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![Page 1: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/1.jpg)
Reaction Forensics: Using a variety of spectroscopic techniques
to elucidate reaction mechanismsSteve Rowling, Brianna Heazlewood and Scott KABLE
guest starring Paul Houston, David Osborn, Arthur Suits, Mike Ashfold, Peter Loock, Meredith Jordan (and groups)
University of SydneySydney, Australia, 2006
![Page 2: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/2.jpg)
Cartoon surfaces for photodissociationh
Dissociation
Bound
h
Dissociation
Repulsive
h
Dissociation
Barrier
Real chemistry is more complex…
![Page 3: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/3.jpg)
h
S1
(excited singlet)
ABC(S0, ground state)
3 or more challenges:- 1 PES… multiple products
![Page 4: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/4.jpg)
S0* (excited ground state)
IC
h
S1
(excited singlet)
ABC(S0, ground state)
3 or more challenges:- 1 PES… multiple products
![Page 5: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/5.jpg)
S0* (excited ground state)
A + BC
B + ACTS
IC
ACB
TS
h
S1
(excited singlet)
ABC(S0, ground state)
3 or more challenges:- 1 PES… multiple products
![Page 6: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/6.jpg)
T1 (triplet)
S0* (excited ground state)
A + BC
B + ACTS
TS
ISC
IC
ACB
TS
h
S1
(excited singlet)
ABC(S0, ground state)
3 or more challenges:- 1 PES… multiple products- multiple PES’s… 1 product
![Page 7: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/7.jpg)
T1 (triplet)
S0* (excited ground state)
A + BC
B + ACTS
TS
ISC
IC
ACB
TS
h
S1
(excited singlet)
H2CO(S0, ground state)
3 or more challenges:- 1 PES… multiple products- multiple PES’s… 1 product- 1 PES… 1 product…
multiple pathways
TS2?
![Page 8: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/8.jpg)
T1 (triplet)
S0* (excited ground state)
H + HCO
H2 + COTS
TS
ISC
IC
h
S1
(excited singlet)
H2CO(S0, ground state)
simple molecular
simple radicalH2CO exhibits all of these complexities!
![Page 9: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/9.jpg)
T1 (triplet)
S0* (excited ground state)
H + HCO
H2 + COTS
TS
ISC
IC
h
S1
(excited singlet)
H2CO(S0, ground state)
simple molecular
simple radicaltriplet
H2CO exhibits all of these complexities!
![Page 10: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/10.jpg)
T1 (triplet)
S0* (excited ground state)
H + HCO
H2 + COTS
TS
ISC
IC
h
S1
(excited singlet)
H2CO(S0, ground state)
simple molecular
simple radicaltriplet
roaming
H2CO exhibits all of these complexities!
“roaming”
![Page 11: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/11.jpg)
Multiple PES’s – 1 productthreshold
phofex
LIF
triplet threshold
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LIF spectrum of nascent HCOPump = 2241
![Page 13: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/13.jpg)
Distributions from Different Excitation
30500
31000
31500
32000
32500
3300024
041
0
23
043
0
11
021
041
0
21
061
0
PhofexLIF
11
041
0 & 51
0
21
042
061
0 E
xcita
tion
ener
gy (c
m-1
)
23
041
0
42
051
0
22
043
0
22
061
0
22
041
0
21
041
061
021
043
0
0
500
1000
1500
2000
2500
Eav
ail (c
m-1
)
2261
2243
2341
2441
112141
PST
244
1
Eav = 2612 cm-1
Eav = 1114 cm-1
0 5 10 15 20
PST
226
1
Re
lativ
e P
op
ula
tion
N
![Page 14: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/14.jpg)
PST
244
1
Eav = 2612 cm-1
Eav = 1114 cm-1
0 5 10 15 20
PST
226
1
Re
lativ
e P
op
ula
tion
N
Fingerprinting with Phofex
Rel
ativ
e P
opul
atio
n
N
2261
Eavail = 11142261
statistical, or S0
2243
non-statistical, or T1
1)12,10(
)1,0(
N
N
32)12,10(
)1,0(
N
N
2441
Eavail = 2612
N(0,1) N(10,12)
![Page 15: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/15.jpg)
30500
31000
31500
32000
32500
3300024
041
0
23
043
0
11
021
041
0
21
061
0
PhofexLIF
11
041
0 & 51
0
21
042
061
0 E
xcita
tion
ener
gy (c
m-1
)
23
041
0
42
051
0
22
043
0
22
061
0
22
041
0
21
041
061
021
043
0
0
500
1000
1500
2000
2500
Eav
ail (c
m-1
)
2261
2243
2341
2441
112141
Triplet dominates
Singlet exclusively
?
