A quadratic-scaling algorithm with guaranteed convergence for quantum coupled-channel calculations

Abstract

Rigorous quantum dynamics calculations provide essential insights into complex scattering phenomena across atomic and molecular physics, chemical reaction dynamics, and astrochemistry. However, the application of the gold-standard quantum coupled-channel (CC) method has been fundamentally constrained by a steep cubic scaling of computational cost $[O(N^3)]$. Here, we develop a general, rigorous, and robust method for solving the time-independent Schrödinger equation for a single column of the scattering S-matrix with quadratic scaling $[O(N^2)]$ in the number of channels. The Weinberg-regularized Iterative Series Expansion (WISE) algorithm resolves the divergence issues affecting iterative techniques by applying a regularization procedure to the kernel of the multichannel Lippmann-Schwinger integral equation. The method also explicitly incorporates closed-channel effects, including those responsible for multichannel Feshbach resonances. We demonstrate the power of this approach by performing rigorous calculations on He + CO and CO + N${}_2$ collisions, achieving exact quantum results with quadratic scaling guaranteed by a contour-integral construction. Our results establish a highly scalable computational paradigm, enabling state-to-state quantum scattering computations for complex molecular systems.

44 pages, 9 figures

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