Accelerating the Design of Multishell Upconverting Nanoparticles through Bayesian Optimization.

The photon upconverting properties of lanthanide-doped nanoparticles drive their applications in imaging, optoelectronics, and additive manufacturing. To maximize their brightness, these upconverting nanoparticles (UCNPs) are often synthesized as core/shell heterostructures. However, the large numbers of compositional and structural parameters in multishell heterostructures make optimizing optical properties challenging. Here, we demonstrate the use of Bayesian optimization (BO) to learn the structure and design rules for multishell UCNPs with bright ultraviolet and violet emission. We leverage an automated workflow that iteratively recommends candidate UCNP structures and then simulates their emission spectra using kinetic Monte Carlo. Yb 3+ /Er 3+ - and Yb 3+ /Er 3+ /Tm 3+ -codoped UCNP nanostructures optimized with this BO workflow achieve 10- and 110-fold brighter emission within 22 and 40 iterations, respectively. This workflow can be expanded to structures with higher compositional and structural complexity, accelerating the discovery of novel UCNPs while domain-specific knowledge is being developed.