Abstract

Following the recent development of a ground-based prototype quantum cascade laser heterodyne radiometer operating in the midinfrared, atmospheric ozone profile retrievals from a solar occultation measurement campaign performed at the Rutherford Appleton Laboratory on 21 September 2006 are presented. Retrieval is based on the optimal estimation method. High resolution (0.0073cm1) atmospheric spectra recorded by the laser heterodyne radiometer and covering a microwindow (1033.81034.5cm1) optimized for atmospheric ozone measurements were used as measurement vectors. As part of the evaluation of this novel instrument, a comprehensive analysis of the retrievals is presented, demonstrating the high potential of quantum cascade laser heterodyne radiometry for atmospheric sounding. Vertical resolutions of 2 km near the ground and about 3 km in the stratosphere were obtained. The information content of the retrieval was found to be up to 48 bits, which is much higher than any other passive ground-based instrument. Frequency mismatches of several absorption peaks between the forward model and experimental spectra have been observed and significantly contribute to the retrieval noise error in the upper-troposphere lower-stratosphere region. Retrieved ozone vertical profiles were compared to ozonesonde data recorded at similar latitudes. The agreement is generally excellent except for the 20 to 25 km peak in ozone concentration, where ozonesonde data were found to be 20% lower than the amount retrieved from the laser heterodyne radiometer spectra. Quantum cascade laser based heterodyne radiometry in the midinfrared has been demonstrated to provide high spectral resolution and unprecedented vertical resolution for a passive sounder in a highly compact and mechanically simple package.

© 2007 Optical Society of America

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  1. D. Weidmann, W. J. Reburn, and K. Smith, "Ground-based prototype quantum cascade laser heterodyne radiometer for atmospheric studies," Rev. Sci. Instrum. 78, 073107 (2007).
    [CrossRef] [PubMed]
  2. P. L. Kinney, "The pulmonary effects of ozone and particle air pollution," Sem. Respir. Crit. Care Med. 20, 601-607 (1999).
    [CrossRef]
  3. R. T. Menzies and R. K. Seals, "Ozone monitoring with an infrared heterodyne radiometer," Science 197, 1275-1277 (1977).
    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
  5. M. M. Abbas, T. Kostiuk, M. J. Mumma, D. Buhl, V. G. Kunde, and L. W. Brown, "Stratospheric ozone measurement with an infrared heterodyne spectrometer," Geophys. Res. Lett. 5, 317-320 (1978).
    [CrossRef]
  6. M. Taguchi, S. Okano, H. Fukunishi, and Y. Sasano, "Comparison of ozone profiles from ground-based laser heterodyne spectrometer and ozonesonde measurements," Geophys. Res. Lett. 17, 2349-2352 (1990).
    [CrossRef]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef]
  25. J. Staehelin and W. Schmid, "Trend analysis of the tropospheric ozone concentration utilizing the 20-years data set of the ozone balloon soundings over Payerne," Atmos. Environ. 25A, 1739-1749 (1991).
  26. X. Liu, K. Chance, C. E. Sioris, T. P. Kurosu, and M. J. Newchurch, "Intercomparison of GOME, ozonesonde, and SAGE II measurements of ozone: demonstration of the need to homogenize available ozonesonde data sets," J. Geophys. Res. 111, D14305, doi:10.1029/2005JD006718 (2006).
  27. "Total Ozone Mapping Spectrometer," http://jwocky.gsfc.nasa.gov/.

2007 (2)

2006 (5)

X. Liu, K. Chance, C. E. Sioris, T. P. Kurosu, and M. J. Newchurch, "Intercomparison of GOME, ozonesonde, and SAGE II measurements of ozone: demonstration of the need to homogenize available ozonesonde data sets," J. Geophys. Res. 111, D14305, doi:10.1029/2005JD006718 (2006).

