arXiv subjects

Rainer F. Mahrt

Publications and source records attributed to Rainer F. Mahrt.

18 recordsLinked to original sources

arXiv2025

Kibble-Zurek mechanism in a polariton supersolid

We study the formation of topological defects via the Kibble-Zurek mechanism in a polariton supersolid in a liquid crystal microcavity with tunable Rashba-Dresselhaus spin-orbit coupling. We predict analytically two different scalings in the slow- and fast-quench regimes, and confirm these predictions numerically. We also present experimental results for the slow-quench regime, demonstrating an original Kibble-Zurek scaling exponent $\eta_{KZM}=1.0\pm 0.2$

cond-mat.mes-hall↗

arXiv2025

Purcell-enhanced single-photon generation from CsPbBr$_3$ quantum dots in in-situ selected Laguerre-Gaussian modes

Single photons in Laguerre-Gaussian (LG) beams, which carry orbital angular momentum (OAM), could enable more robust and efficient photonic quantum communication and information processing, as well as enhanced sensitivity in quantum metrology and imaging. However, as most implementations are indirect or require additional mode-shaping elements, direct generation of single photons with OAM has received growing interest. Colloidal lead halide perovskite quantum dots (QDs) have recently emerged as a versatile material that can produce indistinguishable single photons quasi-deterministically at high rate. Here, we integrate single CsPbBr$_3$ QDs into an open Fabry-Perot microcavity with a nanofabricated Gaussian-shaped deformation, demonstrating Purcell-enhanced single-photon generation into individual cavity modes with up to 18.1 $\pm$ 0.2 times accelerated decay, down to tens of picoseconds. By in-situ tuning of the cavity resonance, we can selectively couple a single QD to different LG modes carrying OAM and observe the spatial patterns of the generated single-photon beams emitted from the cavity. Our findings open the door to high photon rate sources that directly generate single-photon LG beams for advanced quantum photonic applications.

physics.optics↗

arXiv2024

Transition between cooperative emission regimes in giant perovskite nanocrystals

Interactions between emitters within an ensemble can give rise to cooperative processes that significantly alter the properties of the emitted light. One such process is superfluorescence (SF), where excited electric dipoles spontaneously couple coherently and effectively radiate as one macroscopic emitter. It requires low energetic disorder, high temporal coherence and oscillator strength, and sub-wavelength volumes of material can be sufficient. Conversely, amplified spontaneous emission (ASE) originates from an avalanche-like stimulated amplification of initially spontaneously emitted photons and does not necessitate temporally coherent interactions among the emitters, but rather requires spatially long enough light propagation within the material to harvest the optical gain. Cesium lead halide perovskite nanocrystals (NCs) are one of the very few materials where both ASE (in disordered films) and SF (in ordered assemblies) were observed, however leaving unclear whether and how these regimes could be connected. Here, we demonstrate that temperature and excitation density can drive the transition between both regimes in a thin film of giant CsPbBr3 perovskite NCs. At temperatures below 45 K, excitonic SF was observed, whereas above a transition range between 45 K and 100 K, ASE prevails, but requires increased optical excitation and emitter density. Our results work out the different collective effects present in lead halide perovskites, providing fundamental insights into cooperative phenomena and important guidance for the development of compact and bright (quantum) light sources.

cond-mat.mes-hall↗

arXiv2024

A framework to compute resonances arising from multiple scattering

Numerous natural and technological phenomena are governed by resonances. In nanophotonics, resonances often result from the interaction of several optical elements. Controlling these resonances is an excellent opportunity to provide light with properties on demand for applications ranging from sensing to quantum technologies. The inverse design of large, distributed resonators, however, is typically challenged by high computational costs when discretizing the entire system in space. Here, this limitation is overcome by harnessing prior knowledge about the individual scatterers that form the resonator and their interaction. In particular, a transition matrix multi-scattering framework is coupled with the state-of-the-art adaptive Antoulas-Anderson (AAA) algorithm to identify complex poles of the optical response function. A sample refinement strategy suitable for accurately locating a large number of poles is introduced. We tie the AAA algorithm into an automatic differentiation framework to efficiently differentiate multi-scattering resonance calculations. The resulting resonance solver allows for efficient gradient-based optimization, demonstrated here by the inverse design of an integrated exciton-polariton cavity. This contribution serves as an important step towards efficient resonance calculations in a variety of multi-scattering scenarios, such as inclusions in stratified media, periodic lattices, and scatterers with arbitrary shapes.

