arXiv subjects

Alexander Steinhoff

Publications and source records attributed to Alexander Steinhoff.

At least 19 recordsLinked to original sources

arXiv2026

Anisotropic nanoscale coherent polariton transport in CrSBr

In a combined experimental and theoretical study, we demonstrate anisotropic polariton transport on the nanoscale in the van der Waals antiferromagnet CrSBr. While effective cavity-polariton formation emerges via the self-hybridization of ultra-high oscillator strength excitons with a thin slab photonic mode, the absence of external mirrors facilitates spectroscopic investigation of these polaritons via cathodoluminescence (CL) on length scales determined by the electron wavelength. This direct access allows us to perform precise charting of the polariton landscape with nanometric resolution, and to probe polariton interference phenomena. The main finding of the work highlights that the coherent polariton transport follows the $C_{2v}$ symmetry of CrSBr, allowing exclusive transport along the crystallographic a-axis, while no coherent feature is found along the b-axis direction. Our work sets the foundation to use CL spectroscopy in cavity-polaritonics in more advanced landscapes, such as photonic crystals or optical lattices, and establishes the technique as a powerful tool to probe anisotropic expansion and relaxation phenomena on the nanoscale

cond-mat.mtrl-sci↗

arXiv2026

Effective long-range attraction of moir\'e excitons under the influence of atomic reconstructions and anisotropic screening

The moir\'e pattern, which emerges due to a relative rotation between two monolayers of transition metal dichalcogenides, features a long lattice period for small twist angles. The resulting band structure modulation acts as an effective potential for interlayer excitons (IXs), which can realize correlated many-body phenomena. Here, we aim for a material-realistic modelling of the exciton-exciton interaction, taking into account lattice reconstructions and an exciton-exciton potential that incorporates the highly anisotropic screening imposed by the two-dimensional bilayer and the dielectric background. We find strong modifications of the on-site interaction induced by the change of the moir\'e potential during lattice reconstructions, while for long-range interactions on the length scale of the moir\'e period, anisotropic dielectric screening leads to a crossover from a repulsive to an attractive interaction. The interaction potential and hopping amplitudes serve as parameters for a Bose-Hubbard model on the moir\'e lattice, which we use to explain correlated behavior of interlayer excitons.

cond-mat.mtrl-sci↗

arXiv2025

Scalable Quantum Photonic Platform Based on Site-Controlled Quantum Dots Coupled to Circular Bragg Grating Resonators

The scalable integration of solid-state quantum emitters into photonic nanostructures remains a central challenge for quantum photonic technologies. Here, we demonstrate a robust and streamlined integration strategy that tackles the long-standing issue of deterministic fabrication on randomly positioned self-assembled quantum dots (QDs), leveraging a buried-stressor-based site-controlled InGaAs QD platform. We show that this deterministic growth approach enables precise spatial alignment with circular Bragg grating (CBG) resonators for enhanced emission, eliminating the need for complex and time-consuming deterministic lithography techniques. We fabricated a $6\times6$ SCQD-CBG array with 100\% device yield, with 35 devices falling within the radial-offset range where the simulated photon-extraction efficiency (PEE) exceeds 20\%, underscoring the spatial precision and scalability of our fabrication concept. A systematically selected subset of five devices with varying radial displacements reveals clear offset-dependent trends in extraction efficiency, spectral linewidth, and photon indistinguishability, thereby establishing quantitative bounds on spatial alignment tolerances. In the best-aligned QD-CBG device, we achieve a PEE of $(47.1\pm3.8)\%$, a linewidth of $(1.41\pm0.22)$ GHz, a radiative decay lifetime of $(0.80\pm0.02)$~ns, a single-photon purity of $(99.58\pm0.18)\%$, and a Hong-Ou-Mandel two-photon interference visibility of $(81\pm5)\%$ under quasi-resonant excitation at saturation power. We confirm our conceptual understanding of the effect of emitter-position dependent charge-noise fluctuations in terms of a quantum-optical model for the (quantum-)emission properties.

