, Yu Jipan, Shi Weiqun
Summary: Single molecule magnets are magnetic materials composed of a single molecule, with magnetism deriving from the magnetic moment of a single molecule. They are expected to have applications in ultra-high density storage, quantum computers, spintronics, and other fields. Actinide single molecule magnets have attracted increasing attention due to the strong spin-orbit coupling effect and large radial extension of 5f electrons of actinides, showing potential to outperform transition metal and lanthanide complexes in terms of magnetism. However, the relaxation mechanism and factors behind slow magnetic behavior in actinide single molecule magnets remain unclear. This review summarizes the reported actinide single molecule magnets of the past decade, finding inconsistencies between experimental and theoretical values of blocking barriers, which have limited the development of actinide single molecule magnets to some extent. Finally, future research directions for actinide single molecule magnets are proposed.
ACTA CHIMICA SINICA
(2023)
Article
Chemistry, Multidisciplinary
Peng-Bo Jin, Ke-Xin Yu, Yuan-Qi Zhai, Qian-Cheng Luo, Yi-Dian Wang, Xu-Feng Zhang, Yi Lv, Yan-Zhen Zheng
Summary: Two dysprosium(III) complexes have been confirmed as single-molecule magnets, with the dimer showing enhanced magnetic relaxation barrier. Dilution experiments with the yttrium(III) analogue indicate the single-ion nature of the magnetic behavior.
CHINESE JOURNAL OF CHEMISTRY
(2021)
Article
Physics, Applied
Giulia Laghi, Domenico Franco, Guglielmo Guido Condorelli, Riccardo Gallerani, Salvatore Guglielmino, Romolo Laurita, Dario Morganti, Francesco Traina, Sabrina Conoci, Matteo Gherardi
Summary: The validity of the Yasuda parameter W/FM as a controlling parameter for plasma polymerization is demonstrated using an atmospheric pressure single electrode plasma jet. Thin films deposited under different W/FM values exhibit different chemical and physical properties. Coatings with similar characteristics can be obtained regardless of the power and feed rate values adopted. Preliminary results show that the deposited coatings have antiadhesive activity against Pseudomonas aeruginosa and Staphylococcus aureus.
PLASMA PROCESSES AND POLYMERS
(2023)
Article
Chemistry, Multidisciplinary
Felix Houard, Guiseppe Cucinotta, Thierry Guizouarn, Yan Suffren, Guillaume Calvez, Carole Daiguebonne, Olivier Guillou, Franck Artzner, Matteo Mannini, Kevin Bernot
Summary: This study demonstrates the assembly and transfer of single-chain magnets (SCMs) in the gel phase. SCMs based on Tb-III ions and nitronyl-nitroxides radicals with short alkyl chains can form crystalline supramolecular nanotubes interacting with heptane to create a robust gel. The gel is composed of supramolecular nanotubes, as confirmed by small-angle X-ray scattering, and exhibits SCM behavior in magnetism. Gelation on the surface allows for the deposition of supramolecular nanotubes as thick films or sub-monolayers.
