INTRACAVITY LASER SPECTRA OF METHANE 790 AND 861 nm BANDS AT LOW TEMPERATURES SADASIVAN SHAJI and JAMES J O’BRIEN Department of Chemistry & Biochemistry.

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Presentation transcript:

INTRACAVITY LASER SPECTRA OF METHANE 790 AND 861 nm BANDS AT LOW TEMPERATURES SADASIVAN SHAJI and JAMES J O’BRIEN Department of Chemistry & Biochemistry and Center for Nanoscience, University of Missouri, St. Louis, MO

Methane is an important component in the atmospheres of giant planets and their major satellites Laboratory spectral data at low temperatures are required to interpret the planetary data properly Methane spectrum in near-IR region is intrinsically very weak and hence a very sensitive method like intracavity laser spectroscopy (ILS) is needed Absorption lines appear superimposed on the output of the laser which is operated in a time-modulated fashion ILS enhances the sensitivity with its tremendous 'effective pathlength' > 100 km being achieved easily ILS is both ultrasensitive and quantitative method for acquiring weak absorption spectra Introduction "The lakes of Titan" Nature, vol.445, p 61, 2007

Schematic diagram for the intracavity laser spectrometer FM=fold mirror; HR=high reflector; OC=output coupler; AOM=acousto-optic modulator

Schematic of the four walled Cryogenic chamber

Pressure and temperatures of the sample cell for the effective temperature 161 K (-112 ° C) when the set-point temperature is 148 K (-125 °C)

Pressure and temperatures of the sample cell for the effective temperature 131 K (-142 ° C) when the set-point temperature is 108 K (-165 °C)

Pressure and temperatures of the sample cell for the effective temperature 99 K (-174 ° C) when the set- point temperature is 77 K (-196 °C)

Plots indicating the linearity of the ILS results as a function of (a) path length (methane pressure is 8.1 torr) and (b) pressure for a section of the methane (generation time 40 microsec) around cm -1 at 99 K (a) (b)

Plots indicating the linearity of the ILS results as a function of (a) path length (methane pressure is 8.3 torr) and (b) pressure for a section of the methane (generation time 30 microsec) around cm -1 at 131 K (a)(b)

Plots indicating the linearity of the ILS results as a function of (a) path length (methane pressure is 7.3 torr) and (b) pressure for a section of the methane (generation time 30 microsec) around cm -1 at 161 K (a)(b)

A section of the methane 790 nm band around cm -1 at 99K, 131 K and 161 K

A section of the methane 790 nm band around cm -1 normalized to a sample pressure of 4 torr and 4 km pathlength at 99 K, 131 K and 161 K

A section of 99 K Methane spectrum in the 790 nm band showing the original and deconvolved data. The spectrum is normalized to methane conditions of 4 torr and 4 km

Methane absorption coefficients for the 790 nm band averaged per Å derived from ILS spectra of methane at 161 K, 131 K and 99 K.

Methane absorption coefficients for the 790 nm band averaged per cm -1 derived from ILS spectra of methane at 161 K, 131 K and 99 K.

Methane absorption coefficients for the 790 nm band averaged per nm interval derived from ILS spectra of methane at 161 K, 131 K and 99 K.

A section of the methane 861 nm band around cm -1 normalized to a sample pressure of 4 torr and 4 km pathlength at 99 K, 131 K and 161 K

Methane absorption coefficients for the 861 nm band averaged per Å derived from ILS spectra of methane at 161 K, 131 K and 99 K.

Methane absorption coefficients for the 861 nm band averaged per cm -1 derived from ILS spectra of methane at 161 K, 131 K and 99 K.

Methane absorption coefficients for the 861 nm band averaged per nm interval derived from ILS spectra of methane at 161 K, 131 K and 99 K.

Methane 790 and 861 nm band strengths (cm -1 km -1 am -1 ) a comparison 790 nm band861 nm band Karkoschka & Tomasco (R.T) Karkoschka & Tomasco cold temperature (  K, Saturn’s upper troposphere) Ramaprasad et al. (liquid phase) 450 ± ±-300 Ramaprasad et al (calculated gas phase methane) Giver (R T)469±14871 ± 45 ILS (R.T) ILS (77K)638 ILS (161 K) ILS (131 K) ILS (99K) James J O’Brien and Hong Cao, JQSRT 75 (2002)

A four-walled cryogenic chamber for low temperature ILS studies is used to collect the methane spectra The effective temperature in the chamber is in good agreement with that calculated from the gas laws. Linearity of the ILS results as a function of pathlength and pressure are verified at three low temperatures. Methane spectra recorded for 790 and 861 nm bands at different low sample temperatures. Absorption coefficients for the 790 and 861 nm bands at three low temperatures are determined. Conclusions

Acknowledgements Support from NASA’s Planetary Atmospheres Program (NAG ) is gratefully acknowledged. Additional supplemental funding from National Science Foundation (CHE ) and University of Missouri Research Board for the Verdi laser is gratefully acknowledged. Thank you

Å 161 K131 K99 K 7551,56 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , nm band

7603,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , ,

7659,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,5 0, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , ,

7713,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , ,

7769,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 1, , , ,5 0, , , ,50, , , ,50, , , ,50, , , ,50, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,50, , , ,51, , , ,51, , , ,51, , , ,50, , , ,51, , , ,50, , , ,50, , , ,51, , , ,50, , , ,51, , , ,50, , , ,50, , ,

7826,5 1, , , ,5 0, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 2, , , ,5 1, , , ,5 1, , , ,5 2, , , ,5 1, , , ,5 2, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 0, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 0, , , ,5 1, , , ,5 0, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 0, , , ,51, , , ,50, , , ,50, , , ,51, , , ,51, , , ,50, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,50, , , ,50, , , ,51, , , ,51, , , ,51, , , ,50, , , ,50, , , ,50, , , ,51, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , ,

7886,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,50, , , ,51, , , ,50, , , ,50, , , ,50, , , ,51, , , ,50, , , ,51, , , ,51, , , ,50, , , ,50, , , ,51, , , ,51, , , ,50, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,50, , , ,51, , , ,50, , , ,51, , , ,51, , , ,50, , , ,51, , , ,51, , ,

7942,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 0, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,52, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,52, , , ,51, , , ,51, , ,

7997,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 2, , , ,5 2, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 0, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,5 1, , , ,50, , , ,51, , , ,51, , , ,51, , , ,50, , , ,51, , , ,51, , , ,51, , , ,51, , , ,50, , , ,51, , , ,50, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,51, , , ,50, , , ,50, , , ,50, , , ,5 0, , ,

8052,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , , ,50, , ,

8108,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,5 0, , , ,2 0, , ,

Å161 K131 K99 K nm band