arXiv subjects

Andreas Knorr

Publications and source records attributed to Andreas Knorr.

At least 55 records · Page 3Linked to original sources

arXiv2022

Heisenberg treatment of multiphoton pulses in waveguide QED with time-delayed feedback

The dynamics of waveguide-QED systems involving coherent time-delayed feedback give rise to a hierarchy of multi-time correlations within the Heisenberg picture due to the induced non-Markovianity. We propose to perform a projection onto a complete set of states in the Hilbert space to decompose the multi-time correlations into single-time matrix elements. To illustrate the procedure, we consider the paradigmatic example of a two-level system that couples to a semi-infinite waveguide and interacts with quantum light pulses. Our approach complements the range of available methods as it allows calculating the dynamics under the inclusion of additional dissipation channels in a numerically exact and efficient manner for multiphoton pulses of arbitrary shape where memory requirements are known in advance.

quant-ph↗

arXiv2022

Observation of ultrafast interfacial Meitner-Auger energy transfer in a van der Waals heterostructure

Atomically thin layered van der Waals heterostructures feature exotic and emergent optoelectronic properties. With growing interest in these novel quantum materials, the microscopic understanding of fundamental interfacial coupling mechanisms is of capital importance. Here, using multidimensional photoemission spectroscopy, we provide a layer- and momentum-resolved view on ultrafast interlayer electron and energy transfer in a monolayer-WSe$_2$/graphene heterostructure. Depending on the nature of the optically prepared state, we find the different dominating transfer mechanisms: while electron injection from graphene to WSe$_2$ is observed after photoexcitation of quasi-free hot carriers in the graphene layer, we establish an interfacial Meitner-Auger energy transfer process following the excitation of excitons in WSe$_2$. By analysing the time-energy-momentum distributions of excited-state carriers with a rate-equation model, we distinguish these two types of interfacial dynamics and identify the ultrafast conversion of excitons in WSe$_2$ to valence band transitions in graphene. Microscopic calculations find interfacial dipole-monopole coupling underlying the Meitner-Auger energy transfer to dominate over conventional Förster- and Dexter-type interactions, in agreement with the experimental observations. The energy transfer mechanism revealed here might enable new hot-carrier-based device concepts with van der Waals heterostructures.

cond-mat.mtrl-sci↗

arXiv2022

Efficient high-harmonic generation in graphene with two-color laser field at orthogonal polarization

High-order frequency mixing in graphene using a two-color radiation field consisting of the fundamental and the second harmonic fields of an ultrashort linearly polarized laser pulse is studied. It is shown that the harmonics originated from the interband transitions are efficiently generated in the case of the orthogonally polarized two-color field. In this case, the generated high-harmonics are stronger than those obtained in the parallel polarization case by more than two orders of magnitude. This is in sharp contrast with the atomic and semiconductor systems, where parallel polarization case is more preferable. The physical origin of this enhancement is also deduced from the three-step semi-classical electron-hole collision model, extended to graphene with pseudo-relativistic energy dispersion. In particular, we discuss the influence of the many particle Coulomb interaction on the HHG process within dynamical Hartree-Fock approximation. Our analysis shows that in all cases we have an overall enhancement of the HHG signal compared with the free-charged carrier model due to the electron-hole attractive interaction.

cond-mat.mes-hall↗

arXiv2022

Terahertz control of photoluminescence emission in few-layer InSe

A promising route for the development of opto-elelctronic technology is to use terahertz radiation to modulate the optical properties of semiconductors. Here we demonstrate the dynamical control of photoluminescence (PL) emission in few-layer InSe using picosecond terahertz pulses. We observe a strong PL quenching (up to 50%) after the arrival of the terahertz pulse followed by a reversible recovery of the emission on the time scale of 50ps at T =10K. Microscopic calculations reveal that the origin of the photoluminescence quenching is the terahertz absorption by photo-excited carriers: this leads to a heating of the carriers and a broadening of their distribution, which reduces the probability of bimolecular electron-hole recombination and, therefore, the luminescence. By numerically evaluating the Boltzmann equation, we are able to clarify the individual roles of optical and acoustic phonons in the subsequent cooling process. The same PL quenchingmechanismis expected in other van derWaals semiconductors and the effectwill be particularly strong for materials with low carrier masses and long carrier relaxation time, which is the case for InSe. This work gives a solid background for the development of opto-electronic applications based on InSe, such as THz detectors and optical modulators.

