Microscopic Quantum Theory Research Articles

Electronic transport driven by collective light-matter coupled states in a quantum device

In the majority of optoelectronic devices, emission and absorption of light are considered as perturbative phenomena. Recently, a regime of highly non-perturbative interaction, ultra-strong light-matter coupling, has attracted considerable attention, as it has led to changes in the fundamental properties of materials such as electrical conductivity, rate of chemical reactions, topological order, and non-linear susceptibility. Here, we explore a quantum infrared detector operating in the ultra-strong light-matter coupling regime driven by collective electronic excitations, where the renormalized polariton states are strongly detuned from the bare electronic transitions. Our experiments are corroborated by microscopic quantum theory that solves the problem of calculating the fermionic transport in the presence of strong collective electronic effects. These findings open a new way of conceiving optoelectronic devices based on the coherent interaction between electrons and photons allowing, for example, the optimization of quantum cascade detectors operating in the regime of strongly non-perturbative coupling with light.

Multiphoton excitation and high harmonic generation in rectangular graphene quantum dot

The multiphoton excitation and high harmonic generation (HHG) processes are considered using the microscopic quantum theory of nonlinear interaction of strong coherent electromagnetic (EM) radiation with rectangular graphene quantum dot (RGQD). The dynamic Hartree–Fock approximation is developed for the consideration of the quantum dot-laser field nonlinear interaction at the nonadiabatic multiphoton excitation regime. The many-body Coulomb interaction is described in the extended Hubbard approximation. By numerical results, we show the significance of the RGQD lateral size, shape, and EM wavefield orientation in RGQD of the zigzag edge compear to the armchair edge in the HHG process allowing for increasing the cutoff photon energy and the quantum yield of higher harmonics. The differences via edge on the elongated side of the RGQD have been explained by the investigation of the dipole momentum in both cases. Numerical results have shown that the HHG spectra have a strong anisotropy depending on the orientation of the laser wave, and the cutoff photon energy shifts toward blue with an increase in the transverse size of the RGQD.

High harmonic generation with many-body Coulomb interaction in rectangular graphene quantum dots of armchair edge

High harmonic generation (HHG) in graphene quantum dots of armchair edge by strong coherent electromagnetic radiation taking into account collective electron-electron scattering as well in such nanosystems is considered. The microscopic quantum theory describing the plane quantum dot-laser field nonlinear interaction within the dynamic Hartree–Fock approximation is developed. The many-body Coulomb interaction is considered in the extended Hubbard approximation. The obtained results indicate the significance of the nanostructure lateral size, shape, and bandgap width in HHG process that allows to increase in the quantum yield of high-order harmonics and the cutoff photon energy.

Cavity-induced exciton localization and polariton blockade in two-dimensional semiconductors coupled to an electromagnetic resonator

Recent experiments have demonstrated strong light-matter coupling between electromagnetic nanoresonators and pristine sheets of two-dimensional semiconductors, and it has been speculated whether these systems can enter the quantum regime operating at the few-polariton level. To address this question, we present a first-principles microscopic quantum theory for the interaction between excitons in an infinite sheet of two-dimensional material and a localised electromagnetic resonator. We find that the light-matter interaction breaks the symmetry of the otherwise translation-invariant system and thereby effectively generates a localised exciton mode, which is coupled to an environment of residual exciton modes. This dissipative coupling increases with tighter lateral confinement, and our analysis reveals this to be a potential challenge in realising nonlinear exciton-exciton interaction. Nonetheless, we predict that polariton blockade due to nonlinear exciton-exciton interactions is well within reach for nanoresonators coupled to transition-metal dichalcogenides, provided that the lateral resonator mode confinement can be sufficiently small that the nonlinearity overcomes the polariton dephasing caused by phonon interactions.

