Concept, absolute calibration and validation of a new, bench-top laser imaging polar nephelometer

Moallemi, Alireza; Modini, Robin Lewis; Brem, Benjamin Tobias; Bertozzi, Barbara; Giaccari, Philippe; Gysel-Beer, Martin

doi:https://doi.org/10.5194/egusphere-2023-392

Preprints

https://doi.org/10.5194/egusphere-2023-392

Preprints

15 Mar 2023

| 15 Mar 2023

Concept, absolute calibration and validation of a new, bench-top laser imaging polar nephelometer

Alireza Moallemi, Robin Lewis Modini, Benjamin Tobias Brem, Barbara Bertozzi, Philippe Giaccari, and Martin Gysel-Beer

Abstract. Polar nephelometers provide in situ measurements of aerosol angular light scattering and play an essential role in validating numerically calculated phase functions or inversion algorithms used in space-borne and land-based aerosol remote sensing. In this study, we present a prototype of a new polar nephelometer called uNeph. The instrument is designed to measure the phase function, F₁₁, and polarized phase function, –F₁₂/F₁₁ over the scattering range of around 5° to 175° with an angular resolution of 1° at a wavelength of 532 nm. In this work, we present details of the data processing procedures and instrument calibration approaches. The uNeph was validated in a laboratory setting using mono-disperse polystyrene latex (PSL) and Di-Ethyl-Hexyl-Sebacate (DEHS) aerosol particles over a variety of sizes, ranging from 200 nm to 800 nm. An error model was developed and the level of agreement between uNeph measurements and Mie theory was found to be consistent within the uncertainties of the measurements and the uncertainties of the input parameters for the theoretical calculations. The estimated measurement errors were between 5 % to 10 % (relative) for F₁₁ and smaller than ~0.1 (absolute) for –F₁₂/F₁₁. Additionally, by applying the Generalized Retrieval of Aerosol and Surface Properties (GRASP) inversion algorithm to the measurements conducted with broad unimodal DEHS aerosol particles, the volume concentration, size distribution and refractive index of the ensemble of aerosol particles were accurately retrieved. This paper demonstrates that the uNeph prototype can be used to conduct accurate measurements of aerosol phase function and polarized phase function and to retrieve aerosol properties through inversion algorithms.

Received: 13 Mar 2023 – Discussion started: 15 Mar 2023

Download & links

Preprint (PDF, 4606 KB)

Notice on discussion status
The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.
Preprint (4606 KB)

Supplement (8094 KB)

Download & links

The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.

Journal article(s) based on this preprint

08 Aug 2023

Concept, absolute calibration, and validation of a new benchtop laser imaging polar nephelometer

Alireza Moallemi, Robin L. Modini, Benjamin T. Brem, Barbara Bertozzi, Philippe Giaccari, and Martin Gysel-Beer

Atmos. Meas. Tech., 16, 3653–3678, https://doi.org/10.5194/amt-16-3653-2023,https://doi.org/10.5194/amt-16-3653-2023, 2023

Short summary

Alireza Moallemi et al.

Interactive discussion

Status: closed

RC1:
'Comment on egusphere-2023-392', Anonymous Referee #1, 28 Mar 2023
General:
This manuscript presents a newly developed polar nephelometer for aerosol phase function characterisation, along with comprehensive calibration discussion and quantitative error analysis. While other groups have demonstrated polar nephelometry with similar configurations, the novelty of this instrument is its reduced size. The authors provide an extremely detailed and rigorous discussion of the data analysis, including the main sources of uncertainty in the data inversion procedures. The performance of the nephelometer and predicted errors are demonstrated via laboratory experiments using monodisperse and unimodally distributed non-absorbing aerosol with known optical properties. While it would have been interesting to see an exploration of more novel materials or more significant instrumentation developments, the strength of this manuscript is in the thorough analysis. I especially appreciate all the detail discussed in the appendix and shown in Supplementary figures. As such, it is a valuable and excellent piece of research that is highly recommended for publication in AMT after a few minor revisions.