cond-mat.mtrl-sci↗

arXiv2022

Impact of optically pumped non-equilibrium steady states on luminescence emission of atomically-thin semiconductor excitons

The interplay of the non-equivalent corners in the Brillouin zone of transition metal dichalcogenides have been investigated extensively. While experimental and theoretical works contributed to a detailed understanding of the relaxation of selective optical excitations and the related relaxation rates, only limited microscopic descriptions of stationary experiments are available so far. In this manuscript we present microscopic calculations for the non-equilibrium steady state properties of excitons during continuous wave pumping. We find sharp features in photoluminescence excitation spectra and degree of polarization which result from phonon assisted excitonic transitions dominating over exciton recombination and intervalley exchange coupling.

cond-mat.mes-hall↗

arXiv2022

Excitonic theory of doping-dependent optical response in atomically thin semiconductors

The interaction of optically excited excitons in atomically thin semiconductors with residual doping densities leads to many-body effects which are continuously tunable by external gate voltages. Here, we develop a fully microscopic theory to describe the doping-dependent manipulation of the excitonic properties in atomically thin transition metal dichalcogenides. In particular, we establish a diagonalization approach for the Schrödinger equation which characterizes the interaction of a virtual exciton with the Fermi sea of dopants. Solving this many-body Schrödinger equation provides access to trions as well as a continuum of scattering states. The dynamics of coupled excitons, trions, and scattering continua is subsequently described by Heisenberg equations of motion including mean-field contributions and correlation effects due to the interaction of excitons with trions and scattering continuum states. Our calculations for optical excitation close to the band edge reveal the influence of doping on the exciton resonances in combination with the simultaneous identification of not only ground-, but also excited-, state trion resonances.

cond-mat.mes-hall↗

arXiv2022

Doping-induced non-Markovian interference causes excitonic linewidth broadening in monolayer WSe$_2$

Strong Coulomb interactions in atomically thin semiconductors like monolayer WSe$_2$ induce not only tightly bound excitons, but also make their optical properties very sensible to doping. By utilizing a microscopic theory based on the excitonic Heisenberg equations of motion, we systematically determine the influence of doping on the excitonic linewidth, lineshift, and oscillator strength. We calculate trion resonances and demonstrate that the Coulomb coupling of excitons to the trionic continuum generates a non-Markovian interference, which, due to a time retardation, builds up a phase responsible for asymmetric exciton line shapes and increased excitonic linewidths. Our calculated doping dependence of exciton and trion linewidths, lineshifts, and oscillator strengths explains recent experiments. The gained insights provide the microscopic origin of the optical fingerprint of doped atomically thin semiconductors.

cond-mat.mes-hall↗

arXiv2021

Excitonic insulator states in molecular functionalized atomically-thin semiconductors

The excitonic insulator is an elusive electronic phase exhibiting a correlated excitonic ground state. Materials with such a phase are expected to have intriguing properties such as excitonic high-temperature superconductivity. However, compelling evidence on the experimental realization is still missing. Here, we theoretically propose hybrids of two-dimensional semiconductors functionalized by organic molecules as prototypes of excitonic insulators, with the exemplary candidate WS$_2$-F6TCNNQ. This material system exhibits an excitonic insulating phase at room temperature with a ground state formed by a condensate of interlayer excitons. To address an experimentally relevant situation, we calculate the corresponding phase diagram for the important parameters: temperature, gap energy, and dielectric environment. Further, to guide future experimental detection, we show how to optically characterize the different electronic phases via far-infrared to terahertz (THz) spectroscopy.

cond-mat.str-el↗

arXiv2021

Interlayer exciton valley polarization dynamics in large magnetic fields

In van der Waals heterostructures (HS) consisting of stacked MoSe$_2$ and WSe$_2$ monolayers, optically bright interlayer excitons (ILE) can be observed when the constituent layers are crystallographically aligned. The symmetry of the monolayers allows for two different types of alignment, in which the momentum-direct interlayer transitions are either valley-conserving (R-type alignment) or changing the valley index (H-type anti-alignment). Here, we study the valley polarization dynamics of ILE in magnetic fields up to 30~Tesla by time-resolved photoluminescence (PL). For all ILE types, we find a finite initial PL circular degree of polarization ($DoP$) after unpolarized excitation in applied magnetic fields. For ILE in H-type HS, we observe a systematic increase of the PL $DoP$ with time in applied magnetic fields, which saturates at values close to unity for the largest fields. By contrast, for ILE in R-type HS, the PL $DoP$ shows a decrease and a zero crossing before saturating with opposite polarization. This unintuitive behavior can be explained by a model considering the different ILE states in H- and R-type HS and their selection rules coupling PL helicity and valley polarization.

