Toward High-Performances of Halide Light-Emitting Diodes: The Importance of Ligands Engineering

Round 1

Reviewer 1 Report

The manuscript entitled “Toward high-performances of halide light-emitting diodes: The importance of ligands engineering” by Le Ma et al. is a Perspective on the ligand engineering method for CsPbBr₃-based light-emitting diodes. The authors properly classified key points into three categories, and the reviewer agrees that this classification will be helpful to the researchers studying perovskite optoelectronics with ligand engineering. Therefore, the reviewer recommends the publication of this manuscript after some minor corrections for the authors.

 

1.          In the introduction part of line 27, authors must state the full names of the MA and FA. In line 67, external quantum efficiency should be abbreviated as EQE.

2.          Authors should closely check the manuscript to avoid typos and mistakes. In line 112 of the Figure 3 caption, superscripts should be checked, and gamma was omitted in the full name of GABA in line 136.

3.          In the blue emission of LED part, the authors explained low-dimensional perovskites and their application in LEDs. The reviewer recommends the additional citation of a related paper regarding blue PeLEDs [Materials 2022, 15(13), 4571; https://doi.org/10.3390/ma15134571] published by MDPI. The citation will help readers to further understand blue-emissive perovskite LEDs.

 

4.          In the section on the Stabilities of materials and devices, the authors mentioned the higher material stability of CsPbBr₃ than organic cation-based perovskites. However, the authors did not suggest numerical supporting data of photostability for the material stability issue such as PL intensity change or storage lifetime. Therefore, the simple mention of detailed photostability data will be good for readers to understand the higher material stability of CsPbBr₃ than organic cation-base perovskites.

Authors should closely check the manuscript to avoid typos and mistakes.

Author Response

Response to recommendations and criticisms:

 

According to the Referees’ comments, we revised the manuscript. We hope that we have now produced a more balanced and better account for our work. We would like to resubmit our revised manuscript to Inorganics for publication.

We have studied the Referees comments carefully and made major revision of our manuscript as follows.

 

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Reply to the comments of the First Referee

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The manuscript entitled “Toward high-performances of halide light-emitting diodes: The importance of ligands engineering” by Le Ma et al. is a Perspective on the ligand engineering method for CsPbBr₃-based light-emitting diodes. The authors properly classified key points into three categories, and the reviewer agrees that this classification will be helpful to the researchers studying perovskite optoelectronics with ligand engineering. Therefore, the reviewer recommends the publication of this manuscript after some minor corrections for the authors.

 

According to the First Referee comments, we made corrections and revisions. We would like to thank you for your helpful comments. Replies to the listed questions and comments are below.

 

1. In the introduction part of line 27, authors must state the full names of the MA and FA. In line 67, external quantum efficiency should be abbreviated as EQE.

We thank you for your appropriate and helpful comments. We have checked the part you mentioned and revised the MA and FA by their full names.

2. Authors should closely check the manuscript to avoid typos and mistakes. In line 112 of the Figure 3 caption, superscripts should be checked, and gamma was omitted in the full name of GABA in line 136.

Thank you for your helping to check manuscript carefully, we really apologize for such wrong spelling and mistakes. We have revised the part as your kindly mentioned. Thank you very much!

3. In the blue emission of LED part, the authors explained low-dimensional perovskites and their application in LEDs. The reviewer recommends the additional citation of a related paper regarding blue PeLEDs [Materials 2022, 15(13), 4571; https://doi.org/10.3390/ma15134571] published by MDPI. The citation will help readers to further understand blue-emissive perovskite LEDs.

Thank you for great suggesting and we have added the paper as a reference.

4. In the section on the Stabilities of materials and devices, the authors mentioned the higher material stability of CsPbBr₃ than organic cation-based perovskites. However, the authors did not suggest numerical supporting data of photostability for the material stability issue such as PL intensity change or storage lifetime. Therefore, the simple mention of detailed photostability data will be good for readers to understand the higher material stability of CsPbBr₃ than organic cation-base perovskites.

We have further presented the photostability data at the stability parts according referee comments, and thank you for great advices.

 

5. Authors should closely check the manuscript to avoid typos and mistakes.

We further checked the manuscript and revised the manuscript with tracks. Really thank you for kindly and carefully checking.

 

According to the helpful Referees comments and due to the addition of more detailed discussions, we hope that we have now produced better account for our works. We would like to express appreciation to the Referees for suggesting how best to improve our paper. We hope that our manuscript will be accepted for publication in Inorganics with the revisions.

