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Marc Aßmann

Publications and source records attributed to Marc Aßmann.

At least 19 recordsLinked to original sources

Temporal hopping dynamics in exciton-polariton condensation

Polariton condensates provide a versatile platform for exploring non-equilibrium phase transitions and collective phenomena in open quantum systems. Near the condensation threshold, these systems are particularly sensitive to fluctuations and instabilities, which can strongly influence the condensate formation. Using optical trapping and homodyne detection, we directly access the photon statistics and second-order correlation function $g^{(2)}(0)$ of the condensate. We show that polariton condensation near the threshold is not a purely static transition, but instead undergoes a dynamical regime characterized by stochastic hopping between condensed and non-condensed states. These intermittent dynamics are accompanied by a gradual reduction of $g^{(2)}(0)$ towards unity, revealing the progressive build-up of coherence even in the presence of strong temporal fluctuations. Numerical simulations, based on a stochastic Truncated Wigner description of the driven-dissipative polariton field, reproduce these dynamics and capture the essential role of noise and reservoir interactions. This work demonstrates that the observed temporal hopping is an intrinsic feature of polariton condensation, providing a dynamical perspective that goes beyond static descriptions of the condensation phase transition.

cond-mat.mes-hall

Assessing the classicality of photon echo from excitons in lead halide perovskite nanocrystals

Photon echo (PE) spectroscopy is a powerful technique for probing decoherence mechanisms and charge carrier dynamics in semiconductor systems. Beyond traditional coherence measurements, characterizing the photon statistics of the echo signal is important for assessing its potential in quantum information applications and understanding the underlying quantum mechanical processes. Here, we study the photon statistics of PE signals generated by excitons in ensembles of lead halide perovskite CsPbI$_3$ nanocrystals at cryogenic temperature of 2 K using continuous-variable quantum state optical tomography based on homodyne detection. Pronounced Rabi oscillations of the PE amplitude allow us to evaluate the statistics for various pulse areas in the excitation sequence. The damping of the oscillations with increasing pulse area is attributed to spatial excitation inhomogeneity and excitation-induced dephasing. Despite the large ensemble of optically addressed excitons, the efficiency of generated PE signals is low which is attributed to the complex energy level structure of excitons and non-radiative recombination channels in CsPbI$_3$ nanocrystals. We analyze the statistical characteristics of PE via the second-order correlation function $g^{(2)}(0)$ and the characteristic function for different combinations of the areas of the excitation pulses. Our results show that $g^{(2)}(0) = 1$, and the characteristic function of the PE signal corresponds to classical behavior. The formation of photon echoes as well as $g^{(2)}(0) = 1$ at the echo time is reproduced by a quantized free-space multimode model. Despite the relatively low efficiency, the photon echo exhibits a high degree of coherence and minimal classical noise, consistent with Poissonian statistics.

cond-mat.mes-hall

Quantum Resource Theory of Lasers

Lasers serve as the fundamental workhorses of photonic quantum technologies, with perfectly coherent light fields being essential for many protocols that generate nonclassical light, implement coherent control schemes, and initialize qubits. However, no laser is absolutely ideal and the implications of deviations from perfect coherence in quantum technological tasks remain unclear. In this study, we theoretically and experimentally explore the quantum coherence properties of lasers from a resource theory perspective, establishing a significant connection between photonics, quantum optics, and quantum information science. We demonstrate that the maximum achievable quantum coherence for laser light is constrained by spontaneous emission and the purity of the dephased laser field state. As a critical example application in quantum information protocols, we show that the quantum coherence of a laser field with a given mean photon number directly governs the maximum purity attainable when initializing a qubit in a superposition state through resonant driving. Our findings are highly relevant for bridging applied physics and engineering with integrated photonic quantum technologies and resource theories, paving the way for reliable benchmarking of various coherent light sources for applications in photonics and quantum protocols.

