CAREER: NEXT GENERATION THEORY TO PREDICT & CONTROL POLARON FORMATION & TRANSPORT

About This Grant

Andrés Montoya-Castillo of the University of Colorado Boulder is supported by an award from the Chemical Theory, Models and Computational Methods program in the Division of Chemistry to develop accurate and efficient theories to predict and control light-induced currents and reactivity in materials that can convert sunlight into electricity and chemical fuels. While scientific advances over the last decade have enabled researchers to quantify these currents and reactivity, understanding these experiments and predicting how to control and optimize this energy conversion process remains a fundamental challenge – one rooted in the difficulty of describing the quantum mechanical motion of atoms and electrical charges. To address this problem, Montoya-Castillo and his team will develop methods to describe these quantum mechanical processes with unprecedented accuracy and atomistic detail and over experimentally relevant material dimensions and times, and apply them to elucidate and optimize promising light-energy conversion materials. Montoya-Castillo and his team will offer his developments as open-source software for the community to advance their own research on similar problems. These developments should have transformative impact in renewable energy, photocatalysis, and emerging quantum materials. In addition, Montoya-Castillo will develop and offer portable and easily deployable college-level teaching tools that emphasize testable models, observation, and computation to offer students transferable skills needed to advance, thrive, and contribute to modern job market while minimizing their math anxiety and promoting a growth mindset. Transition metal oxides are cheap and promising photocatalysts, except for their low charge mobilities and high recombination rates. These properties are consequences of the material deformation an electronic excitation causes, i.e., polaron formation. While recent microscopies can now track polaron formation and transport, and electronic structure theory can characterize their structure, their quantum dynamics remains a mystery, preventing a full understanding of polaron formation, flow, and reactivity. To address this challenge, Montoya-Castillo and his group will develop scalable and accurate dynamical theories that can employ ab initio energies and forces to probe experimentally relevant sizes and times and interrogate recent experiments on photocatalytically promising Fe2O3 and TiO2. These advances will reveal how to control polaron formation and transport mechanisms via chemical changes to the underlying material, and offer a robust and flexible theoretical framework for related problems involving the dissipative quantum dynamics of many-body systems. Montoya-Castillo will develop and release software to enable researchers in chemistry, materials science, and condensed matter physics to complement their transport research. Further, Montoya-Castillo will develop physical chemistry labs that are easily deployable at primarily undergraduate to research-intensive institutions, unite theory, experiment, and computation to offer students transferable skills needed in the modern STEM-focused job market, and reduce math anxiety via a gradual build-up of skills in a low-stress environment that fosters a growth mindset. This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.