Peer review of: Evolution from unimolecular to colloidal-quantum-dot-like character in chlorine or zinc incorporate (2020)


RR2
REVIEWERS' COMMENTS:
Reviewer #1 (Remarks to the Author):
The manuscript appears to have been revised with great care and attention to the reviewer comments. I believe the work now merits publication.
Reviewer #3 (Remarks to the Author):
The authors have tried hard to “answer” the concerns and suggestions raised. Importantly, they need to “improve” their manuscript, based on the concerns and suggestions raised. Although some explanations or interpretations have been provided, the reviewer believes that the authors are able to push harder to do a better job, so that the study will have a bigger impact. In Discussion, the authors should better reflect what is actually known and unknown about these clusters and the implications. Also, the authors need to improve their English.
Before Reviewer 3 Comment 1, “The structural studies do not seem to be convincing.” The authors may address the reason in their revised manuscript why the cluster structures are difficult to identify at present (as partially indicated by The future of colloidal semiconductor magic-size clusters. ACS Nano 2020, 14, 1227–1235).
It is unclear to the reviewer “Our findings highlight the mechanistic insight that MSCs which appear before the growth to QDs transform by multi-step sequential conversions of MSCs or evolutions of MSCs.” Do they want to say “Our studies introduce the possible pathways, regarding the evolution of MSCs which may include multi-step sequential conversions among MSCs”?
Comment 1: the significant figure should be taken care of for the compositions. The authors should address “the composition-structure-property relationship between Cl-incorporated InP MSC-360 and Cl- incorporated InP MSC-399” in their revised version. In Discussion?
Comment 2: the significant figure should be taken care of for the compositions. On Page 12 of the point- by-point response file, the authors seem to write down a lot. The reviewer recommends that the authors should concisely summarize “the composition-structure-property relationship for Zn- incorporated InP MSC-360, Zn-incorporated InP MSC-408, and Zn-incorporated InP MSC-393” in their revised version. In Discussion?
Comment 3: On Page 14 of the response letter, for the response of reviewer 3, comment 3, the authors claimed that “When In(MA)3 were added into F393-InP : Zn MSCs at room temperature, the absorption peak red-shifted to 404 nm and the second transition disappeared (Figure R9a).”
Here is one example that the authors should carefully improve their English.

Any explanation for the disappearance of the second transition? Is it due to disappearance of the MSCs and the growth of QDs? On Page 15, Figure S8 was presented, showing a sharp absorption peak obtained for a 150 C sample. Why Figures R8 and R9 are presented, while the edited words on Page 15 mentioned Figures S6 and S7?
Again, for the present Figure R8 on Page 15, the two traces for the 110 and 180 C samples look similar. Comment 4: The authors should make a clear statement in their revised version “What is the nature of
the evolution? The authors claimed that the two clusters have different compositions”.
Comment 5: The authors should straightforwardly comprehend in their revised version “do they have different cores?”
Comment 6: The authors should provide an answer in their revised version “the composition-structure- property relationship for MA-capped InP MSC-386 (exhibiting one absorption singlet) and ODPA-capped InP MSC-397 (displaying one absorption doublet)?” For example, if the authors do not have an answer, that is fine. The authors may point out such a concern but without an answer, saying “we do not know why MA-capped .....” This is a kind reminder for to readers to think as well.
Comment 7: The authors edited in their revised manuscript “.....We speculate that these partially-etched 386-MA InP MSCs are 416-IS.” Do the author mean “due to more Cl incorporated”? The reviewer hopes that the authors is able to make their point more directly.
Comment 8: The authors should concisely explain in their revised version “why the experimental observation on “intermediates” is influenced by the temperatures?”
Comment 9: The authors should provide an answer in their revised version “any numbers can be assigned to x”
Comment 10: The authors should improve their revised version answering “ if y = 0, ...?”
Comment 11: The authors should improve their figure presentation. For example, 50 C can be the title of Part a, and does not need to be present for each trace. The four subfigures can be arranged in two panels (two top and two bottom), so do Figure 2.
Figure 8, what is the x axis for Part e? Shall the x axis title of Part f be italic, while the rest titles are not?
There is no need to use “F”, while keep “MSCs”. The author can use, for example, MSC-360 Cl : InP, for their main text and for their figures.