cond-mat.mes-hall↗

arXiv2025

Tunable WS$_2$ Micro-Dome Open Cavity Single Photon Source

Versatile, tunable, and potentially scalable single-photon sources are a key asset in emergent photonic quantum technologies. In this work, a single-photon source based on WS$_2$ micro-domes, created via hydrogen ion irradiation, is realized and integrated into an open, tunable optical microcavity. Single-photon emission from the coupled emitter-cavity system is verified via the second-order correlation measurement, revealing a $g^{(2)}(\tau=0)$ value of 0.3. A detailed analysis of the spectrally selective, cavity enhanced emission features shows the impact of a pronounced acoustic phonon emission sideband, which contributes specifically to the non-resonant emitter-cavity coupling in this system. The achieved level of cavity-emitter control highlights the potential of open-cavity systems to tailor the emission properties of atomically thin quantum emitters, advancing their suitability for real-world quantum technology applications.

quant-ph↗

arXiv2025

Rabi oscillations of a monolayer quantum emitter driven through its excited state

The interaction of a quantum two-level system with a resonant driving field results in the emergence of Rabi oscillations, which are the hallmark of a controlled manipulation of a quantum state on the Bloch sphere. This all-optical coherent control of solid-state two-level systems is crucial for quantum applications. In this work we study Rabi oscillations emerging in a WSe2 monolayer-based quantum dot. The emitter is driven coherently using picosecond laser pulses to a higher-energy state, while photoluminescence is probed from the ground state. The theoretical treatment based on a three-level exciton model reveals the population transfer between the exciton ground and excited states coupled by Coulomb interaction. Our calculations demonstrate that the resulting exciton ground state population can be controlled by varying driving pulse area and detuning which is evidenced by the experimental data. Our results pave the way towards the coherent control of quantum emitters in atomically thin semiconductors, a crucial ingredient for monolayer-based high-performance, on-demand single photon sources.

cond-mat.mes-hall↗

arXiv2025

Tuning the non-linear interactions of hybrid interlayer excitons in bilayer MoS2 via electric fields

Hybrid interlayer excitons in bilayer MoS2 are a promising platform for nonlinear optics due to their intrinsic dipolar character, which combines in-plane and out-ofplane dipole moments. In this work, we directly probe the nonlinear exciton-exciton interactions of hybrid interlayer excitons. By applying an external out-of-plane electric field, we polarize the excitons to enhance their mutual dipolar interactions, thereby deliberately favoring these repulsive contributions over competing attractive manybody corrections. We furthermore establish a fully microscopic theoretical description of these effects to explain the core experimental results. The tuning results in a significantly larger blueshift compared to the zero-field case and perspectively opens an avenue to even switch between repulsive and attractive interaction potentials. Our findings establish that strong nonlinearities can be tuned via an external electric field, providing a new degree of control over exciton interactions beyond density tuning alone.

cond-mat.mtrl-sci↗

arXiv2025

Electronic localization and optical activity of strain-engineered transition-metal dichalcogenide nanobubbles

Strain-engineered transition-metal dichalcogenide nanobubbles are promising platforms for quantum emission, as revealed by recent experimental observations. In this work, we present an \textit{ab initio} investigation of MoS$_2$, WS$_2$, MoSe$_2$, and WSe$_2$ nanobubbles, linking their structural and electronic properties to predictions of their optical activity. Inflating forces yield tunable geometries with non-uniform, apex-concentrated strain, which is sensitive to material rigidity. Strain modifies band gaps and universally induces non-dispersive valence states, exhibiting composition-dependent wave-function character, as revealed by an in-depth analysis of band structures and orbital contributions. Crucially, transitions from these apex-localized valence states are predominantly dark. This characteristic is attributed to their localization at the $\Gamma$-point, inhibiting transitions to the lowest unoccupied states that reside at the K-valley. While revealing that the herein considered sub-10-nm nanobubbles fall short as single-photon emitters, our findings provide essential understanding of the structure-property relations in emerging quantum materials, providing robust design rules to optimize their characteristics for novel quantum applications.

cond-mat.mes-hall↗

arXiv2025

Enhancement of Indistinguishable Photon Emission from a GaAs Quantum Dot via Charge Noise Suppression