Specific comments:
L95: One of the novel features of the uNeph, compared to other polar nephelometers, is its relatively small size. It would be worth reiterating this advantage elsewhere, e.g. the conclusion section.
L97-109: Details on the optical system are scant. It would be useful to provide more details on:
Type of laser and operating mode (i.e. pulsed or cw)

Whether beam was collimated and estimated beam size within the measurement chamber

Range of optical densities for ND filters used

Type of photodetector

L111: Based on Figure 1, it would appear that the camera lens forms part of the chamber seal, and the rooftop reflector is outside a window – is that correct?
L117-121: Can you clarify the dimensions of the region of interest within the camera pixel array that was used, and whether pixels were binned at all? Despite the large pixel array indicated in Section 2.1, Figure S3 indicates a much smaller array.
L120: More details about the objective (lens) would be helpful, e.g. camera position relative to the focal length, the field-of-view…
L162-164: Depending on the CPC mode used, this would imply that the aerosol flow to the uNeph was around 3.5 or 4.7 L min^-1 – can you clarify what you estimate the volume flow in the uNeph to be (and hence the estimated residence time).
L485; L721-22: I believe the N limit in the summations over i indices refers to the number of angles – is that correct? It’s unclear whether this is incremented by pixel angle or by absolute angle. How does the angular resolution of measurements vary across the full range of measurement?
L592: It would appear that the V_tot predicted by the retrieval systematically overestimate the volume when compared to the SMPS measurement. Could this be because the measured size distribution (Figure 8) appears by eye to deviate from an ideal lognormal distribution?
L618-619: It would be interesting and useful to test your calibration and data processing procedures for absorbing spherical particles in the future.
L797: This seems like a very conservative (i.e. erring on the side of large uncertainty) way of quantifying this error. No corrections needed, just an observation!
Table 1: Please clarify whether “q25” and “q75” refer to the 25^th and 75^th percentile quantile points, or other values.
Figure 2: No image appears in the manuscript
Figure 5: It is unclear the purpose for showing the line depicting “3% of uNeph air measurement” in the lefthand panels
Figure 6: Check units on stated number concentrations in caption
Figure 8: The information presented in (b,c) plots might be more clearly depicted in a table

General comments on Figures 6, 7, S2, S4, S8, S9, S11, S12, S13, S14, S15, S16, and S17 : The font size in the axes labels, legends, and/or schematics is far too small.
Citation: https://doi.org/10.5194/egusphere-2023-392-RC1
- AC1: 'Replies to RC1 and RC2', Martin Gysel-Beer, 30 May 2023
  
  Please find our responses to Reviewer 1 and 2 in the attachment.
  
  Citation: https://doi.org/10.5194/egusphere-2023-392-AC1
RC2:
'Comment on egusphere-2023-392', Reed Espinosa, 18 Apr 2023

The manuscript provides a detailed explanation of a new imaging nephelometer called μNeph. Data processing methods are described, followed by validation of the measurements with monodisperse and monomodal polydisperse test aerosols and then finally an example of the potential to perform retrievals of particle size and concentration using μNeph data. The demonstrated accuracy of the μNeph is impressive, especially considering its small size, and I expect it to contribute significantly to our ability to measure aerosol phase matrix elements. Additionally, some aspects of the described data reduction procedure represent advancements over prior approaches, like the use of a monatomic gas (e.g., argon) to characterize the stokes vector of the incoming laser light source. The manuscript is clear and well written making it a very useful resource for future users of μNeph data and other imaging nephelometer efforts. I can thus confidently recommend publication, after the following minor points have been addressed.

