First results from the far-infrared beamline at the Canadian Light Source: High resolution analysis of acrolein in the 600 cm -1 region A.R.W. McKellar.

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Presentation transcript:

First results from the far-infrared beamline at the Canadian Light Source: High resolution analysis of acrolein in the 600 cm -1 region A.R.W. McKellar National Research Council of Canada D.W. Tokaryk, L.-H. Xu University of New Brunswick D.R.T. Appadoo, T. May Canadian Light Source Centre for Laser, Atomic, and Molecular Sciences University of New Brunswick

First results from the far-infrared beamline at the Canadian Light Source: High resolution analysis of acrolein in the 600 cm -1 region A.R.W. McKellar National Research Council of Canada D.W. Tokaryk, L.-H. Xu University of New Brunswick D.R.T. Appadoo, T. May Canadian Light Source

Canadian Light Source Saskatoon, Saskatchewan

Where is Saskatoon?

CLS Parameters Energy: 2.9 GeV Current: 200 mA Circumference: 171 m 12 straight sections, 5.2 m long RF: 500 MHz, 2.4 MV, supercon Injection: 250 MeV LINAC full energy booster ring Main building: ~ 85 x 85 m

Synchrotron IR There are two infrared beamlines at CLS: 1) Far IR (this talk) 2) Mid IR spectromicroscopy (biological / industrial samples) All other CLS beamlines are for x-rays The synchrotron simply replaces the normal source (globar), providing continuum IR radiation to a conventional FTIR spectrometer The high brightness of synchrotron radiation is ideal for the small entrance aperture required for high spectral resolution Bruker IFS 125 HR spectrometer: max optical path difference = 9.4 m; instrumental resolution ~ cm -1 (24 MHz)

Energy / cm -1 SR 23 SR 27 Hg SR 27 /Hg SR 23 /Hg (SR is normalized to 202 mA) SR 23 : Synch. Radiation Run 23 SR 27 : Synch. Radiation Run 27 Hg: internal Hg lamp Synchrotron brightness advantage (the good news)

SR 23 Hg Synchrotron noise (the bad news)

Clearly signal-to-noise ratio is the important factor Our problem is mechanical vibrations in the optics that bring IR radiation from the storage ring to the spectrometer Ring Source Diamond Window Spectrometer Shielding Wall

With successive improvements, the synchrotron now has a significant advantage over the globar from 250 ~ 800 cm -1 But we are aiming for much better performance Reduce noise at source: better isolation of offending cooling pumps, heat exchangers, pipe runs, etc. Reduce noise at beamline: more isolation, better mounting of mirrors Active optics to stabilize the input radiation on the spectrometer aperture

Acrolein CH 2 CHCHO A B C fundamental 8-atom species planar near-prolate asymmetric rotor interstellar molecule combustion byproduct (cigarette smoke) potent respiratory irritant (smog)

17 band of acrolein, CH 2 CHCHO K a = 7 – 6 Q-branch nominal resolution cm -1

Acrolein: center of the 17 band

Acrolein: q Q-branch, center of the 12 band

Acrolein: local perturbation of 17 K a = 13 levels around J = 30, explained by crossing with K a = 13 of 4 18

Ground state v0v (1) (1) (16) A (15) (12) (23) B (44) (44) (42) C (15) (10) (42) x D K (33) (26)-8.303(57) x D JK (74) (20) x D J (71)3.5101(30) x  K 2.18(17)2.09(10) x  J 3.855(63)3.917(33) x H K (49) G a (12,17) (75) G b (12,17) (14) 10 5 x Z 1 (12,17) (37) 10 4 x Z 3 (12,17) -4.29(68) 10 3 x G a (17,18 4 ) 6.533(24) 10 7 x Z 5 (17,18 4 ) -4.17(25) Acrolein: ~2000 lines of the 12 & 17 bands represented in terms of 25 parameters (including ‘dark’ state 4 18 )

Acrolein: local perturbations of K a = 8 and 14 levels of 17 remain unexplained

Acrolein: recently we also studied the 18 fundamental band at 158 cm -1

Acrolein 18 central region

18 Ground state* v0v (1) A (10) B (21) C (17) xDKDK (8) xD JK (8) xDJDJ 3.642(7) x KK -0.08(20) x JJ 4.11(5) xHKHK (28) xH KJ 6.6(31) xLKLK 2.824(27) * Winnewisser, Winnewisser, Honda, & Hirota, Z. Naturforsch. 30a, 1001 (1975) Acrolein 18 parameters

High-resolution synchrotron IR Previous results from MAXlab and LURE were promising -- we hope to do better Presently at CLS: 100 – 200 cm -1 region: SR is ~ 4 times better 250 – 700 cm -1 region: SR is ~ 8 times better Other new synchrotrons (SOLEIL, Australia, Switzerland, Singapore,...) are building hi-res IR facilities Are we the first synchrotron user facility for high- resolution IR spectroscopy of gases ?