X. Liu, K. Chance, C. E. Sioris, M. J. Newchurch, and T. P. Kurosu, "Tropospheric ozone profiles from a ground-based ultraviolet spectrometer: a new retrieval method," Appl. Opt. 45, 2352-2359 (2006).
[CrossRef] [PubMed]

K. Fast, T. Kostiuk, F. Espenak, J. Annen, D. Buhl, T. Hewagama, M. F. A'Hearn, D. Zipoy, T. A. Livengood, G. Sonnabend, and F. Smulling, "Ozone abundance on Mars from infrared heterodyne spectra. I. Acquisition, retrieval, and anticorrelation with water vapor," Icarus 181, 419-431 (2006).
[CrossRef]

Y. J. Meijer, D. P. J. Swart, F. Baier, P. K. Bhartia, G. E. Bodeker, S. Casadio, K. Chance, F. Del Frate, T. Erbertseder, M. D. Felder, L. E. Flynn, S. Godin-Beekmann, G. Hansen, O. P. Hasekamp, A. Kaifel, H. M. Kelder, B. J. Kerridge, J.-C. Lambert, J. Landgraf, B. Latter, X. Liu, I. S. McDermid, Y. Pachepsky, V. Rozanov, R. Siddans, S. Tellmann, R. J. van der A, R. F. van Oss, M. Weber, and C. Zehner, "Evaluation of Global Ozone Monitoring Experiment (GOME) ozone profiles from nine different algorithms," J. Geophys. Res. 111, D21306, doi:10.1029/2005JD006778 (2006).
[CrossRef]

A. J. Geer, W. A. Lahoz, S. Bekki, N. Bormann, Q. Errera, H. J. Eskes, D. Fonteyn, D. R. Jackson, M. N. Juckes, S. Massart, V.-H. Peuch, S. Rharmili, and A. Segers, "The ASSET intercomparison of ozone analyses: method and first results," Atmos. Chem. Phys. 6, 5445-5474 (2006).
[CrossRef]

2005 (5)

C. Brogniez, M. Houët, A. M. Siani, P. Weihs, M. Allaart, J. Lenoble, T. Cabot, A. de la Casinière, and E. Kyrö, "Ozone column retrieval from solar UV measurements at ground level: effects of clouds and results from six European sites," J. Geophys. Res. 110, D24202, doi:10.1029/2005JD005992 (2005).
[CrossRef]

P.-F. Coheur, B. Barret, S. Turquety, D. Hurtmans, J. Hadji-Lazaro, and C. Clerbaux, "Retrieval and characterization of ozone vertical profiles from a thermal infrared nadir sounder," J. Geophys. Res. 110, D24303, doi:10.1029/2005JD005845 (2005).
[CrossRef]

M. Palm, C. v. Savigny, T. Warneke, V. Velazco, J. Notholt, K. Künzi, J. Burrows, and O. Schrems, "Intercomparison of O3 profiles observed by SCIAMACHY and ground based microwave instruments," Atmos. Chem. Phys. 5, 2091-2098 (2005).
[CrossRef]

I. Petropavlovskikh, P. K. Bhartia, and J. DeLuisi, "New Umkehr ozone profile retrieval algorithm optimized for climatological studies," Geophys. Res. Lett. 32, L16808, doi:10.1029/2005GL023323 (2005).
[CrossRef]

L. S. Rothman, D. Jacquemart, A. Barbe, D. Chris Benner, M. Birk, L. R. Brown, M. R. Carleer, C. Chackerian, K. Chance, L. H. Coudert, V. Dana, V. M. Devi, J.-M, Flaud, R. R. Gamache, A. Goldman, J.-M. Hartmann, K. W. Jucks, A. G. Maki, J.-Y. Mandin, S. T. Massie, J. Orphal, A. Perrin, C. P. Rinsland, M. A. H. Smith, J. Tennyson, R. N. Tolchenov, R. A. Toth, J. Vander Auwera, P. Varanasi, and G. Wagner, "The HITRAN 2004 molecular spectroscopic database," J. Quanti. Spectrosc. Radiat. Transfer 96, 139-204 (2005).
[CrossRef]

