Supplemental Material Table 1

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1 Supplemental Material Table. CLARS FTS Measurement Sequence Target Coordinate Target Name Measurement Mode Latitude Longitude Altitude index (degree) (degree) (meter). -. Spectralon SVO. -. Fontana LABS. -. Rancho Cucamunga LABS. -. Riverside LABS. -. Lake Matt LABS. -. Norco LABS. -. Pomona LABS. -. Bend LABS. -. Corona LABS. -. Spectralon SVO. -. North OC LABS. -. Industry LABS. -. SantaFe Dam LABS. -. OC airport LABS. -. Angels Stadium LABS. -. Spectralon SVO. -. Huntinghton beach LABS. -. La Mirada LABS. -. and LABS. -. Santa Anita Park LABS. -. Long Beach LABS. -. Downey LABS. -. ELA water LABS. -. Spectralon SVO. -. Palos Verdes LABS. -. Marina Del Rey LABS. -. Down Town Far LABS. -. Down Town Near LABS. -. Santa Monica LABS. -. Mountains Glendale LABS. -. west Pasadena LABS. -. Universal City LABS Spectralon Viewing Observations Los Angeles Basin Surveys

SVO SVO CLARS CLARS LABS LABS Mt. Mt. Wilson Wilson T T Tn Los Angeles Air Basin Los Angeles Basin Supplemental Material MaterialFigure Figure. Upper.

2 SVO SVO CLARS CLARS LABS LABS Mt. Mt. Wilson Wilson T T Tn Los Angeles Air Basin Los Angeles Basin Supplemental Material MaterialFigure Figure. Upper. (Upper Schematic of spectrometer panel:panel) Schematic diagramdiagram of spectrometer (altitude (altitude of. km) viewing geometry for Los Angeles Basin Surveys (LABS) and of. km) viewing geometry for Los Angeles Basin Surveys (LABS) and Spectralon Spectralon Viewing Observations. (lower the target site location observations of CLARS-FTS Viewing Observations; lower panel: the targetpanel) site location of CLARS-FTS in a observations a measurement over Los Blue balloon measurement in sequence over Los sequence Angeles Basin. BlueAngeles balloon Basin. indicates CLARS site;indicates Yellow CLARS site; Yellow pins showed the The targetmeasurement site location.sequence The measurement sequencedaily is being pins showed the target site location. is being repeated for repeated daily for ~- times. The sequences can be changed to accommodate the needs of ~- times. The sequences can be changed to accommodate the needs of special observations. special observations.

3 Residuals (%) (Solar Transmittance.) X. (H O Transmittance.) X. (CO Transmittance.) Wavenumber (cm ) Supplemental Material Figure. Zoom-in view of MW spectral fitting residuals (black curve) and scaled transmittances of solar spectrum (red curve), major interfering trace gases (green curve: H O spectral features), and CO spectral features (blue curve) within the spectral segments. (top panels) for the measurements over CLARS site; (middle panels) for the measurements along the light path of pointing at the Santa Anita Race Track; and (bottom panels) for the measurements along the light path of pointing at the west Pasadena.

4 Residuals (%) (Solar Transmittance.) X. (H O Transmittance.) X. (CO Transmittance.) Wavenumber (cm ) Supplemental Material Figure. Zoom-in view of MW spectral fitting residuals (black curve) and scaled transmittances of solar spectrum (red curve), major interfering trace gases (green curve: H O spectral features), and CO spectral features (blue curve) within the spectral segments. (top panels) for the measurements over CLARS site; (middle panels) for the measurements along the light path of pointing at the Santa Anita Race Track; and (bottom panels) for the measurements along the light path of pointing at the west Pasadena.

