rotationally resolved a 2 a 1 - x 2 e electronic spectra of symmetric methoxy radicals: ch 3 o and...
TRANSCRIPT
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ROTATIONALLY RESOLVED A2A1 - X2E ELECTRONIC SPECTRA OF
SYMMETRIC METHOXY RADICALS: CH3O AND CD3O (RI08)
MING-WEI CHEN, JINJUN LIU, DMITRY G. MELNIK and TERRY A. MILLER
Laser Spectroscopy FacilityDepartment of ChemistryThe Ohio State University
6/19/2008
~ ~
63rd OSU International Symposium on Molecular Spectroscopy
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Outline
Subsequent talk: Isotope dependence. Asymmetrically deuterated isotopomers.
Subsequent talk: Isotope dependence. Asymmetrically deuterated isotopomers.
Present talk: Motivations and aims. Experiment.
Doable experimental apparatus for both Laser Induced Fluorescence (LIF) and Stimulated Emission Pumping (SEP).
Calibration method. Spectroscopy of CH3O and CD3O.
Global fitting and spectral analysis. Model compounds for other isotopomers.
Summary.
Present talk: Motivations and aims. Experiment.
Doable experimental apparatus for both Laser Induced Fluorescence (LIF) and Stimulated Emission Pumping (SEP).
Calibration method. Spectroscopy of CH3O and CD3O.
Global fitting and spectral analysis. Model compounds for other isotopomers.
Summary.
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Motivations and Aims
Alkoxy radicals (RO·) are key components in the oxidation of hydrocarbons both in combustion and in the atmosphere.
Methoxy (CH3O·), the smallest alkoxy radical is an interesting molecule which has very significant theoretical interest due to the Jahn-Teller effect coupled to spin-orbit interaction, the former is also relevant to conical intersection for chemical reactions.
Benchmark for ab initio calculations and standard for isotopic analysis.
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Spectroscopy of Methoxy Radicals
~2
1AA
~2
1/2EX~
23/2EX
LIF3
SEP
~2
1/2EX
~2
3/2EX
Microwave1,2
1Y. Endo, S. Saito, and E. Hirota, J. Chem. Phys. 81, 122, (1984) 2T. Momose, Y. Endo, E. Hirota, and T. Shida, J. Chem. Phys. 88, 5338 (1988)
5J. Liu, J. T. Yi, V. Starkursky, and T. A. Miller, 61st International Symposium on Molecular Spectroscopy, TJ04&05 (2006).
3D. E. Powers, M. B. Pushkarsky, and T. A. Miller, J. Chem. Phys. 106, 6863 (1997)
resolution~250MHz
resolution~3GHz
4A. Geers, J. Kappert, F. Temps, and J. W. Wiebrecht, J. Chem. Phys. 101, 3618 (1994)
ΔΣ=0ΔP=0
SEP4
~60 cm-1
LIF5
ΔP=±1ΔΣ=±1
p+1-1
Reflection parity (p): Reflection partity (p):
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|J',N', K',p'>
|1/2,0,0,1>
|J",P",Σ",p">
|3/2,3/2,1/2,±1>
|3/2,1/2,-1/2,±1>
|1/2,1/2,-1/2,±1>
|5/2,3/2,1/2,±1>
Pump
Dump
p+1-1
21/ 2X E
21A A
23/ 2X E
Rotationally Resolved SEP
Hund’s case (a)
Hund’s case (b)
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Experimental Apparatus: Overview
