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Semiconductor quantum dots are a versatile source of single photons with tunable properties to be used in quantum-cryptographic applications. A crucial figure of merit of the emitted photons is photon number coherence (PNC), which impacts the security of many quantum communication protocols. In the process of single-photon generation, the quantum dot as a solid-state object is subject to an interaction with phonons, which can therefore indirectly affect the PNC. In this paper, we elaborate on the origin of PNC in optically excited quantum dots and how it is affected by phonons. In contrast to the expectation that phonons always deteriorate coherence, PNC can be increased in a quantum dot-cavity system due to the electron-phonon interaction.

We describe a general-purpose computational toolkit for simulating open quantum systems, which provides numerically exact solutions for composites of zero-dimensional quantum systems that may be strongly coupled to multiple, quite general non-Markovian environments. It is based on process tensor matrix product operators (PT-MPOs), which efficiently encapsulate environment influences. The code features implementations of several PT-MPO algorithms, in particular, Automated Compression of Environments (ACE) for general environments comprised of independent modes as well as schemes for generalized spin boson models. The latter includes a divide-and-conquer scheme for periodic PT-MPOs, which enable million time step simulations for realistic models. PT-MPOs can be precalculated and reused for efficiently probing different time-dependent system Hamiltonians. They can also be stacked together and combined to provide numerically complete solutions of small networks of open quantum systems. The code is written in C++ and is fully controllable by configuration files, for which we have developed a versatile and compact human-readable format.

The algorithm "automated compression of environments" (ACE) [Nat. Phys. 18, 662 (2022)] provides a versatile way of simulating an extremely broad class of open quantum systems. This is achieved by encapsulating the influence of the environment, which is determined by the interaction Hamiltonian(s) and initial states, into compact process tensor matrix product operator (PT-MPO) representations. The generality of the ACE method comes at high numerical cost. Here, we demonstrate that orders-of-magnitude improvement of ACE is possible by changing the order of PT-MPO contraction from a sequential to a tree-like scheme. The problem of combining two partial PT-MPOs with large inner bonds is solved by a preselection approach. The drawbacks of the preselection approach are that the MPO compression is suboptimal and that it is more prone to error accumulation than sequential combination and compression. We therefore also identify strategies to mitigate these disadvantages by fine-tuning compression parameters. This results in a scheme that is similar in compression efficiency and accuracy to the original ACE algorithm, yet is significantly faster. Our numerical experiments reach similar conclusions for bosonic and fermionic test cases, suggesting that our findings are characteristic of the combination of PT-MPOs more generally.

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

Process tensor matrix product operators (PT-MPOs) enable numerically exact simulations for an unprecedentedly broad range of open quantum systems. By representing environment influences in MPO form, they can be efficiently compressed using established algorithms. The dimensions of inner bonds of the compressed PT-MPO may be viewed as an indicator of the complexity of the environment. Here, we show that the inner bonds themselves, not only their dimensions, have a concrete physical meaning: They represent the subspace of the full environment Liouville space which hosts environment excitations that may influence the subsequent open quantum systems dynamics the most. This connection can be expressed in terms of lossy linear transformations, whose pseudoinverses facilitate the extraction of environment observables. We demonstrate this by extracting the environment spin of a central spin problem, the current through a quantum system coupled to two leads, the number of photons emitted from quantum emitters into a structured environment, and the distribution of the total absorbed energy in a driven non-Markovian quantum system into system, environment, and interaction energy terms. Numerical tests further indicate that different PT-MPO algorithms compress environments to similar subspaces. Thus, the physical interpretation of inner bonds of PT-MPOs both provides a conceptional understanding and it enables new practical applications.

Complete quantum control of a stationary quantum bit embedded in a quantum emitter is crucial for photonic quantum information technologies. Recently, the orbital degree of freedom in optically active quantum dots has emerged as a promising candidate. However, the essential ability to perform arbitrary rotations on orbital qubits remains elusive. Here, we demonstrate arbitrary rotation of a hole orbital qubit with direct phase control using picosecond optical pulses. This is achieved by successfully inducing stimulated Raman transitions within $\Lambda$ systems coupled via radiative Auger processes. The new capability enables direct control of polar and azimuth angles of the Bloch vector without requiring timed precession. Our results establish orbital states in solid-state quantum emitters as a viable resource for applications in high-speed quantum information processing., Comment: Manuscript with 7 pages and 4 figures plus Supplementary Material comprising 9 pages and 10 figures

