Article
Multidisciplinary Sciences
Veronica R. Policht, Andrew Niedringhaus, Rhiannon Willow, Philip D. Laible, David F. Bocian, Christine Kirmaier, Dewey Holten, Tomas Mancal, Jennifer P. Ogilvie
Summary: This article reports two-dimensional electronic spectroscopy experiments on the bacterial reaction center, revealing hidden vibrational and excitonic structures. By analyzing the coherent dynamics of the reaction center, multiple quasi-resonances between pigment vibrations and excitonic energy gaps are identified, as well as vibronic coherence transfer processes that are often neglected in standard models. These findings provide insights into the energy transfer and charge separation processes in photosynthesis.
Article
Chemistry, Physical
Adam Srut, Vera Krewald
Summary: In this study, transient absorption spectroscopy and excited state dynamics simulations were used to investigate the electronic and vibrational evolution of a mixed-valent excited state in the reduced form of the Creutz-Taube ion. The results revealed a series of excited states with weak metal-metal interaction, which dominated the electronic population at short time scales. A long-lived vibrational wave packet mainly confined to oscillations of the metal center-bridge distances was observed.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Giuseppe Spedalotto, Marta Lovisari, Aidan R. McDonald
Summary: The researchers synthesized and characterized (NiNiIII)-Ni-II(mu-OH)(2) (2) and Ni-2(III) (mu-OH)(2) (3) species, with 3 demonstrating superior reaction rates and substrate oxidation efficiency compared to 2 and 2'. The kinetic superiority of 3 was attributed to a stronger bond in the product of oxidation for 3.
Article
Chemistry, Multidisciplinary
Yu-Ying Yang, Xiao-Quan Zhu, Jean-Pierre Launay, Cheng-Bin Hong, Shao-Dong Su, Yue-Hong Wen, Xin-Tao Wu, Tian-Lu Sheng
Summary: By synthesizing trimetallic isocyanidometal-bridged compounds with different oxidation states, the electron transfer process in oxidation reactions was investigated. The bridged states and mixed-valence states were simultaneously observed in N3+ compounds, while the electron transfer bridge excited state became more stable in N4+ compounds.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Marcel Krug, Nina Frohlich, Dominik Fehn, Alexander Vogel, Frank Rominger, Karsten Meyer, Timothy Clark, Milan Kivala, Dirk M. Guldi
Summary: Three linear dimers containing two redox-active planarized triphenylamines were synthesized and their structures verified by X-ray crystallography. Investigation of their radical cations using various techniques revealed the significance of using redox centers with low internal reorganization energies. Distance-dependence attenuation factor of the super-exchange mechanisms remained similar when compared with non-planarized nitrogen-centered building blocks.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Vyacheslav V. Sentyurin, Oleg A. Levitskiy, Alexey V. Bogdanov, Tatiana S. Yankova, Sergey G. Dorofeev, Konstantin A. Lyssenko, Victoria E. Gontcharenko, Tatiana V. Magdesieva
Summary: A new type of neutral mixed-valence system was synthesized using a one-pot procedure. The stability and energy barrier of intramolecular electron transfer in this system were influenced by a biphenyl bridge. The radicals in this system were determined to be Class II Robin-Day-mixed-valence systems through experimental and quantum-chemical study, and their structure was confirmed by X-ray data.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Inorganic & Nuclear
S. M. Gulam Rabbani, Andreas J. Achazi, Pere Miro
Summary: A computational study was conducted on the nucleation pathways of a POV alkoxide cluster in the absence of reducing agents, providing insights for controlling and manipulating the properties of the cluster.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Physical
Andrew Palii, Denis Korchagin, Sergey Aldoshin, J. M. Clemente-Juan, Shmuel Zilberg, Boris Tsukerblat
Summary: The vibronic coupling effect in quantum cellular automata based on mixed valence molecular cells significantly enhances the ability to polarize excess electrons in the working cell, leading to a redetermination of the conditions for switching between different spin-states and a significant change in the shapes of the cell-cell response functions.
Article
Chemistry, Inorganic & Nuclear
Stefanie Breimaier, Nina Froehlich, Jan Herberger, Michael Linseis, Milan Kivala, Rainer F. Winter
Summary: This article reports on three new vinylruthenium-triaryl-amine (TA) conjugates and presents a detailed study using various spectroscopic techniques and quantum chemical calculations. By analyzing the intervalence charge-transfer (IVCT) transitions of the mixed-valent radical cations, information on the extent of electronic coupling between chemically different redox sites is obtained. Temperature-dependent spectroscopy reveals the influence of vibrational coupling on the spectral features of these compounds.
