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Laser & Photonics Review

Adiabatic processes in frequency conversion

Haim Suchowski, Gil Porat, Ady Arie

Published Oct 20, 2013• 158 citations
Publisher

Abstract

Adiabatic evolution, an important dynamical process in a variety of classical and quantum systems providing a robust way of steering a system into a desired state 1-5, was introduced only recently to frequency conversion 6-9. Adiabatic frequency conversion allowed the achievement of efficient scalable broadband frequency conversion 8, 9 and was applied successfully to the conversion of ultrashort pulses, demonstrating near-100% efficiency for ultrabroadband spectrum 10-16. The underlying analogy between undepleted pump nonlinear processes and coherently excited quantum systems was extended in the past few years to multi-level quantum systems, demonstrating new concepts in frequency conversion, such as complete frequency conversion through an absorption band 17-20. Additionally, the undepleted pump restriction was removed, enabling the exploration of adiabatic processes in the fully nonlinear dynamics regime of nonlinear optics 21-26. In this article, the basic concept of adiabatic frequency conversion is introduced, and recent advances in ultrashort physics, multi-process systems, and the fully nonlinear dynamics regime are reviewed.

DOI
10.1002/lpor.201300107

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Adiabatic evolution, an important dynamical process in a variety of classical and quantum systems providing a robust way of steering a system into a desired state 1-5, was introduced only recently to frequency conversion 6-9. Adiabatic frequency conversion allowed the achievement of efficient scalable broadband frequency conversion 8, 9 and was applied successfully to the conversion of ultrashort pulses, demonstrating near-100% efficiency for ultrabroadband spectrum 10-16. The underlying analogy between undepleted pump nonlinear processes and coherently excited quantum systems was extended in the past few years to multi-level quantum systems, demonstrating new concepts in frequency conversion, such as complete frequency conversion through an absorption band 17-20. Additionally, the undepleted pump restriction was removed, enabling the exploration of adiabatic processes in the fully nonlinear dynamics regime of nonlinear optics 21-26. In this article, the basic concept of adiabatic frequency conversion is introduced, and recent advances in ultrashort physics, multi-process systems, and the fully nonlinear dynamics regime are reviewed.
In this work, we thoroughly investigated frequency conversion towards ultrashort picosecond (ps) laser pulses in the vacuum ultraviolet (VUV) spectral regime via nonlinear optics in coherently-driven quantum systems at high intensities. We applied approaches of adiabatic quantum dynamics relying on coherent light-matter interactions, which modify the "bare" eigenstates of a quantum system to "dressed" states and exploit slow (i.e., adiabatic) population evolutions via such dressed states. This enables enhancement of typically low-order, low-intensity nonlinear optics (at MW/cm², GW/cm²), where the light field perturbs the atomic level structure only weakly. On the other hand, aiming at nonlinear optics at higher orders, e.g., high-harmonic generation, strong light fields are applied (100 TW/cm², PW/cm²), which modify the Coulomb potential of the atom strongly. In this case, resonances play no role anymore and adiabatic quantum dynamics via atomic resonances will not work. With this work, we demonstrated the implementation of adiabatic quantum dynamics and coherently prepared media for nonlinear optics in an intermediate intensity regime (TW/cm²), i.e., at Keldysh parameters approaching γ≈1. The fundamental question was, whether the high intensities still permit us to drive and exploit coherent-adiabatic dynamics via dressed states for enhancement of frequency conversion processes. We investigated two approaches to enhance the frequency conversion yield applying nonlinear optics in coherently-driven quantum systems (rare gases). In the first approach, we resonantly enhanced harmonic generation via dressed states with large Autler-Townes splittings. With this approach, we demonstrated how to make atomic resonances available for an initially far detuned fixed-frequency pump laser and showed a compensation for inevitable, perturbing Stark shifts. In the second approach, we investigated frequency conversion, enhanced by coherent population return (CPR) and preparation of maximal atomic coherences at high intensities. With this approach, we showed how to maximally benefit from an atomic resonance via adiabatically driven frequency conversion, i.e., by detuning the strong pump laser slightly from the resonance.