physics.comp-ph↗

arXiv2024

Room-temperature cavity exciton-polariton condensation in perovskite quantum dots

The exploitation of the strong light-matter coupling regime and exciton-polariton condensates has emerged as a compelling approach to introduce strong interactions and nonlinearities into numerous photonic applications, ranging from low-threshold topological lasers to ultrafast all-optical logic devices. The use of colloidal semiconductor quantum dots with strong three-dimensional confinement as the active material in these microcavities would be highly advantageous due to their versatile structural and compositional tunability and wet-chemical processability, as well as potentially enhanced, confinement-induced polaritonic interactions. Yet, to date, cavity exciton-polariton condensation has neither been achieved with epitaxial nor with colloidal quantum dots. Here, we demonstrate room-temperature polariton condensation in a thin film of monodisperse, colloidal CsPbBr$_3$ quantum dots placed in a tunable optical resonator with a Gaussian-shaped deformation serving as wavelength-scale potential well for the polaritons. The onset of polariton condensation under pulsed optical excitation is manifested in emission by its characteristic superlinear intensity dependence, reduced linewidth, blueshift, and extended temporal coherence. Our results, based on this highly engineerable class of perovskite materials with unique optical properties, pave the way for the development of polaritonic devices for ultrabright coherent light sources and photonic information processing.

physics.optics↗

arXiv2024

Observation of a supersolid phase in a spin-orbit coupled exciton-polariton Bose-Einstein condensate at room temperature

In Bose-Einstein condensates (BEC), spin-orbit coupling (SOC) produces supersolidity. It is a peculiar state of matter, which, in addition to the superfluid behaviour shows periodic density modulation typical for crystals. Here, we report the fabrication of a new type of optical microcavity allowing to achieve room-temperature supersolidity for a quantum fluid of light. The microcavity is filled with a nematic liquid crystal (LC) and two layers of the organic polymer MeLPPP hosting exciton resonances. We demonstrate exciton-polariton condensation in the two distinct degenerate minima of the dispersion created by the LC induced Rashba-Dresselhaus (RD) SOC. The condensate real-space distribution shows density stripes located randomly from one condensate realization to another despite the presence of a random disorder potential. This demonstrates the immunity of stripes against disorder (that is, superfluidity) and the spontaneous breaking of translational invariance. We also report the random appearance of vortices via the Kibble-Zurek mechanism, another smoking gun of superfluidity.

cond-mat.mes-hall↗

arXiv2024

Perovskite nanocrystal self-assemblies in 3D hollow templates

Highly ordered nanocrystal (NC) assemblies, namely superlattices (SLs), have been investigated as novel building blocks of optical and optoelectronic devices due to their unique properties based on interactions among neighboring NCs. In particular, lead halide perovskite NC SLs have attracted significant attention, owing to their extraordinary optical characteristics of individual NCs and collective emission processes like superfluorescence (SF). So far, the primary method for preparing perovskite NC SLs has been the drying-mediated self-assembly method, in which the colloidal NCs spontaneously assemble into SLs during solvent evaporation. However, this method lacks controllability because NCs form random-sized SLs at random positions on the substrate rendering NC assemblies in conjunction with device structures such as photonic waveguides or microcavities challenging. Here, we demonstrate template-assisted self-assembly to deterministically place perovskite NC SLs and control their geometrical properties. A solution of CsPbBr3 NCs is drop-casted on a substrate with lithographically-defined hollow structures. After solvent evaporation and removal of excess NCs from the substrate surface, NCs only remain in the templates thereby defining the position and size of these NC assemblies. We performed photoluminescence (PL) measurements on these NC assemblies and observed signatures of SF, similar as in spontaneously assembled SLs. Our findings are crucial for optical devices that harness embedded perovskite NC assemblies and prepare fundamental studies on how these collective effects can be tailored through the SL geometry.

cond-mat.soft↗

arXiv2024

In-situ tunable, room-temperature polariton condensation in individual states of a 1D topological lattice

