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1.
The photodissociation coefficient, J NO2 of NO2 in the atmosphere was calculated at 235 and 298 K using the measured temperature dependences of the absorption cross-sections and quantum yields. These calculations gave a ratio J NO2(298 K)/J NO2(235 K)=1.155±0.010 which is only weakly dependent on altitude, surface albedo and solar zenith angle.  相似文献   

2.
Using a filter radiometer, the meridional profile of the NO2 photolysis frequency, J(NO2), was measured between 50° N and 30° S during the cruise ANTVII/1 September/October 1988 of the research vessel Polarstern on the Atlantic Ocean. Simultaneously, global broadband irradiance and acrosol were monitored. Clean marine background air with low aerosol loads (b sp=(1–2)×10-5 m-1) was encountered at the latitudes 25° N–30° N and 18° S–27° S, respectively. Under these conditions and an almost cloudless sky J(NO2) reached 7.3×10-3 s-1 (2 sr) for a zenith angle of 30°. Between 30° N and 30° S, the latitudinal variation of the J(NO2) noontime maxima was less than ± 10%, while the mean value at noon was 7.8×10-3 s-1. For the set of all data between 50° N and 30° S, a nearly linear correlation of J(NO2) vs. global broadland irradiance was found. The slope of (8.24±0.03)×10-5 s-1/mW cm-2 agrees within 10% with observations in Jülich (51° N, 6.2° E).  相似文献   

3.
The photodissociation coefficient of NO2, J NO 2, has been measured from a balloon platform in the stratosphere. Results from two balloon flights are reported. High Sun values of J NO 2 measured were 10.5±0.3 and 10.3±0.3×10-3 s-1 at 24 and 32 km respectively. The decrease in J NO 2 at sunset was monitored in both flights. The measurements are found to be in good agreement with calculations of J NO 2 using a simplified isotropic multiple scattering computer routine.  相似文献   

4.
The latitudinal variation of the photolysis frequency of ozone to O(1D) atoms, J(O1D), was measured using a filter radiometer during the cruise ANT VII/1 of the research vessel Polarstern in September/October 1988. The J(O1D) noon values exhibited a maximum of 3.6×10-5 s-1 (2 sr) at the equator and decreased strongly towards higher latitudes. J(O1D) reached highest values for clean marine background air with low aerosol load and almost cloudless sky. The J(O1D) data, measured under these conditions and a temperature of 295 K, can be expressed by: % MathType!MTEF!2!1!+-% feaafiart1ev1aaatCvAUfeBSjuyZL2yd9gzLbvyNv2CaerbuLwBLn% hiov2DGi1BTfMBaeXatLxBI9gBaerbd9wDYLwzYbItLDharqqtubsr% 4rNCHbGeaGqiVu0Je9sqqrpepC0xbbL8F4rqqrFfpeea0xe9Lq-Jc9% vqaqpepm0xbba9pwe9Q8fs0-yqaqpepae9pg0FirpepeKkFr0xfr-x% fr-xb9adbaqaaeGaciGaaiaabeqaamaabaabaaGcbaGaamOsaiaacI% cacaqGpbWaaWbaaSqabeaaiiaacqWF8baFaaGccaqGebGaaeykaiaa% bccacqWF9aqpcaqGGaGaaeyzaiaabIhacaqGWbGaaeiiaiaabUhacq% GHsislcaaI4aGaaiOlaiaaicdacaaIYaGaeyOeI0IaaGioaiaac6ca% caaI4aGaaiiEaiaaigdacaaIWaWaaWbaaSqabeaacqGHsislcaaIZa% aaaOGaaeiiaiaabIhacaqGGaGaam4uaiabgUcaRiaaiodacaGGUaGa% aGinaiaacIhacaaIXaGaaGimamaaCaaaleqabaGaeyOeI0IaaGOnaa% aakiaadofadaahaaWcbeqaaiaaikdaaaGccaGG9bGaaeikaiaaboha% daahaaWcbeqaaiabgkHiTiaaigdaaaGccaGGPaaaaa!5EE9!\[J({\text{O}}^| {\text{D) }} = {\text{ exp \{ }} - 8.02 - 8.8x10^{ - 3} {\text{ x }}S + 3.4x10^{ - 6} S^2 \} {\text{(s}}^{ - 1} )\] where S represents the product of the overhead ozone column (DU) and the secant of the solar zenith angle. The meridional profile of the primary OH radical production rate P(OH) was calculated from the J(O1D) measurements and simultaneously recorded O3 and H2O mixing ratios. While the latitudinal distribution of J(O1D) and water vapour was nearly symmetric to the equator, high tropospheric ozone levels up to 40 ppb were observed in the Southern Hemisphere, SH, resulting in higher P(OH) in the SH.  相似文献   

