Article
Chemistry, Inorganic & Nuclear
Khetpakorn Chakarawet, Mihail Atanasov, John E. Ellis, Wayne W. Lukens, Victor G. Young, Ruchira Chatterjee, Frank Neese, Jeffrey R. Long
Summary: The spin-vibronic coupling in paramagnetic molecules can lead to spin relaxation, which is detrimental to long spin lifetime. The increase in spin relaxation rate from vanadium to niobium to tantalum was experimentally observed in the isoelectronic and isostructural series of homoleptic zerovalent transition metal triad M(CNDipp)(6). Correlated electronic calculations and first principle spin-phonon computations provide support for the role of spin-orbit coupling in modulating spin-phonon relaxation.
INORGANIC CHEMISTRY
(2021)
Review
Chemistry, Multidisciplinary
Riccardo Marin, Gabriel Brunet, Muralee Murugesu
Summary: Single-molecule magnets play a crucial role in quantum information processing and spintronics. The harmonious combination of magnetism and luminescence within single molecules provides insights for emerging next-generation spintronics devices.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Arpan Mondal, Sanjit Konar
Summary: The study for the first time observed the importance of equatorial crystal fields on the magnetic anisotropy of ytterbium single molecule magnets. Analysis of three similar dinuclear ytterbium complexes revealed weak antiferromagnetic interactions and field-induced slow relaxation of magnetization. Complex 1 showed a higher energy barrier for spin reversal and a remarkable energy barrier within a specific frequency range.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Sourav Dey, Gopalan Rajaraman, Helene Bolvin
Summary: The SMM compound [{Mn(TPA)I}{UO2(Mesaldien)}{Mn(TPA)I}]I has been fully characterized and its spin Hamiltonian parameters extracted using ab initio CAS and DFT methods. The study reveals that the signs of magnetic coupling and g-factors are interconnected, with the central magnetic unit [(UO2)-O-V]+ described by a Kramers Doublet with negative g-factors. Furthermore, the study suggests that the spin polarization on the U(V) center favors ferromagnetic coupling and that the J(Z)/J(perpendicular to) ratio, related to the barrier height, can be estimated from the corresponding g(S)-values.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
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
Chemistry, Multidisciplinary
Celine Pichon, Nicolas Suaud, Valentin Jubault, Carine Duhayon, Nathalie Guihery, Jean-Pascal Sutter
Summary: Trinuclear metal complexes were synthesized to investigate their influence on the magnetic anisotropy of Fe-II derivatives and their Single-Molecule Magnet behaviors, revealing a significant effect of the bending of M-N to C linkages on the slow relaxation of magnetization in [Cr2Fe] complexes. Theoretical calculations emphasized the importance of apical C-N-Fe linkages on the magnetic anisotropy and exchange interactions in these complexes.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Giang Truong Nguyen, Liviu Ungur
Summary: This article presents a theoretical investigation of a series of N23- -radical-bridged diterbium complexes. The study reveals that while promoting strong exchange coupling between the terbium ions, the N23- -radical induces a crystal field that interferes destructively with that of the outer ligands, thereby reducing the overall SMM behavior. Based on the theoretical results, it is concluded that the SMM behavior in this series could be further maximized if the crystal field of the outer ligands is designed to be collinear with that of the radical bridge. This conclusion can be generalized to all exchange-coupled SMMs.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Jules Moutet, Jules Schleinitz, Leo La Droitte, Maxime Tricoire, Fabrice Pointillart, Frederic Gendron, Thomas Simler, Carine Clavaguera, Boris Le Guennic, Olivier Cador, Gregory Nocton
Summary: Divalent lanthanide organometallics are highly reducing compounds known for single electron transfer reactivity and small molecule activation. This study presents a rare organometallic sandwich compound of divalent thulium with the cyclooctatetraenyl ligand, introducing it as an additional strategy for designing high-performing Single Molecule Magnets. The first divalent thulium sandwich complex with f(13) configuration behaves as a single-molecule magnet even in the absence of a DC field.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Inorganic & Nuclear
Qi-Wei Chen, You-Song Ding, Tianjiao Xue, Xiao-Fei Zhu, Zhiping Zheng
Summary: Magneto-structural correlations are crucial for the development of single-molecule magnets. In this study, three cyclooctatetraenylido (COT) ligands with different trimethylsilyl (TMS) substituents were used to prepare Er(III) complexes. The results showed that an increase in the number of TMS substituents led to enhanced molecular vibrations and faster magnetic relaxation.