In recent years, exciton-polariton microcavity arrays have emerged as a promising semiconductor-based platform for analogue simulations of model Hamiltonians and topological effects. To realize experimentally a variety of Hamiltonians and change their parameters, it is essential to have highly tunable and easily engineerable structures. Here, we demonstrate in-situ tunable, room-temperature polariton condensation in individual states of a one-dimensional topological lattice, by utilizing an open-cavity configuration with an organic polymer layer. Angle-resolved photoluminescence measurements reveal the band structure of the Su-Schrieffer-Heeger chain, comprised of S-like and P-like bands, along with the appearance of discrete topological edge states with distinct symmetries. Changing the cavity length in combination with vibron-mediated relaxation in the polymer allows us to achieve selective polariton condensation into different states of the band structure, unveiled by nonlinear emission, linewidth narrowing, energy blue-shift and extended macroscopic coherence. Furthermore, we engineer the bandgap and the edge state localization by adjusting the interaction between adjacent lattice sites. Comparison to first-principles calculations showcases the precision of the polariton simulator. These results demonstrate the versatility and accuracy of the platform for the investigation of quantum fluids in complex potential landscapes and topological effects at room temperature.

cond-mat.mes-hall↗

arXiv2024

Circularly Polarized Luminescence Without External Magnetic Fields from Individual CsPbBr3 Perovskite Quantum Dots

Lead halide perovskite quantum dots (QDs), the latest generation of colloidal QD family, exhibit outstanding optical properties which are now exploited as both classical and quantum light sources. Most of their rather exceptional properties are related to the peculiar exciton fine-structure of band-edge states which can support unique bright triplet excitons. The degeneracy of the bright triplet excitons is lifted with energetic splitting in the order of millielectronvolts, which can be resolved by the photoluminescence (PL) measurements of single QDs at cryogenic temperatures. Each bright exciton fine-structure-state (FSS) exhibits a dominantly linear polarization, in line with several theoretical models based on the sole crystal field, exchange interaction and shape anisotropy. Here, we show that in addition to a high degree of linear polarization, the individual exciton FSS can exhibit a non-negligible degree of circular polarization even without external magnetic fields by investigating the four Stokes parameters of the exciton fine-structure in individual CsPbBr3 QDs through Stokes polarimetric measurements. We observe a degree of circular polarization up to ~38%, which could not be detected by using the conventional polarimetric technique. In addition, we found a consistent transition from left- to right-hand circular polarization within the fine-structure triplet manifold, which was observed in magnetic field dependent experiments. Our optical investigation provides deeper insights into the nature of the exciton fine-structures and thereby drives the yet-incomplete understanding of the unique photophysical properties of this novel class of QDs, potentially opening new scenarios in chiral quantum optics.

physics.app-ph↗

arXiv2024

Integrated, ultrafast all-optical polariton transistors with sub-wavelength grating microcavities

All-optical logic has the potential to overcome the operation speed barrier that has persisted in electronic circuits for two decades. However, the development of scalable architectures has been prevented so far by the lack of materials with sufficiently strong nonlinear interactions needed to realize compact and efficient ultrafast all-optical switches with optical gain. Microcavities with embedded organic material in the strong light-matter interaction regime have recently enabled all-optical transistors operating at room temperature with picosecond switching times. However, the vertical cavity geometry, which is predominantly used in polaritonics, is not suitable for complex circuits with on-chip coupled transistors. Here, by leveraging state-of-the-art silicon photonics technology, we have achieved exciton-polariton condensation at ambient conditions in fully integrated high-index contrast sub-wavelength grating microcavities filled with a pi-conjugated polymer as optically active material. We demonstrate ultrafast all-optical transistor action by coupling two resonators and utilizing seeded polariton condensation. With a device area as small as 2x2 um^2, we realize picosecond switching and amplification up to 60x, with extinction ratio up to 8:1. This compact ultrafast transistor device with in-plane integration is a key component for a scalable platform for all-optical logic circuits that could operate two orders of magnitude faster than electronic ones.