Review
Chemistry, Inorganic & Nuclear
Tomoya Ishizuka, Hideki Sugimoto, Shinobu Itoh, Takahiko Kojima
Summary: Ruthenium and osmium complexes play crucial roles in oxidation reactions, generating high-valent species through peroxide activation and proton-coupled electron transfer. These complexes provide insights into oxidation mechanisms and exhibit unique reactivity.
COORDINATION CHEMISTRY REVIEWS
(2022)
Article
Multidisciplinary Sciences
Suman Mallick, Yuli Zhou, Xiaoli Chen, Ying Ning Tan, Miao Meng, Lijiu Cao, Yi Qin, Zi Cong He, Tao Cheng, Guang Yuan Zhu, Chun Y. Liu
Summary: In this study, the authors examine the characterization of covalency of intermolecular interactions in the van der Waals distance limit by analyzing the electronic states and intermolecular interactions in supramolecular mixed-valence systems. They demonstrate the influence of the solvating C6H6 molecule on the chemical properties and the breakdown of the dielectric solvation theory. This work provides new insights into accurately characterizing van der Waals interactions.
Review
Engineering, Environmental
Long Zhou, Zheng Li, Yunqiang Yi, Eric Pokeung Tsang, Zhanqiang Fang
Summary: This review provides a progress report on the significant developments in electron selectivity (ES) of nanoscale zero-valent iron nanoparticles (nZVI) over the past decade, including the definition of ES, quantification approaches, factors affecting ES, and latest techniques for increasing ES.
JOURNAL OF HAZARDOUS MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Justin T. Henthorn, George E. Cutsail, Thomas Weyhermueller, Serena DeBeer
Summary: This article investigates the electronic structure and spin states of mixed-valent iron-sulfur dimers and discovers a new interaction that can stabilize high spin states. By studying a series of mixed-valent complexes, complex interactions between antiferromagnetic coupling, Heisenberg double-exchange, and vibronic coupling are revealed.
Article
Chemistry, Multidisciplinary
Taeyeon Kim, Yuanning Feng, James P. O'Connor, J. Fraser Stoddart, Ryan M. Young, Michael R. Wasielewski
Summary: Designing and controlling charge transfer pathways in organic semiconductors are crucial for solar energy applications. This study investigates the photoinduced charge transfer and relaxation dynamics in host-guest complexes, and demonstrates that the charge transfer pathway can be controlled by subtle chemical modifications of the acceptor host.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Andrew Palii, Valeria Belonovich, Sergey Aldoshin, Boris Tsukerblat
Summary: A multimode vibronic model is used to analyze the localization-delocalization phenomenon in the two-electron square-planar mixed valence cluster. The dominant coupling with B1g vibration results in the electronic pair being localized on the diagonals of the square, while the dominant coupling with A1g mode leads to fully delocalized electronic pair.
Article
Chemistry, Inorganic & Nuclear
Alvaro Seijas-Da Silva, Jose Alberto Carrasco, Bruno J. C. Vieira, Joao C. Waerenborgh, Eugenio Coronado, Gonzalo Abellan
Summary: In this study, a hybrid NiFe-LDH family is synthesized through anion exchange reactions using surfactant molecules, increasing the interlayer space and achieving complete magnetic decoupling of the layers. The results of magnetic analysis and Mossbauer spectroscopy validate the potential of molecular engineering for designing hybrid layered magnetic materials approaching the 2D magnetic limit.
DALTON TRANSACTIONS
(2023)
Article
Materials Science, Multidisciplinary
Miguel Gavara-Edo, Francisco Javier Valverde-Munoz, Rosa Cordoba, M. Carmen Munoz, Javier Herrero-Martin, Jose Antonio Real, Eugenio Coronado
Summary: In this study, three new neutral Fe(II) SCO molecules belonging to the {Fe[H2B(pz)(2)](2)(L)} family were synthesized, and their crystallographic structure and magnetic properties were investigated. These compounds exhibited thermal- and light-induced SCO transitions with different degrees of cooperativity and effectiveness. Furthermore, two of the compounds were demonstrated to be sublimable, forming homogeneous thin films that retained the chemical integrity of the original molecules. SCO/2D horizontal hybrid devices based on CVD-graphene were successfully produced using these films, enabling the detection of the thermal SCO transition through the electric properties of CVD-graphene.
