Photochemistry h. O h T1T1 O h Acrolein T1T1 Photochemistry.

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Presentation transcript:

Photochemistry h

O h T1T1

O h Acrolein T1T1 Photochemistry

T(n,  * ) T( ,  *) P.E. Twisting coordinate

T 1 (n,  * ) T 1 ( ,  *) P.E. Twisting coordinate T1T1 T1T1 T2T2 T2T2

T 1 (n,  * ) T 1 ( ,  *) T1T1 T1T1 T2T2 T2T2 S0S0 S 1 (n,  * )

T 1 (n,  * )← S 0 S 1 (n,  * )← S 0 Survey at 0.05-nm resolution (Cary-5E) Acrolein (84 T) in 10-cm cell at room temperature 1 1 Prof. William Polik, Hope College

T 1 (n,  * )← S 0 S 1 (n,  * )← S 0 Survey at 0.05-nm resolution (Cary-5E) Acrolein (84 T) in 10-cm cell at room temperature 1 1 Prof. William Polik, Hope College

Dye Laser Telescope Ringdown Cell Photomultiplier OscilloscopeComputer Nd:YAG Laser 10 Hz 355 nm 385 nm, 0.2 mJ/pulse 50 

Dye Laser Telescope Ringdown Cell Photomultiplier OscilloscopeComputer Nd:YAG Laser 10 Hz 355 nm 385 nm, 0.2 mJ/pulse 50  Jordan Valve

T 1 (n,  * )← S 0 S 1 (n,  * )← S 0 Survey at 0.05-nm resolution (Cary-5E) Acrolein (84 T) in 10-cm cell at room temperature 1 1 Prof. William Polik, Hope College

CRD Survey Spectrum T 1 (n,  * )← S 0 S 1 (n,  * )← S 0 Room Temp

T 1 (n,  * )← S 0 S 1 (n,  * )← S 0 CRD Survey Spectrum Room Temp Jet-Cooled

T 1 (n,  * )← S 0 S 1 (n,  * )← S 0 CRD Survey Spectrum Room Temp Jet-Cooled

T 1 (n,  * )← S band

T 1 (n,  * )← S band

Hund’s Case (b)

 J= ±1  N=0, ±1, ±2 N″=1 N′=3 J″=1 N′=2 J′=1 J′=2 J′=3 J′=2 J′=3 J′=4 N′=1 J′=0 J′=1 J′=2 T1T1 S0S0

b a c  J= 0, ±1  K a = 0, ±1, ±2  N=0, ±1, ±2  J= ±1  N=0, ±1, ±2 Singlet-Triplet Selection Rules E rot ≈ BN(N+1) + K a 2 (A – B)

b a c  J= 0, ±1  K a = 0, ±1, ±2  N=0, ±1, ±2  J= ±1  N=0, ±1, ±2 Singlet-Triplet Selection Rules E rot ≈ BN(N+1) + K a 2 (A – B)

T 1 (n,  * )← S band

T 1 (n,  * )← S band Hot bands

Room Temp Jet-Cooled

b a c E rot ≈ BN(N+1) + K a 2 (A – B)

Jet-Cooled b a c K″ = … sub-band origins,  K a =0 E rot ≈ BN(N+1) + K a 2 (A – B)

K″ = 3 Sub-band head,  N = +2, N″ ~ 45 Jet-Cooled STROTA 1 1 Richard Judge et al. E rot ≈ BN(N+1) + K a 2 (A – B)

K″ = 3 Jet-Cooled  K a =0,  N=+2 STROTA E rot ≈ BN(N+1) + K a 2 (A – B)

STROTA

K a ″ = 3 heads K a ″ = 8 head 9 10  N=+1  N=+2 4

K a ″ = 3 heads  N=+2 A″ = cm –1 B″ = cm –1 C″ = cm –1 A′ = cm –1 B′ = cm –1 C′ = cm –1 K a ″ = 8 head 9 10  N=+1 T 1 (n,  *) Microwave Spectroscopy

A″ = cm –1 B″ = cm –1 C″ = cm –1 A′ = cm –1 B′ = cm –1 C′ = cm –1 Room Temp Jet-Cooled T 1 (n,  *) exp sim exp Microwave Spectroscopy

A″ = cm –1 B″ = cm –1 C″ = cm –1 A′ = cm –1 B′ = cm –1 C′ = cm –1 T rot = 63 K  Lor = 0.20 cm -1 T 1 (n,  *) exp sim Microwave Spectroscopy

A″ = cm –1 B″ = cm –1 C″ = cm –1 A′ = cm –1 B′ = cm –1 C′ = cm –1 T rot = 63 K  Lor = 0.20 cm -1 T 1 (n,  *)  = 25 ps T 1 (n,  *) exp sim Microwave Spectroscopy

A″ = cm –1 B″ = cm –1 C″ = cm –1 A′ = cm –1 B′ = cm –1 C′ = cm –1 T rot = 63 K  Lor = 0.20 cm -1 T 1 (n,  *)  = 25 ps T 1 (n,  *) exp sim S 1 (n,  *) 1  = 2 ps 1 K.W. Paulisse et al., J. Chem. Phys. v. 113, p. 184 (2000). Microwave Spectroscopy

T 1 (n,  * ) T 1 ( ,  *) T1T1 T1T1 T2T2 T2T2 S0S0 S 1 (n,  * )

Acknowledgements NSF (CHE ) Camille and Henry Dreyfus Foundation, Inc. (Henry Dreyfus Teacher-Scholar Award) Prof. Richard Judge (UW-Parkside) Prof. William Polik (Hope College)