physics.optics↗

arXiv2021

Organic single-photon switch

The recent progress in nanotechnology [1,2] and single-molecule spectroscopy [3-5] paves the way for cost-effective organic quantum optical technologies emergent with a promise to real-life devices operating at ambient conditions. In this letter, we harness $π$-conjugated segments of an organic ladder-type polymer strongly coupled to a microcavity forming correlated collective dressed states of light, so-called of exciton-polariton condensates. We explore an efficient way for all-optical ultra-fast control over the macroscopic condensate wavefunction via a single photon. Obeying Bose statistics, exciton-polaritons exhibit an extreme nonlinearity undergoing bosonic stimulation [6] which we have managed to trigger at the single-photon level. Relying on the nature of organic matter to sustain stable excitons dressed with high energy molecular vibrations we have developed a principle that allows for single-photon nonlinearity operation at ambient conditions opening the door for practical implementations like sub-picosecond switching, amplification and all-optical logic at the fundamental limit of single light quanta.

cond-mat.mes-hall↗

arXiv2020

All-optical cascadable universal logic gate with sub-picosecond operation

Today, almost all information processing is performed using electronic logic circuits operating with up to several gigahertz frequency. All-optical logic, however, that holds the promise to allow up to three orders of magnitude higher speed [1] has not been able to provide a viable alternative because approaches that had been tried were either not scalable, not energy efficient or did not show a significant speed benefit. Whereas essential all-optical transistor functionalities have been already demonstrated across a range of platforms [2-4], using them to implement the complete Boolean logic gate set and in particular negation - switching off an optical signal with another optical signal - poses a major challenge [5]. Here, we realize a universal NOR logic gate by introducing the concept of non-ground-state dynamic exciton-polariton condensation in an organic semiconductor microcavity under non-resonant pulsed excitation. In the presence of either of the input signals inserted at opposite in-plane momenta, non-ground state dynamic condensation supersedes spontaneous ground-state condensation, resulting in a NOR-operator output signal within less than a picosecond. An additional optical transistor, fed by the output of the NOR gate, is then used to regenerate the output signal such that it is usable as input for cascading gates, a prerequisite for scale up. Our results constitute an essential step towards the realization of more complex logic optical circuitry that could boost future information processing applications.

physics.optics↗

arXiv2019

On-Chip Integrated Quantum-Dot Silicon-Nitride Microdisk Lasers

Hybrid SiN-QD microlasers coupled to a passive SiN output waveguide with 7μm diameter and record low threshold density of 27 μJ cm-2 are demonstrated. A new design and unique processing scheme starting from SiN/QD/SiN stacks offer long term stability and facilitate in depth laser characterization. This approach opens up new paths for optical communication, lab-on-a-chip, gas sensing and, potentially, on-chip cavity quantum electrodynamics and quantum optics.

physics.optics↗

arXiv2019

Zero-dimensional organic exciton-polaritons in tunable coupled Gaussian defect microcavities at room temperature

We demonstrate strong light-matter interaction at ambient conditions between a ladder-type conjugated polymer and the individual modes of a vertical microcavity with tunable resonance frequencies. Zero-dimensional wavelength-scale confinement for the polaritons is achieved through a sub-micron sized Gaussian defect, resulting in a vacuum Rabi splitting of the polariton branches of 2g = 166 meV. By placing a second Gaussian defect nearby, we create a polaritonic molecule with tunnel coupling strength of up to 2J ~ 50 meV. This platform enables the creation of tailor-made potential landscapes with wavelength-scale dimensions and tunable coupling strengths beyond the thermal energy, opening a route towards room-temperature polariton-based quantum simulators.

cond-mat.mes-hall↗

arXiv2019

Room-Temperature Exciton-Polariton Condensation in a Tunable Zero-Dimensional Microcavity

We create exciton-polaritons in a zero-dimensional (0D) microcavity filled with organic ladder-type conjugated polymer in the strong light-matter interaction regime. Photonic confinement at wavelength scale is realized in the longitudinal direction by two dielectric Bragg mirrors and laterally by a sub-micron Gaussian-shaped defect. The cavity is separated into two parts allowing nanometer position control and enabling tuning of exciton and photon fractions of the polariton wavefunction. Polariton condensation is achieved with non-resonant, picosecond optical excitation at ambient conditions and evidenced by a threshold behavior with non-linear increase of the emission intensity, line narrowing and blue-shift of the emission peak. Furthermore, angular emission spectra show that condensation occurs in the ground state of the 0D-cavity, and first order coherence measurements reveal the coherent nature. These experiments open the door for polariton quantum fluids in complex external potentials at room temperature.