JOURNAL OF MATERIALS CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Victor Garcia-Lopez, Hanane El Mansour El Jastimi, Jana Jurakova, Miguel Clemente-Leon, Eugenio Coronado
Summary: In this study, three solvatomorphs of a two-nucleus iron(II) complex were synthesized and characterized. These solvatomorphs exhibited interesting spin crossover properties and could retain their crystallinity while allowing for the entrance or removal of solvent molecules through vapor diffusion. The spin crossover properties of the complex could be reversibly tuned by exposure to different solvents.
CRYSTAL GROWTH & DESIGN
(2023)
Article
Chemistry, Physical
Andrew Palii, Denis Korchagin, Ksenya Kondrina, Sergey Aldoshin, Shmuel Zilberg, Boris Tsukerblat
Summary: This study generalizes the theory of magnetic coupling between localized spins to a trigonal, six-center, four-electron molecule with partial valence delocalization. The combination of electron transfer within the valence-delocalized subsystem and interatomic exchange leads to a special kind of double exchange (DE) called external core double exchange (ECDE). The study compares the effect of ECDE on the ground spin state of the trigonal molecule with the effect produced by DE in a four-electron, mixed-valence (MV) trimer. The results show a high diversity of ground spin states depending on the relative magnitudes and signs of transfer and exchange parameters, suggesting potential applications in molecular electronics and spintronics.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Shmuel Zilberg, Boris Tsukerblat, Andrew Palii
Summary: By studying the cation-radical form of 1,4-diallyl-butane and its derivatives, we found that the electron transfer barrier in compounds with a π-fragment on the bridge is higher compared to those with a saturated bridge. We proposed a model based on the specific polaronic effect of the spacer, which can provide a route to controllable electron transfer in bridged mixed-valence compounds.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Physics, Multidisciplinary
Mattias Matthiesen, Jorrit R. Hortensius, Samuel Manas-Valero, Itzik Kapon, Dumitru Dumcenco, Enrico Giannini, Makars Siskin, Boris A. Ivanov, Herre S. J. van der Zant, Eugenio Coronado, Alexey B. Kuzmenko, Dmytro Afanasiev, Andrea D. Caviglia
Summary: The research focuses on investigating optical methods for generating coherent magnons in antiferromagnetic insulators. It is found that orbital transitions are key targets for magnetic control in insulators with zero orbital angular momentum.
PHYSICAL REVIEW LETTERS
(2023)
Article
Materials Science, Multidisciplinary
Jan N. Kirchhof, Yuefeng Yu, Denis Yagodkin, Nele Stetzuhn, Daniel B. de Araujo, Kostas Kanellopulos, Samuel Manas-Valero, Eugenio Coronado, Herre van der Zant, Stephanie Reich, Silvan Schmid, Kirill Bolotin
Summary: Nanomechanical spectroscopy (NMS) is a new approach to determine optical absorption spectra of nanoscale materials via mechanical measurements. It directly measures absorption by measuring changes in the resonance frequency of a membrane resonator. In this study, a protocol for NMS of 2D materials is developed, which improves sensitivity and simplifies the experiment. The use of low-stress silicon nitride membranes as the substrate reduces noise-equivalent power.