Zoom in
![Page 16: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/16.jpg)
Fingerprinting with Phofex
N = 0 + 1
2243
Eavail ~ 1220 cm-1
![Page 17: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/17.jpg)
Fingerprinting with Phofex
N = 0 + 1
2243
Eavail ~ 1220 cm-1
N = 10 + 12
220+221220, 221
303303+000
220, 221, 303 S0
all others T1
![Page 18: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/18.jpg)
Rydbergtagging experiments
all 2243
Scott Hopkins, Peter Loock, Brid Croonan, Michael Nix, Adam Devine, Richard Dixon, Mike Ashfold, JCP, (in press).
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Comparison
N = 0 + 1
N = 10 + 12
![Page 20: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/20.jpg)
Rydberg tagging experiments
Scott Hopkins, Peter Loock, Brid Croonan, Michael Nix, Adam Devine, Richard Dixon, Mike Ashfold, JCP, (in press).
Ka = 0 1 2 3 4 5Excellent Ka resolution
Partial N resolution
![Page 21: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/21.jpg)
0 1 2 3 4 5 60.00
0.25
0.50
0.75
1.00
1.25
PST
"singlet"
"triplet"
Re
lativ
e P
op
(K
a)
Ka
Comparison of Ka populations
LIF
![Page 22: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/22.jpg)
Comparison of Ka populations
LIF
![Page 23: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/23.jpg)
Comparison of N distributions
0 5 10 15 20 250
2
4"singlet-like" distribution
224
3 22
N
Rydberg tagging LIF
![Page 24: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/24.jpg)
T1 (triplet)
S0* (excited ground state)
H + HCO
H2 + CO
Signatures of each pathway
TS
Triplet HCO: Low NLow KHigh trans
Singlet HCO:Statistical NStatistical KStatistical trans
TS
T.S. CO: High J(CO)Modest vib(H2)High trans
Roaming CO: v. low JHigh vib(H2)Low trans
![Page 25: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/25.jpg)
Now probe roamingchannel with phofex…
Probe J(CO)=15(which has been associated with roaming)
Townsend et al, Science., 306, 1158 (2004)
Experiments: Lahankar and Rowling
![Page 26: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/26.jpg)
Fingerprinting with Phofex
N = 0 + 1
2243
Eavail ~ 1220 cm-1
N = 10 + 12
![Page 27: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/27.jpg)
Fingerprinting with Phofex
2243
Eavail ~ 1220 cm-1
N = 10 + 12
singlet HCO
Roaming scales very closely with S0 HCO!
roaming
![Page 28: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/28.jpg)
how far can H-atom roam? can other moieties roam? what are the requirements for
roaming in larger systems?
Questions from “Roaming atom” mechanism…
Obvious next candidate: CH3CHO
![Page 29: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/29.jpg)
T1 (triplet)
S0* (excited ground state)
CH3 + HCO
CH4 + CO
TS
TS
ISC
IC
CH3COHTS
h
S1
(excited singlet)
CH3CHO(S0, ground state)
CH2CHOHCH2CH2O
TS TS
H2 + CH2CO
H + CH3CO
TS
TS
GOAL = ROAMING??
TS
CH2 + H2CO
![Page 30: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/30.jpg)
T1 (triplet)
S0* (excited ground state)
CH3 + HCOISC
IC
h
S1
(excited singlet)
CH3CHO(S0, ground state)
QCT theoryExperimen
tHCO & CH3
Known acetaldehyde dynamics
![Page 31: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/31.jpg)
T1 (triplet)
S0* (excited ground state)
CH3 + HCO
CH4 + CO
ISC
IC
h
S1
(excited singlet)
CH3CHO(S0, ground state)
TS
QCT theoryExperimen
tHCO & CH3
Known acetaldehyde dynamics
CO PSD
ROAMING??
