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

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Presentation on theme: "Photochemistry h. O h T1T1 O h Acrolein T1T1 Photochemistry."— Presentation transcript:

1 Photochemistry h

2 O h T1T1

3 O h Acrolein T1T1 Photochemistry

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

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

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

7 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

8 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

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

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

11 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

12 CRD Survey Spectrum T 1 (n,  * )← S 0 S 1 (n,  * )← S 0 Room Temp 000000 000000

13 T 1 (n,  * )← S 0 S 1 (n,  * )← S 0 CRD Survey Spectrum Room Temp Jet-Cooled 000000 000000

14 T 1 (n,  * )← S 0 S 1 (n,  * )← S 0 CRD Survey Spectrum Room Temp Jet-Cooled 000000 000000

15 T 1 (n,  * )← S 0 0 0 0 band

16 T 1 (n,  * )← S 0 0 0 0 band

17 Hund’s Case (b)

18  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

19 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)

20 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)

21 T 1 (n,  * )← S 0 0 0 0 band

22 T 1 (n,  * )← S 0 0 0 0 band Hot bands

23 Room Temp Jet-Cooled

24 b a c E rot ≈ BN(N+1) + K a 2 (A – B)

25 Jet-Cooled b a c K″ = 01 2 3 4… sub-band origins,  K a =0 E rot ≈ BN(N+1) + K a 2 (A – B)

26 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)

27 5 6 7 8 K″ = 3 Jet-Cooled  K a =0,  N=+2 STROTA E rot ≈ BN(N+1) + K a 2 (A – B)

28 STROTA

29 K a ″ = 3 heads 5 6 7 8 K a ″ = 8 head 9 10  N=+1  N=+2 4

30 K a ″ = 3 heads 5 6 7 8  N=+2 A″ = 1.580 cm –1 B″ = 0.1554 cm –1 C″ = 0.1415 cm –1 A′ = 1.662 cm –1 B′ = 0.1485 cm –1 C′ = 0.1363 cm –1 K a ″ = 8 head 9 10  N=+1 T 1 (n,  *) Microwave Spectroscopy

31 A″ = 1.580 cm –1 B″ = 0.1554 cm –1 C″ = 0.1415 cm –1 A′ = 1.662 cm –1 B′ = 0.1485 cm –1 C′ = 0.1363 cm –1 Room Temp Jet-Cooled T 1 (n,  *) exp sim exp Microwave Spectroscopy

32 A″ = 1.580 cm –1 B″ = 0.1554 cm –1 C″ = 0.1415 cm –1 A′ = 1.662 cm –1 B′ = 0.1485 cm –1 C′ = 0.1363 cm –1 T rot = 63 K  Lor = 0.20 cm -1 T 1 (n,  *) exp sim Microwave Spectroscopy

33 A″ = 1.580 cm –1 B″ = 0.1554 cm –1 C″ = 0.1415 cm –1 A′ = 1.662 cm –1 B′ = 0.1485 cm –1 C′ = 0.1363 cm –1 T rot = 63 K  Lor = 0.20 cm -1 T 1 (n,  *)  = 25 ps T 1 (n,  *) exp sim Microwave Spectroscopy

34 A″ = 1.580 cm –1 B″ = 0.1554 cm –1 C″ = 0.1415 cm –1 A′ = 1.662 cm –1 B′ = 0.1485 cm –1 C′ = 0.1363 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

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

36 Acknowledgements NSF (CHE-0848615) Camille and Henry Dreyfus Foundation, Inc. (Henry Dreyfus Teacher-Scholar Award) Prof. Richard Judge (UW-Parkside) Prof. William Polik (Hope College)

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