Journal of the Meteorological Society, of Japan, Vol. 75, No. 6, pp , NOTES AND CORRESPONDENCE

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1 Journal of the Meteorological Society, of Japan, Vol. 75, No. 6, pp , NOTES AND CORRESPONDENCE Relative Humidity, Backscattering Ratio and Depolarization Ratio as Derived from Raman Lidar Observations By Tetsu Sakai, Takashi Shibata and Yasunobu Iwasaka Solar-Terrestrial Environment Laboratory, Nagoya University, Chikusa-ku, Nagoya , Japan (Manuscript received 20 November 1996, in revised form 20 September 1997) Abstract Simultaneous observation of the vertical profiles of tropospheric water vapor and the density and nonsphericity of aerosol particles was made with a Raman lidar at Nagoya (35N, 137E). The data from observations made on April 17, 1994 showed the following features of the water vapor and aerosol particles. Temporal and systematic variations of the parameters were observed at the lower altitude range of km, where the mixing ratio of aerosol particles (backscattering ratio) increased and the nonsphericity of the particles (depolarization ratio) decreased with increasing humidity. There was a positive correlation between the vertical profiles of backscattering ratio and the water vapor mixing ratio. The depolarization ratio was positively correlated with the water vapor mixing ratio above 2.2km and negatively correlated below this level. The altitudes where the discontinuities of the water vapor and aerosol parameters were found and that where the correlation between the depolarization ratio and the water vapor mixing ratio changed showed the correspondences with the temperature inversion or wind shears observed at Hamamatsu (35N, 138E). 1. Introduction Condensation of atmospheric water vapor onto atmospheric aerosol particles and evaporation from the particles significantly affect the size, shape and chemical composition of the particles. The hygroscopic behavior of the particles is of great concern since radiative forcing of aerosols and heterogeneous reactions largely depend on the density, size, shape and chemical composition of aerosols which are affected by relative humidity (e.g., Taylor and Penner, 1994; Boucher and Anderson, 1995). Murayama et al. (1996) found a clear negative correlation between the nonsphericity of aerosol particles (depolarization ratio) and the relative humidity in the boundary atmosphere. They suggested that the correlation might be due to the hygroscopic nature of urban aerosol particles. Their measurements was limited to the boundary atmospheric particles, and the two parameters were separately observed: relative humidity near the ground by a hygrometer, and aerosol nonsphericity in the boundary atmosphere ( m altitude) by a polarization lidar. The distribution of free tropospheric aerosol particles is frequently affected by long-range transport from remote areas, as shown by the measurement of dust particles from the Asian mainland over Japan (e.g., Iwasaka et al., 1996). However, the relationship between aerosol sphericity and ambient humidity in the free troposphere has not yet been thoroughly investigated due to technical difficulties. The Raman lidar is a newly developed tool for simultaneously measuring tropospheric water vapor and aerosol density profiles. By using this technique, the relationship between the aerosol backscatter and/or extinction and the humidity in the troposphere has been investigated (Ansmann et al., 1992; Ferrare et al., 1997). Shibata et al. (1996a) and Reichardt et al. (1996) demonstrated the devices applicability for the detection of ice clouds by simultaneously measuring the humidity and the depolarization ratio profiles. Since the depolarization ratio is a measure of the nonsphericity of aerosol particles (e.g., Bohren and Huffman, 1983), it has potential for discriminating the phase of the particles (liquid droplet or solid crystal). Thus the relationship between humidity and the depolarization ratio provides vital infor-

