Energy dissipation and decoherence are at first glance harmful to acquiring long exciton lifetime desired for efficient photovoltaics. In the presence of both optically forbidden (namely, dark) and allowed (bright) excitons, however, they can be instrumental as suggested in photosynthesis. By simulating quantum dynamics of exciton relaxations, we show that the optimized decoherence that imposes a quantum-to-classical crossover with the dissipation realizes a dramatically longer lifetime. In an example of carbon nanotube, the exciton lifetime increases by nearly two orders of magnitude when the crossover triggers stable high population in the dark exciton.
This paper discusses the combined effects of optical excitation power, interface roughness, lattice temperature, and applied magnetic fields on the spin-coherence of excitonic states in GaAs/AlGaAs multiple quantum wells. For low optical powers, at lattice temperatures between 4 K and 50 K, the scattering with acoustic phonons and short-range interactions appear as the main decoherence mechanisms. Statistical fluctuations of the band-gap however become also relevant in this regime and we were able to deconvolute them from the decoherence contributions. The circularly polarized magneto-photolum…
Excitons in a semiconductor monolayer form a collective resonance that can reflect resonant light with extraordinarily high efficiency. Here, we investigate the nonlinear optical properties of such atomistically thin mirrors and show that finite-range interactions between excitons can lead to the generation of highly non-classical light. We describe two scenarios, in which optical nonlinearities arise either from direct photon coupling to excitons in excited Rydberg states or from resonant two-photon excitation of Rydberg excitons with finite-range interactions. The latter case yields conditio…
We study the dark exciton's behavior as a coherent physical two-level spin system (qubit) using an external magnetic field in the Faraday configuration. Our studies are based on polarization-sensitive intensity autocorrelation measurements of the optical transition resulting from the recombination of a spin-blockaded biexciton state, which heralds the dark exciton and its spin state. We demonstrate control over the dark exciton eigenstates without degrading its decoherence time. Our observations agree well with computational predictions based on a master equation model.
Monolayer transition metal dichalcogenides feature Coulomb-bound electron-hole pairs (excitons) with exceptionally large binding energy and coupled spin and valley degrees of freedom. These unique attributes have been leveraged for electrical and optical control of excitons for atomically-thin optoelectronics and valleytronics. The development of such technologies relies on understanding and quantifying the fundamental properties of the exciton. A key parameter is the intrinsic exciton homogeneous linewidth, which reflects irreversible quantum dissipation arising from system (exciton) and bath…
The quantum state of the emitted light from the cascade recombination of a biexciton in a quantum dot is theoretically investigated including exciton fine structure splitting (FSS) and electron-nuclear spin hyperfine interactions. In an ideal situation, the emitted photons are entangled in polarization making the biexciton recombination process a candidate source of entangled photons necessary for the growing field of quantum communication and computation. The coherence of the exciton states in real quantum dots is affected by a finite FSS and the hyperfine interactions via the effective magne…
We present a semi-analytic and asymptotically exact solution to the problem of phonon-induced decoherence in a quantum dot-microcavity system. Particular emphasis is placed on the linear polarization and optical absorption, but the approach presented herein may be straightforwardly adapted to address any elements of the exciton-cavity density matrix. At its core, the approach combines Trotter's decomposition theorem with the linked cluster expansion. The effects of the exciton-cavity and exciton-phonon couplings are taken into account on equal footing, thereby providing access to regimes of co…
Phonon interactions in solid-state photonics systems cause intrinsic quantum decoherence and often present the limiting factor in emerging quantum technology. Due to recent developments in nanophotonics, exciton-cavity structures with very strong light-matter coupling rates can be fabricated. We show that in such structures, a new regime emerges, where the decoherence is completely suppressed due to decoupling of the dominant phonon process. Using a numerically exact tensor network approach, we perform calculations in this non-perturbative, non-Markovian dynamical regime. Here, we identify a s…
We report on the experimental evidence for a nanosecond time-scale spin memory based on nonradiative excitons. The effect manifests itself in magnetic-field-induced oscillations of the energy of the optically active (radiative) excitons. The oscillations detected by a spectrally-resolved pump-probe technique applied to a GaAs/AlGaAs quantum well structure in a transverse magnetic field persist over a time scale, which is orders of magnitude longer than the characteristic decoherence time in the system. The effect is attributed to the spin-dependent electron-electron exchange interaction of the…
A first principles, excited state analysis is carried out to identify ways of producing silicon quantum dots with low excitonic reorganization energy. These focus on the general strategy of either reducing or constraining exciton-phonon coupling, and four approaches are explored. The results can be implemented in quantum dot solids to mitigate polaronic effects and increase the lifetime of coherent excitonic superpositions. It is demonstrated that such designs can also be used to alter the shape of the spectral density for reorganization so as to reduce the rates of both decoherence and dissip…
While valleys (energy extrema) are present in all band structures of solids, their preeminent role in determining exciton resonances and dynamics in atomically thin transition metal dichalcogenides (TMDC) is unique. Using two-dimensional coherent electronic spectroscopy, we find that exciton decoherence occurs on a much faster time scale in MoSe$_2$ bilayers than that in the monolayers. We further identify two population relaxation channels in the bilayer, a coherent and an incoherent one. Our microscopic model reveals that phonon-emission processes facilitate scattering events from the $K$ va…
