This paper presents a class of structure-preserving numerical methods for quantum optimal control problems, based on commutator-free Cayley integrators. Starting from the Krotov framework, we reformulate the forward and backward propagation steps using Cayley-type schemes that preserve unitarity and symmetry at the discrete level. This approach eliminates the need for matrix exponentials and commutators, leading to significant computational savings while maintaining higher-order accuracy. We first recall the standard linear setting and then extend the formulation to nonlinear Schrödinger and Gross-Pitaevskii equations using a Cayley-polynomial interpolation strategy. Numerical experiments on state-transfer problems illustrate that the CF-Cayley method achieves the same accuracy as high-order exponential or Cayley-Magnus schemes at substantially lower cost, especially for longtime or highly oscillatory dynamics. In the nonlinear regime, the structure-preserving properties of the method ensure stability and norm conservation, making it a robust tool for large-scale quantum control simulations. The proposed framework thus bridges geometric integration and optimal control, offering an efficient and reliable alternative to existing exponential-based propagators.

Photon echo (PE) spectroscopy is a powerful technique for probing decoherence mechanisms and charge carrier dynamics in semiconductor systems. Beyond traditional coherence measurements, characterizing the photon statistics of the echo signal is important for assessing its potential in quantum information applications and understanding the underlying quantum mechanical processes. Here, we study the photon statistics of PE signals generated by excitons in ensembles of lead halide perovskite CsPbI_3 nanocrystals at cryogenic temperature of 2 K using continuous-variable quantum state optical tomography based on homodyne detection. Pronounced Rabi oscillations of PE amplitude allow us to evaluate the statistics for various pulse areas in the excitation sequence. The damping of the oscillations with increasing pulse area is attributed to spatial excitation inhomogeneity and excitation-induced dephasing. Despite the large ensemble of optically addressed excitons, the efficiency of generated PE signals is low which is attributed to complex energy structure of excitons and non-radiative recombination channels in CsPbI_3 nanocrystals. We analyze the statistical characteristics of PE via the second-order correlation function g^(2)(0) and the characteristic function for different combinations of the areas of the excitation pulses. Our results show that g^(2)(0) = 1, and the characteristic function of the PE signal corresponds to classical behavior. Despite the relatively low efficiency, the photon echo exhibits a high degree of coherence and minimal classical noise, consistent with Poissonian statistics.

The coherent interaction between quantum light and material excitations in semiconductor nanostructures is investigated using a fully quantized microscopic approach that incorporates many-body Coulomb correlations. The simulations demonstrate that the quantum dynamics is influenced by biexciton continuum states and is highly sensitive to both the frequency of the cavity mode and the strength of the light-matter coupling.

We compute and analyze the dependence of excitonic second-and third-harmonic generation (SHG/THG) as a function of the optical excitation intensity in the presence of static electric fields by solving the semiconductor Bloch equations. Our simulations are performed for excitation of the strongly bound intralayer exciton of an inversion-symmetric homobilayer of MoS2 with in-plane electric fields. We demonstrate that for resonant excitation at the 1s K-exciton the SHG and the THG show complex dependencies on both the strength of the static field and the peak amplitude of the optical pulse. For sufficiently intense optical excitation, the THG increases and the SHG increases superlinearly with the amplitude of the static field as long as exciton ionization is not yet dominating. Microscopic simulations demonstrate that these dependencies arise from an interplay between several effects including static and transient Stark shifts, exciton ionization, off-resonant Rabi oscillations, and a modified interference between optical nonlinearities induced by the intraband acceleration. Our findings offer several new possibilities for controlling the strong-field dynamics of systems with strongly bound excitons.

We demonstrate the novel effect of gain-induced spectral shifts in the type-II parametric down-conversion (PDC) process, which results in a transition from degenerate to non-degenerate PDC with increasing parametric gain. This effect, originating from the second-order dispersion terms, significantly alters the properties of PDC in the high-gain regime, where it leads to increased distinguishability of the generated photon pairs. The effect is established by evaluating a rigorous theoretical model, which is based on solving a system of coupled integro-differential equations for monochromatic operators. The widely used spatially-averaged approximate model fails to reproduce this important effect.