2 1180 Journal of the Meteorological Society of Japan Vol. 75, No. 6 Table 1. Characteristics of the Raman lidar mation on the hygroscopic characteristics of aerosol particles. This paper presents typical results of simultaneous measurements of humidity, depolarization ratio and backscattering ratio from the upper boundary atmosphere to the free troposphere using the Raman lidar; furthermore, it discusses the temporal and vertical relationship among these parameters. 2. Raman lidar measurement of water vapor and aerosols The main characteristics of the Raman lidar used here are shown in Tablel. Three wavelengths (355, 532 and 1064 nm) of linearly-polarized and pulsed Nd:YAG laser beams are transmitted vertically into the atmosphere. The light backscattered by atmospheric gases and aerosol particles is collected with a Cassegrain telescope. The light is simultaneously separated into five spectral components and detected with five photomultiplier tubes (PMTS). The following vertical profiles of atmospheric quantities were obtained in the observations reported in this paper: 1) water vapor mixing ratio; 2) backscattering ratio at 532 nm; and 3) total depolarization ratio at 532 nm. Details of the procedure used to analyze data are summarized in Shibata et al. (1996a, 1996b). The water vapor mixing ratio (q) is derived by the ratio of water vapor Raman to oxygen Raman backscatter signals, which is defined as q(z)=k installed at Nagoya University PH2o (z) T z (o,z) Pot were K is the calibration constant obtained by the coincident radiosonde measurements, P02 (z) and PH2o(z) are lidar signals Raman backscattered by oxygen and water vapor molecules at height z, respectively, and T(zo,z) is the transmission correction term (the ratio of atmospheric transmissivity at the wavelength of oxygen Raman scattering to that of water vapor Raman scattering from the lidar at height zo to height z). The backscattering ratio (R) is obtained from the Mie and Rayleigh backscatter signals at 532 nm by applying an iteration method (Hirono and Shibata, 1983; Shibata et ad., 1996b) and is defined as 3(z) + 13m(z) R(z) 8m (z) where f3 (z) and /3m(z) are the volume backscattering coefficients of aerosol particles and air molecules at height z, respectively. The value of R-1 is approximately proportional to the mixing ratio of aerosol particles. The total depolarization ratio (S) is obtained from the two orthogonal components of the Mie and Rayleigh backscatter signals at 532 nm and is defined as P1(z) 6(z) 1(z) + P11 (z) 3,l(z) + 13m, (Z) p,1(z) + m,11(z) + f,1(z) + m,l(z) where the subscripts // and 1 are the parallel and perpendicular components of the signals with respect to the linearly polarized transmitted laser beam, respectively. The method used to calculate S from the observed signal is described in detail by Shibata et al. (1996b). The depolarization ratio is a measure of the nonsphericity of the scattering particles because nonspherical particles (e.g., solid crystals) backscatter depolarized light with respect to the polarization plane of the incident light. If the backscattered light is only from the spherical particles (e.g., liquid droplets) and/or optically isotropic molecules, the depolarization ratio is zero. The depolarization ratio where aerosol backscattering is negligible (sum of depolarization ratio by Rayleigh scattering and that induced by the system) for this lidar system is 2 % (Kwon et al., 1996). Successive measurements were carried out for 30 minutes (19:18-19:48 JST) on the night of April 17, 1994 on the campus of Nagoya University (35N, 137E). During the observation period, the lidar site was under a high pressure zone after a weak cold front passed its north side. Photon counts were accumulated every five minutes in 50 m intervals. Before the retrieval of the vertical profiles, the signals were smoothed by taking three points running mean, except for taking nine points for the backscattering ratio. In the analysis of the backscattering ratio, data normalization was performed in connection with the stratospheric profile observed about 10 minutes later. Measurement uncertainty was estimated from la confidence of the photon counts.

3 December 1997 T. Sakai, T. Shibata and Y. Iwasaka 1181 (a) (b) (c) (d) Fig. 1. Vertical profiles of water vapor mixing ratio (a), backscattering ratio at a wavelength of 532 nm (b), total depolarization ratio at a wavelength of 532 nm (c) and the relatively humidity over water (d) observed with the Raman lidar at Nagoya (35N, 137E) from 19:18 to 19:48 JST on April 17, Results and Discussion Vertical profiles of water vapor mixing ratio (q), backscattering ratio (R) at 532 nm, total depolarization ratio (S) at 532 nm, and relative humidity (RH) observed on April 17, 1994 are shown in Figs. laid, respectively. Relative humidity was estimated by combining the water vapor mixing ratio observed with the Raman lidar and atmospheric temperature measured with the radiosonde launched at Hamamatsu meteorological observatory (90 km southeast of lidar site) on the same night. The RH profile at Hamamatsu is also shown in Fig. id. Temporal changes of those parameters were found from 19:18 to 19:48 JST at the altitude range of km (Region A in Fig. 1), where q (also RH) and R were increasing, and S was decreasing. The temporal relationship between RH and the values of R and 6 in this region are shown in Figs. 2a and 2b, respectively. A clear positive correlation between RH and R and a clear negative correlation between RH and S were found. These correlations indicated that the total backscattering cross section and the sphericity of the particles were larger in moist air than in dry air in this altitude region. The size of

