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Physical Review A

Many-mode Floquet theoretical approach for coherent control of multiphoton dynamics driven by intense frequency-comb laser fields

Sang-Kil Son, Shih‐I Chu

Published Jun 5, 2008• 19 citations
Publisher

Abstract

We extend the many-mode Floquet theorem (MMFT) for the investigation of multiphoton resonance dynamics driven by intense frequency-comb laser fields. The frequency comb structure generated by a train of short laser pulses can be exactly represented by a combination of the main frequency and the repetition frequency. MMFT allows non-perturbative and exact treatment of the interaction of a quantum system with the frequency-comb laser fields. We observe simultaneous multiphoton resonance processes between a two-level system and frequency-comb laser. The multiphoton processes can be coherently controlled by tuning the laser parameters such as the carrier-envelope phase (CEP) shift. In particular, high-order harmonic generation shows immense enhancement by tuning the CEP shift, due to simultaneous multiphoton resonances.

DOI
10.1103/physreva.77.063406

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We extend the many-mode Floquet theorem (MMFT) for the investigation of multiphoton resonance dynamics driven by intense frequency-comb laser fields. The frequency comb structure generated by a train of short laser pulses can be exactly represented by a combination of the main frequency and the repetition frequency. MMFT allows non-perturbative and exact treatment of the interaction of a quantum system with the frequency-comb laser fields. We observe simultaneous multiphoton resonance processes between a two-level system and frequency-comb laser. The multiphoton processes can be coherently controlled by tuning the laser parameters such as the carrier-envelope phase (CEP) shift. In particular, high-order harmonic generation shows immense enhancement by tuning the CEP shift, due to simultaneous multiphoton resonances.
We present a theoretical investigation of the multiphoton resonance dynamics driven by intense frequency-comb and cavity-mode fields inside a femtosecond enhancement cavity (fsEC). The many-mode Floquet theorem is employed to provide a nonperturbative and exact treatment of the interaction between a quantum system and laser fields. The quasienergy structure driven by the frequency-comb laser field is modified by coupling the cavity-mode field and the multiphoton resonance processes between modified quasienergy states, resulting in the generation of even-order harmonics. The high-order harmonic generation (HHG) from a two-level system driven by the laser fields can be coherently controlled by tuning the laser parameters. In particular, the tuning intensity of the cavity-mode field allows one to coherently control the HHG power spectra without changing the absolute positions of comb frequencies.
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.
This Letter demonstrates control over multiphoton absorption processes in driven two-level systems, which include, for example, superconducting qubits or laser-irradiated graphene, through spectral shaping of the driving pulse. Starting from calculations based on Floquet theory, we use differential evolution, a general purpose optimization algorithm, to find the Fourier coefficients of the driving function that suppress a given multiphoton resonance in the strong field regime. We show that the suppression of the transition probability is due to the coherent superposition of high-order Fourier harmonics which closes the dynamical gap between the Floquet states of the two-level system.
In order to control the state of a two-level quantum system (e.g. the spin state of an ion qubit), optical frequency combs perform a two-photon stimulated Raman process through stimulated absorption from one comb tooth and stimulated emission into another comb tooth. If the two-level energy gap is an integer multiple of the repetition rate of the laser, resonant Rabi oscillations are excited. When these latter have a frequency close to the qubit’s transition one, a strongly anharmonic phase-locked cycle may exist on the Bloch sphere, which generates a sub-harmonic series of very narrow, equally spaced, spectral lines. If the repetition rate of an optical frequency comb is appropriately tuned to these latter (up to the average carrier envelope frequency), a highly resonant dynamical regime of the two-level system should be reached where the Raman stimulated absorption and emission processes would occur for any pair of adjacent comb teeth.
The authors present an exact treatment of two- and multiquantum transitions in three-level systems driven by two intense linearly polarised monochromatic fields based on the semiclassical many-mode Floquet theory developed recently. Further they extend the almost degenerate perturbation theory of Salwen (1955-6) to the two-mode Floquet Hamiltonian and obtain approximate analytical formulae for multiphoton transition probabilities, resonance bichromatic shifts and widths, and absorption lineshapes beyond the conventional rotating-wave approximation (RWA). Detailed comparison of the analytical, the RWA, and the exact results is given. Several novel features of multiphoton lineshape characteristics are pointed out.
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.