formation of astrobiologically important molecules in extraterrestrial environments ralf i. kaiser...
TRANSCRIPT
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Formation of Astrobiologically Important Molecules in
Extraterrestrial Environments
Ralf I. KaiserDepartment of Chemistry
University of Hawai’iHonolulu, HI 96822
[email protected]://www.chem.hawaii.edu/Bil301/welcome.html
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Orion Constellation
Orion Nebula
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H : 1 He : 0.1
O : C : N = 7 : 3 : 1 (0.001)
gas phase solid state99 % 1 %
carbonaceous and silicate-basednanoparticl es
= 10-
molecular clouds and cores
circumstellar envelopes
Interstellar Medium
T = 10 – 4000 K
= 102 – 109 cm-3
T = 10 K
= 10-11 cm-3
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H-H
CH4, C2H2, C2H4, C2H6
H2O, H2S, NH3
CO, CO2
CH3OH, C2H5OH
CH3COCH3, H2CO,CH3CHO
HCOOH, CH3COOH
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Amino Acid
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Characteristics of a Chemical Reaction
1. exoergic vs. endoergic 2. no entrance barrier vs. barrier
3. binary vs. ternary reactions
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The 70es – Bimolecular Ion-Molecule Reactions
k = 10-9 cm3s-1 (Herbst et. al)
O O+ + e-
O+ + H2 OH+ + H
OH+ + H2 OH2+ + H
OH2+ + H2 OH3
+ + H
OH3+ + e- H2O + H
simple hydrides in cold molecular clouds(CH4, NH3, H2O)
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The 80es – Problems with Ion-Molecule Reactions
H C C C N
C2H2
C2H2+ + e-
C2H2+ + CN HCCCN+ + H
HCCCN+ + H2 H2CCCN+ + H
H2CCCN+ + e- HCCCN + H
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The 80es – Problems with Ion-Molecule Reactions
[HCCCN] : [HCCNC] : [HNCCC]
240 : 8 : 1 (models)
1000 : 8 : 1 (TMC-1)
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The 90es – Bimolecular Neutral-Neutral Reactions
CN(X2+) + CnHm CnH(m-1)CN + H
C2H(X2+) + CnHm CnH(m-1)C2H + H
C(3Pj) + CnHm C(n+1)H(m-1) + H
k = 10-10 cm3s-1 (Kaiser et al.; Smith et al.)
C2(X1g+) + CnHm C(n+2)H(m-1) + H
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The 90es – Bimolecular Neutral-Neutral Reactions
Titan IRC+10216
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H : 1 He : 0.1
O : C : N = 7 : 3 : 1 (0.001)
gas phase solid state99 % 1 %
carbonaceous and silicate-basednanoparticl es
= 10-
molecular clouds and cores
circumstellar envelopes
Interstellar Medium
T = 10 – 4000 K
= 102 – 109 cm-3
T = 10 K
= 10-11 cm-3
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UV photons
cosmic ray particles
Cold Molecular Cloud B68
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carbon dioxide carbon monoxide
water
methane ammonia
methanol
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The late 90es – Grain-Surface Reactions
hopping
tunneling
Eley-Rideal
Langmuir-Hinshelwood
accretion
H + H H2
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carbon dioxide carbon monoxidewater
methane ammonia
methanol
RTEaAek
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The 00es - Galactic Cosmic Ray Processing
10 MeV
9 MeV
1. ionization
2. electronic excitation
3. vibrational excitation
4. electron attachment