4 1182 Journal of the Meteorological Society of Japan Vol. 75, No. 6 (a) (a) (b) (b) Fig. 2. Temporal,, relationships between the relative humidity and the quantities backscattering ratio (a), and total depolarization ratio (b) at altitude Region A (1.4, 1.6 and 1.8 km) in Fig. 1 Fig. 3. Vertical relationship of the water vapor mixing ratio and the quantities backscattering ratio (a), and total depolarization ratio (b) (+: z < 2.2 km, 0: z>2.2km). an individual particle would be larger and its shape more spherical in moist air under the condition of a constant mixing ratio of particle number. The sphericity of the hygroscopic particle depends on the phase (liquid droplet or solid crystal), which is controlled by the ambient relative humidity. According to the reported laboratory experiments, relative humidifies at the phase transition points of hygroscopic particles are as follows: 75 % for deliquescence and 40 % for crystallization of an NaCI particle (lunge, 1963); 80 % and % for those of (NH4)2S04, and 40 % and % for those of NH4HSO4 (Tang and Munkelwitz, 1994). In our observation, the values of RH at Region A, where S was negatively correlated with RH, varied between 13 and 38 %. This is near the crystallization humidity of NaCI and (NH4)2S04, and both the deliquescence and crystallization humidifies of NH4HSO4. A similar negative correlation between S and RH was observed by Murayama et al. (1996) in the atmospheric boundary layer in Tokyo. They made hourly observations during both day and night and showed that the S at around an altitude of 100 m was negatively correlated with the RH at 30 m. The

5 December 1997 T. Sakai, T. Shibata and Y. Iwasaka 1183 Fig. 4. Vertical profiles of temperature, wind direction and wind speed at Hamamatsu (35N, 138E) at 21:00 JST on April 17, value of S changed between 2 % and 7 % when the RH changed between 20 % and 65 %. They reported this correlation was generally found independently of the season. Our results in Region A showed that the negative correlation extended vertically for about one kilometer in the lower troposphere and the value of R (mixing ratio of the particles) was also correlated with RH. A similar measurement location (urban area near the bay) and the locality of the source of the lower tropospheric aerosols might result in a similar negative correlation between S and RH. Although a similar temporal variation of the relationship between RH and 6 as observed by Murayama et al. (1996) was found in altitude Region A in Fig. 1, the vertical-spatial variations showed a different relationship from the temporal variation in Region A. At the altitude range of km (Region B in Fig. 1), the value of S was high (6 N 10 %) where RH was as high as the maximum value at km (Region A), in which case RH-S correlation was negative. This difference of the relationship between the parameters depending on the altitude region may be attributed to the difference of the chemical composition of the particulate matter, and/or of the phase which inherits the changes in RH during transportation. Figures 3a and 3b show the vertical relationship between q and R and that between q and 8, respectively. The values of R were positively correlated with q vertically. The values of S were positively correlated with q above 2.2 km and negatively correlated below this level. The different atmospheric processes would be responsible for these temporal and vertical relationships observed by the lidar. Temperature and wind profiles at Hamamatsu are shown in Fig. 4. The wind direction changed for about 15 degrees at boundary of Regions A and B (2.2 km). The altitudes of the wind shears (1.0 km and 5.0 km) and the temperature inversion (3.5 km) corresponded to the vertical discontinuities of the water vapor and aerosol profiles in Figs. 1. The vertical distributions of both water vapor and aerosols would be greatly affected by the horizontal transport process in this case. 4. Conclusions Vertical profiles of tropospheric water vapor and the density and sphericity of aerosol particles were observed simultaneously with a Raman lidar at Nagoya (35N, 137E) on the height of April 17,

