The authors studied the nucleation of lithium on different surface of lithium metal facets via DFT. The aim is to understand origin of lithium dendrites and promote potential dendrite-inhibiting strategies. The topic is very important among the field. The manuscript can be published if the authors can address the following issues:

(1) section of "Li nucleation on defective surfaces", authors consider electrolyte reduction products (SEI) are defective sites for Li deposition. This is an interesting view. Moreover, authors should note that Li metal foil is inherently covered by a layer of native passivation layer (NPL) even prior to be in contact with electrolyte. And the NPL is rather supplier-dependent [suggested reference in this regard Energy Storage Materials, 2025, 76, 104160.]. Authors ought to add these statements in this section to highlight the inherent defective nature of lithium metal anode.

1. The entire study focuses on the early stage Li-clusters formation on varying Li facets. Although all the simulation results point to the inherent preferential adsorption in local spots that explain the propensity of dendritic and non-uniform Li growth pattern. However, beyond the nucleation stage, the energy barrier of Li migration on vary substrates is another factor, the faster migration of Li adatoms can "flatten out" the Li-deposits even if protrusions already formed. If the authors can provide the migration pathways and corresponding energy barrier of Li-atom diffusion along Li(100) and Li(110) surface, the work will be much more convincing.

2. The conclusion part of the paper reveals that dendrite heterogeneous Li deposition on Li metal is inherent and inevitable. However, recently, Li deposition onto varying Li-alloy substrates is emerging fast as effective means to develop dendrite-free lithium metal batteries [e.g., Acta Materialia, 2025, 299, 121405.; Chemical Engineering Journal, 2023, 466, 143084. ]. Authors can discuss these Li vs. Li-alloy interactions and how it can impact Li-deposition heterogeneity referencing these prior studies. This can shed lights on further development of the field: can we avoid using pure Li metal for future LMBs development?

This paper can be published as is.

Alloy-mediated crystallization is indeed an emerging area.