cond-mat.mes-hall

Rydberg excitons in Cu$_2$O at millikelvin temperatures

Rydberg excitons in the semiconductor Cu$_2$O have been observed in absorption experiments up to a principal quantum number of n = 28 at millikelvin temperatures [1]. Here, we extend the experimental parameter space by variing both temperature and excitation power. In particular, we show that the P excitons close to the band gap react more sensitively to an increase of the excitation power than states of the associated D exciton multiplet, even though the latter are located at comparatively higher energy. This finding is similar to the one observed when applying an external electric field, suggesting that the observed behavior arises from internal electric fields created by charged impurities that are optically ionized. At laser intensities below 1 $μ$W/cm$^2$, absorption lines of excitons with n=29 are observed.

cond-mat.mes-hall

Effective interaction dynamics of Rydberg excitons

Rydberg states of excitons in Cu$_2$O are known to interact strongly with other carriers in their surrounding such as other excitons, free charge carriers and static charged impurities. In cw-experiments, discriminating the individual processes is notoriously challenging. Here, we use a time-resolved two-color pump-probe setup and investigate the temporal evolution of Rydberg excitons with a resolution of 15 ns. The dynamic response of the Rydberg system to pump pulses with different energies is analyzed and the elementary processes that constitute the complex decay dynamics are compared among the different excitation scenarios. Our analysis reveals mainly four different timescales on which physical processes occur.

cond-mat.mes-hall

Targeted Polariton Flow Through Tailored Photonic Defects

In non-Hermitian open quantum systems, such as polariton condensates, local tailoring of gains and losses opens up an interesting possibility to realize functional optical elements. Here, we demonstrate that deliberately introducing losses via a photonic defect, realized by reducing the quality factor of a DBR mirror locally within an ultrahigh-quality microcavity, may be utilized to create directed polariton currents towards the defect. We discuss the role of polariton-polariton interactions in the process and how to tailor the effective decay time of a polariton condensate via coupling to the defect. Our results highlight the far-reaching potential of non-Hermitian physics in polaritonics.

cond-mat.mes-hall

Quantum coherence of a long-lifetime exciton-polariton condensate

In recent years, quantum information science has made significant progress, leading to a multitude of quantum protocols for the most diverse applications. States carrying resources such as quantum coherence are a key component for these protocols. In this study, we optimize the quantum coherence of a nonresonantly excited exciton-polariton condensate of long living polaritons by minimizing the condensate's interaction with the surrounding reservoir of excitons and free carriers. By combining experimental phase space data with a displaced thermal state model, we observe how quantum coherence builds up as the system is driven above the condensation threshold. Our findings demonstrate that a spatial separation between the condensate and the reservoir enhances the state's maximum quantum coherence directly beyond the threshold. These insights pave the way for integrating polariton systems into hybrid quantum devices and advancing applications in quantum technologies.

cond-mat.mes-hall

Nonlinear Rydberg exciton-polaritons in Cu$_2$O microcavities

Rydberg excitons (analogues of Rydberg atoms in condensed matter systems) are highly excited bound electron-hole states with large Bohr radii. The interaction between them as well as exciton coupling to light may lead to strong optical nonlinearity, with applications in sensing and quantum information processing. Here, we achieve strong effective photon-photon interactions (Kerr-like optical nonlinearity) via the Rydberg blockade phenomenon and the hybridisation of excitons and photons forming polaritons in a Cu$_2$O-filled microresonators. Under pulsed resonant excitation polariton resonance frequencies are renormalised due to the reduction of the photon-exciton coupling with increasing exciton density. Theoretical analysis shows that the Rydberg blockade plays a major role in the experimentally observed scaling of the polariton nonlinearity coefficient as $\propto n^{4.4 \pm 1.8}$ for principal quantum numbers up to n = 7. Such high principal quantum numbers studied in a polariton system for the first time are essential for realisation of high Rydberg optical nonlinearities, which paves the way towards quantum optical applications and fundamental studies of strongly-correlated photonic (polaritonic) states in a solid state system.

cond-mat.mes-hall

Neutralization of impurities by cw-excitation of high-$n$ Rydberg-excitons

We investigate the neutralization of charged defects in a Cu$_2$O crystal experimentally with a cw two-color pump-probe setup. We demonstrate that the excitation of high-lying Rydberg excitons at low densities generates an enhancement of exciton absorption up to a factor of 3. The result is an overall improvement of the absorption spectrum's quality in terms of increased oscillator strengths and narrower linewidths, referred to as purification. The reduction of the amount of charged impurities in the crystal is further verified by a thorough analysis of impurity photoluminescence signals.