The generation of indistinguishable single photons is a fundamental requirement for future quantum technologies, particularly in quantum repeater networks and for distributed quantum computing based on entanglement distribution. However, spectral jitter, often induced by charge noise in epitaxial quantum dots, leads to exciton dephasing, thereby limiting their practical usage in quantum applications. We present a straightforward approach to mitigate charge noise-induced decoherence in droplet-etched GaAs quantum dots embedded in an n-i-p diode structure and integrated deterministically into an electrically contacted circular Bragg grating resonator for emission enhancement. The quantum device allows for the stabilization of the charge environment by applying an external electrical field while producing a photon extraction efficiency of approximately (37 +- 2)%. Hong-Ou-Mandel two-photon interference measurements reveal a strong voltage dependence of the exciton dephasing time and interference visibility on the applied bias in excellent agreement with our theoretical predictions. Notably, the reduction in visibility from a maximum, charge-stabilized corrected value of 97 percent at the optimum bias point follows an inverse square dependence (proportional to 1/I^2) with increasing diode current (I) in forward direction. Under a quasi-resonant excitation scheme, we achieve a maximum exciton dephasing time (T2*) of approximately (6.8 +-0.5) ns, reaching nearly the Fourier limit (T2 = 2T1) without the need for complex echo schemes like Ramsey or Carr-Purcell-Meiboom-Gill sequences. These findings are consistent with theoretical predictions from rate equation modeling and quantum optical analysis as well as voltage-dependent linewidth measurements, demonstrating optimized electrical control of exciton dephasing.

cond-mat.mes-hall↗

arXiv2025

Wannier-Function-Based Approach to Coupled Exciton-Phonon-Photon Dynamics in Two-Dimensional Semiconductors

Marrying the predictive power of ab initio calculations with many-body effects remains a challenging task in two-dimensional (2d) materials, where efficient carrier-carrier interaction challenges established approximation schemes. In particular, understanding exciton-phonon interaction from first principles is a field of growing interest. Here, we present a many-body theory for coupled free-carrier, exciton, phonon and photon dynamics based on carrier-carrier and carrier-phonon interaction matrix elements obtained via projection on Wannier orbitals. The framework is applied to study the impact of carrier-phonon correlations on optical spectra and coupled nonequilibrium carrier-phonon kinetics in monolayer MoSe$_2$. We find that non-Markovian effects and dynamical buildup of quasi-particles are only properly described if correlations at least on the two-phonon level are included. Our studies open a perspective to advance the material-realistic description of nonequilibrium physics in 2d nanostructures to new many-body realms.

cond-mat.mes-hall↗

arXiv2025

Connection between memory performance and optical absorption in quantum reservoir computing

The fading memory property is a key requirement for reservoir computers -- a specific type of recurrent neural network with fixed internal weights. While mostly undesired in gate-based quantum computing, dissipation due to material imperfections or coupling to the environment acts as a natural mechanism intrinsically providing fading memory to reservoir computers based on dynamical open quantum systems. In this work, we unravel a connection between the physical metric of optical absorption and the performance of quantum reservoir computers in terms of their short-term memory capacity. We establish this link by considering a coherent input encoding in conjunction with tunable qubit decay, giving precise control over the fading memory in the quantum reservoir computer. Our analysis enables us to identify a sweet-spot regime for the dissipation strength at which memory performance is maximized.

quant-ph↗

arXiv2025

Impact of phonon lifetimes on the single-photon indistinguishability in quantum emitters based on 2D materials

Localized excitons in two-dimensional (2D) materials are considered as promising sources of single photons on demand. The photon indistinguishability as key figure of merit for quantum information processing is strongly influenced by the coupling of charge excitations to lattice vibrations of the surrounding semiconductor material. Here, we quantify the impact of exciton-acoustic-phonon-interaction and cavity QED effects on photon indistinguishability in a Hong-Ou-Mandel setup by solving fully quantum mechanical equations for the coupled QD-cavity-phonon system including non-Markovian effects. We find a strong reduction of indistinguishability compared to 3D systems due to increased exciton-phonon coupling efficiency. Moreover, we show that the coherence properties of photons are significantly influenced by the finite phonon lifetime in the surrounding material giving rise to pure dephasing. Only if these limitations are overcome, localized excitons in 2D semiconductors can become a new avenue for quantum light sources.