2004 (2)

P. Keckhut, S. McDermid, D. Swart, T. McGee, S. Godin-Beekmann, A. Adriani, J. Barnes, J.-L. Baray, H. Bencherif, H. Claude, A. G. di Sarra, G. Fiocco, G. Hansen, A. Hauchecorne, T. Leblanc, C. H. Lee, S. Pal, G. Megie, H. Nakane, R. Neuber, W. Steinbrecht, and J. Thayer, "Review of ozone and temperature lidar validations performed within the framework of the Network for the Detection of Stratospheric Change," J. Environ. Monito. 6, 721-733 (2004).
[CrossRef]

K. E. Fast, T. Kostiuk, F. Espenak, T. A. Livengood, T. Hewagama, and M. F. A'Hearn, "Stratospheric ozone profiles from Mauna Kea, Hawai'i (19.8N, 155.5W) using infrared heterodyne spectroscopy, 1988-2003," Geophys. Res. Lett. 31, L08109, doi:10.1029/2004GL019443 (2004).
[CrossRef]

2002 (1)

B. Barret, M. De Maziere, and P. Demoulin, "Retrieval and characterization of ozone profiles from solar infrared spectra at the Jungfraujoch," J. Geophy. Res. 107, D24, 4788, doi:10.1029/2001JD001298 (2002).
[CrossRef]

1999 (2)

M. De Maziere, O. Hennen, and M. Van Roozendael, "Daily ozone vertical profile model built on geophysical grounds, for column retrieval from atmospheric high resolution infrared spectra," J. Geophys. Res. 104, D19, 23855-23869 (1999).
[CrossRef]

P. L. Kinney, "The pulmonary effects of ozone and particle air pollution," Sem. Respir. Crit. Care Med. 20, 601-607 (1999).
[CrossRef]

1995 (1)

M. Beekmann, G. Ancellet, D. Martin, C. Abonnel, G. Duverneuil, F. Eideliman, P. Bessemoulin, N. Fritz, and E. Gizard, "Intercomparison of tropospheric ozone profiles obtained by electrochemical sondes, a ground based lidar and an airborne UV-photometer," Atmos. Environ. 29, 1027-1042 (1995).
[CrossRef]

1991 (1)

J. Staehelin and W. Schmid, "Trend analysis of the tropospheric ozone concentration utilizing the 20-years data set of the ozone balloon soundings over Payerne," Atmos. Environ. 25A, 1739-1749 (1991).

1990 (1)

M. Taguchi, S. Okano, H. Fukunishi, and Y. Sasano, "Comparison of ozone profiles from ground-based laser heterodyne spectrometer and ozonesonde measurements," Geophys. Res. Lett. 17, 2349-2352 (1990).
[CrossRef]

1978 (1)

M. M. Abbas, T. Kostiuk, M. J. Mumma, D. Buhl, V. G. Kunde, and L. W. Brown, "Stratospheric ozone measurement with an infrared heterodyne spectrometer," Geophys. Res. Lett. 5, 317-320 (1978).
[CrossRef]

1977 (2)

R. T. Menzies and R. K. Seals, "Ozone monitoring with an infrared heterodyne radiometer," Science 197, 1275-1277 (1977).
[CrossRef] [PubMed]

M. A. Frerking and D. J. Muehler, "Infrared heterodyne spectroscopy of atmospheric ozone," Appl. Opt. 16, 526-528 (1977).
[CrossRef] [PubMed]

Appl. Opt. (3)

Atmos. Chem. Phys. (2)

M. Palm, C. v. Savigny, T. Warneke, V. Velazco, J. Notholt, K. Künzi, J. Burrows, and O. Schrems, "Intercomparison of O3 profiles observed by SCIAMACHY and ground based microwave instruments," Atmos. Chem. Phys. 5, 2091-2098 (2005).
[CrossRef]