5 XCO (ppm) XCO (ppm) XCO (ppm) MW. MW..... XCO (ppm) XCO (ppm) XCO (ppm) MW.+/.ppm.+/.ppm.+/.ppm Supplemental Material Figure. XCO (in parts per million (ppm)) measured by CLARS- FTS with MW (black dots) and MW (blue circles) on January th, (left panels) and differences of retrieved XCO between the two spectral regions and the histograms (right panels) in the Spectralon viewing geometry (top panels), towards the Arcadia Race Track (middle panels); and towards west Pasadena (bottom panels). Black stars in left panels: XCO obtained using the spectral region of MW. Compared to the background levels of XCO (top panels), XCO over Arcadia Race Track (middle panels) and west Pasadena (bottom panels) show higher values (mean ART-SV:. ppm; mean WP-SV:. ppm) and present stronger diurnal cycles than those measurements over CLARS site. The XCO values retrieved from MW are higher than those of MW. The mean differences between MW and MW are. ppm,. ppm, and. ppm for SV, ART and WP measurements respectively. It was also appeared in the spectral analyses of the TCCON measurements (~. ppm). Both CLARS-FTS and TCCON results, which are using HITRAN line list, show improvements on the band-to-band consistency of XCO, compared to those of using HITRAN line list such as Figure of Washenfelder et al. () with the XCO using MW about. ppm higher than that of MW. These systematic differences of retrieved XCO values between two spectral bands are likely arisen from the discrepancies of spectroscopic parameters between two spectral bands and the amount/intensity of spectral features of interfering species.

6 Resiudal RMS(%) Residual RMS(%) Spectral SNR Spectral SNR Residual RMS(%)..... Spectral SNR Supplemental Material Figure. Root Mean Square (RMS) of spectral fitting residuals (Left panels) and spectral SNR (Right panels) for CO slant column density measurements as a function of time in Spectralon viewing geometry (Top panels); over the Arcadia Race Track (Middle panels); over west Pasadena (Bottom panels). Three spectral bands centered at cm - (black stars, noted as MW thereafter), cm - (blue circles, noted as MW thereafter) and cm - (gold triangles, noted as MW thereafter) are presented, respectively. The spectral SNR were nearly identical over the three spectral bands. The measurements were performed on January th,. The spectral fitting residuals were normalized by the spectral continuum levels prior to the computation of RMS values. The spectral fitting residuals were dominated by the photon shot noise. The RMS of the spectral fitting residuals in both CO bands are reasonably close to the expected values. The Chisquared tests of spectral fitting residuals yielded values generally within..

7 Residuals (%) (Solar Transmittance.) X. (H O Transmittance.) X. (CH Transmittance.) Wavenumber (cm ) Supplemental Material Figure. Zoom-in view of MW spectral fitting residuals (black curve) and scaled transmittances of solar spectrum (red curve), major interfering trace gases (green curve: H O spectral features), and CH spectral features (blue curve) within the spectral segments. (Top panels) for the measurements over CLARS site; (middle panels) for the measurements along the light path of pointing at the Santa Anita Race Track; and (bottom panels) for the measurements along the light path of pointing at the west Pasadena.

8 Residuals (%) (Solar Transmittance.) X. (H O Transmittance.) X. (CH Transmittance.) Wavenumber (cm ) Supplemental Material Figure. Zoom-in view of MW spectral fitting residuals (black curve) and scaled transmittances of solar spectrum (red curve), major interfering trace gases (green curve: H O spectral features) ), and CH spectral features (blue curve) within the spectral segments. (Top panels) for the measurements over CLARS site; (middle panels) for the measurements along the light path of pointing at the Santa Anita Race Track; and (bottom panels) for the measurements along the light path of pointing at the west Pasadena.

9 XCH (ppb) XCH (ppb) XCH (ppb) MW. MW..... XCH (ppb) XCH (ppb) XCH (ppb) MW.+/.ppb.+/.ppb.+/.ppb Supplemental Material Figure. XCH (in parts per billion (ppb)) measured by CLARS- FTS with MW (black dots) and MW (blue circles) on January th, (left panels) and differences of retrieved XCH between the two spectral regions and the histograms (right panels) in the Spectralon Viewing geometry (top panels), towards the Arcadia Race Track (middle panels); and towards west Pasadena (bottom panels). Black stars in left panels: XCH obtained using the spectral region of MW. Compared to the background levels of XCH (top panels), XCH over Arcadia Race Track (middle panels) and west Pasadena (bottom panels) show higher values (mean ART-SV:. ppb; mean WP- SV:. ppb) and present stronger diurnal cycles than those measurements over CLARS site. The XCH values retrieved from MW are higher than those of MW. The mean differences between MW and MW are. ppb,. ppb, and. ppb for SV, ART and WP respectively. These systematic differences of retrieved XCH values between two spectral bands are likely arisen from the discrepancies of spectroscopic parameters between two spectral bands and the amount/intensity of spectral features of interfering species.

