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Ullrich Scherf

Publications and source records attributed to Ullrich Scherf.

15 recordsLinked to original sources

Stimulated cooling in non-equilibrium Bose-Einstein condensate

We report on the experimental observation of stimulated cooling in the non-equilibrium Bose-Einstein condensate (BEC) of weakly interacting exciton-polaritons from approximately room temperature down to 20K. By resolving the condensate in energy-momentum space and performing interferometric measurements, we distinguish the condensate from thermalized particles yet occupying excited states macroscopically. In contrast to the analytical quantum theories of non-equilibrium BEC [Shishkov et al., Phys. Rev. Lett. 128, 065301 (2022)], we observe segmentation of the particle density along the excited states into two fractions both following Bose-Einstein distribution, albeit with different effective temperatures and chemical potentials. Our results indicate that the temperature of the weakly interacting Bose gas is universally set by the density-dependent chemical potential, revealing a defining property of non-equilibrium BECs. Finally, we demonstrate that the stimulated nature of the cooling process directly governs the emergence of quantum coherence of the condensate and shapes the dissipative properties of the excited states.

cond-mat.quant-gas

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 $η_{KZM}=1.0\pm 0.2$

cond-mat.mes-hall

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

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

Temporal bandwidth of consecutive polariton condensation

The advent of organic polaritonics has led to the realisation of all-optical transistors, logic gates, and single photon-switches operating at room temperature. In this Letter, we develop a microscopic theory accounting for thermalisation, vibron-relaxation, and radiative and ballistic polariton losses to investigate the intrinsic limitations of the temporal separation of consecutive polariton condensates. We test and verify our theoretical predictions using an optical pump-pump configuration with different pulse width and unravel the importance of lateral ballistic losses in defining the upper limit of the temporal bandwidth, reaching ~240 GHz.

cond-mat.mes-hall

In-situ tunneling control in photonic potentials by Rashba-Dresselhaus spin-orbit coupling

The tunability of individual coupling amplitudes in photonic lattices is highly desirable for photonic Hamiltonian engineering and for studying topological transitions in situ. In this work, we demonstrate the tunneling control between individual lattice sites patterned inside an optical microcavity. The tuning is achieved by applying a voltage to a liquid crystal microcavity possessing photonic Rashba-Dresselhaus spin-orbit coupling. This type of spin-orbit coupling emerges due to the high birefringence of the liquid crystal material and constitutes an artificial gauge field for photons. The proposed technique can be combined with strong-light matter coupling and non-Hermitian physics already established in liquid crystal microcavities.

physics.optics

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

Ultrafast optical control of polariton energy in an organic semiconductor microcavity

The manipulation of exciton-polaritons and their condensates is of great interest due to their applications in polariton simulators and high-speed, all-optical logic devices. Until now, methods of trapping and manipulating such condensates are not dynamically reconfigurable or result in an undesirable reduction in the exciton-photon coupling strength. Here, we present a new strategy for the ultrafast control of polariton resonances via transient modification of an optical cavity mode. We have constructed multilayer organic semiconductor microcavities that contain two absorbers: one strongly- and one weakly-coupled to the cavity photon mode. By selectively exciting the weakly-coupled absorber with ultrashort laser pulses, we modulate the cavity refractive index and generate fully-reversible blueshifts of the lower polariton branch by up to 8 meV in sub-ps timescales with no corresponding reduction in the exciton-photon coupling strength. Our work demonstrates the ability to manipulate polariton energy landscapes over ultrafast timescales with important applications in emerging computing technologies.

physics.optics

Shaping potential landscape for organic polariton condensates in double-dye cavities

We investigate active spatial control of polariton condensates independently of the polariton-, gain-inducing excitation profile. This is achieved by introducing an extra intracavity semiconductor layer, non-resonant to the cavity mode. Saturation of the optical absorption in the uncoupled layer enables the ultra-fast modulation of the effective refractive index and, through excited-state absorption, the polariton dissipation. Utilising these mechanisms, we demonstrate control over the spatial profile and density of a polariton condensate at room temperature.

cond-mat.mes-hall

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

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

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

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

Direct observation of state-filling at hybrid tin oxide/organic interfaces

Electroluminescence (EL) spectra from hybrid charge transfer excitons at metal oxide/organic type-II heterojunctions exhibit pronounced bias-induced spectral shifts. The reasons for this phenomenon have been discussed controversially and arguments for both electric field-induced effects as well as filling of trap states at the oxide surface have been put forward. Here, we combine the results from EL and photovoltaic measurements to eliminate the disguising effects of the series resistance. For SnOx combined with the conjugated polymer MeLPPP, we find a one-to-one correspondence between the blueshift of the EL peak and the increase of the quasi-Fermi level splitting at the hybrid heterojunction, which we unambiguously assign to state filling. Our data is resembled best by a model considering the combination an exponential density of states with a doped semiconductor.

cond-mat.mtrl-sci

Excitation Dynamics in Low Band Gap Donor-Acceptor Copolymers and Blends

Donor-acceptor (D-A) type copolymers show great potential for the application in the active layer of organic solar cells. Nevertheless the nature of the excited states, the coupling mechanism and the relaxation pathways following photoexcitation are yet to be clarified. We carried out comparative measurements of the steady state absorption and photoluminescence (PL) on the copolymer poly[N-(1-octylnonyl)-2,7-carbazole] -alt-5,5-[4',7' -di(thien-2-yl)-2',1',3' -benzothiadiazole] (PCDTBT), its building blocks as well as on the newly synthesized N-(1-octylnonyl)-2,7-bis-[(5-phenyl)thien-2-yl)carbazole (BPT-carbazole) (see Figure 1). The high-energy absorption band (HEB) of PCDTBT was identified with absorption of carbazoles with adjacent thiophene rings while the low-energy band (LEB) originates instead from the charge transfer (CT) state delocalized over the aforementioned unit with adjacent benzothiadiazole group. Photoexcitation of the HEB is followed by internal relaxation prior the radiative decay to the ground state. Adding PC70BM results in the efficient PL quenching within the first 50 ps after excitation. From the PL excitation experiments no evidence for a direct electron transfer from the HEB of PCDTBT towards the fullerene acceptor was found, therefore the internal relaxation mechanisms within PCDTBT can be assumed to precede. Our findings indicate that effective coupling between copolymer building blocks governs the photovoltaic performance of the blends.

cond-mat.mtrl-sci