A. J. Geer, W. A. Lahoz, S. Bekki, N. Bormann, Q. Errera, H. J. Eskes, D. Fonteyn, D. R. Jackson, M. N. Juckes, S. Massart, V.-H. Peuch, S. Rharmili, and A. Segers, "The ASSET intercomparison of ozone analyses: method and first results," Atmos. Chem. Phys. 6, 5445-5474 (2006).
[CrossRef]

Atmos. Environ. (2)

M. Beekmann, G. Ancellet, D. Martin, C. Abonnel, G. Duverneuil, F. Eideliman, P. Bessemoulin, N. Fritz, and E. Gizard, "Intercomparison of tropospheric ozone profiles obtained by electrochemical sondes, a ground based lidar and an airborne UV-photometer," Atmos. Environ. 29, 1027-1042 (1995).
[CrossRef]

J. Staehelin and W. Schmid, "Trend analysis of the tropospheric ozone concentration utilizing the 20-years data set of the ozone balloon soundings over Payerne," Atmos. Environ. 25A, 1739-1749 (1991).

Geophys. Res. Lett. (4)

M. M. Abbas, T. Kostiuk, M. J. Mumma, D. Buhl, V. G. Kunde, and L. W. Brown, "Stratospheric ozone measurement with an infrared heterodyne spectrometer," Geophys. Res. Lett. 5, 317-320 (1978).
[CrossRef]

M. Taguchi, S. Okano, H. Fukunishi, and Y. Sasano, "Comparison of ozone profiles from ground-based laser heterodyne spectrometer and ozonesonde measurements," Geophys. Res. Lett. 17, 2349-2352 (1990).
[CrossRef]

K. E. Fast, T. Kostiuk, F. Espenak, T. A. Livengood, T. Hewagama, and M. F. A'Hearn, "Stratospheric ozone profiles from Mauna Kea, Hawai'i (19.8N, 155.5W) using infrared heterodyne spectroscopy, 1988-2003," Geophys. Res. Lett. 31, L08109, doi:10.1029/2004GL019443 (2004).
[CrossRef]

I. Petropavlovskikh, P. K. Bhartia, and J. DeLuisi, "New Umkehr ozone profile retrieval algorithm optimized for climatological studies," Geophys. Res. Lett. 32, L16808, doi:10.1029/2005GL023323 (2005).
[CrossRef]

Icarus (1)

K. Fast, T. Kostiuk, F. Espenak, J. Annen, D. Buhl, T. Hewagama, M. F. A'Hearn, D. Zipoy, T. A. Livengood, G. Sonnabend, and F. Smulling, "Ozone abundance on Mars from infrared heterodyne spectra. I. Acquisition, retrieval, and anticorrelation with water vapor," Icarus 181, 419-431 (2006).
[CrossRef]

J. Environ. Monito. (1)

P. Keckhut, S. McDermid, D. Swart, T. McGee, S. Godin-Beekmann, A. Adriani, J. Barnes, J.-L. Baray, H. Bencherif, H. Claude, A. G. di Sarra, G. Fiocco, G. Hansen, A. Hauchecorne, T. Leblanc, C. H. Lee, S. Pal, G. Megie, H. Nakane, R. Neuber, W. Steinbrecht, and J. Thayer, "Review of ozone and temperature lidar validations performed within the framework of the Network for the Detection of Stratospheric Change," J. Environ. Monito. 6, 721-733 (2004).
[CrossRef]

J. Geophy. Res. (1)

B. Barret, M. De Maziere, and P. Demoulin, "Retrieval and characterization of ozone profiles from solar infrared spectra at the Jungfraujoch," J. Geophy. Res. 107, D24, 4788, doi:10.1029/2001JD001298 (2002).
[CrossRef]