SPECIFIC COMMENTS
LN 30: I think this should read "...aerosols makes them difficult to..."
LN 36: It should just be "radiance" here, not "irradiance".
LN 71: It may be good to also cite the very well known Amsterdam–Granada polar nephelometer that is capable of measuring all phase matrix elements (e.g., Muñoz et al. 2012).
LN 95: Would the authors be able to elaborate on potential uses that they envision for the instrument outside of the laboratory (e.g., perhaps onboard a UAV)? The small size of the instrument seems like it would be advantageous for many such applications.
LN 116: Perhaps this would be clearer as greater/less than symbols (e.g., "0≤θ≤90°") to avoid confusion with the minus operator.
LN 117: Presuming the laser beams fill most of the length of the image, this CCD resolution would imply a raw measurement resolution of closer to 0.1°. Are multiple beam cross section integrals averaged to obtain the coarser 1° resolution? Also, how was 1° selected as the final resolution?
LN 118: I assume "A/D" stands for "analog-to-digital" but it still may be good to define the abbreviation explicitly.
LN 121: Please specify the diameter of the pinhole used to image the lasers.
LN 127: It would be helpful to state exactly where the Thorlabs PAX polarimeter was placed in the optical path. Is it possible to place it in the measurement chamber? If so, why are q1 and q2 not known exactly, but instead later solved for using argon measurements? Perhaps this is due to the lack of exact knowledge of the camera's pinhole in the Thorlabs polarimeter's coordinate system? Please elaborate.
LN 180: Apologies if I missed it, but how frequently are dark images obtained? Are these coefficients updated during a given measurement?
LN 194: It would be helpful to replace "several" with the exact number of pinhead positions.
LN 234: While some referencing of supplement figures in the main text in passing is certainly fine, here and in several other places (e.g. LN 258, LN 329, LN 390, LN 499, etc.), a figure from the supplement is described in very significant detail. In these cases where whole sentences or paragraphs are devoted to supplement figures I would suggest either moving that text to the supplement, or the figure into the main text.
LN 240: Are these Ξ limits fixed or a function of scattering angle?
LN 240: Will the value of Ξ at which saturation occurs be dependent on aerosol loading and dark current? The effect is probably small, but it seems that short exposures (low dark current) and high loading (high counts in center of last beam) would be more likely to saturate pixels at the center of the beam than a longer exposure with lower aerosol loading, even if both cases produced the same value of Ξ.
LN 282: Have the authors considered using a beam expander? This was considered for the PI-Neph of Dolgos and Martins (2014) in order to reduce the signal at each individual pixel, while also enlarging the sampled volume providing statistics for a larger number of particles in each image acquisition.
LN 287: Is the precision of the laser reference photodetector known? If so, it would be helpful to state it.
LN 328: Do the authors have any theories as to the primary drivers of the instrument calibration drift?
Eq 3: I'm wondering if something like F∥ and F⊥ would be clearer than F1 and F2, which are very easily confused with phase matrix elements. Although, perhaps the close connection (and same units) with phase matrix elements make the variable names appropriate.
LN 371: Is there a physical basis for the assumption |q1|=|q2|? (Or, more precisely, I think q1=-q2, right?) Are polarization artifacts expected to impact q1 and q2 identically in some way?
LN 384: Please clarify if 1.7% is the width of the PSL size distribution or uncertainty on the mean PSL diameter. If the former, was an uncertainty on mean diameter provided by the PSL manufacturer? If so, how much variation does that uncertainty translate to in terms of Mie calculated F11 and F12?
Sec 4.3: Would it be possible to further refine q, and characterize q1 and q2 separately, using the maxima and minima of the PSL measurements of F1 and F2?
Eq 4: Is instrument stray-light background implicitly included here or is it not considered in the error model?
LN 411: For consistency, maybe drop the squaring "2" on "σ^2_e,l" or add it to the other three variables.
Figure 5: I'm not see a section 3.5.3, as referenced in the caption. Please update to the correct section number.
LN 463: What was the reason the values 1.04 and 1.08 were assumed?
LN 493: This is the second time the blue lines are defined as best fits.
LN 534: Please explain how GRASP was tailored to produce the μNeph-GRASP Inversion. What changes were made relative to the standard build of GRASP? Also, for future work, it may be helpful to note that there was a high size parameter resolution version of the GRASP kernels developed to retrieve PSL properties in Espinosa et al. (2017). Those files are likely available by request from the GRASP team.
LN 549: I think "F11/F12" should be "F12/F11".

REFERENCES
Muñoz, O., Moreno, F., Guirado, D., Dabrowska, D. D., Volten, H., & Hovenier, J. W. (2012). The Amsterdam–Granada light scattering database. Journal of Quantitative Spectroscopy and Radiative Transfer, 113(7), 565-574.

Citation: https://doi.org/10.5194/egusphere-2023-392-RC2
- AC2: 'Replies to RC1 and RC2', Martin Gysel-Beer, 30 May 2023
  
  Please find our responses to Reviewer 1 and 2 in the attachment.
  