5.
A simple model is developed which estimates daily global radiation at the floor of a non-homogeneous Eucalyptus forest. Model input parameters are easily derived from field measurements and consist of individual tree location, tree height, maximum canopy width and its corresponding height, height of the lowest branch and trunk thickness. In addition, the model requires values for global and diffuse irradiance in the open. The tree canopy is represented as a series of spheres containing leaves which are homogeneously spaced but are oriented in the vertical plane. This configuration closely approaches that of actual eucalyptus trees. A Monte-Carlo approach is used to estimate the albedo of the unit sphere as a function of solar zenith angle. At a given combination of solar zenith and azimuth angle, the model estimates the solar irradiance at a specific forest floor location.The model, when tested against pyranometer measurements, predicted daily solar irradiance with a correlation of 0.98 and a standard error of 0.98 MJ m-2 day-1. This good performance is attributed to the spatial averaging of the radiation fluxes over the entire day, and the relatively low sensitivity of the calculated solar irradiance to sphere albedo.  相似文献   

6.
Simulations of polar ozone losses were performed using the three-dimensional high-resolution (1 × 1) chemical transport model MIMOSA-CHIM. Three Arctic winters 1999–2000, 2001–2002, 2002–2003 and three Antarctic winters 2001, 2002, and 2003 were considered for the study. The cumulative ozone loss in the Arctic winter 2002–2003 reached around 35% at 475 K inside the vortex, as compared to more than 60% in 1999–2000. During 1999–2000, denitrification induces a maximum of about 23% extra ozone loss at 475 K as compared to 17% in 2002–2003. Unlike these two colder Arctic winters, the 2001–2002 Arctic was warmer and did not experience much ozone loss. Sensitivity tests showed that the chosen resolution of 1 × 1 provides a better evaluation of ozone loss at the edge of the polar vortex in high solar zenith angle conditions. The simulation results for ozone, ClO, HNO3, N2O, and NO y for winters 1999–2000 and 2002–2003 were compared with measurements on board ER-2 and Geophysica aircraft respectively. Sensitivity tests showed that increasing heating rates calculated by the model by 50% and doubling the PSC (Polar Stratospheric Clouds) particle density (from 5 × 10−3 to 10−2 cm−3) refines the agreement with in situ ozone, N2O and NO y levels. In this configuration, simulated ClO levels are increased and are in better agreement with observations in January but are overestimated by about 20% in March. The use of the Burkholder et al. (1990) Cl2O2 absorption cross-sections slightly increases further ClO levels especially in high solar zenith angle conditions. Comparisons of the modelled ozone values with ozonesonde measurement in the Antarctic winter 2003 and with Polar Ozone and Aerosol Measurement III (POAM III) measurements in the Antarctic winters 2001 and 2002, shows that the simulations underestimate the ozone loss rate at the end of the ozone destruction period. A slightly better agreement is obtained with the use of Burkholder et al. (1990) Cl2O2 absorption cross-sections.  相似文献   

7.
Surface erythemal UV radiation is mainly affected by total column ozone, aerosols, clouds, and solar zenith angle. The effect of ozone on the surface UV radiation has been explored many times in the previous studies due to the decrease of ozone layer. In this study, we calculated the effect of aerosols on the surface UV radiation as well as that of ozone using data acquired from Ozone Monitoring Instrument (OMI). First, ozone, aerosol optical depth (AOD), and surface erythemal UVB radiation measured from satellite are compared with those from ground measurements. The results showed that the comparison for ozone was good with r 2 of 0.92. For aerosol, there was difference between satellite measurements and surface measurements due to the insufficient information on aerosol in the retrieval algorithm. The r 2 for surface erythemal UV radiation was high (~0.94) but satellite measurements showed about 30% larger values than surface measurements on average by not considering the effect of absorbing aerosols in the retrieval process from satellite measurements. Radiative amplification factor (RAF) is used to access the effect of ozone and aerosol quantitatively. RAF for ozone was 0.97~1.49 with solar zenith angle. To evaluate the effect of aerosol on the surface UV radiation, only clear-sky pixel data were used and solar zenith angle and total column amount of ozone were fixed. Also, RAF for aerosol was assessed according to the single scattering albedo (SSA) of aerosols. The results showed that RAF for aerosol with smaller SSA (< 0.90) was larger than that for with larger SSA (> 0.90). The RAF for aerosol was 0.09~0.22 for the given conditions which was relatively small compared to that for ozone. However, considering the fact that aerosol optical depth can change largely in time and space while the total column amount of ozone does not change very much, it needs to include the effect of aerosol to predict the variations of surface UV radiation more correctly.  相似文献   

