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Martin Esmann

Publications and source records attributed to Martin Esmann.

At least 19 recordsLinked to original sources

Coherent interaction of WS$_2$ and quasi-2D perovskite excitons over micrometer distances via a cavity field

The coherent coupling of cavity-confined photons and excitonic matter resonances leads to the formation of cavity polaritons, hybrid light-matter quasi-particles. If multiple exciton resonances couple to the same photonic mode, the resulting polariton constitutes a coherent interaction between matter resonances that can be spatially separated without any direct electronic coupling. In this work, we demonstrate the formation of such a coherent coupling at room temperature using an open optical cavity containing two distinct van der Waals materials - monolayer WS2 and layered quasi-2D halide perovskites (HaPs) - separated by $1.5 \mu\rm m$. The system forms three polariton branches, with the middle branch possessing nearly equal fractions of both excitons and the photonic mode. White-light reflectivity and luminescence measurements are in good agreement with simulations using a coupled harmonic oscillator and a microscopic Wannier-Hopfield framework. Our results lay the foundation to combine highly complementary degrees of freedom in 2D materials in an in-situ tunable fashion to enable new polaritonic functionalities.

cond-mat.mes-hall

Charge Tunable Optical Nonlinearity of Moir\'e Exciton-Polaritons

Transition metal dichalcogenides represent a versatile platform to study strong light-matter interactions based on excitons and electrons in ordered lattices. Twist-engineering of moir\'e structures further enables the manipulation of the polaritonic nonlinearities via engineering the exciton landscape on the nanoscale. In this work, we demonstrate in-situ control of the optical saturation-based nonlinearity of moir\'e exciton-polaritons by phase space restriction via charge doping. Strong exciton-photon coupling is established in a gate-controllable MoTe$_2$-MoSe$_2$ heterobilayer, embedded in a spectrally-tunable open cavity. A small gate voltage can effectively lower the necessary polariton density by one order of magnitude to achieve a similar nonlinear saturation effect as in the charge-neutral case. Our microscopic description successfully explains the observed phenomena in the framework of Pauli blocking for the moir\'e superlattices with charge preoccupation.

cond-mat.mes-hall

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

High-Performance Nanophononic Resonators in Self-Suspended WSe$_2$ Domes and Drums

Van der Waals materials are ideally suited for the implementation of high-frequency nanophononic resonators with atomically flat interfaces. Here, we present two versatile van der Waals-based nanophononic architectures: First, we introduce self-supporting nano-domes of WSe$_2$ as a scalable platform for the simultaneous generation of hundreds of high-quality nanoacoustic resonators with resonance frequencies in the 100 GHz range. Second, we engineer self-supporting nano-drums that reach record-high working frequencies for 2D-semiconductor transducers beyond 1 THz. Through optical pump-probe spectroscopy experiments and photoelastic linear chain model calculations, we gain a detailed understanding of the intricate interplay between phononic mode hybridization across heterostructures, the differences between modes close to the center and edge of the acoustic Brillouin zone, and the temporal structure of the photoelastic response. Both architectures have potential applications in low-cost nanoacoustic probing and the ultrafast modulation of quantum emitters in two-dimensional semiconductors. While nano-drums surpass the THz frequency barrier, nano-domes appear as an accessible, low-cost alternative for developing scalable nanophononic technologies.

cond-mat.mes-hall

Strong coupling regimes of an organic exciton mirror in a microcavity

The coherent, periodic energy transfer between light- and matter excitations characterizes the strong coupling regime of cavity exciton-polaritons, resulting, in the simplest case, in a Rabi-doublet in the spectral domain. We demonstrate a peculiar regime of strong light-matter coupling, which arises when photonic cavity modes couple to an ultra-thin excitonic mirror. We embed a 12 nm J-aggregated thin film in an open microcavity and tune the coupling strength from weak to the onset of ultrastrong coupling. At resonance, the excitonic mirror selectively changes dielectric to metallic field boundary conditions adding a 2{\pi} phase, which links optical cavity modes of different order. Our work gives an exciting perspective to ultra-fast cavity switches and photonic devices based on excitonic optical elements.