10 Resiudal RMS(%) Residual RMS(%) Spectral SNR Spectral SNR Residual RMS(%) Spectral SNR Supplemental Material Figure. Root Mean Square (RMS) of spectral fitting residuals (left panels) and spectral SNR (right panels) as a function of time for the measurements of CH and O column densities in Spectralon viewing geometry (top panels); over the Arcadia Race Track (middle panels); over west Pasadena (bottom panels). Three spectral bands centered at cm - (black stars, noted as MW thereafter), cm - (blue circles, noted as MW thereafter) and cm - (gold triangles, noted as MW thereafter) are presented, respectively. The spectral SNR were nearly identical over the three spectral bands within a measured spectrum, but varies among spectra. The measurements were performed on January th,. The spectral fitting residuals were normalized by the spectral continuum levels prior to the computation of RMS values. The spectral fitting residuals were dominated by the photon shot noise since the RMS of the spectral fitting residuals in both CH bands are reasonably close to the expected values, i.e., /(spectral SNR). The Chi-squared tests of spectral fitting residuals yielded values generally within..

11 Resiudal RMS(%) Residual RMS(%) Spectral SNR Spectral SNR Residual RMS(%)..... Spectral SNR Supplemental Material Figure. Root Mean Square (RMS) of spectral fitting residuals (left panels) and spectral SNR (right panels) as a function of time for the measurements of CO and O column densities in Spectralon viewing geometry (top panels); over the Arcadia Race Track (middle panels); over west Pasadena (bottom panels). Three spectral regions near. µm centered at cm - (black stars, noted as MW thereafter), cm - (blue circles, noted as MW thereafter) and O band near. µm centered at cm - (gold triangles, noted as MW thereafter) are presented, respectively. The spectral SNR were nearly identical over the three spectral bands within a measured spectrum, but varies among spectra. The measurements were performed on January rd,. The spectral fitting residuals were normalized by the spectral continuum levels prior to the computation of RMS values. The strong absorption of inferring gases other than CO gas in MW and MW made spectral fitting residuals be larger than that of CO CH, and O. Previous studies reported similar phenomena.

12 XCO (ppb) XCO (ppb) XCO (ppb) MW. MW..... XCO (ppb) XCO (ppb) XCO (ppb) MW.+/.ppb.+/.ppb.+/.ppb Supplemental Material Figure. XCO (in parts per billion (ppb)) measured by CLARS- FTS with MW (black dots) and MW (blue circles) on January th, (left panels) and differences of retrieved XCO between the two spectral regions and the histograms (right panels) in the Spectralon viewing geometry (top panels), towards the Arcadia Race Track (middle panels); and towards west Pasadena (bottom panels). Compared to the background levels of XCO (top panels), XCO over Arcadia Race Track (middle panels) and west Pasadena (bottom panels) show higher values (mean ART-SV:. ppb; mean WP- SV:. ppb) and present stronger diurnal cycles than those measurements over CLARS site. The XCO values retrieved from MW are higher than those of MW. The mean differences between MW and MW are. ppb,. ppb, and. ppb for SV, ART and WP respectively. These systematic differences of retrieved XCO values between two spectral bands are likely arisen from the discrepancies of spectroscopic parameters between two spectral bands and the amount/intensity of spectral features of interfering species.

Introduction of Anmyeondo FTS Station as a New TCCON Site

Introduction of Anmyeondo FTS Station as a New TCCON Site Tae-Young GOO, Young-Suk OH, Jin-Ho Shin, Mi-Lim OU, and Chun-Ho CHOI Global Environment System Research Division National Institute of Meteorological