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With the realization of controlled quantum systems, exploring excitations beyond the resonant case opens new possibilities. We investigate an extended Jaynes-Cummings model where two photon modes are coupled off-resonantly to a quantum emitter. This allows us to identify few-photon scattering mechanisms that lead to a full inversion of the emitter while transferring off-resonant photons from one mode to another. This behaviour connects to recent measurements of a two-level emitter scattering two off-resonant photons simultaneously. Furthermore, our results can be understood as quantized analogue of the recently developed off-resonant quantum control scheme known as Swing-UP of quantum EmitteR (SUPER). Our intuitive formalism gives a deeper insight into the interaction of a two-level emitter with off-resonant light modes with the prospect of novel photonic applications., Comment: 9 pages, 7 figures (main and appendix)

Entangled photon pairs form the foundation for many applications in the realm of quantum communication. For fiber-optic transfer of entangled photon pairs, time-bin encoding can potentially offer an improved stability compared to polarization encoded qubits. Here, we lay the theoretical foundations to describe the measurement of time-bin entangled photons. We derive multi-time correlation functions of the time-bin encoded photon pairs, corresponding to quantum state tomographic measurements. Our theory can be the starting point to extend the simulations to include all kinds of loss or decoherence effects that apply in a specific quantum system for realistic simulation for time-bin entanglement from quantum emitters., Comment: 8 pages, 3 figures

If a two-level system coupled to a single-mode cavity is strongly driven by an external laser, instead of a continuous accumulation of photons in the cavity, oscillations in the mean photon number occur. These oscillations correspond to peaks of finite width running up and down in the photon number distribution, reminiscent of wave packets in linear chain models. A single wave packet is found if the cavity is resonant to the external laser. Here, we show that for finite detuning multiple packet structures can exist simultaneously, oscillating at different frequencies and amplitudes. We further study the influence of dissipative effects resulting in the formation of a stationary state, which depending on the parameters can be characterized by a bimodal photon number distribution. While we give analytical limits for the maximally achievable photon number in the absence of any dissipation, surprisingly, dephasing processes can push the photon occupations towards higher photon numbers., Comment: 11 pages, 7 figures

Entangled photon pairs are essential for quantum communication technology. They can be generated on-demand by semiconductor quantum dots, but several mechanisms are known to reduce the degree of entanglement. While some obstacles like the finite fine-structure splitting can be overcome by now, the excitation scheme itself can impair the entanglement fidelity. Here, we demonstrate that the swing-up of quantum emitter population (SUPER) scheme applied to a quantum dot in a cavity yields almost perfectly entangled photons. The entanglement degree remains robust against phonon influences even at elevated temperatures, due to decoupling of the excitation and emission process. With this achievement, quantum dots are ready to be used as entangled photon pair sources in applications requiring high degrees of entanglement up to temperatures of about $80\,$K., Comment: 4 pages, 4 figures + appendix

Quantum communication networks rely on quantum cryptographic protocols including quantum key distribution (QKD) using single photons. A critical element regarding the security of QKD protocols is the photon number coherence (PNC), i.e. the phase relation between the zero and one-photon Fock state, which critically depends on the excitation scheme. Thus, to obtain flying qubits with the desired properties, optimal pumping schemes for quantum emitters need to be selected. Semiconductor quantum dots generate on-demand single photons with high purity and indistinguishability. Exploiting two-photon excitation of a quantum dot combined with a stimulation pulse, we demonstrate the generation of high-quality single photons with a controllable degree of PNC. Our approach provides a viable route toward secure communication in quantum networks., Comment: 17 pages

Semiconductor quantum dots have emerged as an especially promising platform for the generation of polarization-entangled photon pairs. However, it was demonstrated recently that the two-photon excitation scheme employed in state-of-the-art experiments limits the achievable degree of entanglement by introducing which-path information. In this work, the combined impact of two-photon excitation and longitudinal acoustic phonons on photon pairs emitted by strongly-confining quantum dots is investigated. It is found that phonons further reduce the achievable degree of entanglement even in the limit of vanishing temperature due to phonon-induced pure dephasing and phonon-assisted one-photon processes, which increase the reexcitation probability. In addition, the degree of entanglement, as measured by the concurrence, decreases with rising temperature and/or pulse duration, even if the excitonic fine-structure splitting is absent and when higher electronic states are out of reach. Furthermore, in the case of finite fine-structure splittings, phonons enlarge the discrepancy in concurrence for different laser polarizations., Comment: 10 pages, 3 figures