cond-mat.mes-hall↗

arXiv2018

Long Exciton Dephasing Time and Coherent Phonon Coupling in CsPbBr$_{2}$Cl Perovskite Nanocrystals

Fully-inorganic cesium lead halide perovskite nanocrystals (NCs) have shown to exhibit outstanding optical properties such as wide spectral tunability, high quantum yield, high oscillator strength as well as blinking-free single photon emission and low spectral diffusion. Here, we report measurements of the coherent and incoherent exciton dynamics on the 100 fs to 10 ns timescale, determining dephasing and density decay rates in these NCs. The experiments are performed on CsPbBr$_{2}$Cl NCs using transient resonant three-pulse four-wave mixing (FWM) in heterodyne detection at temperatures ranging from 5 K to 50 K. We found a low-temperature exciton dephasing time of 24.5$\pm$1.0 ps, inferred from the decay of the photon-echo amplitude at 5 K, corresponding to a homogeneous linewidth (FWHM) of 54$\pm$5 {\mu}eV. Furthermore, oscillations in the photon-echo signal on a picosecond timescale are observed and attributed to coherent coupling of the exciton to a quantized phonon mode with 3.45 meV energy.

cond-mat.mes-hall↗

arXiv2018

Superfluorescence from Lead Halide Perovskite Quantum Dot Superlattices

An ensemble of emitters can behave significantly different from its individual constituents when interacting coherently via a common light field. After excitation, collective coupling gives rise to an intriguing many-body quantum phenomenon, resulting in short, intense bursts of light: so-called superfluorescence. Because it requires a fine balance of interaction between the emitters and their decoupling from the environment, together with close identity of the individual emitters, superfluorescence has thus far been observed only in a limited number of systems, such as atomic and molecular gases and semiconductor crystals, and could not be harnessed for applications. For colloidal nanocrystals, however, which are of increasing relevance in a number of opto-electronic applications, the generation of superfluorescent light was precluded by inhomogeneous emission broadening, low oscillator strength, and fast exciton dephasing. Using caesium lead halide (CsPbX3, X = Cl, Br) perovskite nanocrystals that are self-organized into highly ordered three-dimensional superlattices allows us to observe key signatures of superfluorescence: red-shifted emission with more than ten-fold accelerated radiative decay, extension of the first-order coherence time by more than a factor of four, photon bunching, and delayed emission pulses with Burnham-Chiao ringing behaviour at high excitation density. These mesoscopically extended coherent states can be employed to boost opto-electronic device performances and enable entangled multi-photon quantum light sources.

cond-mat.mes-hall↗

arXiv2017

Bright triplet excitons in lead halide perovskites

Nanostructured semiconductors emit light from electronic states known as excitons[1]. According to Hund's rules[2], the lowest energy exciton in organic materials should be a poorly emitting triplet state. Analogously, the lowest exciton level in all known inorganic semiconductors is believed to be optically inactive. These 'dark' excitons (into which the system can relax) hinder light-emitting devices based on semiconductor nanostructures. While strategies to diminish their influence have been developed[3-5], no materials have been identified in which the lowest exciton is bright. Here we show that the lowest exciton in quasi-cubic lead halide perovskites is optically active. We first use the effective-mass model and group theory to explore this possibility, which can occur when the strong spin-orbit coupling in the perovskite conduction band is combined with the Rashba effect [6-10]. We then apply our model to CsPbX3 (X=Cl,Br,I) nanocrystals[11], for which we measure size- and composition-dependent fluorescence at the single-nanocrystal level. The bright character of the lowest exciton immediately explains the anomalous photon-emission rates of these materials, which emit 20 and 1,000 times faster[12] than any other semiconductor nanocrystal at room[13-16] and cryogenic[17] temperatures, respectively. The bright exciton is further confirmed by detailed analysis of the fine structure in low-temperature fluorescence spectra. For semiconductor nanocrystals[18], which are already used in lighting[19,20], lasers[21,22], and displays[23], these optically active excitons can lead to materials with brighter emission and enhanced absorption. More generally, our results provide criteria for identifying other semiconductors exhibiting bright excitons with potentially broad implications for optoelectronic devices.

cond-mat.mes-hall↗