cleavage of
chemical bonds
‘electronic’interaction
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The 00es - Galactic Cosmic Ray Processing
1. Energy Conservation
10 eV transfer – 4.5 eV bond energy = 5.5 eV maximum kinetic energy
2. Angular Momentum Conservation
H atom (5.15 eV) versus CH3 radical (0.35 eV)
kinetic energy vibrational energy
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Non-Equilibrium Chemistry
1. exoergic vs. endoergic 2. no entrance barrier vs. barrier
3. binary vs. ternary reactions
A* + BC
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C2H4O Isomers
acetaldehyde ethylene oxide vinyl alcohol
H2O, CO, CO2, NH3, CH4, CH3OH
CO/CH4CO2/C2H4 H2O/C2H2
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C2H4O Isomers
acetaldehyde ethylene oxide vinyl alcohol
H
C C
OHH
+ H
H
C C
OHH
H
a b
a
b
b
a
+
+ +
+C O
C
H
HHH
C O
H
C
HH O
C
H
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Surface Scattering Machine
T = 10 – 350 K p = 810-11 torr
LET (5 keV e-) = 3 – 5 keV m-1 = LET (10 MeV H+)
30 min laboratory = 106 years in cold molecular cloud
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1.electron source
2. cation source (positively charged particles)
Sources
3. pyrolytic radical source
4. tunable photon source
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CO/CH4 Ice before Irradiation at 10 K
-0.10
0.00
0.10
0.20
0.30
0.40
0.50
0.60
0.70
0.80
10001500200025003000350040004500
Wavenumber (cm-1)
Ab
sorp
tio
n
45
29
= Methane
= Carbon Monoxide
43
01
42
47
42
03
36
49
30
18
30
03
29
06
28
17
21
34
21
42
20
89
15
29
13
08
25
95
-0.10
0.00
0.10
0.20
0.30
0.40
0.50
0.60
0.70
0.80
10001500200025003000350040004500
Wavenumber (cm-1)
Ab
sorp
tio
n
45
29
= Methane
= Carbon Monoxide
43
01
42
47
42
03
36
49
30
18
30
03
29
06
28
17
21
34
21
42
20
89
15
29
13
08
25
95
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CO/CH4 Ice after Irradiation at 10 K
612 cm-1
2 (CH3 out of plane)
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CO/CH4 Ice after Irradiation at 10 K
1853 cm-1
3 (HCO; CO stretch)
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CO/CH4 Ice after Irradiation at 10 K
1725 cm-1
4 (CH3CHO; CO stretch)
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QMS: CO/CH4 during Irradiation
H + H H2
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CO/CH4 Ices after Irradiation at 10 K
H
C C
OHH
+ H
H
C C
OHH
H
a b
a
b
b
a
+
+ +
+C O
C
H
HHH
C O
H
C
HH O
C
H
[CH4-CO] [CH3…HCO] CH3CHO
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Kinetics
(pseudo) 1st order kinetics
electron induced decomposition
[CH4-CO] [CH3…HCO] CH3CHO
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Kinetics
[CH4-CO] [CH3…HCO] CH3CHOk1 k2
a = 2.32 (0.42) 1015 cm-2
k1<<k2 = 1.13 ( 0.29) 10-11
s-1
a = 2.32 (0.42) 1015 cm-2
k1<<k2 = 1.13 ( 0.29) 10-11
s-1
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CH4 (X1A1) CH3(X2A2’’)
+H(2S1/2) CH4 (X1A1) CH3(X2A2
’’) +H(2S1/2)
CO (X1) +H(2S1/2) HCO (X2A’) CO (X1) +H(2S1/2) HCO (X2A’)
a = 3.87 (0.18) 1015 cm-2
k3 = 4.4 ( 0.37) 10-11 s-1
a = 3.87 (0.18) 1015 cm-2
k3 = 4.4 ( 0.37) 10-11 s-1
a = 3.39 (0.15) 1015 cm-2
k4 = 5.49 ( 0.73) 10-11 s-1
a = 3.39 (0.15) 1015 cm-2
k4 = 5.49 ( 0.73) 10-11 s-1