J. Geophys. Res. (5)

C. Brogniez, M. Houët, A. M. Siani, P. Weihs, M. Allaart, J. Lenoble, T. Cabot, A. de la Casinière, and E. Kyrö, "Ozone column retrieval from solar UV measurements at ground level: effects of clouds and results from six European sites," J. Geophys. Res. 110, D24202, doi:10.1029/2005JD005992 (2005).
[CrossRef]

M. De Maziere, O. Hennen, and M. Van Roozendael, "Daily ozone vertical profile model built on geophysical grounds, for column retrieval from atmospheric high resolution infrared spectra," J. Geophys. Res. 104, D19, 23855-23869 (1999).
[CrossRef]

Y. J. Meijer, D. P. J. Swart, F. Baier, P. K. Bhartia, G. E. Bodeker, S. Casadio, K. Chance, F. Del Frate, T. Erbertseder, M. D. Felder, L. E. Flynn, S. Godin-Beekmann, G. Hansen, O. P. Hasekamp, A. Kaifel, H. M. Kelder, B. J. Kerridge, J.-C. Lambert, J. Landgraf, B. Latter, X. Liu, I. S. McDermid, Y. Pachepsky, V. Rozanov, R. Siddans, S. Tellmann, R. J. van der A, R. F. van Oss, M. Weber, and C. Zehner, "Evaluation of Global Ozone Monitoring Experiment (GOME) ozone profiles from nine different algorithms," J. Geophys. Res. 111, D21306, doi:10.1029/2005JD006778 (2006).
[CrossRef]

P.-F. Coheur, B. Barret, S. Turquety, D. Hurtmans, J. Hadji-Lazaro, and C. Clerbaux, "Retrieval and characterization of ozone vertical profiles from a thermal infrared nadir sounder," J. Geophys. Res. 110, D24303, doi:10.1029/2005JD005845 (2005).
[CrossRef]

X. Liu, K. Chance, C. E. Sioris, T. P. Kurosu, and M. J. Newchurch, "Intercomparison of GOME, ozonesonde, and SAGE II measurements of ozone: demonstration of the need to homogenize available ozonesonde data sets," J. Geophys. Res. 111, D14305, doi:10.1029/2005JD006718 (2006).

J. Quanti. Spectrosc. Radiat. Transfer (1)

L. S. Rothman, D. Jacquemart, A. Barbe, D. Chris Benner, M. Birk, L. R. Brown, M. R. Carleer, C. Chackerian, K. Chance, L. H. Coudert, V. Dana, V. M. Devi, J.-M, Flaud, R. R. Gamache, A. Goldman, J.-M. Hartmann, K. W. Jucks, A. G. Maki, J.-Y. Mandin, S. T. Massie, J. Orphal, A. Perrin, C. P. Rinsland, M. A. H. Smith, J. Tennyson, R. N. Tolchenov, R. A. Toth, J. Vander Auwera, P. Varanasi, and G. Wagner, "The HITRAN 2004 molecular spectroscopic database," J. Quanti. Spectrosc. Radiat. Transfer 96, 139-204 (2005).
[CrossRef]

Rev. Sci. Instrum. (1)

D. Weidmann, W. J. Reburn, and K. Smith, "Ground-based prototype quantum cascade laser heterodyne radiometer for atmospheric studies," Rev. Sci. Instrum. 78, 073107 (2007).
[CrossRef] [PubMed]

Science (1)

R. T. Menzies and R. K. Seals, "Ozone monitoring with an infrared heterodyne radiometer," Science 197, 1275-1277 (1977).
[CrossRef] [PubMed]

Sem. Respir. Crit. Care Med. (1)

P. L. Kinney, "The pulmonary effects of ozone and particle air pollution," Sem. Respir. Crit. Care Med. 20, 601-607 (1999).
[CrossRef]

Other (4)

"ECMWF data archive services," http://www.ecmwf.int/products/data/archive/.

