Single-molecule magnets and polyradicals

Molecules with several unpaired electrons (often called single-molecule magnets) can be used as building blocks of novel magnetic materials and hardware for quantum computers. Typical designs include purely organic molecules (diradicals, triradicals, etc) or molecules with one or several transition metals. We develop new theoretical tools for describing SMMs and use these tools to characterize interesting species, often in collaboration with experimentalists.

301. S. Kaehler, A. Cebreiro, P. Pokhilko, D. Casanova, and A.I. Krylov
State-interaction approach for evaluating g-tensors within EOM-CC and RAS-CI frameworks: Theory and benchmarks
J. Phys. Chem. A  127, 8459 – 8472 (2023) Abstract  PDF Supporting info

290. M. Alessio, S. Kotaru, G. Giudetti, and A.I. Krylov
Origin of magnetic anisotropy in nickelocene molecular magnet and resilience of its magnetic behavior
J. Phys. Chem. C  127, 3647 – 3659 (2023) Abstract  PDF Supporting info

288. S. Kotaru, M. Alessio, S. Kaehler, and A.I. Krylov
Magnetic exchange interactions in binuclear and tetranuclear iron (III) complexes described by spin-flip DFT and Heisenberg effective Hamiltonians
J. Comp. Chem.  44, 367 – 380 (2023) Abstract  PDF 

285. S. Kotaru, P. Pokhilko, and A.I. Krylov
Spin-orbit couplings within spin-conserving and spin-flipping time-dependent density functional theory: Implementation and benchmark calculations
J. Chem. Phys.  157, 224110 (2022) Abstract  PDF Supporting info

267. M. Alessio and A.I. Krylov
Equation-of-motion coupled-cluster protocol for calculating magnetic properties: Theory and applications to single-molecule magnets
J. Chem. Theo. Comp.  17, 4225 – 4241 (2021) Abstract  PDF Supporting info

240. P. Pokhilko and A. I. Krylov
Effective Hamiltonians derived from equation-of-motion coupled-cluster wave-functions: Theory and application to the Hubbard and Heisenberg Hamiltonians
J. Chem. Phys.  152, 094108 (2020) Abstract  PDF Supporting info

236. P. Pokhilko, D. Izmodenov, and A. I. Krylov
Extension of frozen natural orbital approximation to open-shell references: Theory, implementation, and application to single-molecule magnets
J. Chem. Phys.  152, 034105 (2020) Abstract  PDF Supporting info

226. P. Pokhilko and A. I. Krylov
Quantitative El-Sayed rules for many-body wavefunctions from spinless transition density matrices
J. Phys. Chem. Lett.  10, 4857 – 4862 (2019) Abstract  PDF Supporting info

224. P. Pokhilko, E. Epifanovsky, and A. I. Krylov
General framework for calculating spin–orbit couplings using spinless one-particle density matrices: Theory and application to the equation-of-motion coupled-cluster wave functions
J. Chem. Phys.  151, 034106 (2019) Abstract  PDF 

197. N. Orms and A. I. Krylov
Singlet-triplet energy gaps and the degree of diradical character in binuclear copper molecular magnets characterized by spin-flip density functional theory
Phys. Chem. Chem. Phys. 20, 13095 – 13662 (2018) Abstract  PDF Supporting info

194. N. Orms, D. R. Rehn, A. Dreuw, and A. I. Krylov
Characterizing bonding patterns in diradicals and triradicals by density-based wave function analysis: A uniform approach
J. Chem. Theo. Comp. 14, 638 – 648 (2018) Abstract  PDF