8.
In situ measurements of [OH], [HO2] (square brackets denote species concentrations), and other chemical species were made in the tropical upper troposphere (TUT). [OH] showed a robust correlation with solar zenith angle. Beyond this dependence, however, [OH] did not correlate to its primary source, the product of [O3] and [H2O] ([O3]?[H2O]), or its sink [NOy]. This suggests that [OH] is heavily buffered in the TUT. One important exception to this result is found in regions with very low [O3], [NO], and [NOy]. Under these conditions, [OH] is highly suppressed, pointing to the critical role of NO in sustaining OH in the TUT and the possibility of low [OH] over the western Pacific warm pool due to strong marine convections bringing NO-poor air to the TUT. In contrast to [OH], [HOx] ([OH] + [HO2]) correlated reasonably well with [O3]?[H2O]/[NOy], suggesting that [O3]?[H2O] and [NOy] are the significant source and sink, respectively, of [HOx].  相似文献   

9.
Tazhong station, located at the hinterland of the Taklimakan Desert in northwest China, experiences frequent dusty weather events during spring and summer seasons (its dusty season) caused by unstable stratified atmosphere, abundant sand source and strong low-level wind. On average, it has 246.2 dusty days each year, of which 16.2 days are classified as sand and dust storm days. To better understand the characteristic of solar ultraviolet (UV) radiation and factors influencing its variations under such an extreme environment, UV radiation data were collected continuously from 2007 to 2011 at Tazhong station using UVS-AB-T radiometer by Kipp and Zonen. This study documents observational characteristics of the UV radiation variations observed during the five-year period. Monthly UV radiation in this region varied in the range of 14.1–37.8 MJ m?2 and the average annual amount was 320.7 MJ m?2. The highest value of UV radiation occurred in June (62.5 W m?2) while the lowest one in December (29.3 W m?2). It showed a notable diurnal cycle, with peak value at 12:00–13:00 LST. Furthermore, its seasonal variation exhibited some unique features, with averaged UV magnitude showing an order of summer > spring > autumn > winter. The seasonal values were 37.0, 29.1, 24.9 and 15.9 MJ m?2, respectively. In autumn and winter, its daily variations were relatively weak. However, significant daily variations were observed during spring and summer associated with frequent dust weather events occurring in the region. Further analysis showed that there was a significant correlation between the UV radiation and solar zenith angle under different weather conditions. Under the same solar zenith angle, UV radiation was higher during clear days while it was lower in sand and dust storm days. Our observations showed that there was a negative correlation between UV radiation and ozone, but such a relationship became absent in dusty days. The UV radiation was reduced by 6 % when cloud amount was 1–4 oktas, by 12 % when the cloud amount was 5–7 oktas, and by 24 % when the cloud amount was greater than 8 oktas. The relative reduction of UV radiation reached 26, 38, and 45 % in dust day, blowing sand day and sand and dust storm day, respectively. The results revealed that decrease in UV radiation can be attributed to cloud coverage and dust aerosols. Moreover, the reduction of UV radiation caused by dust aerosols was about 2–4 times greater than that caused by cloud coverage. These observational results are of value for improving our understanding of processes controlling UV radiation over sand desert and developing methods for its estimation and prediction.  相似文献   