Entangled photon pairs are essential for a multitude of photonic quantum applications. To date, the best performing solid-state quantum emitters of entangled photons are semiconductor quantum dots operated around liquid-helium temperatures. To favor the widespread deployment of these sources, it is important to explore and understand their behavior at temperatures accessible with compact Stirling coolers. Here we study the polarization entanglement among photon pairs from the biexciton-exciton cascade in GaAs quantum dots at temperatures up to 65 K. We observe entanglement degradation accompanied by changes in decay dynamics, which we ascribe to thermal population and depopulation of hot and dark states in addition to the four levels relevant for photon pair generation. Detailed calculations considering the presence and characteristics of the additional states and phonon-assisted transitions support the interpretation. We expect these results to guide the optimization of quantum dots as sources of highly entangled photons at elevated temperatures., Comment: 12 pages, 3 figures, supplemental material

To coherently control a few-level quantum emitter, typically pulses with an energy resonant to the transition energy are applied making use of the Rabi mechanism, while a single off-resonant pulse does not result in a population inversion. Surprisingly, a two-color excitation with a combination of two off-resonant pulses making use of the Swing-UP of quantum EmitteR population (SUPER) mechanism is able to invert the system. In this paper, we provide an in-depth analysis of the SUPER scheme within the dressed-state picture. We show that the SUPER mechanism can be understood as a driving of the transition between the dressed states. In the two-level system this allows us to derive analytic expressions for the pulse parameters yielding a population inversion. We extend our considerations to the three-level system, where a strong mixing between the bare states takes place. The insights gained from these results help in finding accessible regimes for further experimental realizations of the SUPER scheme and similar two-color excitation schemes., Comment: 12 pages, 8 figures

For a scalable photonic device producing entangled photons, it is desirable to have multiple quantum emitters in an ensemble that can be collectively excited, despite their spectral variability. For quantum dots, Rabi rotation, the most popular method for resonant excitation, cannot assure a universal, highly efficient excited state preparation, because of its sensitivity to the excitation parameters. In contrast, Adiabatic Rapid Passage (ARP), relying on chirped optical pulses, is immune to quantum dot spectral inhomogeneity. Here, we advocate the robustness of ARP for simultaneous excitation of the biexciton states of multiple quantum dots. For positive chirps, we find that there is also regime of phonon advantage that widens the tolerance range of spectral detunings. Using the same laser pulse we demonstrate the simultaneous excitation of energetically and spatially distinct quantum dots. Being able to generate spatially multiplexed entangled photon pairs is a big step towards the scalability of photonic devices.

Entangled photon pairs are essential for many applications in quantum technologies. Recent theoretical studies demonstrated that different types of entangled Bell states can be created in a constantly driven four-level quantum emitter-cavity system. Unlike other candidates for the realization of the four-level emitter, semiconductor quantum dots unavoidably interact with their environment, resulting in carrier-phonon interactions. Surprisingly, phonons change the entanglement of emitted photon pairs in a qualitative way, already at low temperatures on the order of 4 K. While one type of Bell state can still be generated using small driving strengths, the other type is suppressed due to phonon interactions in strongly-confined quantum dots. The degree of entanglement decreases with rising temperature and driving strength until it vanishes at a certain parameter value. Because it remains zero afterward, we encounter a phonon-induced transition between entangled and nonentangled photon emission that resembles a phase transition. The transition occurs at temperatures below 30 K and, independent of the driving strength, the concurrence as a function of the reduced temperature is found to obey a power law with exponent one near the transition point., Comment: 15 pages, 7 figures

Entangled photon pairs are key to many novel applications in quantum technologies. Semiconductor quantum dots can be used as sources of on-demand, highly entangled photons. The fidelity to a fixed maximally entangled state is limited by the excitonic fine-structure splitting. This work demonstrates that, even if this splitting is absent, the degree of entanglement cannot reach unity when the excitation pulse in a two-photon resonance scheme has a finite duration. The degradation of the entanglement has its origin in a dynamically induced splitting of the exciton states caused by the laser pulse itself. Hence, in the setting explored here, the excitation process limits the achievable concurrence for entangled photons generated in an optically excited four-level quantum emitter., Comment: 7 pages, 3 figures, supplemental material

Quantum cryptography harnesses quantum light, in particular single photons, to provide security guarantees that cannot be reached by classical means. For each cryptographic task, the security feature of interest is directly related to the photons' non-classical properties. Quantum dot-based single-photon sources are remarkable candidates, as they can in principle emit deterministically, with high brightness and low multiphoton contribution. Here, we show that these sources provide additional security benefits, thanks to the tunability of coherence in the emitted photon-number states. We identify the optimal optical pumping scheme for the main quantum-cryptographic primitives, and benchmark their performance with respect to Poisson-distributed sources such as attenuated laser states and down-conversion sources. In particular, we elaborate on the advantage of using phonon-assisted and two-photon excitation rather than resonant excitation for quantum key distribution and other primitives. The presented results will guide future developments in solid-state and quantum information science for photon sources that are tailored to quantum communication tasks.