Article
Chemistry, Multidisciplinary
Yishay Zur, Avia Noah, Carla Boix-Constant, Samuel Manas-Valero, Nofar Fridman, Ricardo Rama-Eiroa, Martin E. Huber, Elton J. G. Santos, Eugenio Coronado, Yonathan Anahory
Summary: This work demonstrates direct magnetic imaging of CrSBr flakes using nano-SQUID-on-tip (SOT) microscopy. It is found that the ferromagnetic order and the antiferromagnetic coupling are preserved down to the monolayer. Additionally, spin reorientation and the formation of Neel magnetic domain walls are observed even in the single-layer limit. This highlights the remarkable stability of CrSBr in the 2D limit.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Andrew Palii, Valeria Belonovich, Sergei Aldoshin, Shmuel Zilberg, Boris Tsukerblat
Summary: In this article, the power dissipation in nonadiabatic switching events in mixed-valence molecular cells of quantum cellular automata (QCA) is analyzed. The study shows that while there is a competition between the requirements for a strong nonlinear response and low heat release, it is possible to achieve functional advantages and practical application of QCA through molecular design.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Gabriele Baglioni, Makars Siskins, Maurits Houmes, Martin Lee, Dong Hoon Shin, Samuel Manas-Valero, Eugenio M. Coronado, Yaroslav Blanter, Herre S. J. G. van der Zant, Peter Steeneken
Summary: Magnetostrictive coupling has become a sensitive method for studying magnetism in 2D materials by mechanical means. In this study, we optothermally modulate the magnetization in antiferromagnetic 2D material membranes to induce a high-frequency magnetostrictive driving force. The thermo-magnetostrictive effect near the critical temperature of magnetostrictive 2D materials provides a route for more efficient actuation of nano-magnetomechanical devices and studying the coupling among magnetic, mechanical, and thermodynamic degrees of freedom.
Article
Nanoscience & Nanotechnology
D. Khusyainov, T. Gareev, V. Radovskaia, K. Sampathkumar, S. Acharya, M. Siskins, S. Manas-Valero, B. A. Ivanov, E. Coronado, Th. Rasing, A. V. Kimel, D. Afanasiev
Summary: Using a time-resolved magneto-optical pump-probe technique, the ultrafast laser-induced dynamics of mutually correlated spins and lattice in CoPS3 were experimentally studied. It was found that the femtosecond laser pulse acted as an ultrafast heater and melted the antiferromagnetic order. The resonant pumping of the T-4(1g) ? T-4(2g) electronic transition in Co2+ ions effectively changed their orbital momentum and generated a coherent B-g phonon mode.
Article
Chemistry, Multidisciplinary
Mario Palacios-Corella, Victor Garcia-Lopez, Joao Carlos Waerenborgh, Bruno J. C. Vieira, Guillermo Minguez Espallargas, Miguel Clemente-Leon, Eugenio Coronado
Summary: A bifunctionalized polyoxometalate containing a redox active hexavanadate moiety and two tridentate 2,6-bis(pyrazol-1-yl)pyridine ligands was synthesized and characterized. Reaction with Fe(ii) or Zn(ii) ions resulted in the formation of crystalline 1D networks with tunable magnetic and redox properties. The structures exhibited spin-crossover behavior, which could be induced by light irradiation, and reversible solvent exchange. Additionally, the hexavanadate unit could be reduced and reoxidized, leading to changes in the spin state of Fe(ii) and creating a multifunctional material that can be controlled by various stimuli.
Article
Chemistry, Multidisciplinary
Enrique Burzuri, Maria Jose Martinez-Perez, Carlos Marti-Gastaldo, Marco Evangelisti, Samuel Manas-Valero, Eugenio Coronado, Jesus I. Martinez, Jose Ramon Galan-Mascaros, Fernando Luis
Summary: In this article, a novel 2D heterometallic oxalate complex is presented as a potential candidate for quantum spin liquid (QSL) material. It exhibits strong antiferromagnetic correlations and the absence of magnetic ordering, making it an appealing QSL candidate.
Article
Multidisciplinary Sciences
Junhyeon Jo, Yuan Peisen, Haozhe Yang, Samuel Manas-Valero, Jose J. Baldovi, Yao Lu, Eugenio Coronado, Felix Casanova, F. Sebastian Bergeret, Marco Gobbi, Luis E. Hueso
Summary: We demonstrate novel devices based on the unique properties of two-dimensional materials, including infinite magnetoresistance and nonreciprocal charge transport, using NbSe2/CrSBr van der Waals superconducting spin valves. We also show the realization of a superconductive spin valve with multiple stable resistance states by integrating different CrSBr crystals in a lateral heterostructure.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Miguel Gavara-Edo, Francisco Javier Valverde-Munoz, M. Carmen Munoz, Safaa Elidrissi Moubtassim, Francisco Marques-Moros, Javier Herrero-Martin, Kateryna Znovjyak, Maksym Seredyuk, Jose Antonio Real, Eugenio Coronado
Summary: Materials based on spin crossover molecules have attracted significant attention in molecular magnetism. This study presents a novel spin crossover material that can form thermally stable thin films while retaining its molecular bistability.
CHEMISTRY OF MATERIALS
(2023)
