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Physical Review Letters

Macroscopic Manipulation of High-Order-Harmonic Generation Through Bound-State Coherent Control

Itai Hadas, Alon Bahabad

Published Dec 19, 2014• 8 citations
Publisher

Abstract

We propose a paradigm for macroscopic control of high-order harmonic generation by modulating the bound-state population of the medium atoms. A unique result of this scheme is that apart from regular spatial quasi-phase-matching (QPM), also purely temporal QPM of the emitted radiation can be established. Our simulations demonstrate temporal QPM by inducing homogenous Rabi oscillations in the medium and also spatial QPM by creating a grating of population inversion using the process of rapid adiabatic passage. In the simulations a scaled version of high-order harmonic generation is used: a far off-resonance 2.6 μm source generates UV-visible high-order harmonics from alkali-metal-atom vapor, while a resonant near IR source is used to coherently control the medium.

DOI
10.1103/physrevlett.113.253902

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We propose a paradigm for macroscopic control of high-order harmonic generation by modulating the bound-state population of the medium atoms. A unique result of this scheme is that apart from regular spatial quasi-phase-matching (QPM), also purely temporal QPM of the emitted radiation can be established. Our simulations demonstrate temporal QPM by inducing homogenous Rabi oscillations in the medium and also spatial QPM by creating a grating of population inversion using the process of rapid adiabatic passage. In the simulations a scaled version of high-order harmonic generation is used: a far off-resonance 2.6 μm source generates UV-visible high-order harmonics from alkali-metal-atom vapor, while a resonant near IR source is used to coherently control the medium.
High harmonic generation has been considered for many years to be a coherent source of upconverted laser radiation. We propose a method for the generation of essentially incoherent high harmonic generation with a controlled degree of temporal coherence, obeying random-walk statistics. This is achieved by a unique combination of single-atom and macroscopic effects involving preparation of the medium in an excited state with coordinate-dependent population inversion and using an intense off-resonant and phase-mismatched pumping.
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A theory of quantum control of short-wavelength sum-frequency generation, which employs the continuum states, is developed. The proposed scheme employs all-resonant coupling and trade-off optimization of the accompanying constructive and destructive quantum interference effects in the lower-order and higher-order polarizations controlled by the overlap of two autoionizinglike laser-induced continuum structures. The scheme does not rely on adiabatic passage, coherent population trapping or maximum atomic coherence as a means to facilitate maximum output. The opportunities for manipulating transparency of the medium and refractive index for the fundamental and generated radiations, as well as nonlinear polarization in the multiple-resonant medium, are shown. This opens the feasibility of creating frequency-tunable narrowband filters, polarization rotators, and dispersive elements for vacuum ultraviolet radiation. The features specific for quantum interference in Doppler-broadened media are investigated. The feasibility of almost complete conversion of long-wavelength fundamental radiation into generated short-wavelength radiation, and of a dramatic decrease in the intensity of required fundamental radiations, is shown.
We propose and analyze a scheme for adiabatic creation of maximum coherence of 0.5 with a controllable phase between a ground state and the excited state in a model Λ-structured atom using two short laser pulses. One of the pulses has constant carrier frequency quasi-resonant with transition between an initially empty ground and the excite states. The frequency of the second pulse is swept through the resonance with the adjacent transition between the initially populated ground state and the common excited state of the atom. We demonstrate high degree of robustness of the scheme against variation of parameters of the laser radiation in relatively broad region of values. The proposed scheme may find practical applications in the field of multi-photon ionization, high-order harmonics and Raman sideband generation, as well as in nonlinear wave mixing in coherently prepared media.
We have used quantum control to suppress the impact of random atom positions on coherent population transfer within atom pairs, enabling the observation of dipole-dipole driven Rabi oscillations in a Rydberg gas with hundreds of atoms. The method exploits the reduced coupling-strength sensitivity of the off-resonant Rabi frequency, and coherently amplifies the achievable population transfer in analogy to quasi-phase-matching in nonlinear optics. Simulations reproduce the experimental results and demonstrate the potential benefits of the technique to other many-body quantum control applications.