Exciton-Assisted UV Stimulated Emission with Incoherent Feedback in Polydisperse Crystalline ZnO Powder

Round 1

Reviewer 1 Report

Referee Report

on paper “ Exciton-Assisted UV Stimulated Emission with Incoherent Feedback in Polydisperse Crystalline ZnO Powder “ (coatings-1914081) by authors Leonid Fedorenko, Volodymyr Litovchenko, Vadym Naumov, Dmytro Korbutyak, Volodymyr Yukhymchuk, Olexander Gudymenko, Olexander Dubikovskyi, Hidenori Mimura and Arturs Medvids submitted to Coatings

 

This is interesting paper. It reports a comparative analysis of the features of UV- stimulated emission (SE) of various types of disorder active materials based on ZnO crystallites for a random laser (RL). The superlinear increase in the intensity of the UV photoluminescence (PL) band of polydisperse nano-microcrystalline (PNMC) ZnO powder at a wavelength of λ = 387 nm and some narrowing of its half-width in the range of 20-15 nm with increasing pump intensity were established that indicates a random lasing with incoherent feedback (FB). Properties of similar UV PL bands under the same conditions from a thin film containing hexagonal ZnO microdisks, as well as samples of monodisperse ZnO nanopowder indicate stimulated emission with coherent feedback. It is shown that, among the studied materials, the PNMC ZnO powder with crystallites contained nano-grains with is the most suitable for creating a laser with incoherent feedback at room temperature. The average optical gain coefficient α_g at λ = 387 nm in this RL system is estimated, as αg ~ 150 cm-1. The presented expermental results are reliable without any doubts. However, I have some comments and additions. I would like to note a few points to improve the paper before it can be published:

1.    I fully agree with the authors that different oxides have great technology importance: “One good example of such material became a medium based on ZnO crystallites with extremely high exciton bond energy E_ex excitons (~ 60 meV) [8], in which were obtained both coherent [9] as well as incoherent feedback of UV SE, [5] in the microlasers.”. I understood very well the choice of study object. This is the zinc oxide based composite materials which have excellent electronic properties. However, different oxides exist are also promising for practical applications. It is necessary to give in 1. Introduction information about such oxides:

(1). S.V. Trukhanov, A.V. Trukhanov, V.A. Turchenko, An.V. Trukhanov, D.I. Tishkevich, E.L. Trukhanova, T.I. Zubar, D.V. Karpinsky, V.G. Kostishyn, L.V. Panina, D.A. Vinnik, S.A. Gudkova, E.A. Trofimov, P. Thakur, A. Thakur, Y. Yang, Magnetic and dipole moments in indium doped barium hexaferrites, J. Magn. Magn. Mater. 457 (2018) 83-96. https://doi.org/10.1016/j.jmmm.2018.02.078.

2.    The authors should supplement 2. Materials and Methods information on various methods for obtaining thin films:

(2). S.A. Sharko, A.I. Serokurova, N.N. Novitskii, V.A. Ketsko, M.N. Smirnova, A.H. Almuqrin, M.I. Sayyed, S.V. Trukhanov, A.V. Trukhanov, A new approach to the formation of nanosized gold and beryllium films by ion-beam sputtering deposition, Nanomaterials 12 (2022) 470. https://doi.org/10.3390/nano12030470.

3.    The authors should elucidate in more details in 3. Results and Discussion the state of the oxygen stoichiometry of the obtained samples, since it is well known that complex oxides of transition metals can often experience an excess or deficiency of oxygen anions:

(3). S.V. Trukhanov, A.V. Trukhanov, A.N. Vasil'ev, A. Maignan, H. Szymczak, Critical behavior of La_0.825Sr_0.175MnO_2.912 anion-deficient manganite in the magnetic phase transition region, J. Exp. Theor. Phys. Lett. 85 (2007) 507-512. https://doi.org/10.1134/S0021364007100086.

4.    The proposed 3 papers should be inserted in References.

 

The paper should be sent to me for the second analysis after the moderate revisions.

Comments for author File: Comments.pdf

Author Response

 

Comments and Suggestions for Authors

Referee Report

on paper “ Exciton-Assisted UV Stimulated Emission with Incoherent Feedback in Polydisperse Crystalline ZnO Powder “ (coatings-1914081) by authors Leonid Fedorenko, Volodymyr Litovchenko, Vadym Naumov, Dmytro Korbutyak, Volodymyr Yukhymchuk, Olexander Gudymenko, Olexander Dubikovskyi, Hidenori Mimura and Arturs Medvids submitted to Coatings