cond-mat.mes-hall

Taming Charged Defects: Large Scale Purification in Semiconductors using Rydberg Excitons

We investigate the interaction between highly excited Rydberg excitons and charged impurities in the semiconductor Cuprous Oxide. We find that it is long-ranged and based on charge-induced dipole interactions. We demonstrate that we can utilize this interaction to neutralize impurities throughout the whole crystal - an effect we call purification. Purification reduces detrimental electrical stray fields drastically. We find that the absorption of the purified crystal increases by up to 25 % and that the purification effect is long-lived and may persist for hundreds of microseconds or even longer. Using a time-resolved pump-probe technique, we can discriminate purification from Rydberg blockade, which has been a long-standing goal in excitonic Rydberg systems.

cond-mat.mes-hall

Continuous-variable quantum optics and resource theory for ultrafast semiconductor spectroscopy

In this review, we discuss the use of continuous variable spectroscopy techniques for investigating quantum coherence and light-matter interactions in semiconductor systems with ultrafast dynamics. We focus on multichannel homodyne detection as a powerful tool to measure the quantum coherence and the full density matrix of a polariton system. By monitoring the temporal decay of quantum coherence in the polariton condensate, we observe coherence times exceeding the nanosecond scale. Our findings, supported by proof-of-concept experiments and numerical simulations, demonstrate the enhanced resourcefulness of the produced system states for modern quantum protocols. The combination of tailored resource quantifiers and ultrafast spectroscopy techniques presented here paves the way for future applications of quantum information technologies.

cond-mat.mes-hall

Polariton-dark exciton interactions in bistable semiconductor microcavities

We take advantage of the polariton bistability in semiconductor microcavities to estimate the interaction strength between lower exciton-polariton and dark exciton states. We combine the quasiresonant excitation of polaritons and the nominally forbidden two-photon excitation (TPE) of dark excitons in a GaAs microcavity. To this end, we use an ultranarrow linewidth cw laser for the TPE process that allows us to determine the energy of dark excitons with high spectral resolution. Our results evidence a sharp drop in the polariton transmission intensity and width of the hysteresis cycle when the TPE process is resonant with the dark exciton energy, highly compromising the bistability of the polariton condensate. This behavior demonstrates the existence of a small symmetry breaking such as that produced by an effective in-plane magnetic field, allowing us to directly excite the dark reservoir. We numerically reproduce the collapse of the hysteresis cycle with the increasing dark exciton population, treating the evolution of a polariton condensate in a one-mode approximation, coupled to the exciton reservoir via polariton-exciton scattering processes.

cond-mat.mes-hall

Tracking quantum coherence in polariton condensates with time-resolved tomography

Long-term quantum coherence constitutes one of the main challenges when engineering quantum devices. However, easily accessible means to quantify complex decoherence mechanisms are not readily available, nor are sufficiently stable systems. We harness novel phase-space methods - expressed through non-Gaussian convolutions of highly singular Glauber-Sudarshan quasiprobabilities - to dynamically monitor quantum coherence in polariton condensates with significantly enhanced coherence times. Via intensity- and time-resolved reconstructions of such phase-space functions from homodyne detection data, we probe the systems's resourcefulness for quantum information processing up to the nanosecond regime. Our experimental findings are confirmed through numerical simulations for which we develop an approach that renders established algorithms compatible with our methodology. In contrast to commonly applied phase-space functions, our distributions can be directly sampled from measured data, including uncertainties, and yield a simple operational measure of quantum coherence via the distribution's variance in phase. Therefore, we present a broadly applicable framework and a platform to explore time-dependent quantum phenomena and resources.

