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Physical Review A

Coherent two-photon resonance and Doppler-free population inversion

J. C. Garrison, T. H. Einwohner, Jack Wong

Published Aug 1, 1976• 14 citations
Publisher

Abstract

Doppler-free population inversion induced by coherent two-photon resonance is calculated analytically for a two-photon analog of the hyperbolic-secant pulse and numerically for a Gaussian, linearly chirped pulse. The numerical calculations are carried out for a two-photon resonance of a chirped ruby laser line with the $6{S}_{\frac{1}{2}}\ensuremath{\rightarrow}9{D}_{\frac{3}{2}}$ transition in Cs. Complete inversion is found when the fractional change in frequency during the pulse lies between 6 \ifmmode\times\else\texttimes\fi{} ${10}^{\ensuremath{-}6}$ and 2 \ifmmode\times\else\texttimes\fi{} ${10}^{\ensuremath{-}5}$. The coherent two-photon resonances are described by optical Bloch equations which are derived from a multiple-time-scale perturbation theory.

DOI
10.1103/physreva.14.731

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arXiv:physics/9812010•Journal of Physics B Atomic Molecular and Optical Physics•Jan 1, 1999•11 citations
Doppler-free population inversion induced by coherent two-photon resonance is calculated analytically for a two-photon analog of the hyperbolic-secant pulse and numerically for a Gaussian, linearly chirped pulse. The numerical calculations are carried out for a two-photon resonance of a chirped ruby laser line with the 6S12\ensuremath→9D326{S}_{\frac{1}{2}}\ensuremath{\rightarrow}9{D}_{\frac{3}{2}}6S21​​\ensuremath→9D23​​ transition in Cs. Complete inversion is found when the fractional change in frequency during the pulse lies between 6 \ifmmode\times\else\texttimes\fi{} 10\ensuremath−6{10}^{\ensuremath{-}6}10\ensuremath−6 and 2 \ifmmode\times\else\texttimes\fi{} 10\ensuremath−5{10}^{\ensuremath{-}5}10\ensuremath−5. The coherent two-photon resonances are described by optical Bloch equations which are derived from a multiple-time-scale perturbation theory.
In this research study, we derive the exact solutions of the Bloch equations describing the dynamics of a two-level atom with dephasing. In the two-level atom, a strong laser pump couples a ground state to an upper excited state with a time-dependent Rabi-frequency. The exact solutions are given for the atomic population inversion and the real and imaginary parts of the coherence while the input pulse is an asymmetric hyperbolic cosine form. Additionally, the system is under a chirped detuning. The method of solving the Bloch equations analytically is a very tedious part of the research, and as far as we know, there are few exact solutions available in this field. Hence, our solutions might be of great interest to various research areas, including nuclear magnetic resonance, where analytical solutions to the Bloch equations play a major role in the study of the information on the state of the medium as determined by the NMR signals.
A class of molecular two-photon processes, occurring under transient or steady-state conditions, is analyzed exactly for certain cases using a density-matrix formalism. Our results are relevant to the recently observed phenomena of transient coherent Raman beats and steady-state two-photon absorption of oppositely directed laser beams. Lowest-order perturbation theories have shown that these processes are insensitive to the Doppler effect, and consequently the linewidth is unaffected by Doppler broadening and by elastic collisions that change molecular velocity. The solutions presented here are of the same form for the Raman and two-photon problems and reveal significant power-dependent frequency shifts and line broadening that correct the ideal Doppler-free solutions. For the transient case, we assume a molecular three-level quantum structure that can be switched in or out of optical resonance with cw laser radiation by means of a pulsed dc Stark field, but the solutions also apply when resonant optical pulses are introduced. During the resonant condition when the Stark pulse is on, the three levels are prepared in coherent superposition, and during the nonresonant condition following the Stark pulse, the laser field(s) stimulates the coherently prepared sample in a transient two-photon process. One of these processes, the Ramanbeat effect, has been observed in forward scattering, but the second one, transient two-photon emission, should be observable in backward scattering. Bloch-like