光子学报
光子學報
광자학보
ACTA PHOTONICA SINICA
2010年
10期
1889-1895
,共7页
彭夫敏%罗涛%袁玉鹏%裘灵光%谢品华%刘文清
彭伕敏%囉濤%袁玉鵬%裘靈光%謝品華%劉文清
팽부민%라도%원옥붕%구령광%사품화%류문청
长光程差分吸收光谱%乙二醛%挥发性有机物%光谱插值
長光程差分吸收光譜%乙二醛%揮髮性有機物%光譜插值
장광정차분흡수광보%을이철%휘발성유궤물%광보삽치
Long Path Differential Optical Absorption Spectroscopy (LP-DOAS)%Glyoxal%Volatile organic compounds (VOCs)%Spectral interpolation
针对利用长光程差分吸收光谱技术在实现对大气中乙二醛实时监测中,一些干扰结构(Xe灯结构,H2O、NO2和O4干扰吸收)对长光程差分吸收光谱技术的影响,讨论了乙二醛的光谱反演方法对干扰吸收的准确去除.针对Xe灯结构由于压力和多普勒展宽程度等的变化而引起的Xe灯结构的非线性变化,采用不同时刻的参考灯谱通过光谱插值的方式准确去除,其去除误差引起的剩余结构可降低到比乙二醛的最低理论检测限低3倍;针对H2O的非线性吸收以及特征吸收结构随柱浓度的不同而变化的特点,采用较高和较低浓度H2O吸收光谱插值的方法准确去除了严重干扰乙二醛准确反演的H2O的吸收结构,其去除误差引起的剩余结构可降低到比乙二醛的最低理论检测限低10倍;另外,对于在此波段存在干扰的NO2和O4的吸收结构也实现了准确地去除.干扰结构的准确去除使DOAS对乙二醛的监测实现了较低的实际检测限 (0.15 ppbv)和较低的测量误差 (~10 %).最后,在广州郊区对实际大气进行了实际监测,其浓度范围在低于检测限到1.66 ppbv之间,与文献报道的浓度范围和变化趋势十分吻合.
針對利用長光程差分吸收光譜技術在實現對大氣中乙二醛實時鑑測中,一些榦擾結構(Xe燈結構,H2O、NO2和O4榦擾吸收)對長光程差分吸收光譜技術的影響,討論瞭乙二醛的光譜反縯方法對榦擾吸收的準確去除.針對Xe燈結構由于壓力和多普勒展寬程度等的變化而引起的Xe燈結構的非線性變化,採用不同時刻的參攷燈譜通過光譜插值的方式準確去除,其去除誤差引起的剩餘結構可降低到比乙二醛的最低理論檢測限低3倍;針對H2O的非線性吸收以及特徵吸收結構隨柱濃度的不同而變化的特點,採用較高和較低濃度H2O吸收光譜插值的方法準確去除瞭嚴重榦擾乙二醛準確反縯的H2O的吸收結構,其去除誤差引起的剩餘結構可降低到比乙二醛的最低理論檢測限低10倍;另外,對于在此波段存在榦擾的NO2和O4的吸收結構也實現瞭準確地去除.榦擾結構的準確去除使DOAS對乙二醛的鑑測實現瞭較低的實際檢測限 (0.15 ppbv)和較低的測量誤差 (~10 %).最後,在廣州郊區對實際大氣進行瞭實際鑑測,其濃度範圍在低于檢測限到1.66 ppbv之間,與文獻報道的濃度範圍和變化趨勢十分吻閤.
침대이용장광정차분흡수광보기술재실현대대기중을이철실시감측중,일사간우결구(Xe등결구,H2O、NO2화O4간우흡수)대장광정차분흡수광보기술적영향,토론료을이철적광보반연방법대간우흡수적준학거제.침대Xe등결구유우압력화다보륵전관정도등적변화이인기적Xe등결구적비선성변화,채용불동시각적삼고등보통과광보삽치적방식준학거제,기거제오차인기적잉여결구가강저도비을이철적최저이론검측한저3배;침대H2O적비선성흡수이급특정흡수결구수주농도적불동이변화적특점,채용교고화교저농도H2O흡수광보삽치적방법준학거제료엄중간우을이철준학반연적H2O적흡수결구,기거제오차인기적잉여결구가강저도비을이철적최저이론검측한저10배;령외,대우재차파단존재간우적NO2화O4적흡수결구야실현료준학지거제.간우결구적준학거제사DOAS대을이철적감측실현료교저적실제검측한 (0.15 ppbv)화교저적측량오차 (~10 %).최후,재엄주교구대실제대기진행료실제감측,기농도범위재저우검측한도1.66 ppbv지간,여문헌보도적농도범위화변화추세십분문합.
When measuring glyoxal directly in the atmosphere by Long Path Differential Optical Absorption Spectroscopy (LP-DOAS), the analysis of glyoxal strongly suffers from the cross interference of other absorbers or structure (Xe lamp-structure, H2O, O4 and NO2 absorption). The retrieval method of glyoxal-the elimination of interfering absorption or structure was studied. The Xe lamp-structure will change nonlinearly resulted from the change of pressure broadening and Doppler Broadening with the change of of Xe lamp pressure or temperature. The different lamp reference spectra detected at different time were interpolated to eliminate lamp structure and the resulting residual structures caused by an incorrect elimination were a factor of three below the detection limit of glyoxal; high amount of H2O in the atmosphere cause the nonlinear absorption of H2O and the observed band shape to vary with the column density of H2O. Two H2O absorption spectra with higher and lower column density were interpolated to eliminate nonlinear H2O absorption and the resulting residual structures caused by an incorrect elimination were ten times below the detection limit of glyoxal. In addition, the strong absorption of interfering species NO2 and O4 were also accurately removed. Low detection limit (0.15 ppbv) and low systematic errors (~10 %) were achieved by the accurate elimination of interfering structures. In the end, glyoxal was routinely detected during the daytime on the outskirts of Guangzhou, where mixing ratios ranged from less than detection limit (0.15 ppbv) to 1.66 ppbv. The variation and range of glyoxal concentration detected agreed well with the results reported.