The quest for the perfect single-photon source includes finding the optimal protocol for exciting the quantum emitter. Based on a recently proposed, so-called SUPER (swing-up of quantum emitter population) scheme, we demonstrate experimentally that two red-detuned laser pulses, neither of which could yield a significant upper-level population individually, lead to the coherent excitation of a semiconductor quantum dot. We characterize the emitted single photons and show that they have properties comparable to those achieved under resonant excitation schemes., Comment: 11 pages, 9 figures

When a detuned and strong laser pulse acts on an optical transition, a Stark shift of the corresponding energies occurs. We analyze how this optical Stark effect can be used to prepare and control the dark exciton occupation in a semiconductor quantum dot. The coupling between the bright and dark exciton states is facilitated by an external magnetic field. Using sequences of laser pulses, we show how the dark exciton and different superposition states can be prepared. We give simple analytic formulas, which yield a good estimate for optimal preparation parameters. The preparation scheme is quite robust against the influence of acoustic phonons. We further discuss the experimental feasibility of the used Stark pulses. Giving a clear physical picture our results will stimulate the usage of dark excitons in schemes to generate photons from quantum dots., Comment: 10 pages, 6 figures

The cascaded decay in a four-level quantum emitter is a well established mechanism to generate polarization entangled photon pairs, the building blocks of many applications in quantum technologies. The four most prominent maximally entangled photon pair states are the Bell states. In a typical experiment based on an undriven emitter only one type of Bell state entanglement can be observed in a given polarization basis. Other types of Bell state entanglement in the same basis can be created by continuously driving the system by an external laser. In this work we propose a protocol for time-dependent entanglement switching in a four-level quantum emitter--cavity system that can be operated by changing the external driving strength. By selecting different two-photon resonances between the laser-dressed states, we can actively switch back and forth between the different types of Bell state entanglement in the same basis as well as between entangled and nonentangled photon pairs. This remarkable feature demonstrates the possibility to achieve a controlled, time-dependent manipulation of the entanglement type that could be used in many innovative applications., Comment: 6 pages, 3 figures. The following article has been accepted by Applied Physics Letters. After it is published, it will be found at https://aip.scitation.org/journal/apl

Using a density-functional-theory-based approach, we explore the symmetrization and proton dynamics in ice-VII, for which recent high-pressure NMR experiments indicate significant proton dynamics in the pressure-range of $20-95$ GPa. We directly sample the potential seen by the proton and find a continuous transition from double- to single-well character over the pressure range of 2 to 130 GPa accompanied by proton dynamics in agreement with the NMR experiments., Comment: 7 pages, 6 figures

The central challenge for describing the dynamics in open quantum systems is that the Hilbert space of typical environments is too large to be treated exactly. In some cases, such as when the environment has a short memory time or only interacts weakly with the system, approximate descriptions of the system are possible. Beyond these, numerically exact methods exist, but these are typically restricted to baths with Gaussian correlations, such as non-interacting bosons. Here we present a numerically exact method for simulating open quantum systems with arbitrary environments which consist of a set of independent degrees of freedom. Our approach automatically reduces the large number of environmental degrees of freedom to those which are most relevant. Specifically, we show how the process tensor -- which describes the effect of the environment -- can be iteratively constructed and compressed using matrix product state techniques. We demonstrate the power of this method by applying it to problems with bosonic, fermionic, and spin environments: electron transport, phonon effects and radiative decay in quantum dots, central spin dynamics, anharmonic environments, dispersive coupling to time-dependent lossy cavity modes, and superradiance. The versatility and efficiency of our automated compression of environments (ACE) method provides a practical general-purpose tool for open quantum systems.

