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Physical Review A

Ultrafast saturation of resonant optical processes

Anil K. Patnaik, Sukesh Roy, James R. Gord

Published Dec 10, 2014• 11 citations
Publisher

Abstract

A generalized formulation is presented for determining the saturation thresholds for optical processes excited by ultrafast pulses based on the pulse area of the excitation pulse. It is demonstrated that the threshold of driving-pulse intensity for absorption and fluorescence saturation in a two-level system is inversely proportional to the square of the duration of the excitation pulse. These results are obtained from both a simplified analytical solution assuming a Gaussian excitation pulse shape and a detailed numerical calculation based on density-matrix equations. The calculation is generalized further to obtain the saturation condition for a two-photon Raman process by defining a two-photon pulse area both analytically and numerically. These results not only provide predictive capabilities for determining thresholds of signal saturation using ultrashort durations with arbitrary pulse shapes and durations but also open up possibilities for predetermining the threshold intensities of various resonant nonlinear processes.

DOI
10.1103/physreva.90.063813

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Laser excitation of a two-level atom is analytically studied for arbitrary pulse shape, area, and energy. The ionization mechanism is modeled as a homogeneous width $\ensuremath{\gamma}$ of the atomic excited state. A transformation of the optical Bloch equations allows the dynamics to be completely described by a single equation for the area of the pulse at time $t$, $\ensuremath{\Phi}(t)$. Analytic solutions for the total bound population for a wide variety of pulse shapes can be found in two regions: $\ensuremath{\Phi}(t)\ensuremath{\approx}sin\ensuremath{\Phi}(t)$ and $\ensuremath{\Omega}(t)>\ensuremath{\gamma}$, where $\ensuremath{\Omega}(t)$ is the resonance Rabi frequency. The generalization of the two-level atom results to the $N$-level atom is discussed.

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A generalized formulation is presented for determining the saturation thresholds for optical processes excited by ultrafast pulses based on the pulse area of the excitation pulse. It is demonstrated that the threshold of driving-pulse intensity for absorption and fluorescence saturation in a two-level system is inversely proportional to the square of the duration of the excitation pulse. These results are obtained from both a simplified analytical solution assuming a Gaussian excitation pulse shape and a detailed numerical calculation based on density-matrix equations. The calculation is generalized further to obtain the saturation condition for a two-photon Raman process by defining a two-photon pulse area both analytically and numerically. These results not only provide predictive capabilities for determining thresholds of signal saturation using ultrashort durations with arbitrary pulse shapes and durations but also open up possibilities for predetermining the threshold intensities of various resonant nonlinear processes.
Ultrafast saturation of signals from an optical process occurs when intense laser pulses, with the duration of the driving laser pulse shorter than the effective decay timescales, interact with the target system. Recently, it has been shown that such saturation is marked by transition from transient-absorption to the transient-gain regime, unlike in continuous-wave or long-duration excitations where saturation occurs once the underdamping regime is achieved. The threshold intensities of the drive pulse that drives the optical signal to saturate can be estimated by calculating the area of the pulse. We demonstrate that depending on the shape of the pulse, the saturation behavior differs. The lineshape dependence of ultrafast saturation of absorption and fluorescence is studied for a variety of pulse shapes. We demonstrate that the saturation threshold is lower for super-Gaussian pulses and almost an order of magnitude lower for sech pulses compared to a Gaussian pulse.
The saturation threshold of a probe pulse in an ultrafast electronic-resonance-enhanced (ERE) coherent anti-Stokes Raman spectroscopy (CARS) configuration is calculated. We demonstrate that while the underdamping condition is a sufficient condition for saturation of ERE-CARS with the long-pulse excitations, a transient gain must be achieved to saturate the ERE-CARS signal for the ultrafast probe regime. We identify that the area under the probe pulse can be used as a definitive parameter to determine the criterion for a saturation threshold for ultrafast ERE-CARS. From a simplified analytical solution and a detailed numerical calculation based on density-matrix equations, the saturation threshold of ERE-CARS is compared for a wide range of probe-pulse durations from the 10-ns to the 10-fs regime. The theory explains both qualitatively and quantitatively the saturation thresholds of resonant transitions and also gives a predictive capability for other pulse duration regimes. The presented criterion for the saturation threshold will be useful in establishing the design parameters for ultrafast ERE-CARS.
Resonant two-photon absorption is discussed for the case in which the exciting field may be intense enough and near enough to resonance to cause appreciable saturation. A single pair of levels in an otherwise quite general atom is assumed to satisfy the appropriate resonance condition, and equations are derived governing the time evolution of the associated 2 \ifmmode\times\else\texttimes\fi{} 2 submatrix of the full atomic density matrix. Atomic relaxation is treated explicitly. The analysis, which treats both inversion-symmetric and inversion-nonsymmetric cases within the same general formalism, is developed systematically, the necessary approximations receiving careful discussion. The results are analogous to those for the corresponding one-photon process, but with a shift in the resonance frequency proportional to the intensity of the exciting field. This frequency shift is not identical to the one calculated by time-independent (second-order) perturbation theory, and becomes large when the energy of an intermediate state of the atom approaches the mean of the energies of the active states.
The coupled Maxwell-Schrodinger equations are used to describe propagation of a pulse in a nonlinear absorbing medium. The absorber is assumed to be comprised of a homogeneously broadened system of two-level atoms that are exactly resonant with the field. Numerical calculations have been performed for incident pulses of hyperbolic-secant shape and of duration that is long compared to the atomic phase-memory time. Selected values of input intensity are considered. For intensities below a certain level the calculations nearly agree with rate-equation predictions, but as the incident intensity is increased we find that optical nutation comes into play. The nutation effect leads to pulse breakup as the packet penetrates into the medium. An analytical calculation, for the case of an applied optical field of step-function form, has been performed in order to provide additional insight about the intensity threshold for nutation.
Laser excitation of a two-level atom is analytically studied for arbitrary pulse shape, area, and energy. The ionization mechanism is modeled as a homogeneous width $\ensuremath{\gamma}$ of the atomic excited state. A transformation of the optical Bloch equations allows the dynamics to be completely described by a single equation for the area of the pulse at time ttt, $\ensuremath{\Phi}(t)$. Analytic solutions for the total bound population for a wide variety of pulse shapes can be found in two regions: $\ensuremath{\Phi}(t)\ensuremath{\approx}sin\ensuremath{\Phi}(t)$ and $\ensuremath{\Omega}(t)>\ensuremath{\gamma}$, where $\ensuremath{\Omega}(t)$ is the resonance Rabi frequency. The generalization of the two-level atom results to the NNN-level atom is discussed.