Quantum theory of two-dimensional materials coupled to electromagnetic resonators

We present a microscopic quantum theory of light-matter interaction in pristine sheets of two-dimensional semiconductors coupled to localized electromagnetic resonators such as optical nanocavities or plasmonic particles. The light-matter interaction breaks the translation symmetry of excitons in the two-dimensional lattice, and we find that this symmetry-breaking interaction leads to the formation of a localized exciton state, which mimics the spatial distribution of the electromagnetic field of the resonator. The localized exciton state is in turn coupled to an environment of residual exciton states. We quantify the influence of the environment and find that it is most pronounced for small lateral confinement length scales of the electromagnetic field in the resonator, and that environmental effects can be neglected if this length scale is sufficiently large. The microscopic theory provides a physically appealing derivation of the coupled-oscillator models widely used to model experiments on these types of systems, in which all observable quantities are directly derived from the material parameters and the properties of the resonant electromagnetic field. As a consistency check, we show that the theory recovers the results of semiclassical electromagnetic calculations and experimental measurements of the excitonic dielectric response in the linear excitation limit. The theory, however, is not limited to linear response, and in general describes nonlinear exciton-exciton interactions in the localized exciton state, thereby providing a powerful means of investigating the nonlinear optical response of such systems.

Quantum Susceptibilities in Time‐Domain Sampling of Electric Field Fluctuations

AbstractElectro‐optic sampling has emerged as a new quantum technique enabling measurements of electric field fluctuations on subcycle time scales. In a second‐order nonlinear material, the fluctuations of a terahertz field are imprinted onto the polarization properties of an ultrashort probe pulse in the near infrared. The statistics of this time‐domain signal are calculated, incorporating the quantum nature of the involved electric fields right from the beginning. A microscopic quantum theory of the electro‐optic process is developed adopting an ensemble of noninteracting three‐level systems as a model for the nonlinear material. It is found that the response of the nonlinear medium can be separated into a conventional part, which is exploited also in sampling of coherent amplitudes, and quantum contributions, which are independent of the state of the terahertz input. Interactions between the three‐level systems which are mediated by terahertz vacuum fluctuations are causing this quantum response. Conditions under which the classical response serves as a good approximation of the electro‐optic process are also determined and how the statistics of the sampled terahertz field can be reconstructed from the electro‐optic signal is demonstrated. In a complementary regime, electro‐optic sampling can serve as a spectroscopic tool to study the pure quantum susceptibilities of matter.

Differential Cohomotopy implies intersecting brane observables via configuration spaces and chord diagrams

We introduce a differential refinement of Cohomotopy cohomology theory, defined on Penrose diagram spacetimes, whose cocycle spaces are unordered configuration spaces of points. First we prove that brane charge quantization in this differential 4-Cohomotopy theory implies intersecting p/(p+2)-brane moduli given by ordered configurations of points in the transversal 3-space. Then we show that the higher (co-)observables on these brane moduli, conceived as the (co-)homology of the Cohomotopy cocycle space, are given by weight systems on horizontal chord diagrams and reflect a multitude of effects expected in the microscopic quantum theory of Dp/D(p+2)-brane intersections: condensation to stacks of coincident branes and their Chan-Paton factors, BMN matrix model and fuzzy funnel states, M2-brane 3-algebras, the Hanany-Witten rules, AdS3-gravity observables, supersymmetric indices of Coulomb branches as well as gauge/gravity duality between all these. We discuss this in the context of the hypothesis that the M-theory C-field is charge-quantized in Cohomotopy theory.

Higher Harmonic Generation of Coherent Sub-THz Radiation at Lifshitz Transition in Gapped Bilayer Graphene

The microscopic quantum theory of nonlinear interaction of strong coherent electromagnetic radiation with gapped bilayer graphene is used for consideration of the high harmonic generation at low-energy photon excitation Lifshitz transition. The Liouville–von Neumann equation for the density matrix is solved numerically at the nonadiabatic multiphoton excitation regime. By numerical solutions, we examine the rates of the second and third harmonics generation at the particle-hole annihilation at Lifshitz transitions in the linearly polarized coherent electromagnetic wave. The obtained results show that the gapped bilayer graphene can serve as an effective medium for the generation of even and odd high harmonics in the sub-THz domain of frequencies.

High harmonics generation in bilayer graphene at high Fermi energies induced by coherent THz-radiation

The higher-order harmonic generation process in the nonperturbative regime at the interaction of coherent electromagnetic radiation with the AB-stacked bilayer graphene at high Fermi energies is considered. The applied coherent low-frequency radiation field in the high Fermi energy zone of electrons excludes the interband transitions enhancing high harmonic rates. The developed microscopic nonlinear quantum theory for charged carriers interaction with a strong pump wave is valid near the Dirac points of the Brillouin zone. The Liouville–von Neumann equation for the density matrix in the multiphoton excitation regime is solved both analytically and numerically. Based on the numerical solutions, we examine the rates of higher-order harmonics of the pump wave of arbitrary polarization. Obtained results show that bilayer graphene serves as an effective material for the generation of higher-order harmonics from THz to the mid-IR domain of frequencies at moderate pump wave intensities.

