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arXiv:1905.08362 · Physical review. B./Physical review. B

Ultrafast quantum-path interferometry revealing the generation process of coherent phonons

Kazutaka G. Nakamura, Kensuke Yokota, Yuki Okuda, Rintaro Kase, Takashi Kitashima, yu mishima, Yutaka Shikano, Yōsuke Kayanuma

Published May 20, 2019• 17 citations
arXivHTMLPDF

Abstract

Ultrafast quantum-path interferometry by using a pair of relative-phase-locked femtosecond pulses is proposed to evaluate the contribution of each quantum path in an optical transition. The observed characteristic interference fringes (collapse and revival) reveal that the impulsive stimulated Raman scattering is dominant in the coherent-phonon generation in $n$-type GaAs even in an opaque condition. It is demonstrated that the optical dual-pulse pumping actively creates quantum mechanical superposition of the electronic and phononic states in a bulk solid.

DOI
10.1103/physrevb.99.180301

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EPJ Web of Conferences•Jan 1, 2013•0 citations
Ultrafast quantum-path interferometry by using a pair of relative-phase-locked femtosecond pulses is proposed to evaluate the contribution of each quantum path in an optical transition. The observed characteristic interference fringes (collapse and revival) reveal that the impulsive stimulated Raman scattering is dominant in the coherent-phonon generation in nnn-type GaAs even in an opaque condition. It is demonstrated that the optical dual-pulse pumping actively creates quantum mechanical superposition of the electronic and phononic states in a bulk solid.
We investigated the coherent phonon generation mechanism by irradiation of an ultrashort pulse with a simple two-level model. Our derived formulation shows that both impulsive stimulated Raman scattering (ISRS) and impulsive absorption (IA) simultaneously occur, and phonon wave packets are generated in the electronic ground and excited states by ISRS and IA, respectively. We identify the dominant process from the amplitude of the phonon oscillation. For short pulse widths, ISRS is very small and becomes larger as the pulse width increases. We also show that the initial phase is dependent on the pulse width and the detuning.
The four-wave mixing produced with two ultrashort phase-locked !-3! laser pulses propagating coherently in a two-level system in the infrared spectral region is shown to depend on the pulses relative phase. The Maxwell-Bloch equations are solved beyond the rotating-wave approximation to account for field frequencies which are largely detuned from the atomic resonance. The relative phase dominating the efficiency of the coupling to the 5! anti-Stokes Raman component is determined by sign of the total ac Stark shift induced in the system, in such a way that the phase influence disappears precisely where the ac Stark effect due to both pulses is compensated. This fundamental quantum interference effect can be the basis for nonlinear ultrafast optical spectroscopy techniques. Phenomena arising from the coherent control of nonlinear interactions are of importance in fields as diverse as optoelectronics and materials research, in high harmonic generation, in photoionization or molecular dissociation, and in biological applications such as spectroscopy and imaging, among others [1, 2, 3, 4, 5, 6, 7]. Optical quantum coherent control is based on the fact that the phases of interfering transition amplitudes in light-matter interactions can be controlled through the optical phase of coherent light sources that drive the interaction, in such a way that the transition rates to final states and the dynamics at various stages of the process can be modified [1]. In a recent paper [8], a theoretical investigation on the quantum coherent control of the optical transient four-wave mixing of two intense phase-locked femtosecond laser pulses of central angular frequencies ω and 3ω propagating in a two-level atom (TLA) was reported. It was shown how the nonlinear (χ (3) ) coupling to the antiStokes Raman field at frequency 5ω depends critically on the initial relative phase φ of the propagating pulses. In Ref. [8], the study was centered to intense pulses in the visible and ultraviolet spectral regions, with frequencies at resonance or lower than the atomic transition. The phenomena observed in [8], however, can be scaled to various laser and material parameters. In the infrared spectral range, for instance, experiments on ultrafast molecular dynamics are frequently performed by help of twocolor pump probe nonlinear spectroscopy techniques. In this type of studies, due to the high intensities inherent to ultrashort (subpicosecond) pulses, nonlinear effects such as stimulated Raman processes may become important and are often utilized as a complementary tool to gain information [9]. In this Letter, we address the conditions for quantum coherent control of transient four-wave mixing interactions with two phase-locked ω-3ω femtosecond laser pulses in the mid-IR spectral region. Our purpose is to reveal the basic physics for a strict two-level medium and to this end the Maxwell-Bloch TLA will be considered. We will study pulses with a duration of 300 fs (with a w 5w
Coherent optical phenomena such as the optical Stark effect, Rabi flopping, photon echo and quantum beating which are well-known in atomic spectroscopy can also be observed in semiconductors by using femtosecond laser pulses. On these short time scales, the quantum coherence of the optical excitations in the solid do not only influence the optical properties but change at the same time the relaxation and dephasing kinetics. The quasi-classical Boltzmann kinetics has to be replaced by quantum kinetics. Coherence leads to the appearance of memory in the scattering integrals. For femtosecond four-wave mixing and pump-and-probe spectroscopy the use of quantum kinetics for LO-phonon and for carrier-carrier scattering will be reviewed.
Abstract The interaction between ultrashort light pulses and non-absorbing materials is dominated by impulsive stimulated Raman scattering (ISRS). The description of ISRS in the context of pump&probe experiments is based on effective classical models describing the interaction between the phonon and pulsed electromagnetic fields. Here we report a theoretical description of ISRS where we do not make any semi-classical approximation and we treat both photonic and phononic degrees of freedom at the quantum level. The results of the quantum model are compared with semiclassical results and validated by means of spectrally resolved pump&probe measurements on α-quartz.
Two-phonon bound states have been excited exclusively in ZnTe(110) via impulsive stimulated second-order Raman scattering, essentially being squeezed states due to phase coherent excitation of two identical components anticorrelated in the wave vector. By using coherent control technique with a pair of femtosecond laser pulses, the manipulation of squeezed states has been demonstrated in which both the amplitude and lifetime of coherent oscillations of squeezed states are modulated, indicating the feasibility to control the quantum noise and the quantum nature of phonon squeezed states, respectively.