TY - JOUR
T1 - Magnetic Coupling in a Tris-hydroxo-Bridged Chromium Dimer Occurs through Ligand Mediated Superexchange in Conjunction with Through-Space Coupling
AU - Sharma, Prachi
AU - Truhlar, Donald G.
AU - Gagliardi, Laura
N1 - Publisher Copyright:
© 2020 American Chemical Society
PY - 2020/9/30
Y1 - 2020/9/30
N2 - Quantum chemistry can explain and predict many properties of molecules and materials. However, there are some systems, among which are magnetic systems, that remain a challenge for all electronic structure methods. The tris-hydroxo-bridged chromium dimer, known as Kremer’s dimer, contains two antiferromagnetically coupled chromium(III) metal ions and provides a classic example of a magnetic molecular system that poses a challenge for computational quantum chemistry. In this study we show that combining multiconfiguration pair-density functional theory with large-active-space density matrix renormalization group wave functions can predict the correct spin-state ordering, energy spacing, and magnetic coupling constant. We also use the unpaired electron density to analyze the superexchange contribution. This methodology offers promise for revolutionary rational design of molecular magnets.
AB - Quantum chemistry can explain and predict many properties of molecules and materials. However, there are some systems, among which are magnetic systems, that remain a challenge for all electronic structure methods. The tris-hydroxo-bridged chromium dimer, known as Kremer’s dimer, contains two antiferromagnetically coupled chromium(III) metal ions and provides a classic example of a magnetic molecular system that poses a challenge for computational quantum chemistry. In this study we show that combining multiconfiguration pair-density functional theory with large-active-space density matrix renormalization group wave functions can predict the correct spin-state ordering, energy spacing, and magnetic coupling constant. We also use the unpaired electron density to analyze the superexchange contribution. This methodology offers promise for revolutionary rational design of molecular magnets.
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U2 - 10.1021/jacs.0c06399
DO - 10.1021/jacs.0c06399
M3 - Article
C2 - 32875795
AN - SCOPUS:85092426572
SN - 0002-7863
VL - 142
SP - 16644
EP - 16650
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 39
ER -