Data for: Stereoregular radical polymers enable selective spin transfer - computational studies (Data S1 and S2) and crystal structure of M1

Spintronics offers a promising avenue for surpassing the performance and energy efficiency limits of conventional electronic devices. However, existing spintronic materials, including metals and doped conjugated polymers, face intrinsic stability and performance challenges. To address these limitations, we employed computational methods to investigate the electronic structure, spin transport properties, and crystallographic order of a stereoregular radical polymer. Computational simulations in different stereoregularities were utilized to model spin-spin interactions, charge delocalization, and long-range order within the polymer backbone. Crystallographic data analysis provided insights into the molecular packing of the monomer (M1) and the role of stereochemistry in controlling spin alignment. Our findings highlight how stereoselective polymerization enables persistent radicals in each repeat unit to support long-range spin transport without conventional doping. This computationally g..., Three trimers were analyzed using the Conformer-Rotamer Ensemble Sampling Tool (CREST) and GFN2-xTB semi-empirical potential. The trimers corresponded to the heterotactic (m,r), syndiotactic (r,r), and isotactic (m,m) triads that map to the atactic, syndiotactic, and atactic polymerization scenarios. The universal force field (UFF) in the OpenBabel quantum chemistry file conversion package was used to generate an initial optimized geometry from stereochemically-specific SMILES strings for each triad, which was then optimized using xTB before being subjected to conformational sampling via CREST using the most comprehensive default setting. The initial geometries and outputted conformers were analyzed to ensure no incorrect bond rearrangements or intramolecular radical dimerization had occurred. Separation and alignment analysis was performed on all conformations. Each triad has two pairs of nearest neighbors (i.e., the first and second radicals, and the second and third radicals) wh..., , # Data for: Stereoregular radical polymers enable selective spin transfer - computational studies (Data S1 and S2) and crystal structure of M1

[https://doi.org/10.5061/dryad.44j0zpcr2](https://doi.org/10.5061/dryad.44j0zpcr2)

## Description of the data and file structure

Computational results (Data S1 and S2) and crystal data of M1.

1. .p files are binary files formatted using the pickle module, a built-in Python package. These files are optimized for efficient data storage and can be readily accessed using the pickle module. When loaded, they are automatically interpreted as Python dictionaries, providing a structured and convenient means of storing and retrieving data.
2. **The raw .p files** given correspond to each trimer conformer ensemble tacticity analyzed during the computational section of the results.  They provide the raw data used to determine Boltzmann distributions of radical chain alignment (as defined by the dot product) and radical separation.  Dictionary headings a...,