The last two decades have marked a revolution in materials science with the appearance of two novel groups of materials with promising features for future optoelectronics. The first are artificially fabricated metamaterials, composed of carefully engineered nanoparticle arrays, displaying tailored mie and plasmonic resonant responses [1]. The second are atomically thin two-dimensional (2D) semiconductor crystals, characterized by tightly bound excitons, promising for their flexible heterostructure stacking capabilities [2]. In this work we introduce a novel pulse-shaping approach, to study and control the coherent dynamics of resonant quasparticle excitations in such materials. By constructing a state-of-the-art pulse shaper for controlling the spectral phase of our sub-10 fs laser, we tailor the temporal order of instantaneous frequencies driving the noninstantaneous electronic response of the material on resonance [3]. We measure the response to various pulse shapes through monitoring the four-wave mixing (FWM) generation. Our contribution can be described by to three key aspects: We retrace the resonant dispersion by synchronizing the phase-dependent intra-pulse nonlinear wave-mixing with the prediction of the anharmonic oscillator model (AHO). We disentangle the multitude of interfering quantum pathways caused by the resonant dynamics, and reassemble them to achieve a strong nonlinear enhancement as well as near-complete destruction of the nonlinear yield. By controlling two successive resonant states, we present a glimpse into inter-state selectivity. We display nonlinear generation by improving the coherence in one state while suppressing the coherence in another. We believe this work places the control of coherent quasiparticle dynamics in condensed matter systems as a highly appealing field for both fundamental and applied research, such as improved nonlinear sensing, broadband compressed light sources and various ultrafast optoelectronic applications.
The last two decades have marked a revolution in materials science with the appearance of two novel groups of materials with promising features for future optoelectronics. The first are artificially fabricated metamaterials, composed of carefully engineered nanoparticle arrays, displaying tailored mie and plasmonic resonant responses [1]. The second are atomically thin two-dimensional (2D) semiconductor crystals, characterized by tightly bound excitons, promising for their flexible heterostructure stacking capabilities [2]. In this work we introduce a novel pulse-shaping approach, to study and control the coherent dynamics of resonant quasparticle excitations in such materials. By constructing a state-of-the-art pulse shaper for controlling the spectral phase of our sub-10 fs laser, we tailor the temporal order of instantaneous frequencies driving the noninstantaneous electronic response of the material on resonance [3]. We measure the response to various pulse shapes through monitoring the four-wave mixing (FWM) generation. Our contribution can be described by to three key aspects: We retrace the resonant dispersion by synchronizing the phase-dependent intra-pulse nonlinear wave-mixing with the prediction of the anharmonic oscillator model (AHO). We disentangle the multitude of interfering quantum pathways caused by the resonant dynamics, and reassemble them to achieve a strong nonlinear enhancement as well as near-complete destruction of the nonlinear yield. By controlling two successive resonant states, we present a glimpse into inter-state selectivity. We display nonlinear generation by improving the coherence in one state while suppressing the coherence in another. We believe this work places the control of coherent quasiparticle dynamics in condensed matter systems as a highly appealing field for both fundamental and applied research, such as improved nonlinear sensing, broadband compressed light sources and various ultrafast optoelectronic applications.
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
In this paper, we report on the ultrafast coherent control of excitons in quantum wells using a phase-locked pulse sequence generated by pulse-shaping techniques. The pulse-shaping system with a double liquid-crystal spatial light modulator (SLM), and a Ti3+-sapphire laser is used to generate phase-locked pulses. The ultrafast coherent control of the exciton population and polarization is demonstrated by the observation of the reflectivity change in the pump-probe and the diffracted power in the degenerate-four-wave-mixing (DFWM) measurements. In single quantum wells, good coherent control characteristics with 87% coherent carrier destruction are demonstrated at the low excitation power of 0.15 mW (∼1.1×1010 photons/cm2). In addition, the preliminary manipulation of the exciton population is demonstrated by the phase-locked triple pulses. In the case of coupled quantum wells, the modulation of the SLM is carefully controlled and the coherent control of both the exciton population and the polarization is demonstrated in the two different coupled quantum-well samples.