cond-mat.mes-hall↗

arXiv2021

Optical dipole orientation of interlayer excitons in MoSe$_{2}$-WSe$_{2}$ heterostacks

We report on the far-field photoluminescence intensity distribution of interlayer excitons in MoSe$_{2}$-WSe$_{2}$ heterostacks as measured by back focal plane imaging in the temperature range between 1.7 K and 20 K. By comparing the data with an analytical model describing the dipolar emission pattern in a dielectric environment, we are able to obtain the relative contributions of the in- and out-of-plane transition dipole moments associated to the interlayer exciton photon emission. We determine the transition dipole moments for all observed interlayer exciton transitions to be (99 $\pm$ 1)% in-plane for R- and H-type stacking, independent of the excitation power and therefore the density of the exciton ensemble in the experimentally examined range. Finally, we discuss the limitations of the presented measurement technique to observe correlation effects in exciton ensembles.

cond-mat.mes-hall↗

arXiv2021

Strong coupling regime and hybrid quasinormal modes of a single plasmonic resonator coupled to a TMDC monolayer

We present a rigorous photonic mode model to describe the strong coupling between a monolayer of $\rm MoSe_2$ and a single gold nanoparticle. The onset of strong coupling is quantified by computing the three-dimensional hybrid quasinormal modes of the combined structure, allowing one to accurately model light-matter interactions without invoking the usual phenomenological theories of strong coupling. We explore the hybrid quasinormal modes as a function of gap size and temperature and find spectral splittings in the range of around 80-110 meV, with no fitting parameters for the material models. We also show how the hybrid modes exhibit Fano-like resonances and quantify the complex poles of the hybrid modes as well as the Purcell factor resonances from embedded dipole emitters. These effects cannot be described with the usual heuristic normal mode theories.

physics.optics↗

arXiv2021

Direct measurement of key exciton properties: energy, dynamics and spatial distribution of the wave function

Excitons, Coulomb-bound electron-hole pairs, are the fundamental excitations governing the optoelectronic properties of semiconductors. While optical signatures of excitons have been studied extensively, experimental access to the excitonic wave function itself has been elusive. Using multidimensional photoemission spectroscopy, we present a momentum-, energy- and time-resolved perspective on excitons in the layered semiconductor WSe$_2$. By tuning the excitation wavelength, we determine the energy-momentum signature of bright exciton formation and its difference from conventional single-particle excited states. The multidimensional data allows to retrieve fundamental exciton properties like the binding energy and the exciton-lattice coupling and to reconstruct the real-space excitonic distribution function via Fourier transform. All quantities are in excellent agreement with microscopic calculations. Our approach provides a full characterization of the exciton properties and is applicable to bright and dark excitons in semiconducting materials, heterostructures and devices.

cond-mat.mtrl-sci↗

arXiv2021

Fermi's golden rule for spontaneous emission in absorptive and amplifying media

We demonstrate a fundamental breakdown of the photonic spontaneous emission (SE) formula derived from Fermi's golden rule, in absorptive and amplifying media, where one assumes the SE rate scales with the local photon density of states, an approach often used in more complex, semiclassical nanophotonics simulations. Using a rigorous quantization of the macroscopic Maxwell equations in the presence of arbitrary linear media, we derive a corrected Fermi's golden rule and master equation for a quantum two-level system (TLS) that yields a quantum pumping term and a modified decay rate that is net positive. We show rigorous numerical results of the temporal dynamics of the TLS for an example of two coupled microdisk resonators, forming a gain-loss medium, and demonstrate the clear failure of the commonly adopted formulas based solely on the local density of states.

physics.optics↗

arXiv2021

Continuous and time-discrete non-Markovian system-reservoir interactions: Dissipative coherent quantum feedback in Liouville space