C. D. Rodgers, "Inverse Methods for Atmospheric Sounding: Theory and Practice (World Scientific, 2000).

A. Dudhia, "Reference Forward Model software user's manual," www.atm.ox.ac.uk/RFM/sum.

"Total Ozone Mapping Spectrometer," http://jwocky.gsfc.nasa.gov/.

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Figures (9)

Fig. 1
Fig. 1

Plot of the measured LHR instrument lineshape.

Fig. 2
Fig. 2

(Color online) Simulated analysis of the averaging kernels of the ozone profile retrieval from the infrared quantum cascade laser heterodyne radiometer. Calculations for three different double sideband resolutions are presented with the instrument SNR being kept constant.

Fig. 3
Fig. 3

Plot of the ν 3 band of ozone. The three different spectral windows used to investigate the influence of the frequency coverage on the retrieval quality are indicated. On the right hand side, the LHR window has been expanded.

Fig. 4
Fig. 4

Ozone vertical profiles retrieved for two different sets of a priori conditions.

Fig. 5
Fig. 5

(Color online) (a) Averaging kernels corresponding to the ECMWF a priori retrieval of Fig. 3. (b) Pressure profile and (c) temperature profile interpolated in time and space from the ECMWF dataset.

Fig. 6
Fig. 6

(Color online) Comparison of the ozone profile retrievals from the LHR measurements at RAL with ozonesonde data from the Observatoire de Haute Provence (OHP) and the Payerne Aerological Station (PAS). The inset within the plot focuses on the tropospheric data. The inset map shows the geographical location of the three sites.

Fig. 7
Fig. 7

(Color online) Ozone total column over the Rutherford Appleton Lab (RAL), the Payerne Aerological Station (PAS), and the Observatoire de Haute Provence (OHP) during the two days bracketing the LHR atmospheric campaign. Data are from OMI on the Aura Earth Observing System satellite. On 22nd of September a significant increase in the ozone column above RAL compared to PAS can be seen.

Fig. 8
Fig. 8

(Color online) Retrieval error analysis plots: (a) the diagonal elements of the smoothing error and retrieval noise covariance matrices, (b) the global gain factor, (c) the absolute value of the gain matrix, (d) the corresponding measurement vector, and (e) the corresponding residual between the measurement vector and the forward model applied to the retrieved state.

Fig. 9
Fig. 9

First twelve and most significant singular vectors (SVs) of the K ˜ matrix. These vectors describe the altitudinal location of each independent piece of information retrieved. The corresponding individual degree of freedom, d, quantifies whether the SVs contribute significantly ( d 1 ) to the knowledge of the true atmospheric state, or merely reproduce the a priori conditions ( d 1 ) .

Tables (3)

Tables Icon

Table 1 Specifications of the Laser Heterodyne Radiometer

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Table 2 Summary of the Parameters Used in the Retrieval Algorithm

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Table 3 Most Intense Ozone Rovibrational Transitions Occurring within the LHR Window [Line Intensities > 10−21 cm−1∕(molec. cm−2)]

Equations (12)

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y = F ( x ) + ε .
χ 2 = ( y F ( x n ) ) S ε 1 ( y F ( x n ) ) T + ( x a x n ) S a 1 ( x a x n ) T ,
x i + 1 = x i + [ ( 1 + λ ) S a 1 + K i T S ε 1 K i ] 1 × [ K i T S ε 1 ( y i F ( x i ) ) + S a 1 ( x a x i ) ] .
y = K x + ε .
1033.80   to   1034.50 , Δ σ = 0.0007 cm 1 ,
1030.65   to   1037.65 , Δ σ = 0.007 cm 1 ,
999.15   to   1069.15 , Δ σ = 0.07 cm 1 .
G = ( S a 1 + K T S ε 1 K ) 1 K T S ε 1 ,
G Σ = i = 1 m ( G i ) 2 ,
y ˜ = K ˜ x ˜ + ε ˜ .
H = i 1 2 log ( 1 + λ i 2 ) ,
d = i λ i 2 ( 1 + λ i 2 ) .

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