Molecular isomerization induced by ultrashort infrared pulses. I. Few-cycle to sub-one-cycle Gaussian pulses and the role of the carrier-envelope phase

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-1.0 -0.5 0.0 0.5 1.0

-1 0 1

-1.0 -0.5 0.0 0.5 1.0

-1 0 1

a mp litu de / A

time / T

-1.0 -0.5 0.0 0.5 1.0

-2 -1 0 1 2

-1.0 -0.5 0.0 0.5 1.0

0 1 2 3

fie ld stren g th / A

time / T

po we r / a rbi trar y un its

frequency /

0.00 0.02 0.04 0.06 0.08 0.10 0.12 0.0

0.1 0.2 0.3 0.4

20 18

16 14

12 10

8 6

4 2

0

isom erization probability

A / au

0.5 1.0

1.5 2.0 0.0

0.1 0.2 0.3 0.4

60 80

100

0.5 1.0

1.5 2.0 0.0

0.1 0.2 0.3 0.4

60 80

100

0.5 1.0

1.5 2.0 0.0

0.1 0.2 0.3 0.4

60 80

100

0.5 1.0

1.5 2.0 0.0

0.1 0.2 0.3 0.4

60 80

100

(a)

isomerization probability

(b)

(c)

CEP /

π

optical cycle / fs

CEP /

π

(d)

optical cycle / fs

0.5 1.0

1.5 2.0 0.0

0.1 0.2 0.3 0.4

60 80

100

0.5 1.0

1.5 2.0 0.0

0.1 0.2 0.3 0.4

30 40

0.5 1.0

1.5 2.0 0.0

0.1 0.2 0.3 0.4

30

40 0.5

1.0 1.5 2.0 0.0

0.1 0.2 0.3 0.4

30 40

(a)

isomerization probability

(b)

(c)

CEP /

π

optical cycle / fs

CEP /

π

(d)

optical cycle / fs

0.00 0.25 0.50 0.75 1.00

-20 -10 0 10 20

0.00 0.02 0.04 -0.05 0.00 0.05

0.00 0.20 0.40 0.60

HNC initial

popu lat ion

delocalized

ene rg y / a u HNC

time / fs

fie ld / au

delocalized

0 20 40 60 0.0

0.5 1.0

0 20 40 60

0.0 0.5 1.0

(a) (c)

population (b)

time / fs

(d)

0 20 40 60 -0.01

0.00 0.01 0.02

0 20 40 60

-0.01 0.00 0.01

0.02

(a) (c)

energy / au (b)

time / fs

(d)

0 20 40 0.00

0.25 0.50 0.75 1.00 -0.04 0.00 0.04

0 20 40

product delocalized

initial

time / fs

popu lat ion

HCN/HNC 3d

fi el d st rength / au

product (HNC) delocalized

initial

quartic 1d