quant-ph

Tailored frequency conversion makes infrared light visible for streak cameras

Streak cameras are one of the most common and convenient devices to measure pulsed emission e.g. from semiconductor lightsources with picosecond time resolution. However, they are most sensitive in the visible range and possess low or negligible efficiency in the infrared and telecom regime. In this work, we present a frequency conversion based on sum-frequency generation that converts infrared to visible signals while preserving their temporal properties, making them detectable with a streak camera. We demonstrate and verify the functionality of our device by converting the emission from a quantum dot laser.

physics.optics

Scrutinizing the Debye plasma model: Rydberg excitons unravel the properties of low-density plasmas in semiconductors

For low-density plasmas, the classical limit described by the Debye-Hückel theory is still considered as an appropriate description even though a clear experimental proof of this paradigm is lacking due to the problems in determining the plasma-induced shift of single-particle energies in atomic systems. We show that Rydberg excitons in states with a high principal quantum number are highly sensitive probes for their surrounding making it possible to unravel accurately the basic properties of low-density non-degenerate electron-hole plasmas. To this end, we accurately measure the parameters of Rydberg excitons such as energies and linewidths in absorption spectra of bulk cuprous oxide crystals in which a tailored electron-hole plasma has been generated optically. Since from the absorption spectra exciton energies, as well as the shift of the single-particle energies given by the band edge, can be directly derived, the measurements allow us to determine the plasma density and temperature independently, which has been a notoriously hard problem in semiconductor physics. Our analysis shows unambiguously that the impact of the plasma cannot be described by the classical Debye model, but requires a quantum many-body theory, not only for the semiconductor plasma investigated here, but in general. Furthermore, it reveals a new exciton scattering mechanism with coupled plasmon-phonon modes becoming important even at very low plasma densities.

cond-mat.mes-hall

Quantifying quantum coherence in polariton condensates

We theoretically and experimentally investigate quantum features of an interacting light-matter system from a multidisciplinary perspective, unifying approaches from semiconductor physics, quantum optics, and quantum information science. To this end, we quantify the amount of quantum coherence that results from the quantum superposition of Fock states, constituting a measure of the resourcefulness of the produced state for modern quantum protocols. As an archetypal example of a hybrid light-matter interface, we study a polariton condensate and implement a numerical model to predict its properties. Our simulation is confirmed by our proof-of-concept experiment in which we measure and analyze the phase-space distributions of the emitted light. Specifically, we drive a polariton microcavity across the condensation threshold and observe the transition from an incoherent thermal state to a coherent state in the emission, thus confirming the build-up of quantum coherence in the condensate itself.

quant-ph

Asymmetric Rydberg blockade of giant excitons in Cuprous Oxide

The ability to generate and control strong long-range interactions via highly excited electronic states has been the foundation for recent breakthroughs in a host of areas, from atomic and molecular physics [1, 2] to quantum optics [3, 4] and technology [5-7]. Rydberg excitons provide a promising solid-state realization of such highly excited states, for which record-breaking orbital sizes of up to a micrometer have indeed been observed in cuprous oxide semiconductors [8]. Here, we demonstrate the generation and control of strong exciton interactions in this material by optically producing two distinct quantum states of Rydberg excitons. This makes two-color pump-probe experiments possible that allow for a detailed probing of the interactions. Our experiments reveal the emergence of strong spatial correlations and an inter-state Rydberg blockade that extends over remarkably large distances of several micrometers. The generated many-body states of semiconductor excitons exhibit universal properties that only depend on the shape of the interaction potential and yield clear evidence for its vastly extended-range and power-law character.

cond-mat.mes-hall

Coherent transfer matrix analysis of the transmission spectra of Rydberg excitons in Cuprous Oxide

In this study we analyze the transmission spectrum of a thin plate of Cuprous Oxide in the range of the absorption of the yellow exciton states with the coherent transfer matrix method. We demonstrate that, in contrast to the usual analysis using Beer's law, which turns out to be a rather good approximation only in the spectral region of high principal quantum numbers, a consistent quantitative description over the whole spectral range under consideration is possible. This leads to new and more accurate parameters not only for the Rydberg exciton states, but also for the strengths of indirect transitions. Furthermore, the results have consequences on the determination of the density of electron-hole pairs after optical excitation.

cond-mat.mes-hall