Based on tensor network realizations of path integrals reducing exponential memory scaling to polynomial efficiency and a Liouville space implementation of a time-discrete quantum memory, we investigate a quantum system simultaneously exposed to two structured reservoirs. For this purpose, we employ a numerically exact quasi-2D tensor network combining both diagonal and off-diagonal system-reservoir interactions with a twofold memory for continuous and discrete retardation effects. As a possible example, we study the non-Markovian dynamical interplay between discrete photonic feedback and structured acoustic phonon modes, resulting in emerging inter-reservoir correlations and long-living population trapping within an initially-excited two-level system.

quant-ph↗

arXiv2021

Strongly entangled system-reservoir dynamics with multiphoton pulses beyond the two-excitation limit: Exciting the atom-photon bound state

Within the matrix product state framework, we study the non-Markovian feedback dynamics of a two-level system interacting with the electromagnetic field inside a semi-infinite waveguide where the excitation of an atom-photon bound state is possible. Taking the steady-state excitation of the emitter as a figure of merit, we compare the trapped excitation for an initially excited quantum emitter and an emitter prepared via quantized pulses containing up to four photons. In the latter case, we find that for large feedback delay times, multi-photon pulses can yield a significantly higher steady-state excitation than possible with an initially excited emitter since the stimulated emission process can enhance the trapping probability in comparison to the spontaneous decay of an initially excited emitter.

quant-ph↗

arXiv2020

Unidirectional Quantum Transport in Optically Driven $V$-type Quantum Dot Chains

We predict a mechanism for achieving complete population inversion in a continuously driven InAs/GaAs semiconductor quantum dot featuring $V$-type transitions. This highly nonequilibrium steady state is enabled by the interplay between $V$-type interband transitions and a non-Markovian decoherence mechanism, introduced by acoustic phonons. The population trapping mechanism is generalized to a chain of coupled emitters. Exploiting the population inversion, we predict unidirectional excitation transport from one end of the chain to the other without external bias, independent of the unitary interdot coupling mechanism.

quant-ph↗

arXiv2020

Theory of the Coherent Response of Magneto-Excitons and Magneto-Biexcitons in Monolayer Transition Metal Dichalcogenides

The recent accessibility of high quality, charge neutral monolayer transition metal dichalcogenides with narrow exciton linewidths at the homogeneous limit provides an ideal platform to study excitonic many-body interactions. In particular, the possibility to manipulate coherent exciton-exciton interactions, which govern the ultrafast nonlinear optical response, by applying an external magnetic field has not been considered so far. We address this discrepancy by presenting a nonlinear microscopic theory in the coherent limit for optical excitations in the presence of out-of-plane, in-plane, and tilted magnetic fields. Specifically, we explore the magnetic-field-induced exciton and biexciton fine structure and calculate their oscillator strengths based on a Heisenberg equations of motion formalism. Our microscopic evaluations of pump-probe spectra allow to interpret and predict coherent signatures in future wave-mixing experiments.

cond-mat.mes-hall↗

arXiv2020

Quantized quasinormal mode description of non-linear cavity QED effects from coupled resonators with a Fano-like resonance

We employ a recently developed quantization scheme for quasinormal modes (QNMs) to study a nonperturbative open cavity-QED system consisting of a hybrid metal-dielectric resonator coupled to a quantum emitter. This hybrid cavity system allows one to explore the complex coupling between a low $Q$ (quality factor) resonance and a high $Q$ resonance, manifesting in a striking Fano resonance, an effect that is not captured by traditional quantization schemes using normal modes or a Jaynes-Cummings (JC) type model. The QNM quantization approach rigorously includes dissipative coupling between the QNMs, and is supplemented with generalized input-output relations for the output electric field operator for multiple modes in the system, and correlation functions outside the system. The role of the dissipation-induced mode coupling is explored in the strong coupling regime between the photons and emitter beyond the first rung of the JC dressed-state ladder. Important differences in the quantum master equation and input-output relations between the QNM quantum model and phenomenological dissipative JC models are found. In a second step, numerical results for the Fock distributions and system as well as output correlation functions obtained from the quantized QNM model for the hybrid structure are compared with results from a phenomenological approach. We demonstrate explicitly how the quantized QNM model manifests in multiphoton quantum correlations beyond what is predicted by the usual JC models.

cond-mat.mes-hall↗