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Trans-Influence in Dinuclear Pt(III) Complexes: Electronic Structure, σ-Donation, and Pt-Pt Spin-Spin Coupling

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Author(s):
Oliveira, Pedro P. R. ; Batista, Patrick R. ; Ducati, Lucas C. ; Autschbach, Jochen
Total Authors: 4
Document type: Journal article
Source: Inorganic Chemistry; v. N/A, p. 8-pg., 2025-10-17.
Abstract

This study investigates the trans influence in dinuclear platinum(III) complexes using a combined approach of ab initio molecular dynamics and natural localized molecular orbital (NLMO) analysis. Focusing on pivalamidate-bridged PtIII complexes with axial ligands of varying sigma-donation strength, it is quantified how ligand-metal interactions propagate through the Pt-Pt bond, and how they affect bond polarization, axial water coordination, and 1 J PtPt spin-spin coupling constants. NLMO analysis reveals quantitatively that strong sigma-donating ligands polarize the Pt-Pt bond, shifting the electron density toward the opposite platinum center. The polarization mechanism is identified as the primary reason for the observed reduction of 1 J PtPt, because the bond polarization diminishes the transmission of the nuclear magnetic spin-induced electron spin density through the Pt-Pt bond. Additionally, the destabilization of axial water coordination at the opposite Pt site can be rationalized through a polarization-induced PtIV- PtII-like mixed-valence character. (AU)

FAPESP's process: 24/00633-8 - Probing the Kinetic Trans Effect in Halide Ion Substitution Reactions of Dinuclear Pt(III) Complexes Through Metadynamics Simulations
Grantee:Pedro Paulo Rezende Oliveira
Support Opportunities: Scholarships abroad - Research Internship - Master's degree
FAPESP's process: 24/17236-1 - Solvent Effect on NMR Parameters of Tl(III) and Pt(IV) Complexes by ab initio Molecular Dynamics and Relativistic Calculations
Grantee:Lucas Colucci Ducati
Support Opportunities: Regular Research Grants
FAPESP's process: 21/09687-5 - Assessment of conformational preferences on fluorine-containing molecules and study of transmission pathway for JFH couplings using Car-Parrinello molecular dynamics
Grantee:Patrick Rodrigues Batista
Support Opportunities: Scholarships in Brazil - Post-Doctoral
FAPESP's process: 18/07308-4 - Effect of solvent on shielding tensor and coupling constant calculations of platinum (iii) dinuclear complexes via ab initio molecular dynamics
Grantee:Patrick Rodrigues Batista
Support Opportunities: Scholarships in Brazil - Doctorate
FAPESP's process: 22/12004-0 - Ab Initio Investigation of the Solvent and Different Ligands on the 195Pt NMR Properties in Pt(III) Dinuclear Complexes
Grantee:Pedro Paulo Rezende Oliveira
Support Opportunities: Scholarships in Brazil - Master