Bell states are the most prominent maximally entangled photon states. In a typical four-level emitter, like a semiconductor quantum dot, the photon states exhibit only one type of Bell state entanglement. By adding an external driving to the emitter system, also other types of Bell state entanglement are reachable without changing the polarization basis. In this paper, we show under which conditions the different types of entanglement occur and give analytical equations to explain these findings. We further identify special points, where the concurrence, being a measure for the degree of entanglement, drops to zero, while the coherences between the two-photon states stay strong. Results of this work pave the way to achieve a controlled manipulation of the entanglement type in practical devices., Comment: 14 pages, 7 figures

We explore the impact of a Rashba-type spin-orbit interaction in the conduction band on the spin dynamics of hot excitons in diluted magnetic semiconductor quantum wells. In materials with strong spin-orbit coupling, we identify parameter regimes where spin-orbit effects greatly accelerate the spin decay and even change the dynamics qualitatively in the form of damped oscillations. Furthermore, we show that the application of a small external magnetic field can be used to either mitigate the influence of spin-orbit coupling or entirely remove its effects for fields above a material-dependent threshold., Comment: 9 pages, 5 figures

We theoretically investigate the impact of excited states on the dynamics of the exciton ground state in diluted magnetic semiconductor quantum wells. Exploiting the giant Zeeman shift in these materials, an external magnetic field is used to bring transitions between the exciton ground state and excited states close to resonance. It turns out that, when treating the exciton dynamics in terms of a quantum kinetic theory beyond the Markov approximation, higher exciton states are populated already well below the critical magnetic field required to bring the exciton ground state in resonance to an excited state. This behavior is explained by exciton-impurity correlations that can bridge energy differences on the order of a few meV and require a quantum kinetic description beyond the independent-particle picture. Of particular interest is the significant spin transfer toward states on the optically dark $2p$ exciton parabola which are protected against radiative decay., Comment: 8 pages, 3 figures

We demonstrate theoretically that the single-photon purity of photons emitted from a quantum dot exciton prepared by phonon-assisted off-resonant excitation can be significantly higher in a wide range of parameters than that obtained by resonant preparation for otherwise identical conditions. Despite the off-resonant excitation the brightness stays on a high level. These surprising findings exploit that the phonon-assisted preparation is a two-step process where phonons first lead to a relaxation between laser-dressed states while high exciton occupations are reached only with a delay to the laser pulse maximum by adiabatically undressing the dot states. Due to this delay, possible subsequent processes, in particular multi-photon excitations, appear at a time when the laser pulse is almost gone. The resulting suppression of reexcitation processes increases the single-photon purity. Due to the spectral separation of the signal photons from the laser frequencies this enables the emission of high quality single photons not disturbed by a laser background while taking advantage of the robustness of the phonon assisted scheme.

We investigate the origin of overshoots in the exciton spin dynamics after resonant optical excitation. As a material system, we focus on diluted magnetic semiconductor quantum wells as they provide a strong spin-flip scattering for the carriers. Our study shows that overshoots can appear as a consequence of radiative decay even on the single-particle level in a theory without any memory. The magnitude of the overshoots in this case depends strongly on the temperature as well as the doping fraction of the material. If many-body effects beyond the single-particle level become important so that a quantum-kinetic description is required, a spin overshoot appears already without radiative decay and is much more robust against variations of system parameters. We show that the origin of the spin overshoot can be determined either via its temperature dependence or via its behavior for different doping fractions. The results can be expected to apply to a wide range of semiconductors as long as radiative decay and a spin-flip mechanism are present., Comment: 9 pages, 6 figures

We report on simulations of the degree of polarization entanglement of photon pairs simultaneously emitted from a quantum dot-cavity system that demand revisiting the role of phonons. Since coherence is a fundamental precondition for entanglement and phonons are known to be a major source of decoherence, it seems unavoidable that phonons can only degrade entanglement. In contrast, we demonstrate that phonons can cause a degree of entanglement that even surpasses the corresponding value for the phonon-free case. In particular, we consider the situation of comparatively small biexciton binding energies and either finite exciton or cavity mode splitting. In both cases, combinations of the splitting and the dot-cavity coupling strength are found where the entanglement exhibits a nonmonotonic temperature dependence which enables entanglement above the phonon-free level in a finite parameter range. This unusual behavior can be explained by phonon-induced renormalizations of the dot-cavity coupling $g$ in combination with a nonmonotonic dependence of the entanglement on $g$ that is present already without phonons., Comment: 5 pages, 2 figures, supplemental material