Cooperative effects of multiple quantum emitters are characterized by transitions via delocalized collective states with altered emission properties due to the existence of inter-emitter coherences. When realized with excitonic condensed matter nanostructures, these effects are significantly affected by the presence of strong emitter-phonon coupling, which leads to the formation of polarons. We show that, while for single-emitter emission into free space this formation has no impact on its radiative lifetime, the same is not true for superradiant emission. Considering the case of two indistinguishable quantum emitters, we analyse how polaron dressing affects collective photon emission by mixing bright and dark Dicke states. Our numerical simulations show that this mixing crucially depends on the circumstances of the excitation of the system: Depending on the pulse length of an exciting laser, one can choose to either prepare polaronic Dicke states, or bare electronic Dicke states, changing the superradiant decay characteristics of the system. Additionally, we derive analytic expressions for these limiting cases, which match the results of numerically exact calculations.

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

The interaction of a resonant light field with a quantum two-level system is of key interest both for fundamental quantum optics and quantum technological applications employing resonant excitation. While emission under resonant continuous-wave excitation has been well-studied, the more complex emission spectrum of dynamically dressed states, a quantum two-level system driven by resonant pulsed excitation, has so far been investigated in detail only theoretically. Here, we present the first experimental observation of the complete resonance fluorescence emission spectrum of a single quantum two-level system, in form of an excitonic transition in a semiconductor quantum dot, driven by finite Gaussian pulses. We observe multiple emerging sidebands as predicted by theory with an increase of their number and spectral detuning with excitation pulse intensity and a dependence of their spectral shape and intensity on the pulse length. Detuning-dependent measurements provide additional insights into the emission features. The experimental results are in excellent agreement with theoretical calculations of the emission spectra, corroborating our findings.

While several numerical techniques are available for predicting the dynamics of non-Markovian open quantum systems, most struggle with simulations for very long memory and propagation times, e.g., due to superlinear scaling with the number of time steps $n$. Here, we introduce a numerically exact algorithm to calculate process tensors -- compact representations of environmental influences -- which provides a scaling advantage over previous algorithms by leveraging self-similarity of the tensor networks that represent Gaussian environments. Based on a divide-and-conquer strategy, our approach requires only $\mathcal{O}(n\log n)$ singular value decompositions for environments with infinite memory. Where the memory can be truncated after $n_c$ time steps, a scaling $\mathcal{O}(n_c\log n_c)$ is found, which is independent of $n$. This improved scaling is enabled by identifying process tensors with repeatable blocks. To demonstrate the power and utility of our approach we provide three examples. (1) We calculate the fluorescence spectra of a quantum dot under both strong driving and strong dot-phonon couplings, a task requiring simulations over millions of time steps, which we are able to perform in minutes. (2) We efficiently find process tensors describing superradiance of multiple emitters. (3) We explore the limits of our algorithm by considering coherence decay with a very strongly coupled environment. The algorithm we present here not only significantly extends the scope of numerically exact techniques to open quantum systems with long memory times, but also has fundamental implications for simulation complexity.

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

Coherently driven semiconductor quantum dots are one of the most promising platforms for non-classical light sources and quantum logic gates which form the foundation of photonic quantum technologies. However, to date, coherent manipulation of single charge carriers in quantum dots is limited mainly to their lowest orbital states. Ultrafast coherent control of high-orbital states is obstructed by the demand for tunable terahertz pulses. To break this constraint, we demonstrate an all-optical method to control high-orbital states of a hole via stimulated Auger process. The coherent nature of the Auger process is proved by Rabi oscillation and Ramsey interference. Harnessing this coherence further enables the investigation of single-hole relaxation mechanism. A hole relaxation time of 161 ps is observed and attributed to the phonon bottleneck effect. Our work opens new possibilities for understanding the fundamental properties of high-orbital states in quantum emitters and developing new types of orbital-based quantum photonic devices., Comment: Manuscript with 14 pages and 6 figures plus supplementary Information comprising 15 pages and 14 figures. Nature Nanotechnology (24 July 2023)