  Citation: https://doi.org/10.5194/egusphere-2023-392-AC2

Interactive discussion

Status: closed

RC1:
'Comment on egusphere-2023-392', Anonymous Referee #1, 28 Mar 2023
General:
This manuscript presents a newly developed polar nephelometer for aerosol phase function characterisation, along with comprehensive calibration discussion and quantitative error analysis. While other groups have demonstrated polar nephelometry with similar configurations, the novelty of this instrument is its reduced size. The authors provide an extremely detailed and rigorous discussion of the data analysis, including the main sources of uncertainty in the data inversion procedures. The performance of the nephelometer and predicted errors are demonstrated via laboratory experiments using monodisperse and unimodally distributed non-absorbing aerosol with known optical properties. While it would have been interesting to see an exploration of more novel materials or more significant instrumentation developments, the strength of this manuscript is in the thorough analysis. I especially appreciate all the detail discussed in the appendix and shown in Supplementary figures. As such, it is a valuable and excellent piece of research that is highly recommended for publication in AMT after a few minor revisions.

Specific comments:
L95: One of the novel features of the uNeph, compared to other polar nephelometers, is its relatively small size. It would be worth reiterating this advantage elsewhere, e.g. the conclusion section.
L97-109: Details on the optical system are scant. It would be useful to provide more details on:
Type of laser and operating mode (i.e. pulsed or cw)

Whether beam was collimated and estimated beam size within the measurement chamber

Range of optical densities for ND filters used

Type of photodetector

L111: Based on Figure 1, it would appear that the camera lens forms part of the chamber seal, and the rooftop reflector is outside a window – is that correct?
L117-121: Can you clarify the dimensions of the region of interest within the camera pixel array that was used, and whether pixels were binned at all? Despite the large pixel array indicated in Section 2.1, Figure S3 indicates a much smaller array.
L120: More details about the objective (lens) would be helpful, e.g. camera position relative to the focal length, the field-of-view…
L162-164: Depending on the CPC mode used, this would imply that the aerosol flow to the uNeph was around 3.5 or 4.7 L min^-1 – can you clarify what you estimate the volume flow in the uNeph to be (and hence the estimated residence time).
L485; L721-22: I believe the N limit in the summations over i indices refers to the number of angles – is that correct? It’s unclear whether this is incremented by pixel angle or by absolute angle. How does the angular resolution of measurements vary across the full range of measurement?
L592: It would appear that the V_tot predicted by the retrieval systematically overestimate the volume when compared to the SMPS measurement. Could this be because the measured size distribution (Figure 8) appears by eye to deviate from an ideal lognormal distribution?
L618-619: It would be interesting and useful to test your calibration and data processing procedures for absorbing spherical particles in the future.
L797: This seems like a very conservative (i.e. erring on the side of large uncertainty) way of quantifying this error. No corrections needed, just an observation!
Table 1: Please clarify whether “q25” and “q75” refer to the 25^th and 75^th percentile quantile points, or other values.
Figure 2: No image appears in the manuscript
Figure 5: It is unclear the purpose for showing the line depicting “3% of uNeph air measurement” in the lefthand panels
Figure 6: Check units on stated number concentrations in caption
Figure 8: The information presented in (b,c) plots might be more clearly depicted in a table

General comments on Figures 6, 7, S2, S4, S8, S9, S11, S12, S13, S14, S15, S16, and S17 : The font size in the axes labels, legends, and/or schematics is far too small.
Citation: https://doi.org/10.5194/egusphere-2023-392-RC1
- AC1: 'Replies to RC1 and RC2', Martin Gysel-Beer, 30 May 2023
  
  Please find our responses to Reviewer 1 and 2 in the attachment.
  
  Citation: https://doi.org/10.5194/egusphere-2023-392-AC1
RC2:
'Comment on egusphere-2023-392', Reed Espinosa, 18 Apr 2023

The manuscript provides a detailed explanation of a new imaging nephelometer called μNeph. Data processing methods are described, followed by validation of the measurements with monodisperse and monomodal polydisperse test aerosols and then finally an example of the potential to perform retrievals of particle size and concentration using μNeph data. The demonstrated accuracy of the μNeph is impressive, especially considering its small size, and I expect it to contribute significantly to our ability to measure aerosol phase matrix elements. Additionally, some aspects of the described data reduction procedure represent advancements over prior approaches, like the use of a monatomic gas (e.g., argon) to characterize the stokes vector of the incoming laser light source. The manuscript is clear and well written making it a very useful resource for future users of μNeph data and other imaging nephelometer efforts. I can thus confidently recommend publication, after the following minor points have been addressed.