We investigate the degree of entanglement quantified by the concurrence of photon pairs that are simultaneously emitted in the biexciton-exciton cascade from a quantum dot in a cavity. Four dot-cavity configurations are compared that differ with respect to the detuning between the cavity modes and the quantum dot transitions, corresponding to different relative weights of direct two-photon and sequential single-photon processes. The dependence of the entanglement on the exciton fine-structure splitting $\delta$ is found to be significantly different for each of the four configurations. For a finite splitting and low temperatures, the highest entanglement is found when the cavity modes are in resonance with the two-photon transition between the biexciton and the ground state and, in addition, the biexciton has a finite binding energy of a few meV. However, this widely used configuration is rather strongly affected by phonons such that other dot-cavity configurations, that are commonly regarded as less suited for obtaining high degrees of entanglement, become more favorable already at temperatures on the order of 10 K and above. If the cavity modes are kept in resonance with one of the exciton-to-ground-state transitions and the biexciton binding energy is finite, the entanglement drastically drops for positive $\delta$ with rising temperatures when $T$ is below $\simeq$ 4 K, but is virtually independent of the temperature for higher $T$., Comment: 14 pages, 6 figures

Magnetically doped semiconductors are well known for their giant Zeeman splittings which can reach several meV even in relatively small external magnetic fields. After preparing a nonequilibrium exciton distribution via optical excitation, the spin dynamics in diluted magnetic semiconductor quantum wells is typically governed by spin-flip scattering processes due to the exciton-impurity exchange interaction. Our theoretical calculations show that the giant Zeeman splitting in these materials in combination with the influence of longitudinal acoustic phonons lead to a quantum ratchet-type dynamics, resulting in an almost complete reversal of the carrier spin polarization at very low temperatures. Furthermore, we find that the predictions of a much simpler rate-equation approach qualitatively agree with a more advanced and numerically demanding quantum kinetic description of the spin dynamics for a wide range of temperatures, although quantitative difference are noticeable., Comment: 8 pages, 5 figures

Phonons are well known to be the main mechanism for the coupling between bright and dark excitons in nonmagnetic semiconductors. Here, we investigate diluted magnetic semiconductors where this process is in direct competition with the scattering at localized magnetic impurities. To this end, a recently developed quantum kinetic description of the exciton spin dynamics in diluted magnetic semiconductor quantum wells is extended by the scattering with longitudinal acoustic phonons. A strong phonon impact is found in the redistribution of exciton momenta on the exciton parabola that becomes especially prominent for high temperatures and exciton distributions further away from the exciton resonance which are optically dark. Despite their impact on the energetic redistribution, acoustic phonons virtually do not affected the exciton spin dynamics as the exciton-impurity interaction always dominates. Furthermore, it turns out that the exciton spin lifetime increases by roughly one order of magnitude for nonequilibrium hot exciton distributions and, in addition, pronounced quantum kinetic signatures in the exciton spin dynamics appearing after resonant optical excitation are drastically reduced., Comment: 13 pages, 6 figures

Diluted magnetic semiconductors are materials well known to exhibit strong correlations which typically manifest in carrier-mediated magnetic ordering. In this Rapid Communication, we show that the interaction between excitons and magnetic impurities in these materials is even strong enough to cause a significant deviation from the bare exciton picture in linear absorption spectra of quantum well nanostructures. It is found that exciton-impurity correlations induce a characteristic fingerprint in the form of an additional feature close to the exciton resonance in combination with a shift of the main exciton line of up to a few meV. We trace back these features to the form of the self-energy and demonstrate that reliable values of the average correlation energy per exciton can be extracted directly from the spectra. Since the only requirement for our findings is sufficiently strong correlations, the results can be generalized to other strongly correlated systems., Comment: 4 figures, supplemental material

Using a real-time path integral approach we develop an algorithm to calculate multi-time correlation functions of open few-level quantum systems that is applicable to highly nonequilibrium dynamics. The calculational scheme fully keeps the non-Markovian memory introduced by the pure-dephasing type coupling to a continuum of oscillators. Furthermore, we discuss how to deal consistently with the simultaneous presence of non-Markovian and Markovian system reservoir interactions. We apply the method to a crucial test case, namely the evaluation of emission spectra of a laser-driven two-level quantum dot coupled to a continuum of longitudinal acoustic phonons, which give rise to non-Markovian dynamics. Here, we also account for the coupling to a photonic environment, which models radiative decay and can be treated as a Markovian bath. The phonon side bands are found on the correct side of the zero phonon line in our calculation, in contrast to known results where the quantum regression theorem is applied naively to non-Markovian dynamics. Combining our algorithm with a recently improved iteration scheme for performing the required sum over paths we demonstrate the numerical feasibility of our approach to systems with more than two levels. Results are shown for the second-order photonic two-time correlation function of a quantum dot-cavity system with seven states on the Jaynes-Cummings ladder taken into account., Comment: 11 pages, 2 figures

