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Physical Review Letters

Observation of Broadband Time-Dependent Rabi Shifting in Microplasmas

Ryan Compton, A. I. Filin, Dmitri Romanov, Robert J. Levis

Published Nov 10, 2009• 20 citations
Publisher

Abstract

Coherent broadband radiation in the form of Rabi sidebands is observed when a ps probe laser propagates through a weakly ionized, electronically excited microplasma generated in the focus of an intense pump beam. The sidebands arise from the interaction of the probe beam with pairs of excited states of a constituent neutral atom via the probe-induced Rabi oscillation. Sideband shifting of >90 meV from the probe carrier frequency results in an effective bandwidth of 200 meV. The sidebands are controlled by the intensity and temporal profile of the probe pulse; with amplitude and shift in agreement with the predictions of a time-dependent generalized Rabi cycling model.

DOI
10.1103/physrevlett.103.205001

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International Conference on Ultrafast Phenomena•Jan 1, 2010•0 citations
Coherent broadband radiation in the form of Rabi sidebands is observed when a ps probe laser propagates through a weakly ionized, electronically excited microplasma generated in the focus of an intense pump beam. The sidebands arise from the interaction of the probe beam with pairs of excited states of a constituent neutral atom via the probe-induced Rabi oscillation. Sideband shifting of >90 meV from the probe carrier frequency results in an effective bandwidth of 200 meV. The sidebands are controlled by the intensity and temporal profile of the probe pulse; with amplitude and shift in agreement with the predictions of a time-dependent generalized Rabi cycling model.
Broadband, coherent radiation in the optical-frequency range is generated using microplasma channels in atmospheric gases in a pump-probe experiment. A microplasma medium is created in a gas by a focused intense femtosecond pump pulse. A picosecond probe pulse then interacts with this microplasma channel, producing broad, coherent sidebands that are associated with luminescence lines and are redshifted and blueshifted with respect to the laser carrier frequency. These sidebands originate from the induced Rabi oscillations between pairs of excited states that are coupled by the probe pulse. Thus the sideband radiation intensity tracks the microplasma evolution. The sidebands arise from broad and tunable Rabi shifts corresponding to varying values of the electric-field magnitude in the probe pulse. The \ensuremath{\sim}1010{}^{10}10 W cm${}^{\ensuremath{-}2}$ probe beam creates a maximum sideband shift of >90 meV from the carrier frequency, resulting in an effective bandwidth of 200 meV. The sidebands can be tuned and controlled by the intensity and temporal profile of the probe pulse. The fact that the coherence is observed in a microplasma demonstrates that Rabi cycling is possible at high temperature with moderately high laser intensities as long as transitions close to the driving frequency ($\ensuremath{\Delta}$\ensuremath{\sim}2% ${\ensuremath{\omega}}_{c}$) are available. Plasma excitation combined with Rabi-shifting measurements also serves as a means to simultaneously extract quantitative ratios for the transition-dipole moments between multiple sets of highly excited states with transitions in the optical regime.
Broadband, coherent radiation in the optical frequency range is generated using micro-plasma channels in atmospheric gases in a pump-probe experiment. A micro-plasma medium is created in a gas by a focused intense femtosecond pump pulse. A picosecond probe pulse then interacts with this micro-plasma channel, producing broad, coherent sidebands that are associated with luminescence lines and are red- and blue-shifted with respect to the laser carrier frequency. These sidebands originate from the induced Rabi oscillations between pairs of excited states that are coupled by the probe pulse. These excited states become populated in the process of plasma cooling. Thus, the sideband radiation intensity tracks the micro-plasma evolution. The sidebands incorporate Rabi shifts corresponding to varying value of the electric field magnitude in the probe pulse: this makes them broad and malleable to tuning. The intensity of the probe beam ~ 1010 W cm-2, creates a maximum sideband shift of> 90 meV from the carrier frequency, resulting in an effective bandwidth of 200 meV. The sidebands may be effectively controlled by the intensity and temporal profile of the probe pulse. The giant Rabi shift is both tunable and coherent over a wide range of frequencies and over a wide range of atomic transitions. The fact that the coherence is observed in a micro plasma demonstrates that Rabi cycling is possible at high temperature with moderately high laser intensities (1010 W cm-2) as long as transitions close to the driving frequency ( ~ 2 % c) are available.
We report observation and control of the spatial-spectral distributions of coherent, dynamic Rabi sideband radiation. The Rabi sidebands result from the interaction of a shaped picosecond probe laser of intensity 10(10) W cm(-2), with neutral excited atomic oxygen generated in a laser-induced microplasma. The spatial-spectral distribution is measured and compared for picosecond laser pulses having either an asymmetric temporal shape or a Gaussian temporal shape. The resulting spatial-spectral distributions are in quantitative agreement with theoretical predictions that account for the radial intensity distribution of the picosecond probe pulse.
Characteristic fringe patterns of spectral interference in dynamic Rabi sidebands are used as a means to investigate decoherence phenomena in a highly nonequilibrium underdense microplasma formed in atmospheric-pressure oxygen gas in the wake of a strong-field (\ensuremath{\sim}1013{}^{13}13 W/cm2{}^{2}2) femtosecond pump pulse. The same transient processes in the nonequilibrium plasma work both to create the effective two-level systems producing coherent sidebands and to destroy the coherence and smear the sideband spectral structure; the observed spectral fringe pattern is a result of the trade-off of these two effects. The sidebands generated on a moderately intense (\ensuremath{\sim}1010{}^{10}10 W/cm2{}^{2}2) picosecond laser pulse reveal the decoherence rate as a function of the pump-pulse intensity and the pump-probe delay time. The rate increases with the pump laser intensity and decreases with the delay with corresponding decoherence times in the range of 750 fs to 3 ps, in good agreement with theory revealing that electron scattering dominates the dynamics for the subnanosecond relaxation processes.