This is interesting paper. It reports a comparative analysis of the features of UV- stimulated emission (SE) of various types of disorder active materials based on ZnO crystallites for a random laser (RL). The superlinear increase in the intensity of the UV photoluminescence (PL) band of polydisperse nano-microcrystalline (PNMC) ZnO powder at a wavelength of λ = 387 nm and some narrowing of its half-width in the range of 20-15 nm with increasing pump intensity were established that indicates a random lasing with incoherent feedback (FB). Properties of similar UV PL bands under the same conditions from a thin film containing hexagonal ZnO microdisks, as well as samples of monodisperse ZnO nanopowder indicate stimulated emission with coherent feedback. It is shown that, among the studied materials, the PNMC ZnO powder with crystallites contained nano-grains with is the most suitable for creating a laser with incoherent feedback at room temperature. The average optical gain coefficient αg at λ = 387 nm in this RL system is estimated, as αg ~ 150 cm-1. The presented expermental results are reliable without any doubts. However, I have some comments and additions. I would like to note a few points to improve the paper before it can be published:

1. I fully agree with the authors that different oxides have great technology importance: “One good example of such material became a medium based on ZnO crystallites with extremely high exciton bond energy Eex excitons (~ 60 meV) [8], in which were obtained both coherent [9] as well as incoherent feedback of UV SE, [5] in the microlasers.”. I understood very well the choice of study object. This is the zinc oxide based composite materials which have excellent electronic properties. However, different oxides exist are also promising for practical applications. It is necessary to give in 1. Introduction information about such oxides:

(1). S.V. Trukhanov, A.V. Trukhanov, V.A. Turchenko, An.V. Trukhanov, D.I. Tishkevich, E.L. Trukhanova, T.I. Zubar, D.V. Karpinsky, V.G. Kostishyn, L.V. Panina, D.A. Vinnik, S.A. Gudkova, E.A. Trofimov, P. Thakur, A. Thakur, Y. Yang, Magnetic and dipole moments in indium doped barium hexaferrites, J. Magn. Magn. Mater. 457 (2018) 83-96. https://doi.org/10.1016/j.jmmm.2018.02.078.

2. The authors should supplement 2. Materials and Methods information on various methods for obtaining thin films:

(2). S.A. Sharko, A.I. Serokurova, N.N. Novitskii, V.A. Ketsko, M.N. Smirnova, A.H. Almuqrin, M.I. Sayyed, S.V. Trukhanov, A.V. Trukhanov, A new approach to the formation of nanosized gold and beryllium films by ion-beam sputtering deposition, Nanomaterials 12 (2022) 470. https://doi.org/10.3390/nano12030470.

 

Dear reviewer 1,

thank you for your proposal to introduce the references:

1. S.V. Trukhanov, A.V. Trukhanov, V.A. Turchenko, An.V. Trukhanov, D.I. Tishkevich, E.L. Trukhanova, T.I. Zubar, D.V. Karpinsky, V.G. Kostishyn, L.V. Panina, D.A. Vinnik, S.A. Gudkova, E.A. Trofimov, P. Thakur, A. Thakur, Y. Yang, Magnetic and dipole moments in indium ed in details barium hexaferrites, J. Magn. Magn. Mater. 457 (2018) 83-96. https://doi.org/10.1016/j.jmmm.2018.02.078.
2. S.A. Sharko, A.I. Serokurova, N.N. Novitskii, V.A. Ketsko, M.N. Smirnova, A.H. Almuqrin, M.I. Sayyed, S.V. Trukhanov, A.V. Trukhanov, A new approach to the formation of nanosized gold and beryllium films by ion-beam sputtering deposition, Nanomaterials 12 (2022) 470. https://doi.org/10.3390/nano12030470

After reading the articles that you suggested to be included in the reference list in our article, it turns out that it is about very interesting and important knowledge about magnetic and dipole moments in indium-doped barium hexaferrites, which is far from the topic of our topic. manuscript. Our manuscript does not claim to be an extensive review of CnO applications. In addition, our paper does not consider the production process of disordered material based on ZnO crystals (powder and film), as this information was discussed in previous publications indicated in the reference list. Therefore, we found no reason to include the first two references in our manuscript.

 

3. The authors should elucidate in more details in 3. Results and Discussion the state of the oxygen stoichiometry of the obtained samples, since it is well known that complex oxides of transition metals can often experience an excess or deficiency of oxygen anions:

(3). Trukhanov, S.V.; Trukhanov, A.V.; Vasil'ev, A.N.; Maignan, A.; Szymczak, H. Critical behavior of La0.825Sr0.175MnO2.912 anion-deficient manganite in the magnetic phase transition region, J. Exp. Theor. Phys. Lett. 2007, 85, 507-512. https://doi.org/10.1134/S0021364007100086.

This paper (3) was introduced to the reference list as N [24] with some according text in the line 10page 4 in the paragraph 1.