Optimized light-matter coupling in semiconductor nanostructures is a key to understand their optical properties and can be enabled by advanced fabrication techniques. Using in-situ electron beam lithography combined with a low-temperature cathodoluminescence imaging, we deterministically fabricate microlenses above selected InAs quantum dots (QDs) achieving their efficient coupling to the external light field. This enables to perform four-wave mixing micro-spectroscopy of single QD excitons, revealing the exciton population and coherence dynamics. We infer the temperature dependence of the dep…
The entanglement of an optically generated electron-hole pair in artificial quantum dot molecules is calculated considering the effects of decoherence by interaction with environment. Since the system evolves into a mixed states and due to the complexity of energy level structure, we use the negativity as entanglement quantifier, which is well defined in $d \otimes d^\prime$ composite vector spaces. By a numerical analysis of the non-unitary dynamics of the exciton states, we establish the feasibility of producing protected entangled superpositions by an appropriate tuning of bias electric fie…
Multi-phonon physics is an emerging field that serves as a test bed for fundamental quantum physics and several applications in metrology, on-chip communication, among others. Quantum acoustic cavities or resonators are devices that are being used to study multi-phonon phenomena both theoretically and experimentally. In particular, we study a system consisting of a semiconductor quantum dot pumped by a driving laser, and coupled to an acoustic cavity. This kind of systems has proven to yield interesting multi-phonon phenomena, but the description of the quantum dot has been limited to a two-le…
We demonstrate full suppression of dephasing tied to deformation potential coupling of confined electrons to longitunidal acoustic (LA) phonons in optical control experiments on large semiconductor quantum dots (QDs) with emission compatible with the low-dispersion telecommunications band at 1.3~$μ$m. By exploiting the sensitivity of the electron-phonon spectral density to the size and shape of the QD, we demonstrate a four-fold reduction in the threshold pulse area required to enter the decoupled regime for exciton inversion using adiabatic rapid passage (ARP). Our calculations of the quantum…
Cavity-polaritons in semiconductor microstructures have emerged as a promising system for exploring nonequilibrium dynamics of many-body systems. Key advances in this field, including the observation of polariton condensation, superfluidity, realization of topological photonic bands, and dissipative phase transitions, generically allow for a description based on a mean-field Gross-Pitaevskii formalism. While observation of polariton intensity squeezing and decoherence of a polarization entangled photon pair by a polariton condensate provide counter-examples, quantum effects in these experiment…
In semiconductor quantum dots, the electron hyperfine interaction with the nuclear spin bath is the leading source of spin decoherence at cryogenic temperature. Using high-resolution two-color differential transmission spectroscopy, we demonstrate that such electron-nuclear coupling also imposes a lower limit for the positively charged exciton dephasing rate, γ, in an ensemble of InAs/GaAs quantum dots. We find that the dephasing rate is sensitive to the strength of the hyperfine interaction, which can be controlled through the application of an external magnetic field in the Faraday configura…
We study a pair of quantum dot exciton qubits interacting with a number of fluctuating charges that can induce a Stark shift of both exciton transition energies. We do this by solving the optical master equation using a numerical transfer matrix method. We find that the collective influence of the charge environment on the dots can be detected by measuring the correlation between the photons emitted when each dot is driven independently. Qubits in a common charge environment display photon bunching, if both dots are driven on resonance or if the driving laser detunings have the same sense for …
Electric dipole radiation can be controlled by coherent optical feedback, as has previously been studied by modulating the photonic environment for point dipoles placed both in optical cavities and near metal mirrors. In experiments involving fluorescent molecules, trapped ions and quantum dots the point nature of the dipole, its sub-unity quantum efficiency, and decoherence rate conspire to severely limit any change in total linewidth. Here we show that the transverse coherence of exciton emission in the monolayer two-dimensional (2D) material MoSe${}_2$ removes many of the fundamental physic…
Assessing the classicality of photon echo from excitons in lead halide perovskite nanocrystals
Technische Universität Dortmund（多特蒙德工业大学）；Paderborn University（帕德博恩大学）；St. Petersburg State University（圣彼得堡国立大学）；ITMO University（ITMO大学）；St. Petersburg State Institute of Technology（圣彼得堡国立技术学院）
A semiconductor quantum dot (QD) embedded within an optical microcavity is a system of fundamental importance within quantum information processing. The optimization of quantum coherence is crucial in such applications, requiring an in-depth understanding of the relevant decoherence mechanisms. We provide herein a critical review of prevalent theoretical treatments of the QD-cavity system coupled to longitudinal acoustic phonons, comparing predictions against a recently obtained exact solution. Within this review we consider a range of temperatures and exciton-cavity coupling strengths. Predic…
We propose a scheme to induce weak-light nonlinearity in a double quantum dot. The scheme positively utilizes locality and dissipation of an external auxiliary system. As a plausible setup, we consider a complex system in which a localized plasmon field from a metallic nanotip couples with only one of the coupled quantum dots. The perturbative calculation with respect to the light intensity shows that, even by a sufficiently weak light, a dipole-forbidden two-exciton NOON state is prepared as the steady state. This result can be explained by combining the two factors: decoherence-induced quant…
