AI Article Synopsis
Article Abstract
Single-ion magnets (SIMs) constitute the ultimate size limit in the quest for miniaturizing magnetic materials. Several bottlenecks currently hindering breakthroughs in quantum information and communication technologies could be alleviated by new generations of SIMs displaying multifunctionality. Here, ultrafast optical absorption spectroscopy and X-ray emission spectroscopy are employed to track the photoinduced spin-state switching of the prototypical complex [Co(terpy) ] (terpy = 2,2':6',2″-terpyridine) in solution phase. The combined measurements and their analysis supported by density functional theory (DFT), time-dependent-DFT (TD-DFT) and multireference quantum chemistry calculations reveal that the complex undergoes a spin-state transition from a tetragonally elongated doublet state to a tetragonally compressed quartet state on the femtosecond timescale, i.e., it sustains ultrafast Jahn-Teller (JT) photoswitching between two different spin multiplicities. Adding new Co-based complexes as possible contenders in the search for JT photoswitching SIMs will greatly widen the possibilities for implementing magnetic multifunctionality and eventually controlling ultrafast magnetization with optical photons.
Download full-text PDF |
Source |
|---|---|
| http://www.ncbi.nlm.nih.gov/pmc/articles/PMC10375196 | PMC |
| http://dx.doi.org/10.1002/advs.202206880 | DOI Listing |
Publication Analysis
Top Keywords
Similar Publications
Crystal Lattice-Induced Stress modulates Photoinduced Jahn-Teller Distortion Dynamics.
ACS Phys Chem Au
November 2024
Rosalind Franklin Institute, Harwell OX11 0QX, Oxfordshire, United Kingdom.
Efficient photoredox chemical transformations are essential to the development of novel, cost-effective, and environmentally friendly synthetic methodologies. The concept of the entatic state in bioinorganic catalysis proposes that a preorganized structural configuration can reduce the energy barriers associated with chemical reactions. This concept provides one of the guiding principles to enhance catalytic efficiency by maintaining high-energy conformations close to the reaction's transition state.
View Article and Find Full Text PDFBridge editing of spin-flip emitters gives insight into excited state energies and dynamics.
Chem Sci
December 2024
Department of Chemistry, Johannes Gutenberg University Mainz Duesbergweg 10-14 55128 Mainz Germany
Six-coordinate chromium(iii) complexes with high spin-flip (SF) photoluminescence quantum yields and lifetimes (molecular rubies) have attracted huge interest in the past years due to their applicability in sensing, photocatalysis or circularly polarised emission. However, clearcut design rules for high quantum yields and lifetimes are still lacking due to the multidimensional problem of the non-radiative decay of the SF states. Based on an isostructural series of complexes differing in the ligand backbone, we disentangle decisive structural and electronic features for SF excited state energies and non-radiative decays promoted by spin-orbit coupling, Jahn-Teller distortions and (thermally activated) multiphonon relaxation.
View Article and Find Full Text PDFUnraveling the Mechanisms of the Formations and Transformations of Metal-Ligand Charge Transfer States in [Ru(tpy)]: Consequences of Jahn-Teller Conical Intersections and the Pseudo-Jahn-Teller Effect.
J Phys Chem A
November 2024
State Key Laboratory of Physical Chemistry of Solid Surfaces, Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, Fujian 361005, China.
This work investigates Jahn-Teller conical intersections (CoIns) and the pseudo-Jahn-Teller effect on the formations and transformations of the low-lying singlet metal-ligand charge transfer (MLCT) excited states during the ultrafast evolution process of photoexcited [Ru(tpy)] (tpy = 2,2':6',2″-terpyridine). Longuet-Higgins' geometric phase analyses indicate that the potential energy surface (PES) crossing between charge transfer states MLCT and MLCT is a CoIn, originating from the change in diabatic Hamiltonian matrix elements around the CoIn. Moreover, an ⊗( + ) Jahn-Teller distortion can occur around the Franck-Condon and minimal energy CoIn (MECI) configurations, causing the molecule to distort spontaneously from the high-symmetry configuration to symmetry configurations that are close to it.
View Article and Find Full Text PDFThe phonon-modulated Jahn-Teller distortion of the nitrogen vacancy center in diamond.
Nat Commun
October 2024
Department of Chemistry, New York University, New York, NY, 10003, USA.
The negatively charged nitrogen vacancy (NV) center in diamond is an optically accessible material defect with a unique combination of spin and optical properties that has attracted interest in quantum-information sciences and as a design candidate for nanoscale quantum sensors. Here, we present time-resolved nonlinear optical spectroscopy measurements, conducted with ultrabroadband laser pulses, that reveal strong modulation of the excited-state by the longitudinal optical (LO) phonon of the diamond lattice. The LO phonon and its overtones geometrically distort neighboring NV centers, driving long lived (3.
View Article and Find Full Text PDFOctahedral Mn(iii) ions predominantly exhibit an axially elongated Jahn-Teller (JT) distortion, which is responsible for their large uniaxial magnetic anisotropy. As a result, they are often used in the synthesis of single-molecule magnets (SMMs). Modulation of the JT distortion using femtosecond laser pulses could offer a route to controlling the magnetisation direction, and therefore is promising for the development of data storage devices that work on ultrafast timescales.
View Article and Find Full Text PDFWant AI Summaries of new PubMed Abstracts delivered to your In-box?
Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!