![Page 32: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/32.jpg)
CO product state dist’ns
Roaming TS
CO(J) v.low high
CO(tr) v.low high
CO(v,J) anisotropicv ┴ J
![Page 33: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/33.jpg)
T1 (triplet)
S0* (excited ground state)
CH3 + HCO
CH4 + CO
ISC
IC
h
S1
(excited singlet)
CH3CHO(S0, ground state)
TS
ROAMING??
, known
New experiments
Tune h 1
2
![Page 34: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/34.jpg)
Acetaldehyde action spectra
1 = LIF
2 = Phofex(HCO)
B. Heazlewood, S. RowlingTriplet threshold
HCO formed below T1 barrier= produced on S0
![Page 35: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/35.jpg)
T1 (triplet)
S0* (excited ground state)
CH3 + HCO
CH4 + CO
ISC
IC
h
S1
(excited singlet)
CH3CHO(S0, ground state)
TS
ROAMING??
1, , known
2, CH4
These experiments
![Page 36: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/36.jpg)
FTIR emission
3000
2500
2000
1500
1000
500
0
4500400035003000250020001500
Wavenumber (cm-1)
Tim
e (
s)
Slice
Slice
Brianna Heazlewood, Talitha Selby and David Osborne
![Page 37: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/37.jpg)
FTIR emission
3000
2500
2000
1500
1000
500
0
4500400035003000250020001500
Slice
CH4COHCO
![Page 38: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/38.jpg)
2000 2250 2500 2750 3000 3250 3500
IR emission Max. ent. fit
Wavenumber (cm-1)
Maximum entropy fit
2000 2250 2500 2750 3000 3250 3500
IR emission Max. ent. fit
Wavenumber (cm-1)
• > 3,000,000 CH4 vib. states
• anharmonic (Morse)
oscillators
• harmonic linestrengths
• bin into 10 cm-1 emission
bins
•deconvolve with 400 K
rotational profile
• let all states within a bin be
equally likely
• vary populations to fit
experiment
![Page 39: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/39.jpg)
Maximum entropy pop. distribution
0 5000 10000 15000 20000 25000 30000 35000 40000
Po
pu
la
tio
n (a
rb
.)
Energy (cm-1)
0 100 200 300 400 Energy (kJ/mol)
Emax
![Page 40: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/40.jpg)
Summary of new CH3CHO dynamics
CH3 + HCO channel IS open on S0
HCO is born with low Etrans and higher Erot
CH4 is born extremely hot (vibrationally)
evidence of two distributions of vib. energy
supports a second mechanism for CH4 formation (roaming?)
![Page 41: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/41.jpg)
What is “roaming”?
![Page 42: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/42.jpg)
Acetaldehyde dynamics on a “grown” PES
Movie courtesy Meredith Jordan and Brianna Heazlewood
![Page 43: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/43.jpg)
Roaming?
Roaming might not be so simple in larger systems.
Might there be a continuum between TS and roaming?
Spectroscopic techniques used:• laser induced fluorescence• IR emission• photofragment excitation• photofragment imaging• REMPI• Rydberg tagging• (ab initio + QCT)
![Page 44: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/44.jpg)
Experiments on photodissociation dynamics–Brianna Heazlewood (Hons)
–Klaas Nauta (post doc)
–Steve Rowling (PhD)
–Hongming Yin (post doc)
Theoretical description–Joel Bowman (Emory U.)
–Meredith Jordan (U. Syd.)
–George McBane (Grand Valley U.)
–Ondrej Votava (Heyrovsky Inst.)
$$Funding$$–ARC
–Sydney Univ.
–APAC
Acknowledgements…
Collaborators–Paul Houston (Georgia Tech)
–Arthur Suits (Wayne State)
–Sridhar Lahankar (Wayne State)
–David Osborn (Sandia)
–Talitha Selby (Sandia)
–Mike Ashfold (Bristol)
–Hans-Peter Loock (Queens, CA)
![Page 45: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/45.jpg)
Current laser spectroscopy group (April 2007)…
Tim SchmidtKlaas Nauta
Steve RowlingBrianna Heazlewood
![Page 46: Reaction Forensics: Using a variety of spectroscopic techniques to elucidate reaction mechanisms Steve Rowling, Brianna Heazlewood and Scott KABLE guest.](https://reader035.fdocuments.in/reader035/viewer/2022062714/56649d215503460f949f61f9/html5/thumbnails/46.jpg)