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Chemical Physics Letters

Coupled dressed-states formalism for multiphoton excitation and population inversion by coherent pulses

Tak‐San Ho, Shih‐I Chu

Published Nov 1, 1987• 37 citations
Publisher
DOI
10.1016/0009-2614(87)85031-5

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Tunneling ionization, a fascinating quantum phenomenon, has played the key role in the development of attosecond physics. Upon absorption of a few tens of photons, tunneling ionization creates ions in different excited states and even enables the formation of population inversion between ionic states. However, the underlying physics is still being debated. Here, we demonstrate a significant enhancement in the efficiency of multiphoton excitation when ionization of neutral molecules and resonant excitation of ions coexist in strong laser fields. It facilitates the dramatic increase in population inversion and lasing radiation in N_{2}^{+} around 1000 nm pump wavelength. Utilizing the ionization-coupling theory, we discover that the synergistic interplay between tunneling ionization and multiphoton excitation enables the ionic coherence to be maximized by phase locking of the periodically created ionic dipoles and consistently maintain an optimal phase for the follow-up photoexcitation. This Letter provides new insights into the photoexcitation mechanism of ions in strong laser fields and opens up a route for optimizing ionic lasing radiations.

Physical Review Letters•Sep 13, 2024•16 citations
We analyse the physical origin of population inversion via continuous wave two-colour coherent excitation in three-level systems by dressing the inverted transition. Two different mechanisms are identified as being responsible for the population inversion. For V -configured systems and cascade (Ξ) configured systems with inversion on the lower transition, the responsible mechanism is the selective trapping of dressed states, and the population inversion approaches the ideal value of 1. For Λ-configured systems and Ξ-configured systems with inversion on the upper transition, population inversion is based on the selective excitation of dressed states, with the population inversion tending towards 0.5. As the essential difference between these two mechanisms, the selective trapping of dressed states occurs in systems with strong decay into dressed states while the selective excitation appears in systems with strong decay out of dressed states.
To coherently control a few-level quantum emitter, typically pulses with an energy resonant to the transition energy are applied, making use of the Rabi mechanism, while a single off-resonant pulse does not result in a population inversion. Surprisingly, a two-color excitation with a combination of two off-resonant pulses is able to invert the system. In this paper, we provide an in-depth analysis of two-color excitation schemes within the dressed-state picture. We show that such schemes can be understood as a driving of the transition between the dressed states. In the two-level system this allows us to derive analytic expressions for the pulse parameters yielding a population inversion. We relate our findings to the Swing-UP of quantum EmitteR population (SUPER) mechanism, where the two pulses are red detuned. Our interpretation also holds in the case where one pulse is red detuned while the other pulse is blue detuned, as in dichromatic excitation schemes. We extend our considerations of the SUPER mechanism to the three-level system, where a strong mixing between the bare states takes place. The insights gained from these results help in finding accessible regimes for further experimental realizations of two-color excitation schemes.
Tunneling ionization, a fascinating quantum phenomenon, has played the key role in the development of attosecond physics. Upon absorption of a few tens of photons, tunneling ionization creates ions in different excited states and even enables the formation of population inversion between ionic states. However, the underlying physics is still being debated. Here, we demonstrate a significant enhancement in the efficiency of multiphoton excitation when ionization of neutral molecules and resonant excitation of ions coexist in strong laser fields. It facilitates the dramatic increase in population inversion and lasing radiation in N_{2}^{+} around 1000 nm pump wavelength. Utilizing the ionization-coupling theory, we discover that the synergistic interplay between tunneling ionization and multiphoton excitation enables the ionic coherence to be maximized by phase locking of the periodically created ionic dipoles and consistently maintain an optimal phase for the follow-up photoexcitation. This Letter provides new insights into the photoexcitation mechanism of ions in strong laser fields and opens up a route for optimizing ionic lasing radiations.