Circularly polarized coherent light-induced boosting of polymer solar cells photovoltaic performance

We report a microscopic quantum theory which can be used to study circularly polarized light (CPL) induced singlet to triplet conversions in polymer solar cells (PSCs). We demonstrate that by properly adjusting CPL irradiation parameters, the photo-created singlet excitons can be efficiently converted into non radiative triplet excitons. The maximum singlet–triplet conversion ratio might be reached when the incident CPL frequency is chosen in such a way that the resonant optical excitation occurs between singlet and triplet states. In addition, we also illustrate that with varying CPL oscillating strength, the singlet–triplet conversion patterns behave as the Rabi oscillations and the steadily maintained triplet excitons. The electron-lattice coupling leads to the self-trapping of the excitons, which enhances the coherence between the electron’s and hole’s spin oscillations. This study opens up a novel approach for enhancing and controlling the photovoltaic response of PSCs by an effective all-optical route.

Continuum electron giving birth to terahertz emission

The origin of terahertz (THz) generation in a gas-phase medium is still in controversy, although the THz sources have been applied across many disciplines. Herein, the THz generation in a dual-color field is investigated experimentally by precisely controlling the relative phase and polarization of dual-color lasers, where the accompanying third-harmonic generation is employed for in situ determination of the relative phase up to sub-wavelength accuracy. Joint studies with the strong approximation (SFA) theory reveal that the continuum-continuum (CC) transition within an escaped electron wave packet in the single atom gives birth to THz emission, without the necessity of considering the plasma effect. Meanwhile, we develop the analytic form from SFA-based CC description, which is able to reproduce and decompose the classical photocurrent model from the viewpoint of microscopic quantum theory, establishing the quantum-classical correspondence and bringing a novel insight into the mechanism of THz generation. Present studies leave open the possibility for probing the ultrafast dynamics of continuum electrons and a new dimension for the study of THz-related science and methodology.

High-harmonic generation at particle–hole multiphoton excitation in gapped bilayer graphene

A microscopic nonlinear quantum theory of the interaction of coherent electromagnetic radiation with gapped bilayer graphene is developed. The Liouville-von Neumann equation for the density matrix is solved numerically at the multiphoton excitation regime. The developed theory of interaction of charged carriers with the strong driving wave field is valid near the Dirac points of the Brillouin zone. We consider the harmonic generation process in the nonadiabatic regime of interaction when the Keldysh parameter is of the order of unity. On the basis of numerical solutions, we examine the rates of odd and even high harmonics at the particle–hole annihilation in the field of a strong pump wave of arbitrary polarization. The obtained results show that the gapped bilayer graphene can serve as an effective medium for the generation of even and odd high harmonics in the terahertz and far-infrared domains of frequencies.

Microscopic nonlinear quantum theory of absorption of coherent electromagnetic radiation in doped bilayer graphene

The microscopic quantum theory of nonlinear stimulated scattering of chiral particles in doped $AB$ stacked bilayer graphene on Coulomb field of charged impurities in the presence of strong coherent electromagnetic radiation is presented. The Liouville-von Neumann equation for the density matrix is solved analytically. Here the interaction of electrons with the scattering potential is taken into account as a perturbation. The absorption rate of nonlinear inverse-bremsstrahlung for a grand canonical ensemble of fermionic chiral particles is calculated using the obtained solution. The analysis of the obtained rate shows that in the terahertz and near-infrared range of frequencies there is significant absorption of incident radiation via multiphoton stimulated bremsstrahlung mechanism.

Third harmonic generation in gapped bilayer graphene

With the help of numerical simulations in microscopic nonlinear quantum theory of coherent electromagnetic radiation interaction with a gapped bilayer graphene, we find out the optimal values of pump wave intensity, graphene temperature, and energy gap induced by a constant electric field for practically significant third order harmonic coherent emission. The Liouville-von Neumann equation is treated numerically for the third harmonic generation in multiphoton excitation regime near the Dirac points of the Brillouin zone. We examine the rates of the third harmonic at the particle-hole annihilation in the field of a strong pump wave of linear polarization for practically real/optimal parameters of a considering system. The obtained results show that by choosing the optimal values of the main characteristic parameters, a gapped bilayer graphene can serve as an effective medium for generation of the third harmonic at room temperatures in the terahertz and far infrared domains.