Realising scalable quantum networks requires a meticulous level of understanding and mitigating the deleterious effects of decoherence. Many quantum device platforms feature multiple decoherence mechanisms, often with a dominant mechanism seemingly fully masking others. In this paper, we show how access to weaker dephasing mechanisms can nevertheless be obtained for optically active qubits by performing two-photon coincidence measurements. To this end we theoretically investigate the impact of different decoherence mechanisms on cooperatively emitting quantum dots. Focusing on the typically dominant deformation-potential coupling to longitudinal acoustic phonons and typically much less severe additional sources of pure dephasing, we employ a numerically exact method to show that these mechanisms lead to very different two-photon coincidence signals. Moreover, surprisingly, the impact of the strongly coupled phonon environment is weak and leads to long-lived coherences. We trace this back to the superohmic nature of the deformation-potential coupling causing inter-emitter coherences to converge to a nonzero value on a short timescale, whereas pure dephasing contributions cause a complete decay of coherence over longer times. Our approach provides a practical means of investigating decoherence processes on different timescales in solid state emitters, and thus contributes to understanding and possibly eliminating their detrimental influences.

Indistinguishable quantum emitters confined to length scales smaller than the wavelength of the light become superradiant. Compared to uncorrelated and distinguishable emitters, superradiance results in qualitative modifications of optical signals such as photon coincidences. However, recent experiments revealed that similar signatures can also be obtained in situations where emitters are too far separated to be superradiant if correlations between emitters are induced by the wave function collapse during an emission-angle-selective photon detection event. Here, we compare two sources for cooperative emission, superradiance and measurement-induced cooperativity, and analyze their impact on time-dependent optical signals. We find that an anti-dip in photon coincidences at zero time delay is a signature of inter-emitter correlations in general but does not unambiguously prove the presence of superradiance. This suggests that photon coincidences at zero time delay alone are not sufficient and time-dependent data is necessary to clearly demonstrate a superradiant enhancement of the spontaneous radiative decay rate.

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

We describe here a quantum simulator of extended bipartite Hubbard model with broken sublattice symmetry. The simulator consists of a structured lateral gate confining two dimensional electrons in a quantum well into artificial minima arranged in a hexagonal lattice. The sublattice symmetry breaking is generated by forming an artificial triangular graphene quantum dot (ATGQD) with zigzag edges. The resulting extended Hubbard model generates tunable ratio of tunneling strength to electron-electron interactions and of sublattice symmetry with control over shape. The validity of the simulator is confirmed for small systems using mean-field and exact diagonalization many-body approaches which show that the ground state changes from a metallic to an antiferromagnetic (AF) phase by varying the distance between sites or depth of the confining potential. The one-electron spectrum of these triangular dots contains a macroscopically degenerate shell at the Fermi level. The shell persists at the mean-field level for weak interactions (metallic phase) but disappears for strong interactions, in the AF phase. We determine the effects of electron-electron interactions on the ground state, the total spin, and the excitation spectrum as a function of filling of the ATGQD. We find that the half-filled charge neutral shell leads to a partially spin polarized state in both metallic and AF regimes in accordance with Liebs theorem. In both regimes a relatively large gap separates the spin polarized ground state to the first excited many-body state at half filling of the degenerate shell. By adding or removing an electron, this gap drops dramatically, and alternate total spin states emerge with energies nearly degenerate to a spin polarized ground state., Comment: 7 figures, 11 pages

The controlled preparation of the excited state in a quantum emitter is a prerequisite for its usage as single-photon sources - a key building block for quantum technologies. In this paper we propose a coherent excitation scheme using off-resonant pulses. In the usual Rabi scheme, these pulses would not lead to a significant occupation. This is overcome by using a frequency modulated pulse to swing up the excited state population. The same effect can be obtained using two pulses with different strong detunings of the same sign. We theoretically analyze the applicability of the scheme to a semiconductor quantum dot. In this case the excitation is several meV below the band gap, i.e., far away from the detection frequency allowing for easy spectral filtering, and does not rely on any auxiliary particles such as phonons. Our scheme has the potential to lead to the generation of close-to-ideal photons., Comment: 10 pages, 7 figures

Photon-mediated interactions between atomic systems can arise via coupling to a common electromagnetic mode or by quantum interference. Here, we probe the role of coherence in cooperative emission arising from two distant but indistinguishable solid-state emitters because of path erasure. The primary signature of cooperative emission, the emergence of "bunching" at zero delay in an intensity correlation experiment, is used to characterise the indistinguishability of the emitters, their dephasing, and the degree of correlation in the joint system that can be coherently controlled. In a stark departure from a pair of uncorrelated emitters, in Hong-Ou-Mandel type interference measurements we observe photon statistics from a pair of indistinguishable emitters resembling that of a weak coherent state from an attenuated laser. Our experiments establish techniques to control and characterize cooperative behavior between matter qubits using the full quantum optics toolbox, a key step toward realizing large-scale quantum photonic networks., Comment: Published version. 16 pages, 9 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