CH3ONO (CD3ONO)/ 1st run Ne
General Valve ControllerDG535 Pulse Generator
XeF Excimer Laser
XeCl Excimer Laser
Ar+ Laser
Nd:YAG Laser Sirah Dye Laser
Pulsed Dye Amplifier
PC #1
PC #2
Nozzle
Ring Laser
T0
PMT
SHG
SHG
Frequency reading
Photolysis
Dump
Pump
Q-Switch
Flash Lamp
T0 / GPIB
T0
program
0
11 '
S
SS
synchronizing
Lens
Calibration method Doppler-limited I2
resolution ~0.12cm-1
accuracy ~0.05cm-1
Calibration method Doppler-free I2 +Etalon
resolution ~250MHz
accuracy ~50MHz
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SEP Spectra
CH3O CD3O
32892 32894 32896 32898 32900 32902 32904-25
-20
-15
-10
-5
0
5
32894.0 32894.1
-8
-6
-4
-2
0
2
P2b
pumped, moderate-resolution dump
P2a
pumped, moderate-resolution dump
32892 32894 32896 32898 32900 32902 32904-25
-20
-15
-10
-5
0
5
Dep
letio
n R
ate
(%)
32898.6 32898.7 32898.8
Dump Frequency / cm -1
32901.5 32901.6
P2a
+P2b
pumped, high-resolution dump
32838 32840 32842 32844 32846-15
-10
-5
0
5
32838 32840 32842 32844 32846-15
-10
-5
0
5
32838.7 32838.8
-10
-5
0
5
32842.4 32842.5 32844.7 32844.8
P2b
pumped, moderate-resolution dump
Dep
letio
n ra
te (
%)
P2a
pumped, moderate-resolution dump
Dump Frequency / cm -1
P2a
+P2b
pumped, high-resolution dump
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|N',J',K',p'> → |J,P,Σ,p>
|0,1/2,0,1> → |3/2,1/2,-1/2,-1>
16420.60 16420.65 16420.70 16420.75 16420.80 16420.85 16420.90
16420.60 16420.65 16420.70 16420.75 16420.80 16420.85 16420.90
16420.60 16420.65 16420.70 16420.75 16420.80 16420.85 16420.90
32841.2 32841.3 32841.4 32841.5 32841.6 32841.7 32841.8
wavenumbers / cm -1
Atlas
Iodine
FWHM~30MHz
EtalonFinesse~10
FSR~477MHz
CD3O SEP
FWHM~250MHz
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SEP Results of CH3O
# Pump |J",P", Σ",p "> |N', J', K', p '> |J, P, Σ, p > ΔE / cm-1
1 P1 |3/2,3/2,1/2,-1> |0,1/2,0,1> |1/2,1/2,-1/2,-1> 61.8578
2 P1 |3/2,3/2,1/2,-1> |0,1/2,0,1> |3/2,1/2,-1/2,-1> 64.6635
3 P2a |3/2,3/2,1/2,1> |1,1/2,0,-1> |1/2,1/2,-1/2,1> 61.8393
4 P2a |3/2,3/2,1/2,1> |1,1/2,0,-1> |3/2,1/2,-1/2,1> 64.7106
5 P2b |3/2,3/2,1/2,1> |1,3/2,0,-1> |1/2,1/2,-1/2,1> 61.8411
6 P2b |3/2,3/2,1/2,1> |1,3/2,0,-1> |3/2,1/2,-1/2,1> 64.7070
7 P2b |3/2,3/2,1/2,1> |1,3/2,0,-1> |5/2,1/2,-1/2,1> 69.3856
8 P3 |3/2,3/2,1/2,-1> |2,3/2,0,1> |3/2,1/2,-1/2,-1> 64.6774
9 P4 |1/2,1/2,1/2,-1> |1,1/2,1,1> |3/2,3/2,-1/2,-1> 77.3720
10 P4 |1/2,1/2,1/2,-1> |0,1/2,-1,1> |3/2,3/2,-1/2,-1> 77.3720
11 P4 |1/2,1/2,1/2,1> |1,1/2,1,-1> |3/2,3/2,-1/2,1> 77.3720
12 P4 |1/2,1/2,1/2,1> |0,1/2,-1,-1> |3/2,3/2,-1/2,1> 77.3720
SEPLIFE
P2b
wa
ven
umb
ers
/ cm
-1
P1
P2a
P3
P4
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SEP Results of CD3O
# Pump |J",P", Σ",p"> |N', J', K', p'> |J, P, Σ, p> ΔE / cm-1
1 P1 |3/2,3/2,1/2,-1> |0,1/2,0,1> |1/2,1/2,-1/2,-1> 55.0520
2 P1 |3/2,3/2,1/2,-1> |0,1/2,0,1> |3/2,1/2,-1/2,-1> 57.2713
3 P2a |3/2,3/2,1/2,1> |1,1/2,0,-1> |1/2,1/2,-1/2,1> 55.0291