cond-mat.mes-hall↗

arXiv2024

Material-realistic modelling of quantum many-body effects in a monolayer TMDC nanolaser device

The efficient light-matter interaction in combination with the small volume occupied by monolayer transition-metal dichalcogenides (TMDCs) makes this material class a notable option as gain layer in future opto-electronic devices. Many-body effects of excited carriers influence the emission dynamics due to the introduction of optical non-linearities following excitation, but the exact mechanisms remain unexamined from a theoretical point of view. In this paper, we present a material-realistic microscopic theory of a device based on an MoS2-monolayer, which demonstrates stimulated emission activity at room temperature. The modelling procedure combines Coulomb and light-matter interaction matrix elements with doublet-level Quantum Laser Equations (QLEs). These give access to the dynamics of the photon-assisted polarisation, populations, and photon number while allowing the solution of a multi-scale problem ranging from femto- to nanoseconds. The input-output curve, hole burning and spectral clamping obtained from this theory present strong indications of electron-hole-plasma-based lasing occurring at densities above $5 \cdot 10^{13}\,\text{cm}^{-2}$ in this device.

cond-mat.mtrl-sci↗

arXiv2024

k-resolved ultrafast light-induced band renormalization in monolayer WS$_2$ on graphene

Understanding and controlling the electronic properties of two-dimensional materials is crucial for their potential applications in nano- and optoelectronics. Monolayer transition metal dichalcogenides such as WS$_2$ have garnered significant interest due to their strong light-matter interaction and extreme sensitivity of the band structure to the presence of photogenerated electron-hole pairs. In this study, we investigate the transient electronic structure of monolayer WS$_2$ on a graphene substrate after resonant excitation of the A-exciton using time- and angle-resolved photoemission spectroscopy. We observe a pronounced band structure renormalization including a substantial reduction of the transient band gap that is in good quantitative agreement with our {\it ab initio} theory that reveals the importance of both intrinsic WS$_2$ and extrinsic substrate contributions to the transient band structure of monolayer WS$_2$. Our findings not only deepen the fundamental understanding of band structure dynamics in two-dimensional materials but also offer valuable insights for the development of novel electronic and optoelectronic devices based on monolayer TMDs and their heterostructures with graphene.

cond-mat.mtrl-sci↗

arXiv2023

Exciton-exciton interactions in van der Waals heterobilayers

Exciton-exciton interactions are key to understanding non-linear optical and transport phenomena in van der Waals heterobilayers, which emerged as versatile platforms to study correlated electronic states. We present a combined theory-experiment study of excitonic many-body effects based on first-principle band structures and Coulomb interaction matrix elements. Key to our approach is the explicit treatment of the fermionic substructure of excitons and dynamical screening effects for density-induced energy renormalization and dissipation. We demonstrate that dipolar blue shifts are almost perfectly compensated by many-body effects, mainly by screening-induced self-energy corrections. Moreover, we identify a crossover between attractive and repulsive behavior at elevated exciton densities. Theoretical findings are supported by experimental studies of spectrally-narrow interlayer excitons in atomically-reconstructed, hBN-encapsulated MoSe$_2$/WSe$_2$ heterobilayers. Both theory and experiment show energy renormalization on a scale of a few meV even for high injection densities in the vicinity of the Mott transition. Our results revise the established picture of dipolar repulsion dominating exciton-exciton interactions in van der Waals heterostructures and open up opportunities for their external design.

cond-mat.mes-hall↗

arXiv2023

Engineering the impact of phonon dephasing on the coherence of a WSe$_{2}$ single-photon source via cavity quantum electrodynamics