6 1184 Journal of the Meteorological Society of Japan Vol. 75, No Temporal variations of the parameters were observed at the altitude range of km. The relationship between the aerosol parameters and the relative humidity indicated that the total backscattering cross section and the sphericity of the aerosol particles were larger in moist air than in dry that in this altitude region. The value of relative humidity in the region was near the phase transition (crystallization and/or deliquescence) humidity of major tropospheric hygroscopic particles. The backscattering ratio was positively correlated with the water vapor mixing ratio vertically. The depolarization ratio was positively correlated with the water vapor mixing ratio above an altitude of 2.2 km and negatively correlated below this level. The altitudes where the discontinuities of the water vapor and aerosol parameters were found and that where the correlation between the depolarization ratio and the water vapor mixing ratio changed showed the correspondences with the temperature inversion or wind shears observed at Hamamatsu. Although we have presented only one typical case of the simultaneous measurement of water vapor and aerosol profiles in this paper, the case demonstrates the usefulness of the Raman lidar for study of the hygroscopic nature of the atmospheric aerosols. We are planning to study this relationship's seasonal dependence and it's temporal variation in the nocturnal atmospheric boundary layer. Acknowledgments This research was supported by Japan Ministry of Education, Science, Sports and Culture (Grant-in- Aid for Creative Fundamental Research, Studies of Global Environmental Change with special reference to Asia and Pacific Regions, led by Professors S. Tamura, University of Tokyo, T. Matsuno, Hokkaido University, and M. Tanaka, Tohoku University). References Ansmann, A.M., Riebesell, U. Wandinger, C. Weitkamp, E. Voss, W. Lahmann, and W. Michaelis, 1992: Combined Raman elastic-backscatter LIDAR for vertical profiling of moisture, aerosol extinction, backscatter, and LIDAR ratio, Appl. Phys., B55, Boucher, 0. and T.L. Anderson, 1995: General circulation model assesment of the sensitivity of direct climate forcing by anthropogenic sulfate aerosols to aerosol size and chemistry, J. Geophys. Res., 100, Bohren, C.F. and DR. Huffman, 1983: Absorption and Scattering of Light by Small Particles, Wiley, New York, 530p. Ferrare, R.A., S.H. Melfi, D. Whiteman, K.D. Evans, G. Schwemmer, Y. Kaufman, R. Ellingson, 1997: Raman lidar and sun photometer measurement of aerosols and water vapor, In Advances in atmospheric remote sensing with lidar, Springer-Verlag, Berlin, p Hirono, M and T. Shibata, 1983: Enormous increase of stratospheric aerosols over Fukuoka due to volcanic eruption of El Chichon in 1982, Geophys. Res. Lett., 10, Iwasaka, Y., I. Mori, M. Nagatani, H. Nakada, K. Matsunaga and H. Nakane, 1996: Size distributions of aerosol particles in the free troposphere: aircraft measurements in the Spring of over Japan, Terr. Atm. Ocea. Sci., 7, Junge, CE., 1963: Air chemistry and radioactivity, Academic Press, New York, p Kwon, S.A., Y. Iwasaka and T. Shibata, 1996: Depolarization ratio of air molecules in the free troposphere-lidar measurement in spring 1994-, J. Geomag. Geoelectr., 48, Murayama, T., M. Furushima, A. Oda, N. Iwasaka and K. Kai, 1996: Depolarization ratio measurements in the atmospheric boundary layer by lidar in Tokyo, J. Meteor. Soc. Japan, 74, Reichardt, J., A. Ansmann, M. Serwazi, C. Weitkamp, W. Michaelis, 1996: Unexpectedly low ozone concentration in midlatitude tropospheric ice clouds: A case study, Geophys. Res. Lett., 23, Shibata, T., T. Sakai, M. Hayashi, T. Ojio, S.A. Kwon and Y. Iwasaka, 1996a, Raman lidar observations: simultaneous measurements of water vapor, temperature and aerosol vertical profiles, Part I, J. Geomag. Geoelectr., 48, Shibata, T., T. Sakai, M. Hayashi, T. Ojio, S.A. Kwon and Y. Iwasaka,1996b, Raman lidar observations: simultaneous measurements of water vapor, temperature and aerosol vertical profiles, Part II, J. Geomag. Geoelectr., 48, Tang, IN. and H.R. Munkelwitz,1994: Water activities, densities, and refractive indices of aqueous sulfates and sodium nitrate droplets of atmospheric importance, J. Geophys. Res., 99, Taylor, K.E. and J.E. Penner,1994: Response of the climate system to atmospheric aerosols and greenhouse gases, Nature, 369,

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