SPECIFIC COMMENTS
LN 30: I think this should read "...aerosols makes them difficult to..."
LN 36: It should just be "radiance" here, not "irradiance".
LN 71: It may be good to also cite the very well known Amsterdam–Granada polar nephelometer that is capable of measuring all phase matrix elements (e.g., Muñoz et al. 2012).
LN 95: Would the authors be able to elaborate on potential uses that they envision for the instrument outside of the laboratory (e.g., perhaps onboard a UAV)? The small size of the instrument seems like it would be advantageous for many such applications.
LN 116: Perhaps this would be clearer as greater/less than symbols (e.g., "0≤θ≤90°") to avoid confusion with the minus operator.
LN 117: Presuming the laser beams fill most of the length of the image, this CCD resolution would imply a raw measurement resolution of closer to 0.1°. Are multiple beam cross section integrals averaged to obtain the coarser 1° resolution? Also, how was 1° selected as the final resolution?
LN 118: I assume "A/D" stands for "analog-to-digital" but it still may be good to define the abbreviation explicitly.
LN 121: Please specify the diameter of the pinhole used to image the lasers.
LN 127: It would be helpful to state exactly where the Thorlabs PAX polarimeter was placed in the optical path. Is it possible to place it in the measurement chamber? If so, why are q1 and q2 not known exactly, but instead later solved for using argon measurements? Perhaps this is due to the lack of exact knowledge of the camera's pinhole in the Thorlabs polarimeter's coordinate system? Please elaborate.
LN 180: Apologies if I missed it, but how frequently are dark images obtained? Are these coefficients updated during a given measurement?
LN 194: It would be helpful to replace "several" with the exact number of pinhead positions.
LN 234: While some referencing of supplement figures in the main text in passing is certainly fine, here and in several other places (e.g. LN 258, LN 329, LN 390, LN 499, etc.), a figure from the supplement is described in very significant detail. In these cases where whole sentences or paragraphs are devoted to supplement figures I would suggest either moving that text to the supplement, or the figure into the main text.
LN 240: Are these Ξ limits fixed or a function of scattering angle?
LN 240: Will the value of Ξ at which saturation occurs be dependent on aerosol loading and dark current? The effect is probably small, but it seems that short exposures (low dark current) and high loading (high counts in center of last beam) would be more likely to saturate pixels at the center of the beam than a longer exposure with lower aerosol loading, even if both cases produced the same value of Ξ.
LN 282: Have the authors considered using a beam expander? This was considered for the PI-Neph of Dolgos and Martins (2014) in order to reduce the signal at each individual pixel, while also enlarging the sampled volume providing statistics for a larger number of particles in each image acquisition.
LN 287: Is the precision of the laser reference photodetector known? If so, it would be helpful to state it.
LN 328: Do the authors have any theories as to the primary drivers of the instrument calibration drift?
Eq 3: I'm wondering if something like F∥ and F⊥ would be clearer than F1 and F2, which are very easily confused with phase matrix elements. Although, perhaps the close connection (and same units) with phase matrix elements make the variable names appropriate.
LN 371: Is there a physical basis for the assumption |q1|=|q2|? (Or, more precisely, I think q1=-q2, right?) Are polarization artifacts expected to impact q1 and q2 identically in some way?
LN 384: Please clarify if 1.7% is the width of the PSL size distribution or uncertainty on the mean PSL diameter. If the former, was an uncertainty on mean diameter provided by the PSL manufacturer? If so, how much variation does that uncertainty translate to in terms of Mie calculated F11 and F12?
Sec 4.3: Would it be possible to further refine q, and characterize q1 and q2 separately, using the maxima and minima of the PSL measurements of F1 and F2?
Eq 4: Is instrument stray-light background implicitly included here or is it not considered in the error model?
LN 411: For consistency, maybe drop the squaring "2" on "σ^2_e,l" or add it to the other three variables.
Figure 5: I'm not see a section 3.5.3, as referenced in the caption. Please update to the correct section number.
LN 463: What was the reason the values 1.04 and 1.08 were assumed?
LN 493: This is the second time the blue lines are defined as best fits.
LN 534: Please explain how GRASP was tailored to produce the μNeph-GRASP Inversion. What changes were made relative to the standard build of GRASP? Also, for future work, it may be helpful to note that there was a high size parameter resolution version of the GRASP kernels developed to retrieve PSL properties in Espinosa et al. (2017). Those files are likely available by request from the GRASP team.
LN 549: I think "F11/F12" should be "F12/F11".