Emitter dephasing is one of the key issues in the performance of solid-state single photon sources. Among the various sources of dephasing, acoustic phonons play a central role in adding decoherence to the single photon emission. Here, we demonstrate, that it is possible to tune and engineer the coherence of photons emitted from a single WSe$_2$ monolayer quantum dot via selectively coupling it to a spectral cavity resonance. We utilize an open cavity to demonstrate spectral enhancement, leveling, and suppression of the highly asymmetric phonon sideband, finding excellent agreement with a microscopic description of the exciton-phonon dephasing in a truly two-dimensional system. Moreover, the impact of cavity tuning on the dephasing is directly assessed via optical interferometry, which points out the capability to utilize light-matter coupling to steer and design dephasing and coherence of quantum emitters in atomically thin crystals.

quant-ph↗

arXiv2023

In-situ spontaneous emission control of MoSe$_2$-WSe$_2$ interlayer excitons with near-unity quantum yield

Optical resonators are a powerful platform to control the spontaneous emission dynamics of excitons in solid-state nanostructures. Here, we study a MoSe$_2$-WSe$_2$ van-der-Waals heterostructure that is integrated in a widely tunable open optical microcavity to gain insights into fundamental optical properties of the emergent interlayer charge-transfer excitons. First, we utilize an ultra-low quality factor open planar vertical cavity and investigate the modification of the excitonic lifetime as on- and off-resonant conditions are met with consecutive longitudinal modes. Time-resolved photoluminescence measurements reveal that the interlayer exciton lifetime can thus be periodically tuned with an amplitude of 110 ps. The resulting oscillations of the interlayer exciton lifetime allows us to extract a 0.5 ns free-space radiative lifetime and a quantum efficiency as high as 81 \%. We subsequently engineer the local density of optical states by introducing a spatially confined and fully spectrally tunable Tamm-plasmon resonance. The dramatic redistribution of the local optical modes in this setting allows us to encounter a profound inhibition of spontaneous emission of the interlayer excitons by a factor of 3.2. We expect that specifically engineering the inhibition of radiation from moir\'e excitons is a powerful tool to steer their thermalization, and eventually their condensation into coherent condensate phases.

cond-mat.mtrl-sci↗

arXiv2023

Non-linear and negative effective diffusivity of optical excitations in moir\'e-free heterobilayers

Interlayer exciton diffusion is studied in atomically-reconstructed MoSe2/WSe2 heterobilayers with suppressed disorder. Local atomic registry is confirmed by characteristic optical absorption, circularly-polarized photoluminescence, and g-factor measurements. Using transient microscopy we observe propagation properties of interlayer excitons that are independent from trapping at moir\'e- or disorder-induced local potentials. Confirmed by characteristic temperature dependence for free particles, linear diffusion coefficients of interlayer excitons at liquid helium temperature and low excitation densities are almost 1000 times higher than in previous observations. We further show that exciton-exciton repulsion and annihilation contribute nearly equally to non-linear propagation by disentangling the two processes in the experiment and simulations. Finally, we demonstrate effective shrinking of the light-emission over time across several 100's of picoseconds at the transition from exciton- to the plasma-dominated regimes. Supported by microscopic calculations for bandgap renormalization to identify Mott threshold, this indicates transient crossing between rapidly expanding, short-lived electron-hole plasma and slower, long-lived exciton populations.

cond-mat.mes-hall↗

arXiv2023

Confined-state physics and signs of fermionization of moir\'e excitons in WSe$_2$/MoSe$_2$ heterobilayers

We revisit and extend the standard bosonic interpretation of interlayer excitons in the moir\'e potential of twisted heterostructures of transition-metal dichalcogenides. In our experiments, we probe a high quality MoSe$_2$/WSe$_2$ van der Waals bilayer heterostructure via density-dependent photoluminescence spectroscopy and reveal strongly developed, unconventional spectral shifts of the emergent moir\'e exciton resonances. The observation of saturating blueshifts of successive exciton resonances allow us to explain their physics in terms of a model utilizing fermionic saturable absorbers. This approach is strongly inspired by established quantum-dot models, which underlines the close analogy of interlayer excitons trapped in pockets of the moir\'e potential, and quantum emitters with discrete eigenstates.

cond-mat.mes-hall↗