  The paper should be sent to me for the second analysis after the moderate revisions.

peer-review-22357328.v2.pdf

Submission Date

29 August 2022

Date of this review

05 Sep 2022 11:12:56

Author Response File: Author Response.docx

Reviewer 2 Report

Referee reports on paper coatings-1914081

 

In my opinion this paper may be published in Coatings. However, some additions are needed:

1.      The authors should mention the certain zinc oxide based composites efficient for practical application:

(i). R.G.M. Oliveira, D.C. Souza, J.E.V. de Morais, G.S. Batista, M.A.S. Silva, D.X. Gouveia,·S. Trukhanov, A. Trukhanov, L. Panina, C. Singh, D. Zhou, A.S.B. Sombra, High thermal stability of RF dielectric properties of BiVO₄ matrix with added ZnO, J. Mater. Sci.: Mater. Electron. 31 (2020) 13078–13087. https://doi.org/10.1007/s10854-020-03858-x.

(ii). M.A. Almessiere, S. Güner, Y. Slimani, M. Hassan, A. Baykal, M.A. Gondal, U. Baig, S.V. Trukhanov, A.V. Trukhanov, Structural and magnetic properties of Co_0.5Ni_0.5Ga_0.01Gd_0.01Fe_1.98O₄/ZnFe₂O₄ spinel ferrite nanocomposites: Comparative study between sol-gel and pulsed laser ablation in liquid approaches, Nanomaterials 11 (2021) 2461. https://doi.org/10.3390/nano11092461.

(iii). R.G.M. Oliveira, J.E.V. de Morais, D.C. Souza, M.A.S. Silva, D.X. Gouveia, S. Trukhanov, A. Trukhanov, L. Panina, C. Singh, D. Zhou, A.S.B. Sombra, High-bandwidth microwave dielectric resonator antennas from BiVO₄/ZnO composites, J. Austr. Cer. Soc. 57 (2021) 369-377. https://doi.org/10.1007/s41779-020-00559-w.

2.      All the 3 proposed citation should be taken into account in the literature.

 

I suggest the moderate revision. I need post-corrected viewing and evaluation. My final verdict will be after completing the required additions.

Comments for author File: Comments.pdf

Author Response

Referee reports on paper coatings-1914081

 In my opinion this paper may be published in Coatings. However, some additions are needed:

1. The authors should mention the certain zinc oxide based composites efficient for practical application:

(i). R.G.M. Oliveira, D.C. Souza, J.E.V. de Morais, G.S. Batista, M.A.S. Silva, D.X. Gouveia,·S. Trukhanov, A. Trukhanov, L. Panina, C. Singh, D. Zhou, A.S.B. Sombra, High thermal stability of RF dielectric properties of BiVO₄ matrix with added ZnO, J. Mater. Sci.: Mater. Electron. 31 (2020) 13078–13087. https://doi.org/10.1007/s10854-020-03858-x.

(ii). M.A. Almessiere, S. Güner, Y. Slimani, M. Hassan, A. Baykal, M.A. Gondal, U. Baig, S.V. Trukhanov, A.V. Trukhanov, Structural and magnetic properties of Co_0.5Ni_0.5Ga_0.01Gd_0.01Fe_1.98O₄/ZnFe₂O₄ spinel ferrite nanocomposites: Comparative study between sol-gel and pulsed laser ablation in liquid approaches, Nanomaterials 11 (2021) 2461. https://doi.org/10.3390/nano11092461.

(iii). R.G.M. Oliveira, J.E.V. de Morais, D.C. Souza, M.A.S. Silva, D.X. Gouveia, S. Trukhanov, A. Trukhanov, L. Panina, C. Singh, D. Zhou, A.S.B. Sombra, High-bandwidth microwave dielectric resonator antennas from BiVO₄/ZnO composites, J. Austr. Cer. Soc. 57 (2021) 369-377. https://doi.org/10.1007/s41779-020-00559-w.

2. All the 3 proposed citation should be taken into account in the literature.

I suggest the moderate revision. I need post-corrected viewing and evaluation. My final verdict will be after completing the required additions.

 Dear Reviewer 2, thanks for your kind proposal. We did not find areas of overlap with the topics and issues addressed in our manuscript sufficient to refer to the above 3 articles, unfortunately, but we have inserted 1 reference to the article of the group of authors you recommended to us.

peer-review-22357667.v2.pdf

Submission Date

29 August 2022

Date of this review

05 Sep 2022 11:19:13

 

Reviewer 3 Report

 The manuscript entitled “Exciton-Assisted UV Stimulated Emission with Incoherent 2 Feedback in Polydisperse Crystalline ZnO Powder”. It’s very interesting on A comparative analysis of the features of UV- stimulated emission (SE) of various types 15 of disorder active materials based on ZnO crystallites for a random laser (RL). The manuscript could be suitable published after the authors are correction for the following points:

1. Abstract is very well only needs included some of optimum result numbers.

2. There are a good introduction but need expansion the last paragraph and focusing on novelty this work.

3.Figure 1 is unimportant, please removed.