Hybrid quantum photonics seeks to combine the complementary advantages of continuous- and discrete-variable quantum optics. This typically entails photon-counting measurements on entangled states generated by interfering many single-mode squeezed-vacuum (SMSV) states. However, because conventional photon-counting schemes are mode-insensitive, it is critical that the SMSV states occupy a single, well-defined mode. Achieving this requires careful engineering of the process, which determines both the spatial and spectro-temporal properties of the generated state. In addition, the ideal source must be massively scalable, capable of efficiently generating strong squeezing, and remain compatible with existing detection schemes and fiber networks. Although many platforms address one or more of these requirements, satisfying all of them simultaneously remains challenging. Here, we present a source that meets all of these requirements: a single-pass, periodically poled, Type-II potassium titanyl phosphate (KTP) waveguide optimized for scalable hybrid quantum-photonic architectures. The SMSV state produced by the source has a measured effective mode number of 1.24. Furthermore, the source is extremely bright (producing up to 40 000 photons per pulse) and operates at a central wavelength of 1546nm, optimized for fiber-network compatibility and which, in combination with picosecond duration, also enables intrinsic photon-number resolution in superconducting nanowire single-photon detectors. Although this source constitutes an ideal source in a simplified picture, the ultimate limitations of any source will be governed by complex dynamics that arise when the system is driven at high-gain or due to unavoidable loss during state generation. We have therefore developed a complete theoretical framework that enables a comprehensive photon-counting-based characterization of the source.

Low-order harmonics, normally valued for their efficiency but often viewed as perturbative, are shown here to arise from a strongly non-perturbative intraband response, enabling halfcycle switching. In wide-bandgap dielectrics near the damage threshold, a gas-phase-inspired injection current has gained broad attention as a putative third radiation channel beyond the intra- and interband responses. Combining phase-locked ω–3ω spectroscopy in crystalline α-quartz and fused silica with orientation-resolved measurements in α-quartz, we determine the contributing microscopic channels of low-order harmonics. A polarization-consistent decomposition demonstrates that this gas-phase analogy cannot be directly transferred to solids: the injection contribution cancels from the total current and does not survive as an independent radiation channel. Experimentally, the third and fifth harmonics follow the optical waveform and switch every 3.3 fs between ON and OFF states, exhibiting nearly 100-fold signal contrast. A field-driven evolution from crystallographic anisotropy to near-isotropic emission is observed in α-quartz. These measurements, together with the large nonlinear indicator previously reported for wave mixing1, are all accounted for by the intraband current. Our results reveal a distinctively band-structure-driven route to strongly non-perturbative nonlinearity at low harmonic orders, extending subcycle lightwave control from transient conductivity to bright, petahertz-bandwidth subcycle harmonic switching.

In this paper, we theoretically study the spectral and temporal properties of pulsed spontaneous parametric down-conversion (SPDC) generated in lossy waveguides. Our theoretical approach is based on the formalism of Gaussian states and the Langevin equation, which is elaborated for weak parametric down-conversion and photon-number-unresolved click detection. Using the example of frequency-degenerate type-II SPDC generated under the pump-idler group-velocity-matching condition, we show how the joint-spectral intensity, mode structure, normalized second-order correlation function, and Hong-Ou-Mandel interference pattern depend on internal losses of the SPDC process. We found that the joint-spectral intensity is almost insensitive to internal losses, while the second-order correlation function shows a strong dependence on them, being different for the signal and idler beams in the presence of internal losses. Based on the sensitivity of the normalized second-order correlation function, we show how its measurement can be used to experimentally determine internal losses.

Static electric fields lead to Stark shifts and ionization of excitons. For a bi-layer of MoS 2 we demonstrate that electric fields of intermediate strength can significantly increase excitonic third harmonic generation before ionization dominates.

