Tuning symmetry and magnetic blocking of an exchange-coupled lanthanide ion in isomeric, tetrametallic complexes: [LnCl6(TiCp2)3]

Paramagnetic molecules with a metal ion as an electron spin center are promising building blocks for molecular qubits and high-density memory arrays. However, fast spin relaxation and decoherence in these molecules lead to a rapid loss of magnetization and quantum information. Nonadiabatic coupling (NAC), closely related to spin-vibrational coupling, is the main source of spin relaxation and decoherence in paramagnetic molecules at higher temperatures. Predicting these couplings using numerical differentiation requires a large number of computationally intensive ab initio or crystal field electronic structure calculations. To reduce computational cost and improve accuracy, we derive and implement analytical NAC and state-specific energy gradient for the ab initio parametrized crystal field Hamiltonian describing single-ion molecular magnets. Our implementation requires only a single crystal field calculation. In addition, the accurate NACs and state-specific energy gradients can be used to model spin relaxation using sophisticated nonadiabatic molecular dynamics, which avoids the harmonic approximation for molecular vibrations. To test our implementation, we calculate the NAC values for three lanthanide complexes. The predicted values support the relaxation mechanisms reported in previous studies.

show abstract

scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.

Contact Info

customersupport@researchsolutions.com

10624 S. Eastern Ave., Ste. A-614

Henderson, NV 89052, USA

This site is protected by reCAPTCHA and the Google Privacy Policy and Terms of Service apply.

Blog Terms and Conditions API Terms Privacy Policy Contact Cookie Preferences Do Not Sell or Share My Personal Information

Made with 💙 for researchers

Part of the Research Solutions Family.

Tuning symmetry and magnetic blocking of an exchange-coupled lanthanide ion in isomeric, tetrametallic complexes: [LnCl₆(TiCp₂)₃]

Abstract: The synthesis and magnetic properties of two pairs of isomeric, exchange-coupled complexes, [LnCl6(TiCp2)3] (Ln = Gd, Tb), are reported. In each isomeric pair, the central lanthanide ion adopts either a...

Cited by 3 publications

References 49 publications

Engineering a high-barrier d-f single-molecule magnet centered with hexagonal bipyramidal Dy(III) unit

Engineering a high-barrier d-f single-molecule magnet centered with hexagonal bipyramidal Dy(III) unit

Predicting Magnetic Barriers in Lanthanide Complexes with Electrostatic Potential Charges

Analytical nonadiabatic coupling and state-specific energy gradient for the crystal field Hamiltonian describing lanthanide single-ion magnets

Contact Info

Product

Resources

About