We compare three different notions of concurrence to measure the polarization entanglement of two-photon states generated by the biexciton cascade in a quantum dot embedded in a microcavity. We focus on the often-discussed situation of a dot with finite biexciton binding energy in a cavity tuned to the two-photon resonance. Apart from the time-dependent concurrence, which can be assigned to the two-photon density matrix at any point in time, we study single- and double-time integrated concurrences commonly used in the literature that are based on different quantum state reconstruction schemes. We argue that the single-time integrated concurrence can be thought of as the concurrence of photons simultaneously emitted from the cavity without resolving the common emission time, while the more widely studied double-time integrated concurrence refers to photons that are neither filtered with respect to the emission time of the first photon nor with respect to the delay time between the two emitted photons. Analytic and numerical calculations reveal that the single-time integrated concurrence indeed agrees well with the typical value of the time-dependent concurrence at long times, even in the presence of phonons. Thus, the more easily measurable single-time integrated concurrence gives access to the physical information represented by the time-dependent concurrence. However, the double-time integrated concurrence shows a different behavior with respect to changes in the exciton fine structure splitting and even displays a completely different trend when the ratio between the cavity loss rate and the fine structure splitting is varied while keeping their product constant. This implies the non-equivalence of the physical information contained in the time-dependent and single-time integrated concurrence on the one hand and the double-time integrated concurrence on the other hand., Comment: 18 pages, 10 figures

We investigate theoretically the influence of an external magnetic field on the spin dynamics of excitons in diluted magnetic semiconductor quantum wells. To this end, we apply a quantum kinetic theory beyond the Markov approximation which reveals that non-Markovian effects can significantly influence the exciton spin dynamics. If the magnetic field is oriented parallel to the growth direction of the well, the Markovian spin-transfer rate decreases monotonically with increasing field as predicted by Fermi's golden rule. The quantum kinetic theory follows this result qualitatively but predicts pronounced quantitative differences in the spin-transfer rate as well as in the long-time spin polarization. However, for an in-plane magnetic field, where the Markovian spin-transfer rate first drops and then increases again, quantum kinetic effects become so pronounced that the Markovian trend is completely reversed. This is made evident by a distinct maximum of the rate followed by a monotonic decrease. The deviations can be traced back to a redistribution of carriers in energy space caused by correlations between excitons and magnetic dopants. The same effect leads to a finite electron-spin polarization at long times in longitudinal as well as transverse fields which is much larger than the corresponding Markovian prediction., Comment: 17 pages, 7 figures

The generation of photons in a microcavity coupled to a laser-driven quantum dot interacting with longitudinal acoustic (LA) phonons is studied in the regime of simultaneously strong driving and strong dot-cavity coupling. The stationary cavity photon number is found to depend in a non-trivial way on the detuning between the laser and the exciton transition in the dot. In particular, the maximal efficiency of the cavity feeding is obtained for detunings corresponding to transition energies between cavity-dressed states with excitation numbers larger than one. Phonons significantly enhance the cavity feeding at large detunings. In the strong-driving, strong-coupling limit, the photon statistics is highly non-Poissonian. While without phonons a double-peaked structure in the photon distribution is predicted, phonons make the photon statistics thermal-like with very high effective temperatures $\sim 10^5$ K, even for low phonon temperatures $\sim 4$ K. These results were obtained by numerical calculations where the driving, the dot-cavity coupling and the dot-phonon interactions are taken into account without approximations. This is achieved by a reformulation of an exact iterative path-integral scheme which is applicable for a large class of quantum-dissipative systems and which in our case reduces the numerical demands by 15 orders of magnitude., Comment: 6 pages, 3 figures

Quantum kinetic equations of motion for the description of the exciton spin dynamics in II-VI diluted magnetic semiconductor quantum wells with laser driving are derived. The model includes the magnetic as well as the nonmagnetic carrier-impurity interaction, the Coulomb interaction, Zeeman terms, and the light-matter coupling, allowing for an explicit treatment of arbitrary excitation pulses. Based on a dynamics-controlled truncation scheme, contributions to the equations of motion up to second order in the generating laser field are taken into account. The correlations between the carrier and the impurity subsystems are treated within the framework of a correlation expansion. For vanishing magnetic field, the Markov limit of the quantum kinetic equations formulated in the exciton basis agrees with existing theories based on Fermi's golden rule. For narrow quantum wells excited at the $1s$ exciton resonance, numerical quantum kinetic simulations reveal pronounced deviations from the Markovian behavior. In particular, the spin decays initially with approximately half the Markovian rate and a non-monotonic decay in the form of an overshoot of up to $10\,\%$ of the initial spin polarization is predicted., Comment: 17 pages, 3 figures, typographical errors corrected (Erratum published in Phys. Rev. B 96, 239904)