A unified theoretical approach to describe the properties of multimode squeezed light generated in a lossy medium is presented. This approach is valid for Markovian environments and includes both a model of discrete losses based on the beamsplitter approach and a generalized continuous loss model based on the spatial Langevin equation. For an important class of Gaussian states, we derive master equations for the second-order correlation functions and illustrate their solution for both frequency-independent and frequency-dependent losses. Studying the mode structure, we demonstrate that in a lossy environment no broadband basis without quadrature correlations between the different broadband modes exists. Therefore, various techniques and strategies to introduce broadband modes can be considered. We show that the Mercer expansion and the Williamson-Euler decomposition do not provide modes in which the maximal squeezing contained in the system can be measured. In turn, we find a new broadband basis that maximizes squeezing in the lossy system and present an algorithm to construct it.

A microscopic many-body approach describing semiconductor nanostructures excited by quantum light is presented. The coupled dynamics of photons and electron-hole-pair excitations highlights the importance of a microscopic modeling, in particular the relevance biexcitonic continuum states.

Entangled two-mode Gaussian states constitute an important building block for continuous variable quantum computing and communication protocols and are thus of high demand for many experiments. In this work, we study such kind of states which are extracted from multimode light generated via type-II parametric down-conversion (PDC) in lossy waveguides. For such states, we demonstrate that the squeezing quantifies entanglement and we construct a measurement basis which results in the maximal bipartite entanglement. We illustrate our findings by numerically solving the spatial master equation for PDC in a Markovian environment. The optimal measurement modes are compared with two widely-used broadband bases: the Mercer-Wolf basis (the first-order coherence basis) and the Williamson-Euler basis.

We compute and analyze the dependence of excitonic second- and third-harmonic generation (SHG/THG) as a function of the optical excitation intensity in the presence of static electric fields by solving the semiconductor Bloch equations. Our simulations are performed for excitation of the strongly bound intralayer exciton of an inversion-symmetric homobilayer of MoS2 with in-plane electric fields. We demonstrate that for resonant excitation at the 1s K-exciton the SHG and the THG show complex dependencies on both the strength of the static field and the peak amplitude of the optical pulse. For sufficiently intense optical excitation, the THG increases and the SHG increases superlinearly with the amplitude of the static field as long as exciton ionization is not yet dominating. Microscopic simulations demonstrate that these dependencies arise from an interplay between several effects including static and transient Stark shifts, exciton ionization, Wannier-Stark localization, off-resonant Rabi oscillations, and a modified interference between optical nonlinearities induced by the intraband acceleration. Our findings offer several new possibilities for controlling the strong-field dynamics of systems with strongly bound excitons.

We present a microscopic and fully quantized model to investigate the interaction between semiconductor nanostructures and quantum light fields including the many-body Coloumb interaction between photoexcited electrons and holes. Our approach describes the coupled dynamics of the quantum light field and single and double electron-hole pairs, i.e., excitons and biexcitons, and exactly accounts for Coulomb many-body correlations and carrier band dispersions. Using a straightforward yet exact approach, we study a one-dimensional twoband system interacting with a single-mode, two-photon quantum state within a Tavis-Cummings framework. By employing an exact coherent factorization scheme, the computational complexity is reduced significantly enabling numerical simulations. We also derive a simplified model that includes only the bound 1s-exciton and biexciton states for comparison. Our simulations reveal distinct single- and two-photon Rabi oscillations, corresponding to photon-exciton and exciton-biexciton transitions. We demonstrate, in particular, that biexciton continuum states significantly modify the dynamics in a way that cannot be captured by simplified models that consider only bound states. Our findings emphasize the importance of a comprehensive microscopic modeling in order to accurately describe quantum optical phenomena of interacting electronic many-body systems.