equations are derived for this three-level problem that facilitate an exact pulse solution for state preparation. Following the pulse, transient decay is well-approximated by a perturbation calculation. For the steady-state case, an exact solution is also obtained and is of interest for continuous-wave spectroscopy or for transient experiments requiring an initial preparation of quantum states, prior to Stark switching. These solutions exhibit a power-dependent line broadening and a frequency shift of magnitude $\ensuremath{\sim}\frac{\ensuremath{\Delta}({\ensuremath{\alpha}}^{2}\ensuremath{-}{\ensuremath{\beta}}^{2})}{({\ensuremath{\Delta}}^{2}+\frac{1}{{T}_{2}^{2}})}$, in agreement with our earlier estimate, where $\ensuremath{\alpha}$ and $\ensuremath{\beta}$ are the Rabi flopping frequencies for the two intermediate transitions and $\ensuremath{\Delta}$ is the off-resonance tuning behavior for one of them.
In this project I developed a general method of finding the optimal laser excitation for an ensemble of two-level atoms with the primary goal of exciting as many atoms as possible, as quickly as possible, for as long as possible, in order of decreasing priority. Specifically, I simulated the laser excitation of a collection of Rubidium-87 atoms from (n=5, L=0, S=1/2, J=1/2) to (n=5, L=1, S=1/2, J=3/2), by finding numerical solutions to the optical Bloch equations. I optimized the parameters of a linear chirp paired with a Gaussian intensity pulse first neglecting and then including spontaneous emission, and then for a hyperbolic-tangent chirp paired with a squared-hyperbolic-secant intensity pulse including spontaneous emission. Comparing the optimal parameters for the linear chirp both with and without spontaneous emission demonstrated that neglecting spontaneous emission will lead to significant errors, at least when considering Rubidium-87. Comparing the linear chirp to the hyperbolic-tangent chirp (both with spontaneous emission) showed that both chirp shapes lead to excitation of greater than 96% of the population, and that based on my simulations, the linear chirp was slightly better at meeting all three goals of ceiling, speed and endurance. The best of all the excitations that I found using a linear chirp is to use a chirp rate between 0.2 and 0.65 GHz/ns and to use a pulse with a FWHM of 100 ns and a peak intensity of 10 W/cm^2.
Detailed theoretical analysis and numerical simulation indicate that nearly complete electronic population inversion of molecular systems can be achieved with intense positively chirped broadband laser pulses. To provide a simple physical picture, a two-level model is used to examine the condition for the so-called π pulses and a four-level model is designed to demonstrate for molecular systems the correlation between the sign of the chirp and the excited state population. The proposed molecular π pulse is the combined result of vibrational coherence in the femtosecond regime and adiabatic inversion in the picosecond regime. Numerical results for a displaced oscillator, for LiH and for I2, show that the proposed molecular π pulse scheme is robust with respect to changes in field parameters such as the linear positive chirp rate, field intensity, bandwidth, and carrier frequency, and is stable with respect to thermal and condensed phase conditions including molecular rotation, rovibronic coupling, and electronic dephasing.
Via a non-perturbative method we study the population dynamics and photoelectron spectra of Cs atoms subject to intense chirped laser pulses, with Gaussian beams. We include above threshold ionization spectral peaks. The frequency of the laser is near resonance with the 6s-7p transition. Dominant couplings are included exactly, weaker ones accounted for perturbatively. We calculate the relevant transition matrix elements, including spin-orbit coupling. The pulse is taken to be a hyperbolic secant in time and the chirping a hyperbolic tangent. This choice allows the equations of motions for the probability amplitudes to be solved analytically as a series expansion in the variable , where is a measure of the pulse length. We find that the chirping changes the ionization dynamics and the photoelectron spectra noticeably, especially for longer pulses of the order of au. The peaks shift and change in height, and interference effects between the 7p levels are enhanced or diminished according to the amount of chirping and its sign. The integrated ionization probability is not strongly affected.