Enhanced harmonic generation in double-well potentials

Abstract

Recently, a new 3-level structure, called the Γ-system, has been identified and studied, which shows strong multiphoton coupling and harmonic generation. Under certain circumstances, the Γ-system appears in 1D double well potentials, suggesting that strong multiphoton excitation and harmonic generation may be seen in molecules at favorable internuclear separations, as various aspects of molecules in strong fields can be modeled by 1D potentials. However, even 1D potentials will have additional states, besides the Γ-system, which may interfere with these multiphoton processes. This paper presents numerical solutions to the time-dependent Schrödinger equation (TDSE) of two electrons in a double well potential approximating a dication (A 2+ 2) at various internuclear separations R. These calculations are compared to 2-and 3-level approximations of the full energy level structure. We show 1) the presence of the Γ-system in the 1D double-well potential; 2) that harmonic generation is enhanced at certain R; 3) the enhancement is due to the Γ-system by showing that the 3-level system shows the enhancement, while the 2-level system does not. This goes beyond the work of [M. Berent and R. Parzyński, Phys. Rev. A 82, 023804 (2010)] by demonstrating that the additional levels in the full TDSE calculation do not disrupt this response. In addition, we investigate a neutral double well potential (A 2) with both TDSE and 5-level calculations. While the level structure is not as clear as the dication, enhanced harmonic generation is still present from which we conclude that the Γ-system inherent in the double well potential still allows for a strong multiphoton coupling, even in the presence of other levels. From these calculations, we expect that neutral diatomic molecules at intermediate R should be a strong source of harmonic generation when exposed to intense laser fields. Indeed, in both charge states, the harmonic radiation is highly non-perturbative, as the power in the harmonics grows with harmonic order from 3 to 17, under certain conditions.

Enhanced high-order-harmonic generation and wave mixing via two-color multiphoton excitation of atoms and molecules

“…in quantum control, spectroscopy, sensing and imaging etc.. Depending on the laser-atom interaction parameters, harmonic generation may arise from bound-bound [7][8][9][10][11] and bound-free-bound transitions via continuum spectrum [12,13]. Bound-bound mechanism of harmonic generation without ionization is more efficient for generation of moderately high harmonics [8,9].…”