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

Understanding strongly interacting electrons enables the design of materials, nanostructures and devices. Developing this understanding relies on the ability to tune and control electron-electron interactions by, e.g., confining electrons to atomically thin layers of 2D crystals with reduced screening. The interplay of strong interactions on a hexagonal lattice with two nonequivalent valleys, topological moments, and the Ising-like spin-orbit interaction gives rise to a variety of phases of matter corresponding to valley and spin polarized broken symmetry states. In this work we describe a highly tunable strongly interacting system of electrons laterally confined to monolayer transition metal dichalcogenide MoS$_2$ by metalic gates. We predict the existence of valley and spin polarized broken symmetry states tunable by the parabolic confining potential using exact diagonalization techniques for up to $N=6$ electrons. We find that the ground state is formed by one of two phases, either both spin and valley polarized or valley unpolarised but spin intervalley antiferromagnetic, which compete as a function of electronic shell spacing. This finding can be traced back to the combined effect of Ising-like spin-orbit coupling and weak intervalley exchange interaction. These results provide an explanation for interaction-driven symmetry-breaking effects in valley systems and highlight the important role of electron-electron interactions for designing valleytronic devices.

We present a method to calculate many-body states of interacting carriers in million atom quantum nanostructures based on atomistic tight-binding calculations and a combination of iterative selection of configurations and perturbation theory. This method enables investigations of large excitonic complexes and multi-electron systems with near full configuration interaction accuracy, even though only a small subspace of the full many-body Hilbert space is sampled, thus saving orders of magnitudes in computational resources. Important advantages of this method are that the convergence is controlled by a single parameter, the threshold, and that ground and excited states can be treated on an equal footing. We demonstrate the extreme efficiency of the method by numerical studies of complexes composed of up to 13 excitons, which requires filling of states up to the fourth electronic shell. We find that the method generally converges fast as a function of the threshold, profiting from a significant enhancement due to the perturbative corrections. The role of the choice of single-particle basis states is discussed. It is found that the algorithm converges faster in the Hartree-Fock basis only for highly charged systems, where Coulomb repulsion dominates. Finally, based on the observation that second order perturbative energy corrections only depend on off-diagonal elements of the many-body Hamiltonian, we present a way to accurately calculate many-body states that requires only a relatively small number of Coulomb matrix elements.

We present here an atomistic theory of the electronic and optical properties of hexagonal InAsP quantum dots in InP nanowires in the wurtzite phase. These self-assembled quantum dots are unique in that their heights, shapes, and diameters are well known. Using a combined valence-force-field, tight-binding, and configuration-interaction approach we perform atomistic calculations of single-particle states and excitonic, biexcitonic and trion complexes as well as emission spectra as a function of the quantum dot height, diameter and As versus P concentration. The atomistic tight-binding parameters for InAs and InP in the wurtzite crystal phase were obtained by ab initio methods corrected by empirical band gaps. The low energy electron and hole states form electronic shells similar to parabolic or cylindrical quantum confinement, only weakly affected by hexagonal symmetry and As fluctuations. The relative alignment of the emission lines from excitons, trions and biexcitons agrees with that for InAs/InP dots in the zincblende phase in that biexcitons and positive trions are only weakly bound. The random distribution of As atoms leads to dot-to-dot fluctuations of a few meV for the single-particle states and the spectral lines. Due to the high symmetry of hexagonal InAsP nanowire quantum dots the exciton fine structure splitting is found to be small, of the order a few $\mu$eV with significant random fluctuations in accordance with experiments.

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

We study theoretically the ultrafast spin dynamics of II-VI diluted magnetic quantum wells in the presence of spin-orbit interaction. We extend a recent study where it was shown that the spin-orbit interaction and the exchange sd coupling in bulk and quantum wells can compete resulting in qualitatively new dynamics when they act simultaneously. We concentrate on Hg$_{1-x-y}$Mn$_x$Cd$_y$Te quantum wells, which have a highly tunable Rashba spin-orbit coupling. Our calculations use a recently developed formalism which incorporates electronic correlations originating from the exchange $sd$-coupling. We find that the dependence of electronic spin oscillations on the excess energy changes qualitatively depending on whether or not the spin-orbit interaction dominates or is of comparable strength with the sd interaction., Comment: 4 pages, 5 figures, EDISON'19, 29 June - 2 July, 2015, Salamanca. Spain

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