The recent advent of optical metasurfaces, ultra-thin structures composed of nanoresonators facilitating strong light concentration [1–3], opens the path towards efficient \nfrequency conversion [4–7] in a material thousand times thinner than a human hair [8]. \nThere is a remarkable capacity to individually shape each nanoresonator of the metasurface to spatially and spectrally control the conversion process with unprecedented \nnanoscale resolution, facilitating an ultimate flexibility to selectively convert, focus, \nand image different colours with a single metasurface. The strong enhancement of the \nnonlinear processes in dielectric nanoresonators is largely due to the absence of material \nabsorption and the excitation of Mie-type bulk resonances [2]. The highest conversion \nefficiency to date has been achieved employing III-V semiconductor nanostructures, \nsuch as AlGaAs which is a non-centrosymmetric material with high quadratic nonlinear \nsusceptibility. In particular, second-harmonic generation efficiencies up to 10−4 have \nbeen recently demonstrated [8–12], six orders of magnitude higher than in plasmonics. \nSuch capabilities can make an immense fundamental and practical impact, including \nthe quantum state generation in nonlinear metasurfaces as we discuss in this chapter. \nThe quantum state of correlated photon-pairs is the essential building block for photon entanglement [13, 14], which underpins many quantum applications, including secure networks, enhanced measurement and lithography, and quantum information processing [15]. One of the most versatile techniques for the generation of correlated photons is the process of spontaneous parametric down-conversion (SPDC) [16, 17], see \nFig. 1. It allows for an arbitrary choice of energy and momentum correlations between \nthe generated photons, robust operation at room temperature, as well as for spatial and \ntemporal coherence between simultaneously pumped multiple SPDC sources. Alternative approaches based on atom-like single photon emitters, such as solid-state fluorescent atomic defects [18], quantum dots [19, 20], and 2D host materials [21, 22], have \nreached a high degree of frequency indistinguishability, purity and brightness [19, 20]. \nHowever, this comes with the expense of operation at cryogenic temperatures and lack \nof spatial coherence between multiple quantum emitters. These features might limit \npossible applications and reduce the potential for device scalability. Furthermore, the \nsmall size of the atomic sources often requires complex schemes aimed at coupling to \noptical nanoantennas and improving the photon extraction efficiency [21]. \nThe miniaturization of SPDC quantum-light sources to micro and nanoscale dimensions is a continuing quest, as it enables denser integration of functional quantum \ndevices. Traditionally, bulky cm-sized crystals were utilized for SPDC, entailing the \ndifficulty of aligning multiple optical elements after the SPDC crystal, while offering \nrelatively low photon-pair rates [17]. As a first step of miniaturization, SPDC was \nrealized in low-index-contrast waveguides, which allowed confining light down to several square micrometers transversely to the propagation direction, significantly enhancing the conversion efficiency [23]. However, this approach still requires centimetres \nof propagation length, which makes the on-chip integration with other elements challenging [24]. The introduction of high-index contrast waveguides and ring resonators \nallowed for shrinking the sizes necessary for SPDC to millimetres [25], and to tens \nof micrometers [26]. However, further miniaturisation down to the metasurfaces composed of nanoresonators requires conceptually different approaches.
The three-dimensional confinement created by the ultrasmall semiconductor structures known as quantum dots greatly modifies the optical properties of the spatially localized carriers. These systems are presently of great interest to the research community, both for the improved understanding of the physics of confined structures, and for the potential applications of these systems to areas such as optoelectronics and quantum computing. Here, the techniques of transient coherent nonlinear optical spectroscopy are applied to the investigation of excitons confined within InAs/GaAs self-assembled quantum dots. These methods provide a powerful tool for the study of dynamic processes in these novel materials. The nonlinear measurements are based on the differential transmission experimental geometry, and utilize ultrafast pulsed lasers in order to temporally resolve the carrier dynamics after excitation. The experiments performed here are resonant with the ground state absorption of the quantum dots, as evidenced by comparison with the photoluminescence measurements which are used to characterize the sample. The incoherent relaxation dynamics of the population of photoexcited excitons are examined, allowing for a determination of both the lifetime of the excitons and the time scale for relaxation between the two polarization eigenstates of the system. The three-dimensional quantum confinement results in the suppression of these relaxation processes, as predicted. The use of coherent spectroscopic techniques allows for the first unambiguous demonstration of an optically-induced nonradiative Raman coherence in these quantum dots. Simultaneous excitation of both polarization states of the exciton results in a coherent superposition state, whose temporal evolution is observed through the homodyne-detection scheme. In these transient experiments, this is manifested as a beating in the nonlinear response, which allows us to directly measure the fine-structure splitting between the polarization states. Utilizing optical pulse shaping techniques, transient spectral hole burning is performed, which allows for the nonlinear response to be spectrally resolved. As expected for the strongly confined quantum dot excitons, the results show that diffusion among the localized states is not a significant effect. Temperature dependent measurements show that at elevated temperatures, extra dephasing processes, potentially related to acoustic phonon scattering, become important. Finally, this technique allows for the first direct observation of the induced absorption from the exciton to biexciton transition in these InAs quantum dots, and a measurement of the associated binding energy. These results lay the foundation for future studies in this material system, and for the possible development of quantum logic devices utilizing quantum dots.