We investigate the dynamics of wave packets in a parabolic optical lattice formed by combining an optical lattice with a global parabolic trap. Our study examines the phase space representation of the system's eigenstates by comparing them to the classical phase space of a pendulum, to which the system effectively maps. The analysis reveals that quantum states can exhibit mixed dynamics by straddling the separatrix. A key finding is that the dynamics around the separatrix enables the controlled creation of highly nonclassical states, distinguishing them from the classical oscillatory or rotational dynamics of the pendulum. By considering a finite momentum of the initial wave packet, we demonstrate various dynamical regimes. Furthermore, a slight energy mismatch between nearly degenerate states localized at opposite turning points of the trap potential results in controlled long-range dynamical tunneling. These results can be interpreted as quantum beating between a clockwise rotating and a counterclockwise rotating pendulum.

We introduce a new classification of multimode states with a fixed number of photons. This classification is based on the factorizability of homogeneous multivariate polynomials and is invariant under unitary transformations. The classes physically correspond to field excitations in terms of single and multiple photons, each of which is in an arbitrary irreducible superposition of quantized modes. We further show how the transitions between classes are rendered possible by photon addition, photon subtraction, and photon-projection nonlinearities. We explicitly put forward a design for a multilayer interferometer in which the states for different classes can be generated with state-of-the-art experimental techniques. Limitations of the proposed designs are analyzed using the introduced classification, providing a benchmark for the robustness of certain states and classes.

Experiments with ultracold atoms in optical lattices usually involve a weak parabolic trapping potential which merely serves to confine the atoms, but otherwise remains negligible. In contrast, we suggest a different class of experiments in which the presence of a stronger trap is an essential part of the set-up. Because the trap-modified on-site energies exhibit a slowly varying level spacing, similar to that of an anharmonic oscillator, an additional time-periodic trap modulation with judiciously chosen parameters creates nonlinear resonances which enable efficient Floquet engineering. We employ a Mathieu approximation for constructing the near-resonant Floquet states in an accurate manner and demonstrate the emergence of effective ground states from the resonant trap eigenstates. Moreover, we show that the population of the Floquet states is strongly affected by the phase of a sudden turn-on of the trap modulation, which leads to significantly modified and rich dynamics. As a guideline for further studies, we argue that the deliberate population of only the resonance-induced effective ground states will allow one to realize Floquet condensates which follow classical periodic orbits, thus providing challenging future perspectives for the investigation of the quantum-classical correspondence.

The dynamics of semiconductor quantum wires and wells that are coupled to a single-mode quantum field are analyzed. Within a two-band tight-binding model the Coulomb interaction between electrons and holes is included on a microscopic basis and the light-matter interaction is quantized. The dynamics of the system is described by equations of motion for the relevant set of expectation values of the coupled electronic-photonic system. Starting from the initial condition of a single photon occupying the field mode, we study the dynamics of the mean photon number. To analyze effects arising from the many-body Coulomb interaction, we use an exact truncation of the electronic hierarchy problem by employing the fact that N photons cannot excite more than N electron-hole pairs. We compare Rabi oscillations with and without Coulomb interaction for different excitation conditions. When the quantum field mode is initially occupied by two photons, two interacting electron-hole pairs, i.e., biexcitons, can be generated which characteristically modify the dynamics. Within a consistent and fully-quantized approach we show consequences of biexcitonic many-body correlations that are coupled to a quantum field and discuss the obtained dynamics.

Tunneling ionization is a crucial process in the interaction between strong laser fields and matter which initiates numerous nonlinear phenomena including high-order harmonic generation, photoelectron holography, etc. Both adiabatic and nonadiabatic tunneling ionization are well understood in atomic systems. However, the tunneling dynamics in solids, especially nonadiabatic tunneling, has not yet been fully understood. Here, we study the sub-cycle resolved strong-field tunneling dynamics in solids via a complex saddle-point method. We compare the instantaneous momentum at the moment of tunneling and the tunneling distances over a range of Keldysh parameters. Our results demonstrate that for nonadiabatic tunneling, tunneling ionization away from Γ point is possible. When this happens the electron has a nonzero initial velocity when it emerges in the conduction band. Moreover, consistent with atomic tunneling, a reduced tunneling distance as compared to the quasi-static case is found. Our results provide remarkable insight into the basic physics governing the sub-cycle electron tunneling dynamics with significant implications for understanding subsequent strong-field nonlinear phenomena in solids.