MATERIALS HORIZONS
(2023)
Article
Chemistry, Multidisciplinary
Alessandro Chiesa, Alberto Privitera, Emilio Macaluso, Matteo Mannini, Robert Bittl, Ron Naaman, Michael R. Wasielewski, Roberta Sessoli, Stefano Carretta
Summary: Molecular spins are potential building blocks for future quantum technologies due to the flexibility provided by chemistry. However, their weak interaction with external stimuli makes it difficult to access their state at the single-molecule level. A solution using the chirality-induced spin selectivity effect on electron transfer processes is envisioned, which enables initialization, manipulation, and single-spin readout of molecular qubits and qudits even at relatively high temperatures.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Giuseppe Tranchida, Rachela Gabriella Milazzo, Marco Leonardi, Silvia Scalese, Luca Pulvirenti, Guido G. Condorelli, Corrado Bongiorno, Salvatore Lombardo, Stefania M. S. Privitera
Summary: In this study, Fe-based nanoparticles with different morphology were deposited on carbon cloth via drop-casting and chemical reduction. The catalyst activity was evaluated and optimized, resulting in a significant increase in ammonia production. The optimized catalysts produced ammonia with a yield of 26.44 μg mgcat-1h-1 and a Faradaic efficiency of 20.4%, more than five times higher than without activation.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Chemistry, Physical
Amandine Bellec, Massine Kelai, Arthur Tauzin, Anastasia Railean, Vincent Repain, Jerome Lagoute, Yann Girard, Sylvie Rousset, Edwige Otero, Talal Mallah, Marie-Laure Boillot, Cristian Enachescu
Summary: In this study, the photoexcitation of ultrathin films of [FeII((3, 5-(CH3)2Pz)3BH)2] (Pz = pyrazolyl) adsorbed on a special substrate was investigated. The anomalous light-induced spin-state switching was observed for sub-monolayer coverage, while the well-known light-induced excited spin-state trapping effect was recovered for higher coverages. The combination of continuous light excitation and thermal cycling revealed light-induced thermal hysteresis for thicker films and extended thermal conversion over a large temperature range for sub-monolayer coverage. Mechanoelastic simulations showed opposite behaviors in different layers of the films due to intermolecular interactions.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Crystallography
Fabio Santanni, Laura Chelazzi, Lorenzo Sorace, Grigore A. Timco, Roberta Sessoli
Summary: Heterotopic ligands with chemically different binding centers are used to obtain heteronuclear metal complexes with different paramagnetic centers. This molecular approach has the potential to yield multi-spin adducts for quantum information processing. This study reports the structural and magnetic characterization of a novel adduct {Cr(pybd)(3)[Cu(cyclen)](2)}(BF4)(4), which demonstrates weak magnetic couplings and maintains distinctive EPR signals for Cr3+ and Cu2+ moieties.
Article
Chemistry, Physical
Claudio Pereti, Kevin Bernot, Thierry Guizouarn, Frantisek Laufek, Anna Vymazalova, Luca Bindi, Roberta Sessoli, Duccio Fanelli
Summary: We propose an approach based on DeepSet technology for supervised classification and regression of superconductive materials. The method takes the chemical constituents as input, avoiding artefacts from ordering in the list. Successful performance is achieved in classifying superconducting materials and quantifying their critical temperature. Using the trained neural network, we searched the International Mineralogical Association list and identified three superconducting candidates, confirming superconductivity in the synthetic analogue of michenerite and observing it for the first time in monchetundraite with critical temperatures in good agreement with theory predictions. This marks the first certified superconducting material identified through artificial intelligence methodologies.
NPJ COMPUTATIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Francesca Portone, Mattia Amorini, Matteo Montanari, Roberta Pinalli, Alessandro Pedrini, Roberto Verucchi, Roberto Brighenti, Enrico Dalcanale
Summary: This study presents the first example of a synthetic molecular auxetic polymer obtained by embedding a conformationally expandable cavitand as a crosslinker into a rigid polymer of intrinsic microporosity. The auxetic behavior of the material is predicted and supported by a specific micromechanical model, and experimentally verified through mechanical tests. The results show that the conformational expansion of the cavitand crosslinker is responsible for the observed negative Poisson's ratio.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Materials Science, Multidisciplinary
Ameen Uddin Ammar, Feray Bakan-Misirlioglu, Mohamad Hasan Aleinawi, Giorgia Franzo, Guglielmo Guido Condorelli, Fatma Nur Tuzluca Yesilbag, Yasar Ozkan Yesilbag, Salvo Mirabella, Emre Erdem
Summary: In this study, high-performance supercapacitor devices were developed using manganese-doped zinc oxide nanowires and copper-doped zinc oxide nanoparticles as a positive electrode, with MXene as a negative electrode. The performance of transition metal-based electrodes in combination with MXene was found to significantly enhance the supercapacitors' performance. The highest-performance supercapacitor achieved a specific capacitance of 151 F/g, an energy density of 84 Wh/kg, and a power density of 75 kW/kg. The presence of intrinsic and extrinsic defects in the Mn/Cu-doped ZnO was found to optimize the intrinsic properties and improve reaction kinetics, leading to enhanced electrochemical activity and superior supercapacitor device performance.