cond-mat.mes-hall

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

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

Tuning relaxation and nonlinear upconversion of valley-exciton-polaritons in a monolayer semiconductor

Controlling exciton relaxation and energy conversion pathways via their coupling to photonic modes is a central task in cavity-mediated quantum materials research. In this context, the light-matter hybridization in optical cavities can lead to intriguing effects, such as modified carrier transport, enhancement of optical quantum yield, and control of chemical reaction pathways. Here, we investigate the impact of the strong light-matter coupling regime on energy conversion, both in relaxation and upconversion schemes, by utilizing a strongly charged MoSe2 monolayer embedded in a spectrally tunable open-access cavity. We find that the charge carrier gas yields a significantly modified photoluminescence response of cavity exciton-polaritons, dominated by an intra-cavity like pump scheme. In addition, upconversion luminescence emerges from a population transfer from fermionic trions to bosonic exciton-polaritons. Due to the availability of multiple optical modes in the tunable open cavity, it seamlessly meets the cavity-enhanced double resonance condition required for an efficient upconversion. The latter can be actively tuned via the cavity length in-situ, displaying nonlinear scaling in intensity and fingerprints of the valley polarization. This suggests mechanisms that include both trion-trion Auger scattering and phonon absorption as its underlying microscopic origin.

cond-mat.mes-hall

Exciton-polariton condensate in the van der Waals magnet CrSBr

Van der Waals magnets are an emergent material class of paramount interest for fundamental studies in coupling light with matter excitations, which are uniquely linked to their underlying magnetic properties. Among these materials, the semiconducting magnet CrSBr is possibly a first playground where we can study simultaneously the interaction of photons, magnons, and excitons at the quantum level. Here we demonstrate a coherent macroscopic quantum phase, the bosonic condensation of exciton-polaritons, emerging in a CrSBr flake embedded in a fully tunable cryogenic open optical cavity. The Bose condensate is characterized by a highly non-linear threshold-like behavior, and coherence manifests distinctly via its first and second order quantum correlations. We find that the condensate's non-linearity is highly susceptible to the magnetic order in CrSBr. Specially, it can encounter a sign change from attractive to repulsive interactions when the intrinsic antiferromagnetic order transforms to the forced ferromagnetic order. Our findings open a route towards magnetically controllable quantum fluids of light, and optomagnonic devices where spin magnetism is coupled to on-chip Bose-Einstein condensates.

cond-mat.mtrl-sci

Room-temperature polariton condensate in a two-dimensional hybrid perovskite

Layered 2D halide perovskites are chemically synthesized realizations of quantum well stacks with giant exciton oscillator strengths, tunable emission spectra and very large exciton binding energies. While these features render 2D halide perovskites a promising platform for room-temperature polaritonics, bosonic condensation and polariton lasing in 2D perovskites have so far remained elusive at ambient conditions. Here, we demonstrate room-temperature cavity exciton-polariton condensation in mechanically exfoliated crystals of the 2D Ruddlesden-Popper iodide perovskite $(BA)_{2}(MA)_{2}Pb_{3}I_{10}$ in an open optical microcavity. We observe a polariton condensation threshold of $P_{th}=6.76 fJ$ per pulse and detect a strong non-linear response. Interferometric measurements confirm the spontaneous emergence of spatial coherence across the condensate with an associated first-order autocorrelation reaching $g^{(1)}\approx 0.6$. Our results lay the foundation for a new class of room-temperature polariton lasers based on 2D halide perovskites with great potential for hetero-integration with other van-der-Waals materials and combination with photonic crystals or waveguides.

physics.optics

Infrared magneto-polaritons in MoTe$_2$ mono- and bilayers

MoTe$_2$ monolayers and bilayers are unique within the family of van-der-Waals materials since they pave the way towards atomically thin infrared light-matter quantum interfaces, potentially reaching the important telecommunication windows. Here, we report emergent exciton-polaritons based on MoTe$_2$ monolayer and bilayer in a low-temperature open micro-cavity in a joint experiment-theory study. Our experiments clearly evidence both the enhanced oscillator strength and enhanced luminescence of MoTe$_2$ bilayers, signified by a 38 \% increase of the Rabi-splitting and a strongly enhanced relaxation of polaritons to low-energy states. The latter is distinct from polaritons in MoTe$_2$ monolayers, which feature a bottleneck-like relaxation inhibition. Both the polaritonic spin-valley locking in monolayers and the spin-layer locking in bilayers are revealed via the Zeeman effect, which we map and control via the light-matter composition of our polaritonic resonances.

