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Physical Review A

Phase-coherent multilevel two-photon transitions in cold Rb atoms: Ultrahigh-resolution spectroscopy via frequency-stabilized femtosecond laser

Tai Hyun Yoon, Adela Marian, J. L. Hall, Jun Ye

Published Dec 6, 2000• 37 citations
Publisher

Abstract

A two-photon transition in cold Rb atoms will be probed with a phase-coherent wide bandwidth femtosecond laser comb. Frequency domain analysis yields a high-resolution picture where phase coherence among various transition pathways through different intermediate states produces interference effects on the resonantly enhanced transition probability. This result is supported by the time domain Ramsey interference effect. The two-photon transition spectrum is analyzed in terms of the pulse repetition rate and carrier frequency offset, leading to a cold-atom-based frequency stabilization scheme for both degrees of freedom of the femtosecond laser.

DOI
10.1103/physreva.63.011402

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A two-photon transition in cold Rb atoms will be probed with a phase-coherent wide bandwidth femtosecond laser comb. Frequency domain analysis yields a high-resolution picture where phase coherence among various transition pathways through different intermediate states produces interference effects on the resonantly enhanced transition probability. This result is supported by the time domain Ramsey interference effect. The two-photon transition spectrum is analyzed in terms of the pulse repetition rate and carrier frequency offset, leading to a cold-atom-based frequency stabilization scheme for both degrees of freedom of the femtosecond laser.
An alternate method of two-photon spectroscopy is presented where cesium atoms interact with a phase-modulated laser beam. Doppler-free two-photon spectroscopy of the cesium atom $6S\ensuremath{\rightarrow}8S$ hyperfine transition was used to experimentally demonstrate quantum interfered two-photon spectra. We calculated the photon-atom interaction by second-order perturbation theory and assumed that the one-photon frequency is detuned far from any intermediate state. Then we calculated the relative transition rates of all spectral lines resolved by the laser carrier and sidebands. A physical picture of multipathway quantum interference in the frequency domain is given that explains the unusual line strength, based on the trick that a phase-modulated laser beam can be decomposed into a series of coherent and collinear laser modes (carrier and sidebands). For all pairs of modes in which the sum frequency of each pair was on resonance with the cesium atom $6S\ensuremath{\rightarrow}8S$ transition, the superposition of all pathways induced by the different mode pairs resulted in a destructive interference, which then leads to a lack of absorption. We have shown in this paper that our calculation agrees very well with our experimental results in terms of the relative interfered line strengths, which were functions of modulation depth. We further discuss some related issues concerning laser stabilization and we demonstrate an approach for simultaneously comparing two cesium cells.
We present experiments demonstrating high-resolution and wide-bandwidth coherent control of a four-level atomic system in a diamond configuration. A femtosecond frequency comb is used to excite a specific pair of two-photon transitions in cold 87Rb. The optical-phase-sensitive response of the closed-loop diamond system is studied by controlling the phase of the comb modes with a pulse shaper. Finally, the pulse shape is optimized resulting in a 256% increase in the two-photon transition rate by forcing constructive interference between the mode pairs detuned from an intermediate resonance.
Coherent control of the atomic two-photon absorption with shaped single-cycle pulses is examined theoretically in the weak-field regime. The control over the stabilized carrier-envelope phase (CEP) of the pulses is determined as a key parameter allowing the full utilization of the ultrabroad pulse spectrum. This bandwidth is sufficient to provide besides the sequential two-photon pathways, additional Raman-type pathways coupling between the ground and the excited states. The interference between the different pathways is efficiently controlled via the control over the CEP. Simplified two-level model is analyzed in the frequency domain where the rational pulse shaping is applied. The developed intuition is applied to atomic Cs and verified by the exact numerical solution of time-dependent Schrodinger equation.
Coherent control of femtosecond two-photon absorption in the intermediate-field regime is analyzed in detail in the powerful frequency domain using an extended 4th-order perturbative description. The corresponding absorption is coherently induced by the weak-field non-resonant two-photon transitions as well as by four-photon transitions involving three absorbed photons and one emitted photons. The interferences between these two groups of transitions lead to a difference between the intermediate-field and weak-field absorption dynamics. The corresponding interference nature (constructive or destructive) strongly depends on the detuning direction of the pulse spectrum from half the two-photon transition frequency. The model system of the study is atomic sodium, for which both experimental and theoretical results are obtained. The detailed understanding obtained here serves as a basis for coherent control with rationally-shaped femtosecond pulses in a regime of sizable absorption yields.
Weak-field coherent phase control of atomic non-resonant multiphoton excitation induced by shaped femtosecond pulses is studied theoretically in the single-cycle regime. The carrier-envelope phase (CEP) of the pulse, which in the multi-cycle regime does not play any control role, is shown here to be a new effective control parameter that its effect is highly sensitive to the spectral position of the ultrabroad spectrum. Rationally chosen position of the ultrabroadband spectrum coherently induces several groups of multiphoton transitions from the ground state to the excited state of the system: transitions involving only absorbed photons as well as Raman transitions involving both absorbed and emitted photons. The intra-group interference is controlled by the relative spectral phase of the different frequency components of the pulse, while the inter-group interference is controlled jointly by the CEP and the relative spectral phase. Specifically, non-resonant two- and three-photon excitation is studied in a simple model system within the perturbative frequency-domain framework. The developed intuition is then applied to weak-field multiphoton excitation of atomic cesium (Cs), where the simplified model is verified by non-perturbative numerical solution of the time-dependent Schrödinger equation. We expect this work to serve as a basis for a new line of femtosecond coherent control experiments.