4 P2a |3/2,3/2,1/2,1> |1,1/2,0,-1> |3/2,1/2,-1/2,1> 57.3134
5 P2b |3/2,3/2,1/2,1> |1,3/2,0,-1> |1/2,1/2,-1/2,1> 55.0293
6 P2b |3/2,3/2,1/2,1> |1,3/2,0,-1> |3/2,1/2,-1/2,1> 57.3128
7 P2b |3/2,3/2,1/2,1> |1,3/2,0,-1> |5/2,1/2,-1/2,1> 61.0088
8 P3 |3/2,3/2,1/2,-1> |2,3/2,0,1> |3/2,1/2,-1/2,-1> 57.2715
9 P3 |3/2,3/2,1/2,-1> |2,3/2,0,1> |3/2,1/2,-1/2,-1> 61.0731
10 P4 |3/2,3/2,1/2,-1> |3,5/2,0,1> |5/2,1/2,-1/2,-1> 61.0739
11 P5 |1/2,1/2,1/2,-1> |1,1/2,1,1> |3/2,3/2,-1/2,-1> 63.9904
12 P5 |1/2,1/2,1/2,-1> |0,1/2,-1,1> |3/2,3/2,-1/2,-1> 63.9904
13 P5 |1/2,1/2,1/2,1> |1,1/2,1,-1> |3/2,3/2,-1/2,1> 63.9904
14 P5 |1/2,1/2,1/2,1> |0,1/2,-1,-1> |3/2,3/2,-1/2,1> 63.9904
SEPLIFE
P2b
wa
ven
um
be
rs /
cm-1
P1
P2a
P3P
4
P5
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ground state (2E):a
HEFF = HROT + HCOR + HSO + HSR + HJT + HCD
Effective Hamiltonian:
Rotational Hamiltonian
Coriolis interaction
Spin-orbit interaction
Spin-rotation interaction
Jahn-Teller interaction
Centrifugal distortion
excited state (2A1):b,c,d
HEFF = HROT + HCOR + HSR + HCD
aY. Endo, S. Saito, and E. Hirota, J. Chem. Phys. 81, 122, (1984)
bX. Liu, C. P. Damo, T.-Y. Lin, S. C. Foster, P. Misra, L. Yu, and T. A. Miller, J. Phys. Chem. 92, 5914 (1988)cX. Liu, S. C. Foster, J. M. Williamson, L. Yu, and T. A. Miller, Mol. Phys. 69, 357 (1990)dD. E. Powers, M. B. Pushkarsky, and T. A. Miller, J. Chem. Phys. 106, 6863 (1997)
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Correction of CH3O Assignment
aζed1,2 = −62.24(17)cm-1
1Y. Endo, S. Saito, and E. Hirota, J. Chem. Phys. 81, 122, (1984) 2T. Momose, Y. Endo, E. Hirota, and T. Shida, J. Chem. Phys. 88, 5338 (1988)
21/ 2X E
23/ 2X E
21A A
aζed = −61.4994(39) cm-1
|N',J',K',p'>
|1,3/2,0,-1>
|J",P",Σ",p">
|3/2,3/2,1/2,±1>
|J,P,Σ,p>
|5/2,1/2,-1/2,±1>
|3/2,1/2,-1/2,±1>|1/2,1/2,-1/2,±1>
|5/2,3/2,1/2,±1>
p
+1
-1
MW
LIF
SEP
|N',J',K',p'>
|1,3/2,0,-1>
|J",P",Σ",p">
|3/2,3/2,1/2,±1>
|J,P,Σ,p>
|5/2,1/2,-1/2,±1>
|3/2,1/2,-1/2,±1>|1/2,1/2,-1/2,±1>
|5/2,3/2,1/2,±1>
|N',J',K',p'>
|1,3/2,0,-1>
|J",P",Σ",p">
|3/2,3/2,1/2,±1>
|J,P,Σ,p>
|5/2,1/2,-1/2,±1>
|3/2,1/2,-1/2,±1>|1/2,1/2,-1/2,±1>
|5/2,3/2,1/2,±1>
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Global Summary of Data
CH3O CD3O
46 40
118 105
320 Band 101 165
610 Band 77 75
12 14
0.05 0.05
1 1
50 50
70 70
0.04 0.09
3.82 0.35
320 Band 33 40
610 Band 78 36
49 44
microwavea
LIFc
SEPc
SEPc
Standard Deviation of Fitting (σ, MHz)LIFc
extended microwaveb
Transitions involved in Global Fitting
SEPc
microwavea
Experimental Accuracy (σ, MHz)
microwavea
extended microwaveb
extended microwaveb
LIFc
Number of assigned transitions
aCH3O: Y. Endo, S. Saito, and E. Hirota, J. Chem. Phys. 81, 122, (1984) ; CD3O: Y. Endo, private communication.bCH3O: T. Momose, Y. Endo, E. Hirota, and T. Shida, J. Chem. Phys. 88, 5338 (1988); CD3O: Y. Endo, private communication.cThis work.