cond-mat.mes-hall

Polarization-controlled Brillouin scattering in elliptical optophononic resonators

The fast-growing development of optomechanical applications has motivated advancements in Brillouin scattering research. In particular, the study of high frequency acoustic phonons at the nanoscale is interesting due to large range of interactions with other excitations in matter. However, standard Brillouin spectroscopy schemes rely on fixed wavelength filtering, which limits the usefulness for the study of tunable optophononic resonators. It has been recently demonstrated that elliptical optophononic micropillar resonators induce different energy-dependent polarization states for the Brillouin and the elastic Rayleigh scattering, and that a polarization filtering setup could be implemented to increase the contrast between the inelastic and elastic scattering of the light. An optimal filtering configuration can be reached when the polarization states of the laser and the Brillouin signal are orthogonal from each other. In this work, we theoretically investigate the parameters of such polarization-based filtering technique to enhance the efficiency of Brillouin scattering detection. For the filtering optimization, we explore the initial wavelength and polarization state of the incident laser, as well as in the ellipticity of the micropillars, and reach an almost optimal configuration for nearly background-free Brillouin detection. Our findings are one step forward on the efficient detection of Brillouin scattering in nanostructures for potential applications in fields such as optomechanics and quantum communication.

physics.optics

Topologically tunable polaritons based on two-dimensional crystals in a photonic lattice

Topological photonics is an emergent research discipline which interlinks fundamental aspects of photonics, information processing and solid-state physics. Exciton-polaritons are a specifically interesting platform to study topological phenomena, since the coherent light matter coupling enables new degrees of freedom such as tunable non-linearities, chiralities and dissipation. Room-temperature operation of such exciton-polaritons relies on materials comprising both, large exciton binding energies and oscillator strength. We harness widely spectrally tunable, room temperature exciton-polaritons based on a WS2 monolayer in an open optical cavity to realize a polariton potential landscape which emulates the Su-Schrieffer-Heeger (SSH) Hamiltonian. It comprises a domain boundary hosting a topological, exponentially localized mode at the interface between two lattices characterized by different Zak-phases which features a spectral tunability over a range as large as 80 meV. Moreover, we utilize the unique tilt-tunability of our implementation, to transform the SSH-lattice into a Stark-ladder. This transformation couples the topologically protected defect mode to propagating lattice modes, and effectively changes the symmetry of the system. Furthermore, it allows us to directly quantify the Zak-phase difference $\Delta_{Zak}=(1.13\pm 0.11)\pi$ between the two topological phases. Our work comprises an important step towards in-situ tuning topological lattices to control and guide light on non-linear chips.

physics.optics

Correlated magnetism of moir\'e exciton-polaritons on a triangular electron-spin lattice

We demonstrate evidence of correlated magnetism for exciton-polaritons in a MoSe$_{2}$/WS$_{2}$ moir\'e heterostructure with near-parallel alignment subject to electron doping. In our experiments, interactions between electrons and moir\'e excitons are controlled electrostatically by field-effect doping, and the polaritonic regime of strong light-matter coupling is established in an open cryogenic microcavity. Remarkably, at filling fractions around one electron per moir\'e cell, we observe drastic and nonlinear enhancement of the effective polariton Land\'e factor as a hallmark of correlated magnetism, which is cavity-controlled via resonance tuning of light and matter polariton constituents. Our work establishes moir\'e van der Waals heterostructures as an outstanding platform for studies of correlated phenomena in the presence of strong light-matter coupling and many-body phases of lattice-ordered excitons, charges and spins.

cond-mat.mes-hall

Second-order temporal coherence of polariton lasers based on an atomically thin crystal in a microcavity