The electron spin dynamics in an optically excited narrow quantum well is studied, where the electron spins precess in a k-dependent magnetic field while the electrons scatter at localized impurities. For the resulting spin decay, which is commonly known as the D'yakonov-Perel' mechansim, analytical expressions in the strong- and weak-scattering limits are available. It is found by the numerical solution of quantum kinetic equations in a broad range of parameters that, in situations that are typically relevant for ultrafast optical experiments, the dynamics of the total spin polarization significantly deviates from the pertinent analytical results. This is attributed to the broad spectral width of the optically excited spin-polarized electron distribution, which gives rise to a spin dephasing due to inhomogeneous broadening. Furthermore, it is found that the decay of the spin polarization need not be exponential. The notion of a spin decay time becomes ambiguous and different definitions of spin decay times can lead to different outcomes. The long-term dynamics of the decay of the spin polarization is even dominated by an algebraically decaying component. These findings highlight the importance of the effects of the broad spectral distribution of optically excited carriers in ultrashort magneto-optical experiments., Comment: 13 pages, 6 figures

The doping of semiconductors with magnetic impurities gives rise not only to a spin-spin interaction between quasi-free carriers and magnetic impurities, but also to a local spin-independent disorder potential for the carriers. Based on a quantum kinetic theory for the carrier and impurity density matrices as well as the magnetic and non-magnetic carrier-impurity correlations, the influence of the non-magnetic scattering potential on the spin dynamics in DMS after optical excitation with circularly polarized light is investigated using the example of Mn-doped CdTe. It is shown that non-Markovian effects, which are predicted in calculations where only the magnetic carrier-impurity interaction is accounted for, can be strongly suppressed in the presence of non-magnetic impurity scattering. This effect can be traced back to a significant redistribution of carriers in $\mathbf{k}$-space which is enabled by the build-up of large carrier-impurity correlation energies. A comparison with the Markov limit of the quantum kinetic theory shows that, in the presence of an external magnetic field parallel to the initial carrier polarization, the asymptotic value of the spin polarization at long times is significantly different in the quantum kinetic and the Markovian calculations. This effect can also be attributed to the formation of strong correlations which invalidates the semiclassical Markovian picture and it is stronger when the non-magnetic carrier-impurity interaction is accounted for. In an external magnetic field perpendicular to the initial carrier spin, the correlations are also responsible for a renormalization of the carrier spin precession frequency.

Quantum kinetic equations of motion for carrier and impurity spins in paramagnetic II-VI diluted magnetic semiconductors in a $\mathbf{k}$-dependent effective magnetic field are derived, where the carrier-impurity correlations are taken into account. In the Markov limit, rates for the electron-impurity spin transfer can be derived for electron spins parallel and perpendicular to the impurity spins corresponding to measurable decay rates in Kerr experiments in Faraday and Voigt geometry. Our rigorous microscopic quantum kinetic treatment automatically accounts for the fact that, in an individual spin flip-flop scattering process, a spin flip of an electron is necessarily accompanied by a flop of an impurity spin in the opposite direction and the corresponding change of the impurity Zeeman energy influences the final energy of the electron after the scattering event. This shift in the electron energies after a spin flip-flop scattering processes, which usually has been overlooked in the literature, turns out to be especially important in the case of extremely diluted magnetic semiconductors in an external magnetic field. As a specific example for a $\mathbf{k}$-dependent effective magnetic field the effects of a Rashba field on the dynamics of the carrier-impurity correlations in a Hg$_{1-x-y}$Cd$_y$Mn$_x$Te quantum well are described. It is found that, although accounting for the Rashba interaction in the dynamics of the correlations leads to a modified $\mathbf{k}$-space dynamics, the time evolution of the total carrier spin is not significantly influenced. Furthermore, a connection between the present theory and the description of collective carrier-impurity precession modes is presented., Comment: 18 pages, 7 figures

The non-Markovian effects in the spin dynamics in diluted magnetic semiconductors found in quantum kinetic calculations can be reproduced very well by a much simpler effective single electron theory, if a finite memory is accounted for. The resulting integro-differential equation can be solved by a differential transform method, yielding the Taylor series of the solution. From the comparison of both theories it can be concluded that the non-Markovian effects are due to the spectral proximity of the excited electrons to the band edge.