INORGANIC CHEMISTRY FRONTIERS
(2023)
Review
Chemistry, Inorganic & Nuclear
Lucinda R. B. Wilson, Marco Coletta, Marco Evangelisiti, Stergios Piligkos, Scott J. Dalgarno, Euan K. Brechin
Summary: The calix[4]arene scaffold is a versatile supramolecular platform that can be used to synthesize a variety of polymetallic clusters with consistent coordination preferences and assembly behaviors.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Physical
Dongmei Zhang, Yong Lu, Jie Wang, Chu Gong, Xuesen Hou, Xinxing Zhang, Jun Chen
Summary: This study re-examines the synthesis method of the cyclohexanehexone molecule, confirming its structure and chemical bonding through mass spectrometry and theoretical calculations. It provides a benchmark understanding of the historically elusive C6O6.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Inorganic & Nuclear
Amaleswari Rasamsetty, Sakshi Mehta, Kamal Uddin Ansari, Pardeep Kumar, Abhishake Mondal, Maheswaran Shanmugam
Summary: The research discovers a weak antiferromagnetic coupling in rare six-coordinated dinuclear Ln(III) complexes, and emphasizes the importance of the amide ligand at the coordination site of Dy(III) which results in slow relaxation of magnetization. This finding is supported by detailed ab initio calculations and electronic structure determination of the complexes.
DALTON TRANSACTIONS
(2021)
Article
Chemistry, Multidisciplinary
Gao-Peng Li, Hong-Fang Xie, Shi-Rui Yang, Yun-Long Fu, Yi-Quan Zhang, Yao-Yu Wang
Summary: The study investigates the control of intramolecular magnetic interactions and relaxation dynamics by introducing two structurally related heterometal SMMs. It is found that changing the coordination geometries significantly affects the magnetic interactions and single-ion anisotropy.
CHINESE JOURNAL OF CHEMISTRY
(2022)
Article
Chemistry, Inorganic & Nuclear
Fabio Manna, Mariangela Oggianu, Narcis Avarvari, Maria Laura Mercuri
Summary: Lanthanide metal-organic frameworks (Ln-MOFs) with single-molecule magnet (SMM) properties are a growing family of materials where magnetic properties can be controlled by interrelated parameters, such as solvent, temperature, organic linkers, lanthanide ions, and coordination environment. This overview discusses synthetic methods for accessing MOFs/Ln-MOFs and controlling/fine-tuning their SMM behavior. It also explores challenging strategies for inducing SMM/SIM behavior, including redox activity and chirality, as well as intriguing physical phenomena such as the CISS effect and CPL.
Article
Chemistry, Physical
Tilmann Bodenstein, Andreas Heimermann, Karin Fink, Christoph van Wuellen
Summary: The spin-orbit configuration interaction program presented in this study is tailored for describing the magnetic properties of polynuclear metal complexes with partially filled d- and f-shells. It uses spin-orbit operators directly within a configuration interaction program based on Slater determinants, allowing for efficient calculation of magnetic parameters and temperature-dependent properties. This program demonstrates fast convergence and high efficiency in analyzing the magnetic behavior of transition metal complexes.
Article
Chemistry, Physical
Diana Dulic, Alfredo Rates, Edison Castro, Jacqueline Labra-Munoz, Daniel Aravena, Alvaro Etcheverry-Berrios, Daniel Riba-Lopez, Eliseo Ruiz, Nuria Aliaga-Alcalde, Monica Soler, Luis Echegoyen, Herre S. J. van der Zant
JOURNAL OF PHYSICAL CHEMISTRY C
(2020)
Article
Chemistry, Physical
Yolimar Gil, Leonel Llanos, Patricio Cancino, Pablo Fuentealba, Andres Vega, Evgenia Spodine, Daniel Aravena
JOURNAL OF PHYSICAL CHEMISTRY C
(2020)
Article
Chemistry, Multidisciplinary
Albert C. Aragones, Alejandro Martin-Rodriguez, Daniel Aravena, Josep Puigmarti-Luis, David B. Amabilino, Nuria Aliaga-Alcalde, Arantzazu Gonzalez-Campo, Eliseo Ruiz, Ismael Diez-Perez
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2020)
Article
Chemistry, Inorganic & Nuclear
Leonel Llanos, Cristian Vera, Andres Vega, Daniel Aravena, Luis Lemus
INORGANIC CHEMISTRY
(2020)
Article
Chemistry, Physical
Chen Sun, Leonel Llanos, Pablo Arce, Allen Oliver, Reinhold Wannemacher, Juan Cabanillas-Gonzalez, Luis Lemus, Daniel Aravena
Summary: This study reports on the thermally activated delayed fluorescence (TADF) properties of a novel iodine-bridged Cu-I dimeric complex and its structurally related monomer. Efficient room-temperature TADF was observed in both compounds, with similar singlet-triplet splittings but longer triplet lifetime in the dimer. Key structural factors determining TADF properties, such as the role of iodine in spin-orbit coupling mixing and near degeneracies in donor and acceptor orbitals, were identified through computational calculations.