We discuss theoretically and demonstrate experimentally the robustness of the adiabatic sum frequency conversion method. This technique, borrowed from an analogous scheme of robust population transfer in atomic physics and nuclear magnetic resonance, enables the achievement of nearly full frequency conversion in a sum frequency generation process for a bandwidth up to two orders of magnitude wider than in conventional conversion schemes. We show that this scheme is robust to variations in the parameters of both the nonlinear crystal and of the incoming light. These include the crystal temperature, the frequency of the incoming field, the pump intensity, the crystal length and the angle of incidence. Also, we show that this extremely broad bandwidth can be tuned to higher or lower central wavelengths by changing either the pump frequency or the crystal temperature. The detailed study of the properties of this converter is done using the Landau-Zener theory dealing with the adiabatic transitions in two level systems.
We present experimental data on adiabatically driven frequency conversion with ultrashort (picosecond) laser pulses towards the vacuum-ultraviolet regime, enhanced by coherent population return and preparation of maximal atomic coherences. We generate the sum frequency of an intense pump pulse and a probe pulse via a two-photon resonance in xenon. When we slightly detune the pump laser from two-photon resonance, the atomic populations are adiabatically driven forth and back from the atomic ground state to an excited state. This coherent population return (CPR) prepares the medium in a transient state of maximal atomic coherence, which enhances frequency mixing with a probe laser. We thoroughly study the variation of CPR-enhanced frequency conversion with experimental parameters and compare CPR with conventional, resonantly enhanced frequency conversion. In particular, we investigate the temporal evolution of the atomic coherence and the effect of inevitable ac Stark shifts. We find that ac Stark shifts induce an asymmetry in the spectral characteristics of CPR, which nevertheless permits enhanced frequency conversion. For the case of resonantly enhanced frequency conversion, we show that the atomic coherences are maintained for several tens of picoseconds after the pump pulse, which permits time-delayed frequency conversion. Moreover, we analyze the pressure dependence of the atomic coherence' lifetime and observe a free induction decay at the two-photon coherence with the generation of a second harmonic field. These findings shall push applications of adiabatic light-matter interactions also to the regime of nonlinear optics, driven by intense laser pulses.
A comprehensive study of two simultaneous three wave mixing processes, a second harmonic generation followed by difference frequency generation, under nonlinear stimulated Raman adiabatic passage (STIRAP) is presented. An input pump is up-converted to its second harmonic, which then gets down-converted to a signal and idler pair with frequencies lying very close to the input pump in such a manner that complete conversion from the pump to the signal and idler takes place without exciting the second harmonic under counterintuitive adiabatic passage. This process involves nonlinear STIRAP with a nonlinear dark state similar to atomic population transfers, and we bring an analogy from atomic systems to our nonlinear dynamics to linearize the problem and analytically obtain the adiabaticity condition required for complete conversion. We also show that the nonlinear STIRAP mechanism results in a large bandwidth of about 380 nm with almost complete conversion of the pump to the signal and idler.
Single-photon frequency upconversion is a nonlinear process where the frequency of the signal photon is translated to the higher frequency with the complete preservation of all the quantum characteristics of the “flying” qubits [1,2]. One promising application of the singlephoton frequency upconversion is converting the infrared photons to the desired spectral regime (usually visible regime) where the high performance detectors are available for sensitive detections [3-6]. The infrared single-photon frequency upconversion detection technique has been successfully used in a variety of applications, including infrared imaging [7] and infrared ultra-sensitive spectroscopy [8,9]. Additionally, such upconversion detector has greatly benefited the applications stringently requiring efficient photon detection in optical quantum computation and communication [10-12]. Furthermore, due to the phase-matching requirement in the frequency upconversion process, the upconversion detectors have some unique features, such as narrow-band wavelength acceptance [13] and polarization sensitivity [14], both of which render them very useful for fiber based quantum systems [15]. In the recent decade, experiments bear that the photon correlation, entanglement, and photon statistics are all well preserved in the coherent frequency upconversion [16-18].