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LIF Spectra and Simulations
32960 32965 32970 32975
wavenumbers / cm -1
experimental
simulation
32895 32900 32905 32910
wavenumbers / cm -1
experimental
simulation
CH3O, 320 band CD3O, 32
0 band
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SEP Spectra and Simulations
CH3O CD3O
32892 32894 32896 32898 32900 32902 32904-25-20-15-10
-505
32894.0 32894.1
-8
-6
-4
-2
0
2
32894.0 32894.1
P2a
pumped, moderate-resolution dump
32892 32894 32896 32898 32900 32902 32904-25-20-15-10
-505
Dep
letio
n R
ate
(%)
P2b
pumped, moderate-resolution dump
32898.6 32898.7 32898.8 32901.5 32901.6
P2a
+P2b
pumped, high-resolution dump
Simulation
32898.6 32898.7 32898.8
Dump Frequency / cm -132901.5 32901.6
32838 32840 32842 32844 32846 32848-15
-10
-5
0
5
32838 32840 32842 32844 32846 32848-15
-10
-5
0
5
32838.7 32838.8
-10
-5
0
5
32842.4 32842.5 32844.7 32844.8
32838.7 32838.8 32842.4 32842.5 32844.7 32844.8
De
ple
tion
ra
te (
%) P
2b pumped, moderate-resolution dump
P2a
pumped, moderate-resolution dump
P2a
+P2b
pumped, high-resolution dump
Dump Frequency / cm -1
Simulation
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A 154960 (570) 160050 (315) 154800 (50) 78391 (23)
B 27931.140 (46) 27929.849 (59) 27930.36 (4) 22194.05 (2)D k 2.11 e 2.11 e 2.11 e 0.39 f
D N 0.7699 (38) 0.76963 (108) 0.7693 (20) 0.4040 (3)
D NK 0.07553 (44) 0.075788 (96) 0.07565 (40) 0.04214 (6)
Aζ t 54330 (270) 52273 (124) 52241 (83) 22293 (24)
η e ζ t 1.82 (92) -0.936 (118) 0.264 (74) 0.713 (39)
η K ζt 131.9 (181) 153.1 (58) 31.6 (145) 16.7 (10)
aζ e d -1865980 (5030) -1873283 (1023) -1843707 (113) -1648372 (101)
a D ζ e d 134 (75) 363 (25) 176 (22) 77 (5)
ε aa -40930 (1700) -36897 (508) -37375 (88) -23097 (71)
ε bc -1428 (66) -1579.4 (160) -1111 (3) -841 (2)
ε 1 -171.670 (38) -171.590 (85) 172.65 (13) 142.09 (15)
ε 2a 2420 (1080) -984 (418) -534 (86) -192 (42)
ε 2b 436 c -172 c -96 c -54 c
h 1 75.446 (178) 76.380 (82) -77.68 (214) -88.71 (10)
h 2 1398 (40) 1280.7 (54) -1326 (3) -847 (1)
h 1N 0 e -0.001848 (298) 0.0011 (8) 0.000899 (4)
h 2N -0.0047 (41) -0.01239 (67) -0.0301 (106) -0.0091 (20)
h 1K 0.2356 (116) -0.644 (85) 2.476 (2139) -0.199 (78)h 2K -0.522 (47) -0.519 (17) 0.201 (8) 0.127 (7)h 4 0.00188 (138) -0.00038 (29) -0.00120 (45) -0.00009 (34)
microwavea,e+LIFb+SEPb microwavea,e+LIFb+SEPbextended microwaveemicrowavea
CH3O CD3O
Ground State Parameters
Rotational
Spin-Orbit
Coriolis
Centrifugal Distortion
Spin-Rotation
Jahn-Teller
bThis work cFixed to ε2a*(B/A) d2.5σ in parentheseseT. Momose, Y. Endo, E. Hirota, and T. Shida, J. Chem. Phys. 88, 5338 (1988)
aY. Endo, S. Saito, and E. Hirota, J. Chem. Phys. 81, 122, (1984)
ffixed to CD3F value.gY. Endo, private communication.
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Summary
LIF and SEP spectra are taken with both high-resolution (FWHM~250MHz) and high-accuracy (σ~50MHz).
Direct measurement of E1/2 component of the electronic ground state. Spin-orbit splitting ( )
Correction to parity assignments and Jahn-Teller related parameters (ε1, h1, h2…) from the global fitting involving microwave, LIF, and SEP
Available isotope (CH3O, CD3O) data for isotopic analysis. (RI09)
LIF and SEP spectra are taken with both high-resolution (FWHM~250MHz) and high-accuracy (σ~50MHz).
Direct measurement of E1/2 component of the electronic ground state. Spin-orbit splitting ( )
Correction to parity assignments and Jahn-Teller related parameters (ε1, h1, h2…) from the global fitting involving microwave, LIF, and SEP
Available isotope (CH3O, CD3O) data for isotopic analysis. (RI09)
ea d
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AcknowledgementThe METHOXY team:
Dr. Miller
Dmitry Melnik
Jinjun Liu (alumni)
Funding: NSF
Your attention!NEXT: RI09, given by Dmitry Melnik
Other Miller group members:
Shenghai Wu (alumni)
Patrick Rupper (alumni)
John T. Yi (alumni)
Jinjun Liu (alumni)
Erin Sharp (alumni)
Gabriel Just
Phillip Thomas
Linsen Pei
Rabi Chhantyal-Pun