arXiv subjects

Manuel Katzer

Publications and source records attributed to Manuel Katzer.

13 recordsLinked to original sources

arXiv2023

Fermionic vs. bosonic thermalization in the phonon-driven exciton dynamics: An analytic dimensionality study

Excitons are compound particles formed from an electron and a hole in semiconductors. The impact of this substructure on the phonon-exciton interaction is described by a closed system of microscopic scattering equations. To calculate the actual excitonic thermalization properties beyond the pure bosonic picture, this equation is derived directly from an electron-hole picture within the Heisenberg equation of motion framework. In addition to the well-known bosonic character of the compound particles, we identified processes of a repulsive, fermionic type, as well as attractive carrier exchange contributing to the scattering process. In this analytical study we give general statements about the thermalization of excitons in two and three dimensional semiconductors. We give insights on the strong dependence of the thermalization characteristics of the exciton Bohr radius and the thermalization wavelength. Above all, we analytically provide arguments why a bosonic behavior of excitons - such as an enhanced ground state occupation - requires the dominant phonon scattering to be quasielastic. Acoustic phonons tend to fulfil this, as each scattering event only takes small amounts of energy out of the distribution, while optical phonons tend to prevent macroscopic occupations of the lowest exciton state, since the Pauli repulsion between the individual carriers will then dominate the thermalization dynamics.

cond-mat.mes-hall↗

arXiv2023

Time-domain observation of interlayer exciton formation and thermalization in a MoSe$_2$/WSe$_2$ heterostructure

Vertical heterostructures (HS) of transition metal dichalcogenides (TMDs) host interlayer excitons (ILX), with electrons and holes residing in different layers. With respect to their intralayer counterparts, ILX feature much longer lifetimes and diffusion lengths, paving the way to excitonic optoelectronic devices operating at room temperature. While the recombination dynamics of ILX has been intensively studied, the formation process and its underlying physical mechanisms are still largely unexplored. Here we use ultrafast transient absorption spectroscopy with a white-light probe, spanning both intralayer and interlayer exciton resonances, to simultaneously capture and time-resolve interlayer charge transfer and ILX formation dynamics in a MoSe$_2$/WSe$_2$ HS. We find that the ILX formation timescale is nearly an order of magnitude (~1 ps) longer than the interlayer charge transfer time (~100 fs). Microscopic calculations attribute the relative delay to an interplay between a phonon-assisted interlayer exciton cascade and subsequent cooling processes, and excitonic wave-function overlap. Our results provide an explanation to the efficient photocurrent generation observed in optoelectronic devices based on TMD HS, as the ILX have an opportunity to dissociate during their thermalization process.

cond-mat.mtrl-sci↗

arXiv2023

Exciton-phonon-scattering: A competition between bosonic and fermionic nature of bound electron-hole pairs

The question of macroscopic occupation and spontaneous emergence of coherence for exciton ensembles has gained renewed attention due to the rise of van der Waals heterostructures made of atomically thin semiconductors. The hosted interlayer excitons exhibit nanosecond lifetimes, long enough to allow for excitonic thermalization in time. Several experimental studies reported signatures of macroscopic occupation effects at elevated exciton densities. With respect to theory, excitons are composite particles formed by fermionic constituents, and a general theoretical argument for a bosonic thermalization of an exciton gas beyond the linear regime is still missing. Here, we derive an equation for the phonon mediated thermalization at densities above the classical limit, and identify which conditions favor the thermalization of fermionic or bosonic character, respectively. In cases where acoustic, quasielastic phonon scattering dominates the dynamics, our theory suggests that transition metal dichalcogenide (TMDC) excitons might be bosonic enough to show bosonic thermalization behaviour and decreasing dephasing for increasing exciton densities. This can be interpreted as a signature of an emerging coherence in the exciton ground state, and agrees well with the experimentally observed features, such as a decreasing linewidth for increasing densities.

cond-mat.mes-hall↗

arXiv2023

Extended spatial coherence of interlayer excitons in MoSe$_2$/WSe$_2$ heterobilayers

We report on the spatial coherence of interlayer exciton ensembles as formed in MoSe$_2$/WSe$_2$ heterostructures and characterized by point-inversion Michelson-Morley interferometry. Below 10 K, the measured spatial coherence length of the interlayer excitons reaches values equivalent to the lateral expansion of the exciton ensembles. In this regime, the light emission of the excitons turns out to be homogeneously broadened in energy with a high temporal coherence. At higher temperatures, both the spatial coherence length and the temporal coherence time decrease, most likely because of thermal processes. The presented findings point towards a spatially extended, coherent many-body state of interlayer excitons at low temperature.

