Enhanced harmonic generation in double-well potentials George N. Gibson University of Connecticut...
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![Page 1: Enhanced harmonic generation in double-well potentials George N. Gibson University of Connecticut Graduate students: Katya Sergen Dale Smith James Dragan.](https://reader035.fdocument.org/reader035/viewer/2022062504/5a4d1b6e7f8b9ab0599b4537/html5/thumbnails/1.jpg)
Enhanced harmonic generation in double-well potentials
George N. GibsonUniversity of Connecticut
Graduate students:Katya SergenDale SmithJames Dragan
Funding: NSF
DAMOP 2015Columbus, OHJune 8-12, 2015
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OutlineHigh multiphoton susceptibility of the Γ-
system:– Strong multiphoton excitation– Strong harmonic generation
Double-well potentials contain the Γ-system– Doubly ionized potentials work well (A2
2+)– What about neutral potentials (A2)?
These are much more practicalPerformed both n-level and TDSE calculationsDouble-well potentials have large MP
susceptibility, even in the presence of other levels.
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What is special about even-charged diatomic molecules?
Strongly coupled pair of excited states and a weakly coupled ground state.
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3-Level Model System
This system can be solved exactly for the n-photon Rabi frequency!
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Γ-system Literature
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Γ-system: Harmonic Generation
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Γ-system: Harmonic Generation
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1-D 2-electron double-well model:),,(),,(),,( 212121 txxtxxHtxx
ti
))(()(
1
)()(
)()(
212221
222
222
2
1
221
222
1
1
xxtEaxxadx
Z
adx
Zadx
Z
adx
ZH S
mp
mpHP 22
22
21
Harmonic generation:
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Double well energy levels:
A2+ + A2+
A3+ + A1+
Ionic
Ionic
Covalent Covalent
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Double well energy levels:Ionic
Ionic
Covalent
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Harmonic generation from A22+
Small R Intermediate R
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Harmonic generation from A22+
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Harmonic generation from A2Small R Intermediate R
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Harmonic generation from A2
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Double well energy levels:Ionic
Ionic
Covalent
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Double well energy levels:
A2+ + A2+
A3+ + A1+
Ionic
Ionic
Covalent Covalent
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Dipole couplings at large R:
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Conclusions A pair of nearly degenerate strongly coupled states,
like those found in diatomic molecules greatly enhances multiphoton couplings.
In particular, low order harmonic generation is strongly enhanced and becomes non-perturbative.
Presence of covalent states in the neutral molecule are not detrimental.
Requires diatomic molecules at moderate internuclear separations.
Question: what is the optimal energy level structure for a particular nonlinear process?
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Thank you for listening!
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Perfect Floquet Ladder of States:Level 1 couples to the -(n-1) Floquet state through 12. Since this is only a 1-photon interaction the AC Stark shift is small.