Quantum hardware calculations of the activation and dissociation of nitrogen on iron clusters and surfaces

Catalytic processes are the cornerstone of chemical industry, and catalytic conversion of nitrogen to ammonia remains one of the largest industrial processes implemented. Rational design of catalysts and catalytic reactions largely depends on approximate computational chemistry methods, such as density functional theory, which, however, suffer from limited accuracy, especially for strongly-correlated materials. Rigorous ab initio methods which account for static and dynamic electron correlation, while arbitrarily accurate for small systems, are generally too expensive to be applied to modelling of catalytic cycles, due to prohibitive time and space computational complexity with respect to the size of the active space. Recent advances in quantum computing give hope for enabling access to accurate ab initio methods at scale. Herein, we present a prototype hybrid quantum-classical workflow for modeling chemical reactions on surfaces, applied to proof-of-concept models of activation and dissociation of nitrogen on small Fe clusters and a single-layer (221) iron surface. First, we determined the structures of species present in the catalytic cycle at DFT level and studied their electronic structure using CASSCF. We show that it is possible to decouple the half-filled Fe-3d band from the Fe-N and N-N bond orbitals, thereby reducing the active space significantly. Subsequently, we translated the CASSCF wavefunctions into corresponding qubit quantum states, using the Adaptive Variational Quantum Eigensolver, and estimated their energies using a state vector simulator, H1-1E quantum emulator and (for selected systems) H1-1 quantum computer. We demonstrated that if a sufficiently small active orbital space is chosen, ground state energies obtained with classical methods and with the quantum computer are in reasonable agreement. We argue that once quantum computing methods are scaled up so that larger active spaces are accessible, they can offer a tremendous practical advantage to the computational catalysis community.