Review Reports - Performance Enhancement and Stability Improvement in Perovskite Solar Cells via Interface Functionalization

Round 1

Reviewer 1 Report

This review is timely and well-organized by the authors from two aspects of interfaces in perovskite solar cells. Thus, I recommend publication of this review after addressing the revision/commends as followed:

1. Typos should be revised. For example, “works” should be revised to “works” at line 353.

2. The latest certified PCE of perovskite solar cells is 26%. This is suggested to be updated.

3. The spelling of “Spiro-OMeTAD” is wrong in figures and text of this review. The author should carefully check the spelling of this abbreviation.

4. In figure 3, “MAPBI₃” should be revised to “MAPbI₃”.

5. These two papers might fit the topic of this manuscript.

In situ growth of graphene on both sides of a Cu-Ni alloy electrode for perovskite solar cells with improved stability

DOI: 10.1038/s41560-022-01038-1

Stabilizing heterostructures of soft perovskite semiconductors

DOI: 10.1126/science.aax8018

Typos should be revised.

Author Response

Reply: We thank the reviewer for his/her positive opinion about our manuscript. All the changes made in text have been highlighted in yellow color in the revised version of the manuscript. Besides, we thank the reviewer for his/her valuable comments which helped us overall to improve the quality of our manuscript.

1. Typos should be revised. For example, “works” should be revised to “works” at line 353.

Reply: We thank the reviewer for the careful consideration of our work. The word is corrected to the text.

2. The latest certified PCE of perovskite solar cells is 26%. This is suggested to be updated.

Reply: We thank the reviewer for his/her constructive remark. The efficiency is corrected both in abstract and the introduction section.

3. The spelling of “Spiro-OMeTAD” is wrong in figures and text of this review. The author should carefully check the spelling of this abbreviation.

Reply: We thank the reviewer for his/her constructive remark. The spelling of “Spiro-OMeTAD” is now corrected in the text and in the Figures (namely: Figures 2, 3, 4, 6, 7, 8, 10 and 11 are now corrected).

4. In figure 3, “MAPBI3” should be revised to “MAPbI3”.

Reply: We thank the reviewer for the careful consideration of our work. The word is corrected to the text.

5. These two papers might fit the topic of this manuscript.

-In situ growth of graphene on both sides of a Cu-Ni alloy electrode for perovskite solar cells with improved stability DOI: 10.1038/s41560-022-01038-1

-Stabilizing heterostructures of soft perovskite semiconductors DOI: 10.1126/science.aax8018

Reply: Indeed, after a thorough consideration of suggested literature, the suggested papers were analyzed and incorporated in the manuscript: in the corresponding section elaborating the stabilizing role of graphene. (After Figure 6, page 8, first paragraph)

Comments on the Quality of English Language

Typos should be revised.

Reply: We thank the reviewer for the careful consideration of our work. Typos were thoroughly checked and corrected in the entire document

Reviewer 2 Report

Interface functionalization is of great importance for the development of efficient and robust chalcogenide devices. The authors have reviewed the interface engineering through both ETL/Perovskite and perovskite HTL, which is well laid out and has certain features. However, there are several aspects that need to be improved as follows.

1. The diagrams in the paper are so monotonous, either molecular formula or device structure, can there be more in-depth principle content? For example, why the use of this material can improve the interface quality.

2. When explaining the role of both ETL/Perovskite and perovskite HTL in the article, the authors seem to mention only the structure on the left side of Figure 1. The ETL/Perovskite and perovskite HTL aspects in the structure on the right of Figure 2 should also be mentioned.

3. Why graphene-based nanomaterials can solve the challenges of stability, scalability and flexibility that limit the industrial applications of PSC.

4. The interface functionalization realized through perovskite dimension (3D/0D, 3D/1D, 3D/2D), is mentioned in the paper. Figure 7 can depict the schematic diagram of 3D/0D, 3D/1D, 3D/2D. Wouldn't it be better to use 3D/1D as an example to illustrate this structure?

5. Statistical analysis and machine learning (ML) is very important, but there is basically no systematic description of statistical analysis and machine learning (ML) in your text, and it is very abrupt to suddenly propose these lines (456-464). If the author thinks this is important, at least 1-2 paragraphs of content to give examples of statistical analysis and machine learning (ML) is important.

6. In line 353, ‘works’ is written wrongly.

can express in English very clearly

Author Response

Comments and Suggestions for Authors

The diagrams in the paper are so monotonous, either molecular formula or device structure, can there be more in-depth principle content? For example, why the use of this material can improve the interface quality.

Reply: We thank the reviewer for his/her constructive remark. Indeed, the diagrams include formulas and/or device architecture and the selected configuration will permit the journal audience to perform a direct comparison of the main modifications and corresponding interface engineering strategies, without the need to make any additional (duplicate) description in the text. In the revised version of the manuscript an effort has also been made to add details concerning the role of the functional materials.

