Reply to Reviewer #1’s Comments

Manuscript #EMID:1044e1894f49d457: Pinning and Depinning Dynamics of an

Evaporating Sessile Droplet Containing Mono- and Bidispersed Colloidal Particles on a
Nonheated/Heated Hydrophobic Substrate
Authors: Suryansh Gupta, Mahesh R. Thombare, Nagesh D. Patil

The authors thank the reviewer for the valuable comments, suggestions and giving us an
opportunity to revise our work. We have worked towards incorporating all the comments.
The comments are copied below in italic and followed by our responses. The modifications
in the revised manuscript are marked in red color.

General Comments:
The authors studied the coupled effects of substrate heating, colloidal dispersion, and
particle size variation on the contact line pinning-depinning dynamics of evaporating
droplets containing mono- and bidispersed polystyrene colloidal particles. The work is
interesting and it may be publishable after the appropriate revision.
Response: We are thankful to the reviewer for finding our work interesting and for giving a
positive recommendation on the publication of this work. We have performed the required
modifications in the revised manuscript, by incorporating all the valuable comments/
suggestions put forth by the reviewer.

Specific Comments:
Comment 1: The introduction should be more concise for highlighting the motivation of
this work.
Response: Thank you for this suggestion/comment. Following the reviewer’s suggestion, we
have revised the introduction section to improve the overall conciseness in the revised
manuscript. (Please refer page no. 2 to 5)

Comment 2: Please give more information such as methods on measuring the advancing
and receding contact angles.
Response: We are sorry to the reviewer for not including the information regarding the
methods for the measurement of the advancing and receding contact angles. We used a tilting
plate method and measured the advancing and receding contact angles at the front and back
of the droplet, moving along the tilted surface, respectively; as done by Patil et al. [1]. Based
on the reviewer’s comment, we have included this information in the revised manuscript
under the section 2.1. (Please refer page no 7, lines 7-9)

Comment 3: Page 18, Line 23: Please specify the interfacial tension in “a decrease in the
interfacial tension”.
Response: We are sorry to the reviewer for the typographical mistake associated with the
description of the interfacial tension in the aforementioned line. We have corrected the
corresponding line in revised manuscript as follows.
“Incidentally, similar findings have also been reported in the previous studies, which also
attributed the cause of the prolonged CL pinning to a decrease in the liquid-gas interfacial
tension35. (Please refer page no 16, line 11)

Comment 4: Page24, Line 7: Please check “the corresponding pinning durations remained
20% and 25% respectively”.
Response: Thank you for bringing this to our attention, we have checked and corrected the
sentence in the revised manuscript. (Please refer page no 22, lines 2-4)

Comment 5: What is the initial contact angles of sessile droplets? If it is greater than 90
degrees, how can the difference in temperature between the apex and the contact line can be
obtained from the top view images? Moreover, the droplets have a spherical profile, so can
the temperature distribution be accurately obtained?
Response: We thank the reviewer for this insightful remark. Based on the contact angle
measurements for the 1.5 μL sessile droplets deposited on the PDMS substrate, the
equilibrium contact angle is found to be 109±4°. It is rightly pointed out by the reviewer that
since the initial contact angle is greater than 90°, the acquisition of the liquid-vapor
interfacial temperature closer to the contact line may be hindered due to the curvature effects.
However, note that in such type of study considering the size/volume of the droplet, the
relative discrepancy due to curvature effect in the measurement of liquid-gas interface
temperature values from the side view and top view was found to be in the order of ±1°C; as
observed in the findings by Josyula et al. [2]. In their study, the sessile droplet contact angle
was 113◦, which is in the same range as was observed in the present study.
Further, to address the reviewer’s comment on the measurement of the liquid-gas interface
temperature for the spherical profile, we would like to highlight that the focal length of the IR
camera (30 cm) is much larger than the field of view (or wetted diameter ~ 1.4 mm). Thus,
the maximum angle of view in the measurements is much less than 1°. Therefore, any
uncertainty in the temperature measurements due to spherical profile of droplet is almost zero
at very low values of the angle of view, as was also reported by Cheng et al. [3]. Further, it is
to be noted that the water is generally opaque to the infrared radiation, so the measured
temperature from the top view essentially corresponds to the liquid−gas interface temperature
[4].

Comment 6: Page 25, Line 44: Please check “… the contact line which will Marangoni
circulation”.
Response: Thank you for pointing this grammatical mistake. We have corrected the sentence
in the revised manuscript. (Please refer page no 23, line 23)

Comment 7: Why are colloidal particles with diameters of 3.0 um and 4.5 um choosed
rather than those with a larger difference in particle diameter?
Response: Thanks for commenting on it. We would like to clarify that the selection of the
particle combination was based on the findings obtained from the trial experiments in our lab
and the previous studies in the literature [4, 5]. Following the literature, we had performed
multiple experiments by considering different particle size combinations with particle sizes
0.5 µm, 1 µm, 3 µm, and 4.5 µm (as per the easy availability of these particle sizes at our
lab). Based on our experimental findings, it was observed that for the particle concentration
of 0.1% (w/v) (as used for the current study), the colloidal dispersion containing 3.0 µm and
4.5 µm particles showed substantial difference in the CL pinning-depinning dynamics at
different substrate temperatures and colloidal dispersion (mono- and bidispersed).
Subsequently, we tried to understand it through the theoretical model, and it was well
corroborated with the findings of experiments. In future, we would extend this study to
investigate the effect of different particle size combinations (involving greater as well as
smaller difference in the particle size) based on the valuable insights gained from the present
study. It has been planned to try the different particle size combinations by defining the
particle size ratio (R) for a given bidispersed suspensions, which can be defined as the ratio of
smaller size particle diameter to the larger size particle diameter.
Once again, we would like to thank the reviewer for dedicating his/her time and providing us
the valuable comments/suggestions. It has contributed significantly to increase the overall
quality and in bringing out an improved version of this manuscript.

References:
1. Patil, N. D.; Bhardwaj, R.; Sharma, A. Droplet Impact Dynamics on Micropillared
Hydrophobic Surfaces. Exp Therm Fluid Sci 2016, 74, 195–206.
2. Josyula, T., Wang, Z., Askounis, A., Orejon, D., Harish, S., Takata, Y., ... & Pattamatta,
A. (2018). Evaporation kinetics of pure water drops: Thermal patterns, Marangoni flow,
and interfacial temperature difference. Physical Review E, 98(5), 052804.
3. Cheng, T. Y., Deng, D., & Herman, C. (2012). Curvature Effect Quantification for In-
Vivo IR Thermography. International Mechanical Engineering Congress and Exposition
: [proceedings]. International Mechanical Engineering Congress and Exposition, 2,
10.1115/IMECE2012-88105.
4. Patil, N. D.; Bange, P. G.; Bhardwaj, R.; Sharma, A. Effects of Substrate Heating and
Wettability on Evaporation Dynamics and Deposition Patterns for a Sessile Water
Droplet Containing Colloidal Particles. Langmuir 2016, 32 (45), 11958–11972.
5. Malla, L. K.; Bhardwaj, R.; Neild, A. Colloidal Deposit of an Evaporating Sessile
Droplet on a Non-Uniformly Heated Substrate. Colloids Surf A Physicochem Eng Asp
2020, 584, 124009.