It is well known that area pulses make Rabi oscillation and chirped pulses in the adiabatic interaction regime induce complete population inversion of a two-state system. Here we show that chirped zero-area pulses could engineer an interplay between the adiabatic evolution and Rabi-like rotations. In a proof-of-principle experiment utilizing spectral chirping of femtosecond laser pulses with a resonant spectral hole, we demonstrate that the chirped zero-area pulses could induce, for example, complete population inversion and return of the cold rubidium atom two-state system. Experimental result agrees well with the theoretically considered overall dynamics, which could be approximately modeled to a Ramsey-like three-pulse interaction, where the $x$ and $z$ rotations are driven by the hole and the main pulse, respectively.It is well known that area pulses make Rabi oscillation and chirped pulses in the adiabatic interaction regime induce complete population inversion of a two-state system. Here we show that chirped zero-area pulses could engineer an interplay between the adiabatic evolution and Rabi-like rotations. In a proof-of-principle experiment utilizing spectral chirping of femtosecond laser pulses with a resonant spectral hole, we demonstrate that the chirped zero-area pulses could induce, for example, complete population inversion and return of the cold rubidium atom two-state system. Experimental result agrees well with the theoretically considered overall dynamics, which could be approximately modeled to a Ramsey-like three-pulse interaction, where the $x$ and $z$ rotations are driven by the hole and the main pulse, respectively.

arXiv:1508.05584Physical Review AFeb 23, 20167 citations

Molecular “ π Pulse” for Total Inversion of Electronic State Population

Jianshu Cao, Christopher J. Bardeen, Kent R. Wilson

Theoretical analysis leads us to the intriguing conclusion that nearly complete electronic population inversion of molecules can be achieved with intense positively chirped broadband laser pulses, as a combined result of vibrational coherence and adiabatic inversion. Strong field quantum calculations demonstrate inversion probabilities of up to 99%. The results are robust with respect to changes in light field parameters as well as to thermal and condensed phase conditions, are supported by experimental evidence, and have many potential applications in chemistry, biochemistry, biology, and physics.Theoretical analysis leads us to the intriguing conclusion that nearly complete electronic population inversion of molecules can be achieved with intense positively chirped broadband laser pulses, as a combined result of vibrational coherence and adiabatic inversion. Strong field quantum calculations demonstrate inversion probabilities of up to 99%. The results are robust with respect to changes in light field parameters as well as to thermal and condensed phase conditions, are supported by experimental evidence, and have many potential applications in chemistry, biochemistry, biology, and physics.

Physical Review LettersFeb 16, 1998154 citations

Multiband Adiabatic Inversion Pulses

Gadi Goelman, J.S. Leigh

Journal of Magnetic Resonance Series AFeb 1, 199316 citations

CROSSING OF OPTICAL RESONANCES BY CHIRPED PULSES

Angelo Turrin

Jan 1, 19800 citations

Laser pulse control of Raman processes by chirped non-adiabatic passage

François Légaré, Szczepan Chelkowski, André D. Bandrauk

Chirped pulses allow for non-adiabatic passage between dressed states of Raman processes. It is shown that using an appropriately chirped pulse, one can control the interference between resonant and non-resonant pathways in stimulated Raman processes. A three-level system is studied in detail and application to complete ro-vibrational level inversion to high vibration quantum numbers (v > 10) in H2 via RCNAP (Raman chirped non-adiabatic passage) is presented. Copyright © 2000 John Wiley & Sons, Ltd.Chirped pulses allow for non-adiabatic passage between dressed states of Raman processes. It is shown that using an appropriately chirped pulse, one can control the interference between resonant and non-resonant pathways in stimulated Raman processes. A three-level system is studied in detail and application to complete ro-vibrational level inversion to high vibration quantum numbers (v > 10) in H2 via RCNAP (Raman chirped non-adiabatic passage) is presented. Copyright © 2000 John Wiley & Sons, Ltd.

Journal of Raman SpectroscopyJan 1, 200026 citations

x

and

z

rotations are driven by the hole and the main pulse, respectively.