All Paths All at Once: A Quantum Monte Carlo and Neural Committor Approach to Reaction Pathway Search
Year: 2026
Type: preprint
Abstract: Locating competing reaction pathways is difficult when potential-energy gradients are unavailable. Here we present tReax_expedition, an energy-only approach combining coupled Monte Carlo exploration, stochastic quench labelling and restrained continuation. Exploration identifies connected states, while continuation resolves candidate channels and records sampled chain maxima. Single-search benchmarks on three two-dimensional potentials recovered an intermediate and competing routes without transition-state guesses. For eight of nine gas-phase reactions on GFN2-xTB, sampled chain maxima differed from independently refined saddle energies by less than 0.76 kJ mol -1 . Alanine dipeptide instead revealed incomplete conformational relaxation, showing that route connectivity can persist despite structural and energetic errors. Neural committor learning and local straddling-pair sampling connect the resulting paths to transition-region sampling, although molecular shooting diagnostics indicate limited committor calibration. These results show how energy-only exploration and continuation recover candidate pathways, while distinguishing route connectivity from geometric localization, barrier resolution and finite-temperature transition statistics.
Source: Research Square
Author: Chien-Chai Chang
Institution: National Tsing Hua University
Language: English
Subfield: Physical and Theoretical Chemistry
Field: Chemistry
Domain: Physical Sciences
Open Access status: green
OpenAlex ID: W7225055589