10.
Abstract

Ground‐based measurements of stratospheric NO2, using absorption spectroscopy of twilight sky in the spectral region 437–451 nm, have been made at Calgary (51.08°N, 114.13°W), Alberta, Canada, during the period December 1978‐March 10, 1979. The NO2 showed a rather steady behaviour in the month of December when there was no stratospheric warming in progress; the monthly average of the afternoon vertical column abundance for December was 1.7 × 1015 cm2. In the rest of the observation period the NO2 showed a complex behaviour, but this behaviour appears to be explicable in terms of the stratospheric circulation changes taking place in that period due to the occurrence of a stratospheric warming event.  相似文献   

11.
NO2的光解速率j(NO2)是对流层化学研究中的一个重要的参数,它是对流层臭氧(O3)和OH自由基的形成关键影响因子之一。本文利用香河站2017年11月至2018年1月的观测资料对NO2的光解速率j(NO2)、太阳辐射的变化特征,及光解速率与分波段辐射相关性进行分析,在此基础上建立了一套适合于构建香河地区j(NO2)的参数化方案。结果表明,香河地区的j(NO2)与太阳辐射的变化趋势基本一致,日变化均呈正午高、早晚低的单峰型。香河地区冬季j(NO2)的变化范围是0.00046~0.0044 s-1,平均值为0.0029 s-1。j(NO2)与晴空指数(KS)和定义的紫外辐射晴空指数(KUV)存在很好的相关性,因此,利用j(NO2)与大气质量数和晴空指数的相互依赖关系,基于KUV构建了适合于香河地区j(NO2) 的估算方程。由于总辐射是气象站的常规观测要素,晴空指数KS更容易获取,继而建立了通过KS参数化计算j(NO2)的估算方程。利用KUV和KS建立的j(NO2)估算方程的瞬时估算值与观测值的平均相对误差分别为6.5%和13.9%,均方根误差分别为0.00029和0.00051。  相似文献   

12.
Surface ozone is mainly produced by the photodissociation of nitrogen dioxide (NO2) by solar UV radiation. Subsequently, solar eclipses provide one of the unique occasions to explore the variations in the photolysis rate of NO2 and their significant impact on the production of ozone at a location. This study aims to examine the diurnal variations in the photodissociation rate coefficient of NO2, (j(NO2*)), and mixing ratios of surface ozone and NO X * (NO?+?NO2*) during the solar eclipse that occurred on 15 January 2010 at Kannur (11.9°N, 75.4°E, 5?m amsl), a tropical coastal site on the Arabian Sea in South India. This investigation was carried out on the basis of the ground level observations of surface ozone and its prominent precursor NO2*. The j(NO2*) values were estimated from the observed solar UV-A flux data. A sharp decline in j(NO2*) and surface ozone was observed during the eclipse phase because of the decreased efficiency of the ozone formation from NO2. The NO2* levels were found to increase during this episode, whereas the NO levels remained unchanged. The surface ozone concentration was reduced by 57.5%, whereas, on the other hand, that of NO X * increased by 62.5% during the solar eclipse. Subsequently a reduction of *% in the magnitude of j(NO2*) was found here during the maximum obscuration. Reductions in solar insolation, air temperature and wind speed were also observed during the solar eclipse event. The relative humidity showed a 6.4% decrease during the eclipse phase, which was a unique observation at this site.  相似文献   

13.
地面热红外发射率的天顶角变化效应   总被引:1,自引:0,他引:1  
孙毅义  李治平 《气象学报》2001,59(3):373-376
文中着重研究了自然地表面的红外辐射的方向特征 ,实地测量了发射率随观测天顶角的变化 ,分别对卫星资料反演地面温度和地面辐射测量作出红外发射率的观测天顶角修正 ,两者比较的结果表明 ,发射观测天顶角修正在精确地面温度的反演计算中不可忽视 ,尤其在大角度观测情况下 ,对某些地物发射率方向特征的修正比发射率本身的修正更重要。  相似文献   

14.
Measurements of NO2, HCHO, and H2O2 were made by the highly specific method of mid infra-red absorption spectroscopy using tunable diode lasers (TDLAS) during the 1988 Polarstern expedition. The TDLAS data are compared to those obtained during the cruise using less direct methods. Southern Hemisphere NO2 levels suggest nett photochemical destruction of O3 in the boundary layer. Northern Hemisphere HCHO averaged 0.47±0.2 ppbv; the HCHO measurements are used in a simple calculation to estimate OH noontime maxima of 3–6×106 cm-3.  相似文献   