We investigate the transfer between carrier and Mn spins due to the s-d-exchange interaction in a Mn doped bulk semiconductor within a microscopic quantum kinetic theory. We demonstrate that the spin transfer dynamics is qualitatively different for components of the carrier spin parallel and perpendicular to the Mn magnetization. From our quantum kinetic equations we have worked out the corresponding Markov limit which is equivalent to rate equations based on Fermi's golden rule. The resulting equations resemble the widely used Landau-Lifshitz-Gilbert-equations, but also describe genuine spin transfer due to quantum corrections. Although it is known that the Markovian rate description works well for bulk systems when the initial Mn magnetization is zero, we find large qualitative deviations from the full quantum kinetic theory for finite initial Mn magnetizations. These deviations mainly reflect corrections of higher than leading order in the interaction which are not accounted for in golden rule-type rates.

The effects of carrier-impurity correlations due to a Kondo-like spin-spin interaction in diluted magnetic semiconductors are investigated. These correlations are not only responsible for a transfer of spins between the carriers and the impurities, but also produce non-perturbative effects in the spin dynamics such as renormalization of the precession frequency of the carrier spins, which can reach values of several percent in CdMnTe quantum wells. In two-dimensional systems, the precession frequency renormalization for a single electron spin with defined wave vector shows logarithmic divergences similar to those also known from the Kondo problem in metals. For smooth electron distributions, however, the divergences disappear due to the integrability of the logarithm. A possible dephasing mechanism caused by the wave-vector dependence of the electron spin precession frequencies is found to be of minor importance compared to the spin transfer from the carrier to the impurity system. In the Markov limit of the theory, a quasi-equilibrium expression for the carrier-impurity correlation energy can be deduced indicating the formation of strongly correlated carrier-impurity states for temperatures in the mK range.

We study theoretically the ultrafast spin dynamics of II-VI diluted magnetic semiconductors in the presence of spin-orbit interaction. Our goal is to explore the interplay or competition between the exchange $sd$-coupling and the spin-orbit interaction in both bulk and quantum well systems. For bulk materials we concentrate on Zn$_{1-x}$Mn$_x$Se and take into account the Dresselhaus interaction, while for quantum wells we examine Hg$_{1-x-y}$Mn$_x$Cd$_y$Te systems with a strong Rashba coupling. Our calculations were performed with a recently developed formalism which incorporates electronic correlations beyond mean-field theory originated from the exchange $sd$-coupling. For both bulk and quasi-two-dimensional systems we find that, by varying the system parameters within realistic ranges, both interactions can be chosen to play a dominant role or to compete on an equal footing with each other. The most notable effect of the spin-orbit interaction in both types of systems is the appearance of strong oscillations where the exchange $sd$-coupling by itself only causes an exponential decay of the mean electronic spin components. The mean-field approximation is also studied and it is interpreted analytically why it shows a strong suppression of the spin-orbit-induced dephasing of the spin component parallel to the Mn magnetic field., Comment: 9 pages, 5 figures

Starting from a quantum kinetic theory for the spin dynamics in diluted magnetic semiconductors, we derive simplified equations that effectively describe the spin transfer between carriers and magnetic impurities for an arbitrary initial impurity magnetization. Taking the Markov limit of these effective equations, we obtain good quantitative agreement with the full quantum kinetic theory for the spin dynamics in bulk systems at high magnetic doping. In contrast, the standard rate description where the carrier-dopant interaction is treated according to Fermi's golden rule, which involves the assumption of a short memory as well as a perturbative argument, has been shown previously to fail if the impurity magnetization is non-zero. The Markov limit of the effective equations is derived, assuming only a short memory, while higher order terms are still accounted for. These higher order terms represent the precession of the carrier-dopant correlations in the effective magnetic field due to the impurity spins. Numerical calculations show that the Markov limit of our effective equations reproduces the results of the full quantum kinetic theory very well. Furthermore, this limit allows for analytical solutions and for a physically transparent interpretation., Comment: 15 pages, 3 figures

A quantum kinetic theory of the spin transfer between carriers and Mn atoms in a Mn doped diluted magnetic semiconductor is presented. It turns out that the typical memory time associated with these processes is orders of magnitude shorter than the time scale of the spin transfer. Nevertheless, Markovian rate equations, which are obtained by neglecting the memory, work well only for bulk systems. For quantum wells and wires the quantum kinetic results qualitatively deviate from the Markovian limit under certain conditions. Instead of a monotonic decay of an initially prepared excess electron spin, an overshoot or even coherent oscillations are found. It is demonstrated that these features are caused by energetic redistributions of the carriers due to the energy-time uncertainty.