Globally Accurate Gaussian Process Potential Energy Surface and Quantum Dynamics Studies on the Li(2S) + Na2 → LiNa + Na Reaction at Low Collision Energies
Round 1
Reviewer 1 Report
The paper “Globally accurate Gaussian process potential energy surface and quantum dynamics studies on the Li(2S) + Na2 → LiNa + Na reaction at low collision energies” by Zijiang, Yang et. al. is well written and meet the standards of the Journal “Molecules” for publication. But, I have certain queries/ suggestions regarding this work:
1. Page-1, Line No. 153, “matrixes” should be “matrices”.
2. Page 3, Line 156 “……is enough large, limiting significantly the subsequent dynamics calculations.”---This sentence needs a change for better clarity.
Author Response
Dear Reviewer,
We appreciate your thoughtful comment earnestly and point out the critical English problem. We have checked the manuscript carefully and tried our best to correct the grammatical, spelling, and stylistic errors, and we hope that the correction will meet with approval. Once again, thank you very much for your comments.
Reviewer 2 Report
This paper demonstrated the construction of global potential energy surface of Li(Na)2 system using Gaussian Process regression approach and applied this surface to quantum dynamics simulation of the reaction. The computational approaches are carefully illustrated and the results are well presented. The constructed PES is of high-quality in both short-range and long-range regimes and enables quantum wavepacket dynamics calculations. More extensive quantum dynamics simulation could be conducted using this PES and provides important insights for the exciting field of ultracold reaction dynamics. Thus I would like to suggest the publication of this paper to Molecules
My additional minor comments are:
(1) On page 2, line 69, it should be "Feshbach resonance"
(2) On page 3, line 128, the authors should mention what are the permutaion invariant polynomials and how they are applied to the PES construction.
Author Response
Please see the attachment.
Author Response File: 
Author Response.pdf
Reviewer 3 Report
This paper presents a novel approach to constructing the first globally accurate ground-state LiNa2 potential energy surface (PES) using the Gaussian process model, overcoming previous challenges in ultracold chemical reaction studies. The authors achieve a high-precision and generalizable PES using 1776 high-level ab initio training points calculated with the icMRCI +Q method. They perform quantum dynamics calculations on the Li(2S) + Na2(v = 0, j = 0) → LiNa + Na reaction using the improved time-dependent wave packet (TDWP) method.
The improved grid-based TDWP method overcomes the limitations of both time-independent close coupling (TICC) and conventional TDWP methods, effectively addressing the challenges of large de Broglie wavelengths in ultracold scattering. The authors accurately calculate the adiabatic and non-adiabatic dynamics of triatomic reactive systems, demonstrating the reaction is dominated by a complex-forming mechanism with LiNa molecules favouring low-vibrational and high-rotational states.
The paper is well-structured, and the methodology is sound, providing a significant contribution to the field of ultracold chemical reactions. The results build upon the work by Son et al. ("Control of reactive collisions by quantum interference", PMID: 35239387, DOI: 10.1126/science.abl7257), advancing the understanding of ultracold chemical reactions and offering valuable insights for future experimental research and theoretical explorations in this area.
Author Response
Dear Reviewer,
We sincerely thank you for thoroughly examining our manuscript and providing very good comments on our work. These comments are very valuable and have an important guiding significance to our research. In the further study, we will perform further dynamics study on this reactive system based on the newly constructed potential energy surface in this paper. Once again, thank you very much for your thoughtful comment sincerely.