15.
The available energy (AE), driving the turbulent fluxes of sensible heat and latent heat at the earth surface, was estimated at four partly complex coniferous forest sites across Europe (Tharandt, Germany; Ritten/Renon, Italy; Wetzstein, Germany; Norunda, Sweden). Existing data of net radiation were used as well as storage change rates calculated from temperature and humidity measurements to finally calculate the AE of all forest sites with uncertainty bounds. Data of the advection experiments MORE II (Tharandt) and ADVEX (Renon, Wetzstein, Norunda) served as the main basis. On-site data for referencing and cross-checking of the available energy were limited. Applied cross checks for net radiation (modelling, referencing to nearby stations and ratio of net radiation to global radiation) did not reveal relevant uncertainties. Heat storage of sensible heat J H, latent heat J E, heat storage of biomass J veg and heat storage due to photosynthesis J C were of minor importance during day but of some importance during night, where J veg turned out to be the most important one. Comparisons of calculated storage terms (J E, J H) at different towers of one site showed good agreement indicating that storage change calculated at a single point is representative for the whole canopy at sites with moderate heterogeneity. The uncertainty in AE was assessed on the basis of literature values and the results of the applied cross checks for net radiation. The absolute mean uncertainty of AE was estimated to be between 41 and 52 W m?2 (10–11 W m?2 for the sum of the storage terms J and soil heat flux G) during mid-day (approximately 12% of AE). At night, the absolute mean uncertainty of AE varied from 20 to about 30 W m?2 (approximately 6 W m?2 for J plus G) resulting in large relative uncertainties as AE itself is small. An inspection of the energy balance showed an improvement of closure when storage terms were included and that the imbalance cannot be attributed to the uncertainties in AE alone.  相似文献   

16.
This study explores the influence of air gaseous pollutants–aerosols and solar zenith angle (SZA) on the spectral diffuse-to-direct beam E /E irradiances ratio. It does so using ground-based spectroradiometric measurements taken over the Athens atmosphere during May 1995. It was found that the spectral E /E ratio decreases rapidly with increasing wavelength and regression curves of the form E /E  = aλ?b fitted the experimental data. These curves are strongly modified by aerosols–air pollutants, aerosol optical properties, and SZA. The log–log plot of E /E versus λ reveals a significant departure from linearity, which is likely to be associated with aerosol physical properties and SZA effects. The effect of atmospheric turbidity, as expressed through the aerosol optical at 500 nm and SZA on the spectral E /E ratio, is investigated in detail for two discernible atmospheric conditions observed in the urban Athens atmosphere. The first case includes different atmospheric turbidity levels under the same SZA, while the second corresponds to different SZA values under the same turbidity levels. It was found that the correlation between E /E and spectral aerosol optical depth can be a useful tool in determining the aerosol optical properties and aerosol types composition.  相似文献   

17.
Measurements of the photodissociation constant for nitrous acid (j HONO) were made at an urban site in Toronto, Canada, during the months of May–July 2005, using an optically thin actinometer. Operating details of the j HONO monitor are reported, along with laboratory tests. Measurements of j HONO were obtained for solar zenith angles ranging from 20–75, under clear and cloudy skies. Maximum error estimates on j HONO under clear skies range from 11% at sunrise, to 4% at solar noon, with a minimum detection limit of 5.7 × 10−4/sec for our actinometer. Measured clear-sky values of j HONO were compared with values calculated by a four-stream discrete ordinate radiative transfer (RT) model (ACD TUV version 4.1), and were found to be within better than 10% agreement for solar zenith angles < 65. For conditions of scattered cloud, enhancement and suppression of the j HONO values occurred by as much as 16%–70%, and 59%–80%, respectively. The integrated band area of the nπ transition for gas-phase nitrous acid yields an oscillator strength, f = (1.06 ± 0.044)×10−3 (based on clear-sky data), 19.1% higher than the value reported by Bongartz et al. (1991).  相似文献   