When explaining the role of both ETL/Perovskite and perovskite HTL in the article, the authors seem to mention only the structure on the left side of Figure 1. The ETL/Perovskite and perovskite HTL aspects in the structure on the right of Figure 2 should also be mentioned.

Reply: We thank the reviewer for his/her constructive remark. The corresponding description was improved and includes the features (ITO glass substrate, ETL, HTM, evaporated metal) of the inverted structure (page 2, first paragraph, lines 3-4)

Why graphene-based nanomaterials can solve the challenges of stability, scalability and flexibility that limit the industrial applications of PSC.

Reply: We thank the reviewer for his/her constructive remark. Graphene-based materials present excellent optoelectronic properties and a number of oxygen functionalities that make them ideal candidates for industrially compatible interface engineering applications. The oxygen functional groups can strongly interact with the cell components (especially forming strong bonds with the perovskite and HTM), passivating structural defects and fine tuning the interface energetics. This becomes more evident in the revised manuscript including the analysis of two additional works elaborating the use of graphene nanomaterials in robust and highly efficient PSCs (page 7).

The interface functionalization realized through perovskite dimension (3D/0D, 3D/1D, 3D/2D), is mentioned in the paper. Figure 7 can depict the schematic diagram of 3D/0D, 3D/1D, 3D/2D. Wouldn't it be better to use 3D/1D as an example to illustrate this structure?

Reply: We thank the reviewer for his/her constructive remark. We totally agree with the reviewer and his/her observation was incorporated into the manuscript. In addition, the caption of Figure 7 was modified to include interface engineering employing 3D/0D and 3D/2D structures.

Statistical analysis and machine learning (ML) is very important, but there is basically no systematic description of statistical analysis and machine learning (ML) in your text, and it is very abrupt to suddenly propose these lines (456-464). If the author thinks this is important, at least 1-2 paragraphs of content to give examples of statistical analysis and machine learning (ML) is important.

Reply: We thank the reviewer for his/her constructive remark. A recent study further elaborating the dye-modification approach by using machine learning and symbolic regression methods was added, to better highlights the importance and high potential of ML platforms to accelerate the design of functional interfaces enabling the development of efficient and robust devices and their long-term operation in extreme environmental conditions (pages 11-12).

In line 353, ‘works’ is written wrongly.

Reply: We thank the reviewer for the careful consideration of our work. The word is corrected to the text.

Reviewer 3 Report

Please see teh attached file

Comments for author File: Comments.pdf

Please see the attached file

Author Response

This paper reports the interface modification effects on the enhancement of the photovoltaic (PV) performance of perovskite solar cells (PSCs). The paper is suitable for publication in the journal “Electronics” subject to some major revisions. Following are comments in detail:

The interface modification effects on the enhancement of the photovoltaic (PV) performance of “inverted” PSCs should be included in the article.

Reply: We thank the reviewer for his/her constructive remark. A number of additional works on inverted device architectures was analyzed and included in the manuscript (pages 1-3, page 11)

There are many functionalized polymers have been reported as the interfacial modifier of PSCs. However, only a few polymer materials as interfacial modifier of PSCs was discussed in the article. This issue should be further discussed.

Reply: We thank the reviewer for his/her constructive remark. As suggested, the issue of functional polymers was further discussed in the manuscript, including the addition of three papers (two in section 2 –inverted PSCs and one as additives in conventional architecture).

The following literature regarding the interfacial modifier of PSCs were suggested to be cited as the references in the article: (1) J. Phys. Chem. C 2019, 123, 23826; (2) Applied Surface Science 548 (2021) 149276; (3) Polymers, 2023, 15, 437.

Reply: We thank the reviewer for his/her remark. The suggested papers were thoroughly analyzed and reported in the revised manuscript.

Round 2

Reviewer 2 Report

Articles can be accepted by modifying the following problems.

1.There's a problem with the syntax.（page 7，lines 263-264）

2.The first paragraph needs a blank line. (page 8, lines 300-306)

Grammar and syntax should be revised.

Author Response

Articles can be accepted by modifying the following problems.

Reply: We thank the reviewer for his/her positive opinion about our manuscript. All the changes made in text have been highlighted in yellow color in the revised version of the manuscript.

There's a problem with the syntax.（page 7，lines 263-264）

Reply: We thank the reviewer for the careful consideration of our work and we totally agree with his/her remark. The last sentence of the paragraph is rephrased.

The first paragraph needs a blank line. (page 8, lines 300-306)

Reply: We thank the reviewer for the careful consideration of our work and we totally agree with his/her remark. We put extra space in the beginning of the specific paragraph.

Reviewer 3 Report

The authors have revised their manuscript according to the referee’s comments. Therefore, the paper can be accepted in present form.

Dear Editor:

The authors have revised their manuscript according to the referee’s comments. Therefore, the paper can be accepted in present form.

Author Response

Reply: We thank the reviewer for his/her positive opinion about our manuscript. All the changes (grammatical errors, etc.) made in text have been highlighted in yellow color in the revised version of the manuscript.