cond-mat.mes-hall↗

arXiv2023

Suppression and amplification of phonon sidebands in transition metal dichalcogenides by optical feedback

Transition metal dichalcogenides (TMDCs) combine both strong light-matter-interaction and strong Coulomb-interaction for the formation of optically excitable excitons. Through radiative feedback control, a mechanism to control the linewidth can be applied, which modifies optical transition spectra. Here, we extend these investigations to the absorption spectra of TMDCs in a variety of geometries with respect to non-Markovian exciton-phonon-scattering contributions. Our approach is based on the self consistent solution of the microscopic Bloch equations and the macroscopic solution of the wave equation. We discuss the formation of a phonon sideband for MoSe$_2$ embedded in SiO$_2$, and two setups for enhancing or suppressing the phonon sideband in the spectrum.

cond-mat.mtrl-sci↗

arXiv2023

Impact of dark excitons on F\"orster type resonant energy transfer between dye molecules and atomically thin semiconductors

Interfaces of dye molecules and two-dimensional transition metal dichalcogenides (TMDCs) combine strong molecular dipole excitations with high carrier mobilities in semiconductors. F\"orster type energy transfer is one key mechanism for the coupling between both constituents. We report microscopic calculations of a spectrally resolved F\"orster induced transition rate from dye molecules to a TMDC layer. Our approach is based on microscopic Bloch equations which are solved self-consistently together with Maxwells equations. This approach allows to incorporate the dielectric environment of a TMDC semiconductor, sandwiched between donor molecules and a substrate. Our analysis reveals transfer rates in the meV range for typical dye molecules in closely stacked structures, with a non-trivial dependence of the F\"orster rate on the molecular transition energy resulting from unique signatures of dark, momentum forbidden TMDC excitons.

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↗

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↗

arXiv2020

Non-equilibrium non-Markovian steady-states in open quantum many-body systems: Persistent oscillations in Heisenberg quantum spin chains

We investigate the effect of a non-Markovian, structured reservoir on an open Heisenberg spin chain. We establish a coherent self-feedback mechanism as the reservoir couples frequency-dependent to the spin chain. Thus, loss and driving take place due to the interaction of the spin chain with its own past. This new paradigm of non-Markovian imposed boundary-driving allows to discuss a new kind of non-equilibrium steady-state. We show that for certain parameters even in the long-time limit persistent oscillations occur within the chain. Moreover, we demonstrate that the conditions for these oscillations and excitation trapping depend on the characteristics of the chain, thus making it possible to characterize a chain by detection of its emitted signal under influence of self-feedback.

quant-ph↗

arXiv2020

Long-range interaction in an open boundary-driven Heisenberg spin lattice: A far-from-equilibrium transition to ballistic transport

We study an open Heisenberg XXZ spin chain with long-range Ising-type interaction, which is incoherently driven at its boundaries and therefore a far-from-equilibrium steady state current is induced. Quantum Monte Carlo techniques make a regime accessible, where the system size is large enough to examine the transition from a diffusive to a ballistic transport regime. We find that the chain lengths for this transition are increasing with decreasing range of the Ising-type interactions between distant spins, while the strength of the incoherent driving does not have a relevant effect on the transport transition. The transition can be explained by the suppression of ferromagnetic domains at the edges of the chain.

quant-ph↗

arXiv2017

Quantum cascade driving: Dissipatively mediated coherences

Quantum cascaded systems offer the possibility to manipulate a target system with the quantum state of a source system. Here, we study in detail the differences between a direct quantum cascade and coherent/incoherent driving for the case of two coupled cavity-QED systems. We discuss qualitative differences between these excitations scenarios, which are particular strong for higher-order photon-photon correlations: $g^{(n)}(0)$ with $ n>2 $. Quantum cascaded systems show a behavior differing from the idealized cases of individual coherent/incoherent driving and allow to produce qualitatively different quantum statistics. Furthermore, the quantum cascaded driving exhibits an interesting mixture of quantum coherent and incoherent excitation dynamics. We develop a measure, where the two regimes intermix and quantify these differences via experimentally accessible higher-order photon correlations.

quant-ph↗