CHEMISTRY OF MATERIALS
(2021)
Article
Chemistry, Applied
Tamara Maldonado, Erick Flores, Leonel Llanos, Daniel Aravena, Andres Vega, Fernando Godoy, Alexis Aspee, Nicolas Arancibia-Miranda, Guillermo Ferraudi, Alejandra Gomez
Summary: The spectroscopic properties and tautomeric behavior of five novel Rhenium (I) tricarbonyl complexes with an azo ligand are presented. The organic ligand remains stable as the hydrazone tautomer in solution, but complexation with a strong electron-withdrawing fragment induces tautomerism in the organic moiety.
Review
Chemistry, Multidisciplinary
Yolimar Gil, Alejandro Castro-Alvarez, Pablo Fuentealba, Evgenia Spodine, Daniel Aravena
Summary: Enhancement of axial magnetic anisotropy is the central objective to improve the performance of Single-Molecule Magnet (SMM) complexes. Tuning the chemical environment around the paramagnetic ion is crucial in mononuclear lanthanide complexes. The use of highly structured, chelating ligands and macrocycles in a belt conformation can provide precise chemical environments for metal centers and allow for axial-equatorial control.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Chemistry, Inorganic & Nuclear
Yolimar Gil, Raquel Gimeno-Munoz, Ricardo Costa de Santana, Nuria Aliaga-Alcalde, Pablo Fuentealba, Daniel Aravena, Arantzazu Gonzalez-Campo, Evgenia Spodine
Summary: In this study, two mononuclear DyIII complexes were immobilized on functionalized silicon-based surfaces using microcontact printing technique, allowing control over the position of the molecules on the surface. The successful functionalization of the surfaces was confirmed through various measurements, and the optical properties of the compounds were investigated. The results showed that the immobilized complexes emitted deep blue and white light at room temperature, while retaining their bulk emissive properties.
INORGANIC CHEMISTRY
(2022)
Article
Physics, Multidisciplinary
Katy Aruachan, Yamil J. Colon, Daniel Aravena, Felipe Herrera
Summary: Understanding the physical processes that determine the relaxation and dephasing times of molecular spin qubits is crucial for their applications in quantum metrology and information processing. Recent spin-echo measurements in solid-state molecular spin qubits have led to the development of quantum mechanical models for predicting qubit timescales. In this study, a semi-empirical approach is used to construct Redfield quantum master equations for molecular spin qubits, taking into account the effects of spin-lattice interaction and interactions with lattice spins. The model is validated using two vanadium-based spin qubits, and it demonstrates good agreement with experimental data over a wide range of conditions. The model's ability to describe the temperature dependence of the T2/T1 ratio is discussed, and potential applications for designing molecule-based quantum magnetometers are suggested.
NEW JOURNAL OF PHYSICS
(2023)
Article
Chemistry, Inorganic & Nuclear
Shuting Liu, Yolimar Gil, Chen Zhao, Jinjiang Wu, Zhenhua Zhu, Xiao-Lei Li, Daniel Aravena, Jinkui Tang
Summary: This study synthesized two new belt macrocycle complexes through self-condensation reaction and other steps, and conducted magnetic measurements on them. The experimental results indicate that these complexes exhibit typical single-molecule magnet behavior.
INORGANIC CHEMISTRY FRONTIERS
(2022)
Article
Chemistry, Physical
Lucia Velasco, Leonel Llanos, Pedro Levin, Andres Vega, Jin Yu, Xiaoyi Zhang, Luis Lemus, Daniel Aravena, Dooshaye Moonshiram
Summary: Time-resolved X-ray and optical transient absorption spectroscopy were combined with DFT and XANES calculations to study the photoexcitation dynamics of three homoleptic Cu(i) dimeric chromophores. Results showed distinct excited state lifetimes for different complexes, which were attributed to solvent effects and ligand flexibility upon copper flattening. These findings are important for understanding the structural dynamics of Cu-based compounds and their potential integration into solar energy conversion systems.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Inorganic & Nuclear
Yolimar Gil, Pablo Fuentealba, Andres Vega, Evgenia Spodine, Daniel Aravena
DALTON TRANSACTIONS
(2020)
Article
Chemistry, Inorganic & Nuclear
Alejandro Castro-Alvarez, Yolimar Gil, Leonel Llanos, Daniel Aravena
INORGANIC CHEMISTRY FRONTIERS
(2020)
Review
Chemistry, Inorganic & Nuclear
Daniel Aravena, Eliseo Ruiz
DALTON TRANSACTIONS
(2020)
Article
Chemistry, Multidisciplinary
Patricio Cancino, Luis Santibanez, Christian Stevens, Pablo Fuentealba, Nathalie Audebrand, Daniel Aravena, Julia Torres, Sebastian Martinez, Carlos Kremer, Evgenia Spodine
NEW JOURNAL OF CHEMISTRY
(2019)