Bosonic condensation and lasing of exciton-polaritons in microcavities is a fascinating solid-state phenomenon. It provides a versatile platform to study out-of-equilibrium many-body physics and has recently appeared at the forefront of quantum technologies. Here, we study the photon statistics via the second-order temporal correlation function of polariton lasing emerging from an optical microcavity integrated with an atomically thin MoSe2 crystal. Furthermore, we investigate the macroscopic polariton phase transition for varying excitation powers and temperatures. The lower-polariton exhibits photon bunching below the threshold, implying a dominant thermal distribution of the emission, while above the threshold, the second-order correlation transits towards unity, which evidences the formation of a coherent state. Our findings are in agreement with a microscopic numerical model, which explicitly includes scattering with phonons on the quantum level.

cond-mat.mes-hall

Excitons in epitaxially grown WS2 on Graphene: a nanometer-resolved EELS and DFT study

In this study, we investigate excitonic properties of epitaxially grown WS2, which is of particular interest for various applications due to its potential for upscaling to wafer sized structures. Understanding the effect of the dielectric environment due to changing layer numbers and multi-material heterostructures on the optical properties is crucial for tailoring device properties. Monochromated electron energy loss spectroscopy in a scanning transmission electron microscope is employed to characterize the excitonic spectrum of WS2 on graphene grown by metal organic chemical vapor deposition. This technique provides the required spatial resolution at the nanometer scale in combination with high quality spectra. To complement the experimental results, theoretical investigations using density functional theory and applying the Bethe-Salpeter equations are conducted. We find that by transitioning from mono- to bi- to multilayers of WS2 the spectra show redshifts for both, the K-valley excitons at about 2.0 and 2.4 eV as well as excitonic features of higher energies. The latter features originate from so called band nesting of transitions between the Gamma- and K-point. In summary, this study provides valuable insights into the excitonic properties of WS2 in different layer configurations and environments, which are realistically needed for future device fabrication and property tuning. Finally, we can show that nanometer scale electron spectroscopy supported by careful theoretical modelling can successfully link atomic structure and optical properties, such as exciton shifts, in non-idealized complex material systems like multilayer 2D heterostructures.

cond-mat.mtrl-sci

Organic room-temperature polariton condensate in a higher-order topological lattice

Organic molecule exciton-polaritons in photonic lattices are a versatile platform to emulate unconventional phases of matter at ambient conditions, including protected interface modes in topological insulators. Here, we investigate bosonic condensation in the most prototypical higher-order topological lattice: a 2D-version of the Su-Schrieffer-Heeger (SSH) model, supporting both 0D and 1D topological modes. We study fluorescent protein-filled, structured microcavities defining a staggered photonic trapping potential and observe the resulting first- and higher-order topologically protected modes via spatially resolved photoluminescence spectroscopy. We account for the spatial mode patterns by tight-binding calculations and theoretically characterize the topological invariants of the lattice. Under strong optical pumping, we observe bosonic condensation into the topological modes. Via interferometric measurements, we map the spatial first-order coherence in the protected 1D modes extending over 10 microns. Our findings pave the way towards organic on-chip polaritonics using higher-order topology as a tool for the generation of robustly confined polaritonic lasing states.

physics.optics

Revealing dark exciton signatures in polariton spectra of 2D materials

Dark excitons in transition metal dichalcogenides (TMD) have been so far neglected in the context of polariton physics due to their lack of oscillator strength. However, in tungsten-based TMDs, dark excitons are known to be the energetically lowest states and could thus provide important scattering partners for polaritons. In this joint theory-experiment work, we investigate the impact of the full exciton energy landscape on polariton absorption and reflectance. By changing the cavity detuning, we vary the polariton energy relative to the unaffected dark excitons in such a way that we open or close specific phonon-driven scattering channels. We demonstrate both in theory and experiment that this controlled switching of scattering channels manifests in characteristic sharp changes in optical spectra of polaritons. These spectral features can be exploited to extract the position of dark excitons. Our work suggests new possibilities for exploiting polaritons for fingerprinting nanomaterials via their unique exciton landscape.

cond-mat.mes-hall