18.
A new version of an atmospheric pressure chemical ionisation mass spectrometer has been developed for ground based in situ atmospheric measurements of OH and total peroxy (HO2 + organic peroxy) radicals. Based on the previously developed principle of chemical conversion of OH radicals to H2SO4 in reaction with SO2 and detection of H2SO4 using an ion molecule reaction with NO3, the new instrument is equipped with a turbulent chemical conversion reactor allowing for measurements in moderately polluted atmosphere at NO concentrations up to several ppb. Unlike other similar devices, where the primary NO3 ions are produced using radioactive ion sources, the new instrument is equipped with a specially developed corona discharge ion source. According to laboratory measurements, the overall accuracy and detection limits are estimated to be, respectively, 25% and 2 × 105 molecule cm-3 for OH and 30% and 1 × 105 molecule cm-3 for HO2 at 10 min integration times. The detection limit for measurements of OH radicals under polluted conditions is 5 × 105 molecules cm-3 at 10 min integration times. Examples of ambient air measurements during a field campaign near Paris in July 2007 are presented demonstrating the capability of the new instrument, although with reduced performance due to the employment of non isotopic SO2.  相似文献   

19.
The interpretation of atmospheric measurements and the forecasting of the atmospheric composition require a hierarchy of accurate chemical transport and global circulation models. Here, the results of studies using Bremens Atmospheric Photochemical Model (BRAPHO) are presented. The focus of this study is given to the calculation of the atmospheric photolysis frequencies It is shown that the spectral high resolved simulation of the O2 Schumann–Runge bands leads to differences in the order of 10% in the calculated O2 photolysis frequency when compared with parameterizations used in other atmospheric models. Detailed treatment of the NO absorption leads to even larger differences (in the order of 50%) compared to standard parameterizations. Refraction leads to a significant increase in the photolysis frequencies at large solar zenith angles and, under polar spring conditions, to a significant change in the nighttime mixing ratio of some trace gases, e.g., NO3. It appears that recent changes in some important rate constants significantly alter the simulated BrOx- and HOx-budgets in the mid-latitude stratosphere.  相似文献   

20.
Plants require solar radiation for photosynthesis and their growth is directly related to the amount received, assuming that other environmental parameters are not limiting. Therefore, precise estimation of photosynthetically active radiation (PAR) is necessary to enhance overall accuracies of plant growth models. This study aimed to explore the PAR radiant flux in the San Francisco Bay Area of northern California. During the growing season (March through August) for 2?years 2007?C2008, the on-site magnitudes of photosynthetic photon flux densities (PPFD) were investigated and then processed at both the hourly and daily time scales. Combined with global solar radiation (R S) and simulated extraterrestrial solar radiation, five PAR-related values were developed, i.e., flux density-based PAR (PPFD), energy-based PAR (PARE), from-flux-to-energy conversion efficiency (fFEC), and the fraction of PAR energy in the global solar radiation (fE), and a new developed indicator??lost PARE percentages (LPR)??when solar radiation penetrates from the extraterrestrial system to the ground. These PAR-related values indicated significant diurnal variation, high values occurring at midday, with the low values occurring in the morning and afternoon hours. During the entire experimental season, the overall mean hourly value of fFEC was found to be 2.17???mol?J?1, while the respective fE value was 0.49. The monthly averages of hourly fFEC and fE at the solar noon time ranged from 2.15 in March to 2.39???mol?J?1 in August and from 0.47 in March to 0.52 in July, respectively. However, the monthly average daily values were relatively constant, and they exhibited a weak seasonal variation, ranging from 2.02?mol?MJ?1 and 0.45 (March) to 2.19?mol?MJ?1 and 0.48 (June). The mean daily values of fFEC and fE at the solar noon were 2.16?mol?MJ?1 and 0.47 across the entire growing season, respectively. Both PPFD and the ever first reported LPR showed strong diurnal patterns. However, they had opposite trends. PPFD was high around noon, resulting in low values of LPR during the same time period. Both were found to be highly correlated with global solar radiation R S, solar elevation angle h, and the clearness index K t. Using the best subset selection of variables, two parametric models were developed for estimating PPFD and LPR, which can easily be applied in radiometric sites, by recording only global solar radiation measurements. These two models were found to be involved with the most commonly measured global solar radiation (R S) and two large-scale geometric parameters, i.e., extraterrestrial solar radiation and solar elevation. The models were therefore insensitive to local weather conditions such as temperature. In particular, with two test data sets collected in USA and Greece, it was verified that the models could be extended across different geographical areas, where they performed well. Therefore, these two hourly based models can be used to provide precise PAR-related values, such as those required for developing precise vegetation growth models.  相似文献   

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