REFERENCES
Muñoz, O., Moreno, F., Guirado, D., Dabrowska, D. D., Volten, H., & Hovenier, J. W. (2012). The Amsterdam–Granada light scattering database. Journal of Quantitative Spectroscopy and Radiative Transfer, 113(7), 565-574.

Citation: https://doi.org/10.5194/egusphere-2023-392-RC2
- AC2: 'Replies to RC1 and RC2', Martin Gysel-Beer, 30 May 2023
  
  Please find our responses to Reviewer 1 and 2 in the attachment.
  
  Citation: https://doi.org/10.5194/egusphere-2023-392-AC2

Peer review completion

AR: Author's response | RR: Referee report | ED: Editor decision | EF: Editorial file upload

AR by Martin Gysel-Beer on behalf of the Authors (19 Jun 2023) Author's response Author's tracked changes Manuscript

ED: Publish as is (21 Jun 2023) by Mingjin Tang

AR by Martin Gysel-Beer on behalf of the Authors (23 Jun 2023) Manuscript

Journal article(s) based on this preprint

08 Aug 2023

Concept, absolute calibration, and validation of a new benchtop laser imaging polar nephelometer

Alireza Moallemi, Robin L. Modini, Benjamin T. Brem, Barbara Bertozzi, Philippe Giaccari, and Martin Gysel-Beer

Atmos. Meas. Tech., 16, 3653–3678, https://doi.org/10.5194/amt-16-3653-2023,https://doi.org/10.5194/amt-16-3653-2023, 2023

Short summary

Alireza Moallemi et al.

Supplement

https://doi.org/10.5194/egusphere-2023-392-supplement

Model code and software

Platform for GRASP open source code Get public access to the code, documentation and user assistance GRASP-SAS https://www.grasp-sas.com/

miepython: a pure Python module to calculate light scattering by non-absorbing, partially-absorbing, or perfectly conducting spheres Scott Prahl https://github.com/scottprahl/miepython

Alireza Moallemi et al.

Viewed

Total article views: 334 (including HTML, PDF, and XML)

HTML	PDF	XML	Total	Supplement	BibTeX	EndNote
204	114	16	334	41	9	9

HTML: 204
PDF: 114
XML: 16
Total: 334
Supplement: 41
BibTeX: 9
EndNote: 9

Views and downloads (calculated since 15 Mar 2023)

Month	HTML	PDF	XML	Total
Mar 2023	99	44	7	150
Apr 2023	43	16	3	62
May 2023	22	10	0	32
Jun 2023	15	16	1	32
Jul 2023	22	22	5	49
Aug 2023	3	6	0	9

Cumulative views and downloads (calculated since 15 Mar 2023)

Month	HTML	PDF	XML	Total
Mar 2023	99	44	7	150
Apr 2023	43	16	3	62
May 2023	22	10	0	32
Jun 2023	15	16	1	32
Jul 2023	22	22	5	49
Aug 2023	3	6	0	9

Viewed (geographical distribution)

Total article views: 321 (including HTML, PDF, and XML) Thereof 321 with geography defined and 0 with unknown origin.

Country	#	Views	%

Latest update: 08 Aug 2023

Download

The requested preprint has a corresponding peer-reviewed final revised paper. You are encouraged to refer to the final revised version.

Preprint (4606 KB)
Metadata XML

Short summary

Polarimetric data, that is angular and polarization dependence of light scattering by an aerosol, contain ample information on its optical and microphysical properties. Retrieval of these properties is a central approach in aerosol remote sensing. We present a description, calibration, validation and a first application of a new benchtop polar nephelometer, which provides in situ polarimetric measurements of an aerosol. Such data facilitate closure between retrieval results and independent data.


Total:	0
HTML:	0
PDF:	0
XML:	0