MATERIALS RESEARCH BULLETIN
(2023)
Article
Chemistry, Multidisciplinary
Alejandro Nunez-Lopez, Ramon Torres-Cavanillas, Marc Morant-Giner, Natalia Vassilyeva, Richard Mattana, Sergio Tatay, Philippe Ohresser, Edwige Otero, Emiliano Fonda, Michael Paulus, Victor Rubio-Gimenez, Alicia Forment-Aliaga, Eugenio Coronado
Summary: In this research, ultrathin films of spin-crossover materials were grown on 2D materials, and the properties and spin transition of these hybrid structures were studied. When using 2H MoS2 as the substrate, the spin transition in films thinner than 8 nm was hindered by Fe3+; while using 1T MoS2, the spin transition was preserved in films as thin as 4 nm.
Article
Chemistry, Physical
Anna L. Pellegrino, Cristina Tudisco, Francesca Lo Presti, Emil Milan, Adolfo Speghini, Guglielmo G. Condorelli, Graziella Malandrino
Summary: For the first time, a gas-phase route called molecular layer deposition (MLD) was used to create a monolayer of metalorganic Eu(III) molecules on a NiO oxide layer. The NiO layer was activated using H2O/O2 vapors and then functionalized with molecules of the Eu complex at different temperatures to promote the chemisorption process. The effects of activation process and MLD temperature on the chemisorption of the Eu complex were evaluated using X-ray photoelectron and luminescence spectroscopy. The research findings defined the stoichiometry of the chemisorbed Eu moiety and optimized a strategy for synthesizing hybrid metalorganic/inorganic systems. The luminescence properties of the hybrid system confirmed energy conversion phenomena of the monolayer and provided information about the local environment of the Eu(III) complex anchored on the NiO surface.
Article
Chemistry, Multidisciplinary
Jacob O. Rothbaum, Alessandro Motta, Yosi Kratish, Tobin J. Marks
Summary: In this study, the mechanism of aldehyde and ketone hydroboration catalyzed by La[N(SiMe3)(2)](3) was investigated, revealing that aldehydes and ketones undergo initial carbonyl oxygen coordination to the acidic La center, followed by ligand-assisted intramolecular hydroboration. The study also identified a bidentate acylamino lanthanide complex associated with the aldehyde hydroboration and an aminomonoboronate-lanthanide complex produced under excess HBpin conditions, providing insights into the ligand-assisted hydroboration pathway and previously unknown catalyst deactivation pathways.
Article
Chemistry, Inorganic & Nuclear
Marius Retegan, Sadaf Fatima Jafri, Leonardo Curti, Laurent Lisnard, Edwige Otero, Eric Riviere, Maurits W. Haverkort, Anne Bleuzen, Philippe Sainctavit, Marie-Anne Arrio
Summary: This study investigates the contribution of the orbital magnetic moment to magnetization in a potassium hexacyanoferrate(III) sample using X-ray magnetic circular dichroism and molecular multiconfigurational ab initio calculations. The results demonstrate a significant proportion of the total magnetization attributed to the orbital magnetic moment, which is exceptional for 3d transition metal ions. The study also analyzes the impact of crystal field strength and distortion, pi back-bonding, spin-orbit coupling, and external magnetic induction on the spin and orbital magnetic anisotropies, providing a deeper understanding of these phenomena.
INORGANIC CHEMISTRY
(2023)