 

Sincerely,

 

Feijiu Wang

Reviewer 2 Report

The authors have reported the perspective on ligands engineering halide perovskite-based light-emitting diodes. Especially, this draft summarizes the efficiency of LEDs, quantum confinement, and stability enhancement by the addition of various ligands on bromide-based perovskites and gives some perspective on it. In general, this is an interesting collection and outlook in this field of research. The manuscript is well written. I recommend its publication in Inorganics after improving the following details.  

1.      The authors have mentioned in the manuscript the enhancement of stability by the addition of ligands on the perovskites, I would suggest adding the reasons by referring to some related papers.

2.       On page 4, the statement by the author “Cl vacancies, easily formed in perovskites because of their low formation energy”. I am not convinced by that statement. Please add some evidence/calculations.

3.      The authors are suggested to make the font in each figure identical and readable.

4.      The authors are suggested to follow some important ligands-controlled halide perovskites papers: J. Phys. Chem. C 2018, 122, 26, 15041–15046; Nanoscale Adv., 2019,1, 1791-1798

 

5.      Overall, the manuscript is well written. However, there are some typos or jumbled sentences that should be corrected. For example, the caption of Figure 1: “Evolution of EQEs of green-LEDs employed CsPbBr₃ emitting layer. performance”. Also, the last sentence of the perspective and summary section, and so on.

Needs minor improvement

Author Response

Response to recommendations and criticisms:

 

According to the Referees’ comments, we revised the manuscript. We hope that we have now produced a more balanced and better account for our work. We would like to resubmit our revised manuscript to Inorganics for publication.

We have studied the Referees comments carefully and made major revision of our manuscript as follows.

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Reply to the comments of the Second Referee

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The authors have reported the perspective on ligands engineering halide perovskite-based light-emitting diodes. Especially, this draft summarizes the efficiency of LEDs, quantum confinement, and stability enhancement by the addition of various ligands on bromide-based perovskites and gives some perspective on it. In general, this is an interesting collection and outlook in this field of research. The manuscript is well written. I recommend its publication in Inorganics after improving the following details.

According to the Second Referee comments, we made corrections and revisions. We would like to thank you for your helpful comments. Replies to the listed questions and comments are below.

1. The authors have mentioned in the manuscript the enhancement of stability by the addition of ligands on the perovskites, I would suggest adding the reasons by referring to some related papers.

We added the reasons in the section of “Stabilities of materials and devices” and thank you for good comments.

2. On page 4, the statement by the author “Cl vacancies, easily formed in perovskites because of their low formation energy”. I am not convinced by that statement. Please add some evidence/calculations.

We thank you for the good comments, the “Cl vacancies, easily formed in perovskites because of their low formation energy” is come from the reference [Bi, C.et al., Perovskite Quantum Dots with Ultralow Trap Density by Acid Etching-Driven Ligand Exchange for High Luminance and Stable Pure-Blue Light-Emitting Diodes. Adv. Mater. 2021, 33, 2006722–2006730, doi:10.1002/adma.202006722.]. But recently, we did not find the theoretically calculation or explanation. In avoid misunderstanding, we changed the sentence as follows:’In addition, Cl vacancies in mixed halide perovskites easily create relatively deeper defect level in the bandgap, which could capture the carriers and increase the nonradiative recombination[73]. Moreover, the defects, which act as hoping sites to induce the halide ion migration and result the perovskite more vulnerable under operational conditions, have also been reported [74]. Compared to Cl vacancies in CsPbBr_xCl_3-x, the CsPbBr₃ exhibits great “defect-tolerant” nature, which could reduce the related nonradiative recombination[75].’

 We really thank you for the academic discussion.

3. The authors are suggested to make the font in each figure identical and readable.

Thank you for great suggestion, we change the font in each figure for better identification.

4. The authors are suggested to follow some important ligands-controlled halide perovskites papers: J. Phys. Chem. C 2018, 122, 26, 15041–15046; Nanoscale Adv., 2019,1, 1791-1798

  We have cited the paper as you mentioned and thank you for good comments.

5. Overall, the manuscript is well written. However, there are some typos or jumbled sentences that should be corrected. For example, the caption of Figure 1: “Evolution of EQEs of green-LEDs employed CsPbBr₃ emitting layer. performance”. Also, the last sentence of the perspective and summary section, and so on.

  We really thank referee great contributions on the manuscript checking. The part you mentioned have been revised. Also, we have revised the manuscript with carefully reading and understanding. Thank you again.

 

According to the helpful Referees comments and due to the addition of more detailed discussions, we hope that we have now produced better account for our works. We would like to express appreciation to the Referees for suggesting how best to improve our paper. We hope that our manuscript will be accepted for publication in Inorganics with the revisions.

 

Sincerely,

 

Feijiu Wang

Round 2

Reviewer 2 Report

This version of the manuscript is not necessary for further review.