4.Write sequential references [ 1,2,3….. ] into []1-5] along manuscript.

5. The authors have excellent discussion of the results; needs add reference agreements with previous research.

6. All equations along the manuscript needs references, except in the case of this empirical equation and researcher concluded from the practical results

7. Providing high-resolution some figures (not less than 300dpi).

8.re-write conclusions as paragraphs not numbers.

9- Arrangement the manuscript &references according to journal template exactly.

10-Update references into 2021.

11-The language of the article has to be slightly revised. There are some grammar, spelling, and punctuation mistakes.

Author Response

Comments and Suggestions for Authors

 The manuscript entitled “Exciton-Assisted UV Stimulated Emission with Incoherent 2 Feedback in Polydisperse Crystalline ZnO Powder”. It’s very interesting on A comparative analysis of the features of UV- stimulated emission (SE) of various types 15 of disorder active materials based on ZnO crystallites for a random laser (RL). The manuscript could be suitable published after the authors are correction for the following points:

Dear reviewer 3, thanks for your notes.  Replay is below.

 

1. Abstract is very well only needs included some of optimum result numbers.

Abstract was fulfilled by the next additions words:

There was:

The properties of similar UV PL bands under the same conditions of a thin film containing hexagonal ZnO microdisks, as well as samples of monodisperse ZnO nanopowder, indicate stimulated radiation with coherent feedback. It is shown that, among the studied materials, PNMC ZnO powder is the most suitable for creating a random laser with incoherent feedback at room temperature.

It became:

The properties of similar UV PL bands under the same conditions of a thin film containing hexagonal ZnO microdiscs, as well as samples of monodisperse ZnO nanopowder with nanoparticles size of 100 nm, indicate stimulated radiation with coherent feedback. It is shown that, among the studied materials, PNMC ZnO powder with widely dispersed crystallites ranging in size from 50 nm to a few microns, which in turn consist of nanograins with dimensions of ~ 25 nm, is the most suitable for creating a random laser with incoherent feedback at room temperature.

 

2. There are a good introduction but need expansion the last paragraph and focusing on novelty this work.

 

The following sentence was added to the text to the introduction:

 

In addition, the influence of the size dispersion of crystallites in disordered photonic media (in particular, ZnO) on the type of feedback of SE is also insufficiently studied.

3. Figure 1 is unimportant, please removed.

Agree, Figure 1 is removed

4. Write sequential references [ 1,2,3….. ] into []1-5] along manuscript.

 It's done

5. The authors have excellent discussion of the results; needs add reference agreements with previous research.

In our text, reference is made to our work [12] for conceptual considerations regarding the possible influence of interfaces and surfaces of nanocrystallites on photoluminescence efficiency. There are also references [20, 26] to previous works on the stimulated emission of ZnO thin films consisting of hexagonal microcrystals. Our earlier experimental studies of ZnO crystals concerned laser modification (irreversible structural rearrangement) in the solid phase, that is, from a slightly different direction [L. Fedorenko, A. Medvids. Optical Excitation of the Surface Plasmon-Polariton Resonance in Zn Nanoparticles Formed by Laser Radiation in ZnO Crystal. VІI VII Ukrainian scientific conference on semiconductor physics: abstracts of reports, Ukraine, Dnepropetrovsk, 26-30 September, 2016]. We jointed to the researches of ZnO crystallites as photonic elements of the disordered media in the random laser relative recently.

6.  All equations along the manuscript needs references, except in the case of this empirical equation and researcher concluded from the practical results

It's done

7. Providing high-resolution some figures (not less than 300 dpi)

 It's done

8. re-write conclusions as paragraphs not numbers.

It's done

9-  Arrangement the manuscript & references according to journal template exactly.

10 - Update references into 2021.

It's done by reference [10]

 

The development of the principles of RL made it possible to develop the system of eliminating or suppress all artifacts caused by the speckles by fine-tuning the spatial coherence of illumination [10].

 

11-The language of the article has to be slightly revised. There are some grammar, spelling, and punctuation mistakes.

 

It's done

 

Submission Date

29 August 2022

Date of this review

Round 2

Reviewer 1 Report

Referee Report

on paper “ Exciton-Assisted UV Stimulated Emission with Incoherent Feedback in Polydisperse Crystalline ZnO Powder “ (coatings-1914081-v2) by authors Leonid Fedorenko, Volodymyr Litovchenko, Vadym Naumov, Dmytro Korbutyak, Volodymyr Yukhymchuk, Olexander Gudymenko, Olexander Dubikovskyi, Hidenori Mimura and Arturs Medvids submitted to Coatings

 

This paper has been well corrected and it should be published.

Comments for author File: Comments.doc

Reviewer 3 Report

no comments