Microscopic nonlinear quantum theory of absorption of strong electromagnetic radiation in doped graphene

Microscopic nonlinear quantum theory of absorption of strong electromagnetic radiation in doped graphene

Evolution of Temporal Coherence in Confined Exciton-Polariton Condensates.

We study the influence of spatial confinement on the second-order temporal coherence of the emission from a semiconductor microcavity in the strong coupling regime. The confinement, provided by etched micropillars, has a favorable impact on the temporal coherence of solid state quasicondensates that evolve in our device above threshold. By fitting the experimental data with a microscopic quantum theory based on a quantum jump approach, we scrutinize the influence of pump power and confinement and find that phonon-mediated transitions are enhanced in the case of a confined structure, in which the modes split into a discrete set. By increasing the pump power beyond the condensation threshold, temporal coherence significantly improves in devices with increased spatial confinement, as revealed in the transition from thermal to coherent statistics of the emitted light.

Excitonic transitions in highly efficient (GaIn)As/Ga(AsSb) type-II quantum-well structures

The excitonic transitions of the type-II (GaIn)As/Ga(AsSb) gain medium of a “W”-laser structure are characterized experimentally by modulation spectroscopy and analyzed using microscopic quantum theory. On the basis of the very good agreement between the measured and calculated photoreflectivity, the type-I or type-II character of the observable excitonic transitions is identified. Whereas the energetically lowest three transitions exhibit type-II character, the subsequent energetically higher transitions possess type-I character with much stronger dipole moments. Despite the type-II character, the quantum-well structure exhibits a bright luminescence.

Microscopic nonlinear relativistic quantum theory of absorption of powerful x-ray radiation in plasma

The microscopic quantum theory of plasma nonlinear interaction with the coherent shortwave electromagnetic radiation of arbitrary intensity is developed. The Liouville-von Neumann equation for the density matrix is solved analytically considering a wave field exactly and a scattering potential of plasma ions as a perturbation. With the help of this solution we calculate the nonlinear inverse-bremsstrahlung absorption rate for a grand canonical ensemble of electrons. The latter is studied in Maxwellian, as well as in degenerate quantum plasma for x-ray lasers at superhigh intensities and it is shown that one can achieve the efficient absorption coefficient in these cases.

Quantum-mechanical diffraction theory of light from a small hole: Extinction-theorem approach

In a recent paper [Phys. Rev. A 90, 043830 (2014)] it was shown that the so-called aperture response tensor is the central concept in the microscopic quantum theory of light diffraction from a small hole in a flat screen. It was further shown that the quantum mechanical theory of diffraction only requires a preknowledge of the incident field plus the electronic properties of identical screens with and without a hole. Starting from the quantum mechanical expression for the linear conductivity tensor, we study the related causal conductivity tensor paying particular attention to diamagnetic electron dynamics. Using a nonlocal-potential separation assumption, we present a calculation of the diamagnetic causal surface conductivity for a jellium quantum-well screen using a two-dimensional Hartree-Fock model. In the diamagnetic case the difference between the light-unperturbed electron densities for screens with $({n}^{0})$ and without $({n}_{\ensuremath{\infty}}^{0})$ holes are the primary quantities for the diffraction theory. In a central part (Sec. IV) of this article we determine ${n}^{0}$ via a quantum-mechanical two-dimensional extinction-theorem approach related to elastic electron scattering from a hole with an electronic selvedge. For heuristic purposes we illustrate aspects of the extinction-theorem theory by applying the approach for an infinitely high potential barrier to the vacuum hole. Finally, we calculate and discuss the aperture response tensor in the small hole limit and in the zeroth-order Born approximation. Our final result for the aperture response tensor establishes the bridge to the anisotropic electric dipole polarizability tensor of the hole. It turns out that the effective optical aperture (hole) size relates closely to the extension of the relevant electronic wave functions scattered from the hole.

Novel type-II material system for laser applications in the near-infrared regime.

The design and experimental realization of a type-II "W"-multiple quantum well heterostructure for emission in the λ > 1.2 μm range is presented. The experimental photoluminescence spectra for different excitation intensities are analyzed using microscopic quantum theory. On the basis of the good theory-experiment agreement, the gain properties of the system are computed using the semiconductor Bloch equations. Gain values comparable to those of type-I systems are obtained.