k3k3 k4k4
Kinetics
[CH4-CO] [CH3…HCO] CH3CHO
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Electronic Structure Calculations
Osamura et al. 2004
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C2H4O Isomers
acetaldehyde ethylene oxide vinyl alcohol
H2O, CO, CO2, NH3, CH4, CH3OH
CO/CH4CO2/C2H4 H2O/C2H2
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CO2/C2H4 Ices after Irradiation at 10 K
0.00
0.02
0.04
0.06
0.08
0.10
0.12
0.14
0.16
0.18
21102115212021252130213521402145215021552160
Wavenumber (cm-1)
Ab
sorp
tion
2139
(ν 1
fro
m C
O)
2139 cm-1
1 (CO; stretch)
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CO2/C2H4 Ices after Irradiation at 10 K
16801700172017401760
Wavenumber (cm-1)
0.000
0.005
0.010
0.015A
bsor
ptio
n
1723 cm-1
4 (CH3CHO; CO stretch)
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CO2/C2H4 Ices after Irradiation at 10 K
850860870880890
Wavenumber (cm-1)
0.000
0.002
0.004
0.006
0.008
0.010A
bsor
ptio
n
868 cm-1
12 (c-C2H4O; ring)
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Kinetics
(pseudo) 1st order kinetics
electron induced decomposition
[C2H4-CO2] [C2H4…O…CO] [C2H4O+CO]
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C2H4 + O CH3CHO C2H4 + O CH3CHO
a = 2.10 (0.09) 1015 cm-2
k1 = 5.22 ( 0.37) 10-12 s-1
a = 2.10 (0.09) 1015 cm-2
k1 = 5.22 ( 0.37) 10-12 s-1
a = 1.77 (0.05) 1015 cm-2
k2 = 6.29 ( 0.34) 10-12 s-1
a = 1.77 (0.05) 1015 cm-2
k2 = 6.29 ( 0.34) 10-12 s-1
k1k1
Kinetics
0 5 10 15 20 25 30
Time (min)
0.0
0.5
1.0
1.5
2.0x1015
Mol
ecul
escm
-2
0 5 10 15 20 25 30
Time (min)
0.0
0.5
1.0
1.5x1015
Mol
ecul
escm
-2
C2H4 + O c-C2H4O C2H4 + O c-C2H4O
k2k2
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Mechanism
+ OCC
H
HH
H
CC
H
HH
H
O
CC
H
HH
H
O
H3C H
O
CC
O
HH
H H
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Mechanism
‘cone of acceptance’ favors attack of bond (formation of acetaldehyde and ethylene oxide)
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Mechanisms
[CH4-CO] [CH3…HCO] CH3CHOa = 2.32 (0.42) 1015 cm-2
k = 1.13 ( 0.29) 10-11 s-1
a = 2.32 (0.42) 1015 cm-2
k = 1.13 ( 0.29) 10-11 s-1
[C2H4-CO2] [C2H4…O…CO] [C2H4O+CO]
a = 2.10 (0.09) 1015 cm-2
k = 5.22 ( 0.37) 10-12 s-1
a = 2.10 (0.09) 1015 cm-2
k = 5.22 ( 0.37) 10-12 s-1
a = 1.77 (0.05) 1015 cm-2
k = 6.29 ( 0.34) 10-12 s-1
a = 1.77 (0.05) 1015 cm-2
k = 6.29 ( 0.34) 10-12 s-1
CH3CHO c-C2H4O
kinetics versus dynamics
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C2H4O Isomers
acetaldehyde ethylene oxide vinyl alcohol
H2O, CO, CO2, NH3, CH4, CH3OH
CO/CH4 CO2/C2H4H2O/C2H2
synchrotron irradiations are crucial to discriminate between O(3P) and O(1D)
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H : 1 He : 0.1
O : C : N = 7 : 3 : 1 (0.001)
gas phase solid state99 % 1 %
carbonaceous and silicate-basednanoparticl es
= 10-
molecular clouds and cores
circumstellar envelopes
Interstellar Medium
T = 10 – 4000 K
= 102 – 109 cm-3
T = 10 K
= 10-11 cm-3
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Crossed Molecular Beams Machine
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Acknowledgements
Chris Bennett (UH, USA)
Corey Jamieson (UH, USA)
Prof. Nigel Mason (OU, UK)
Prof. Yoshihiro Osamura (Tokyo, Japan)