Over the past 15 years, researchers have extended the multidimensional techniques which originated with NMR in the 1970s to infrared and visible coherent spectroscopy. These advances have dramatically enhanced the temporal resolution from the microsecond to the femtosecond regime. NMR spectroscopists have developed principles for the design of pulse sequences that enhance selected spectral features and reveal desired dynamical events. Extending these principles to the optical regime offers numerous opportunities for narrowing the line shapes in specific directions, unraveling weak cross-peaks from otherwise congested spectra, and controlling the interferences between quantum pathways. We can achieve these enhancements by shaping the spectral and temporal profiles of the pulses. Pulse polarization shaping may lead to unique probes of time-dependent chirality. In this Account, we compare two types of signals. The first, the photon echo, is generated in the direction -k(1) + k(2) + k(3), and the second, double quantum coherence, is detected at +k(1) + k(2) - k(3). Here k(1), k(2), and k(3) are the wave vectors of the three incoming pulses in chronological order. We illustrate the novel information extracted from these signals by simulations of three physical systems. In the first system, spectra of GaAs semiconductor quantum wells provide a direct look at many-body electron correlation effects. We directly observe specific projections of the many-electron wave function, which we can use to test the quality of various levels of computational techniques for electronic structure. Secondly, the spectra of photosynthetic aggregates reveal couplings between chromophores, quantum coherence signatures of chromophore entanglement, and energy-transfer pathways. Using some fundamental symmetries of pulse polarization configurations of nonlinear signals, we can construct superpositions of signals designed to better distinguish among various coherent and incoherent exciton transport pathways and amplify subtle variations among different species of the Fenna-Matthews-Olson (FMO) antenna complex. Both of the first two applications require femtosecond pulses of light in the visible range. The third application demonstrates how resonant core spectroscopy may be used to generate core excitations that are highly localized at selected atoms. Such signals can monitor the motions of valence electron wavepackets in real space with atomic spatial resolution. These future X-ray applications will require attosecond bright X-ray sources, which are currently being developed in several labs. Common principles underlie these techniques in coherent spectroscopy for spins, valence electrons, and core electronic excitations, spanning frequencies from radiowaves to hard X-rays.
Quasiparticles are fundamental in describing the complex many-body interactions underlying single-particle excitations, playing a key role in understanding the macroscopic properties of quantum materials. Recent advancements in ultrafast laser technology, combined with various detection methods, have enabled precise monitoring and manipulation of quantum states and their dynamic processes. These developments not only enhance our comprehension of quasiparticle excitation mechanisms but also facilitate driving materials into non-equilibrium states, uncovering novel physical phenomena and advancing the design and application of innovative functional materials. The computational approach based on real-time time-dependent density functional theory (rt-TDDFT) transcends the limitations of linear response theory, enabling first-principles simulations of the dynamic response of strongly coupled quasiparticles under non-equilibrium conditions. The proposed method provides accurate predictions of highly nonlinear phenomena induced by strong laser fields, offering deeper insights into the underlying physical mechanisms. These theoretical insights are crucial for optimizing the performance of optoelectronic devices. This paper introduces the theoretical foundations of Ehrenfest dynamics within the framework of rt-TDDFT and presents case studies on the evolution of various quasiparticles under laser excitation. The results demonstrate the significant potential of ultrafast lasers for probing and controlling the properties of quantum materials, while also underscoring the vital role of dynamic simulations for studying non-equilibrium states and their time-domain characteristics.