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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 19 records

Direct measurement of polariton-polariton interaction strength in the Thomas-Fermi regime of exciton-polariton condensation

Bosonic condensates of exciton polaritons (light-matter quasiparticles in a semiconductor) provide a solid-state platform for studies of nonequilibrium quantum systems with a spontaneous macroscopic coherence. These driven, dissipative condensates typically coexist and interact with an incoherent reservoir, which undermines measurements of key parameters of the condensate. Here, we overcome this limitation by creating a high-density exciton-polariton condensate in an optically induced box trap. In this so-called Thomas-Fermi regime, the condensate is fully separated from the reservoir and its behavior is dominated by interparticle interactions. We use this regime to directly measure the polariton-polariton interaction strength, and reduce the existing uncertainty in its value from four orders of magnitude to within three times the theoretical prediction. The Thomas-Fermi regime has previously been demonstrated only in ultracold atomic gases in thermal equilibrium. In a nonequilibrium exciton-polariton system, this regime offers a novel opportunity to study interaction-driven effects unmasked by an incoherent reservoir.

36 MATERIALS SCIENCE↗

Enhancement and Tunability of Near-Field Radiative Heat Transfer Mediated by Surface Plasmon Polaritons in Thin Plasmonic Films

The properties of thermal radiation exchange between hot and cold objects can be strongly modified if they interact in the near field where electromagnetic coupling occurs across gaps narrower than the dominant wavelength of thermal radiation. Using a rigorous fluctuational electrodynamics approach, we predict that ultra-thin films of plasmonic materials can be used to dramatically enhance near-field heat transfer. The total spectrally integrated film-to-film heat transfer is over an order of magnitude larger than between the same materials in bulk form and also exceeds the levels achievable with polar dielectrics such as SiC. We attribute this enhancement to the significant spectral broadening of radiative heat transfer due to coupling between surface plasmon polaritons (SPPs) on both sides of each thin film. We show that the radiative heat flux spectrum can be further shaped by the choice of the substrate onto which the thin film is deposited. In particular, substrates supporting surface phonon polaritons (SPhP) strongly modify the heat flux spectrum owing to the interactions between SPPs on thin films and SPhPs of the substrate. The use of thin film phase change materials on polar dielectric substrates allows for dynamic switching of the heat flux spectrum between SPP-mediated and SPhP-mediated peaks

42 ENGINEERING↗

Analytic rate theory of polariton relaxation that explains long polariton lifetime

Hybridization of a molecular exciton with a quantized photon creates a polariton. Despite extensive experimental investigations, the apparent lifetime of the exciton–polariton is not well-understood. For this work, we examined the steady-state population dynamics for a Holstein–Tavis–Cumming Hamiltonian to illuminate the long-term polaritonic dynamics and lifetime of the exciton–polariton in an optical cavity. For a realistic description of polariton relaxation, cavity loss and various exciton decay channels are included in the model. We found that in the presence of weak but finite exciton loss, the apparent lifetime of the lower polariton coincides with the out-of-cavity exciton lifetime and is independent of cavity-matter detuning. This is a simple explanation for the experimentally observed lifetimes for exciton polaritons and theoretically justifies the dark state reservoir hypothesis. Furthermore, if the upper polariton is initially populated, the system reaches the steady state very quickly, leading to single-exponential polariton relaxation. Starting from the lower polariton leads to a longer pre-steady-state time period, leading to double-exponential relaxation. Finally, we considered the effect of site orientational disorders and the exciton frequency disorderers. Under the collective limit, the effects of this disorder can be included in Fermi’s golden rule population dynamics without explicit sampling. For the exciton energy disorders, numerical calculations are needed. Our theoretical framework is applicable to interpret exciton–polariton experiments, especially related to the measured apparent lifetime of polaritons.

Chemical dynamics↗

Twin Polaritons: Classical versus Quantum Features in Polaritonic Spectra

Understanding whether a polaritonic phenomenon is fundamentally quantum or classical is essential for building accurate theoretical models and guiding experimental design. Here, in this work, we address this question in the context of polaritonic spectra and report an intriguing new feature: the twin polariton, an additional splitting beyond the primary resonant polariton splitting originating from vacuum field fluctuations. We show that the twin polariton persists in the many-molecule limit under permutationally symmetrical initial-state constraint and that it follows the same linear dependence on coupling strength as the primary polariton splitting. This establishes a novel mechanism by which a quantum feature (the twin polariton) can be tuned through a classical one (the primary polariton), offering new opportunities to probe and control the fundamental nature of polaritonic systems.

classical optics↗

Reanalysis of Experimental Determinations of Polariton-Polariton Interactions in Microcavities

The polariton-polariton interaction strength is an important parameter for all kinds of applications using the nonlinear properties of polaritons, such as optical switching and single-photon blockade devices. In this paper, we review and compare the results of a series of experiments on polariton-polariton interactions in GaAs/AlxGa1-xAs microcavity polariton structures and present an updated analysis of these experiments. We show that not just the energy shift of the spectral lines but also the results of measurements sensitive to the polariton scattering rate are important for the calibration of the interaction parameter at low excitation density. We find that when adjustments are made to correct for recent understanding of the experiments, the value of the interaction parameter at low density is lower than previous reported, but still significantly higher than theoretically predicted.

CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SU↗

Doping-tunable thermal emission from plasmon polaritons in semiconductor epsilon-near-zero thin films

We utilize the unique dispersion properties of leaky plasmon polaritons in epsilon-near-zero (ENZ) thin films to demonstrate thermal radiation control. Owing to its highly flat dispersion above the light line, a thermally excited leaky wave at the ENZ frequency out-couples into free space without any scattering structures, resulting in a narrowband, wide-angle, p-polarized thermal emission spectrum. We demonstrate this idea by measuring angle- and polarization-resolved thermal emission spectra from a single layer of unpatterned, doped semiconductors with deep-subwavelength film thickness (d/λ{sub 0} ∼ 6×10{sup −3}, where d is the film thickness and λ{sub 0} is the free space wavelength). We show that this semiconductor ENZ film effectively works as a leaky wave thermal radiation antenna, which generates far-field radiation from a thermally excited mode. The use of semiconductors makes the radiation frequency highly tunable by controlling doping densities and also facilitates device integration with other components. Therefore, this leaky plasmon polariton emission from semiconductor ENZ films provides an avenue for on-chip control of thermal radiation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Enabling multiple intercavity polariton coherences by adding quantum confinement to cavity molecular polaritons

In this study, the “particle in a box” idea, which was broadly developed in semiconductor quantum dot research, was extended into mid-infrared (IR) cavity modes by applying lateral confinement in an optical cavity. The discrete cavity modes hybridized with molecular vibrational modes, resulting in a quartet of polariton states that can support multiple coherence states in the IR regime. We applied tailored pump pulse sequences to selectively prepare these coherences and verified the multi-coherence existence. The simulation based on Lindblad equation showed that because the quartet of polariton states resided in the same cavity, they were specifically robust toward decoherence caused by fluctuations in space. The multiple robust coherences paved the way for entangled states and coherent interactions between cavity polaritons, which would be critical for advancing polariton-based quantum information technology.

2D IR↗

When are Surface Plasmon Polaritons Excited in the Kretschmann-Raether Configuration?

It is widely believed that the reflection minimum in a Kretschmann-Raether experiment results from direct coupling into surface plasmon polariton modes. Our experimental results provide a surprising discrepancy between the leakage radiation patterns of surface plasmon polaritons (SPPs) launched on a layered gold/germanium film compared to the K-R minimum, clearly challenging this belief. We provide definitive evidence that the reflectance dip in K-R experiments does not correlate with excitation of an SPP mode, but rather corresponds to a particular type of perfectly absorbing (PA) mode. Results from rigorous electrodynamics simulations show that the PA mode can only exist under external driving, whereas the SPP can exist in regions free from direct interaction with the driving field. These simulations show that it is possible to indirectly excite propagating SPPs guided by the reflectance minimum in a K-R experiment, but demonstrate the efficiency can be lower by more than a factor of 3. We find that optimal coupling into the SPP can be guided by the square magnitude of the Fresnel transmission amplitude.

Foley IV, Jonathan J.↗

Ab initio polaritonic potential-energy surfaces for excited-state nanophotonics and polaritonic chemistry

Advances in nanophotonics, quantum optics, and low-dimensional materials have enabled precise control of light–matter interactions down to the nanoscale. Combining concepts from each of these fields, there is now an opportunity to create and manipulate photonic matter via strong coupling of molecules to the electromagnetic field. Toward this goal, here we demonstrate a first principles framework to calculate polaritonic excited-state potential-energy surfaces, transition dipole moments, and transition densities for strongly coupled light–matter systems. In particular, we demonstrate the applicability of our methodology by calculating the polaritonic excited-state manifold of a formaldehyde molecule strongly coupled to an optical cavity. This proof-of-concept calculation shows how strong coupling can be exploited to alter photochemical reaction pathways by influencing avoided crossings with tuning of the cavity frequency and coupling strength. Therefore, by introducing an ab initio method to calculate excited-state potential-energy surfaces, our work opens a new avenue for the field of polaritonic chemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Molecular Polaritonics: Chemical Dynamics Under Strong Light–Matter Coupling

Chemical manifestations of strong light–matter coupling have recently been a subject of intense experimental and theoretical studies. Here we review the present status of this field. Section 1 is an introduction to molecular polaritonics and to collective response aspects of light–matter interactions. Section 2 provides an overview of the key experimental observations of these effects, while Section 3 describes our current theoretical understanding of the effect of strong light–matter coupling on chemical dynamics. A brief outline of applications to energy conversion processes is given in Section 4. Pending technical issues in the construction of theoretical approaches are briefly described in Section 5. Finally, the summary in Section 6 outlines the paths ahead in this exciting endeavor.

Chemistry↗

Terahertz instability of surface optical-phonon polaritons that interact with surface plasmon polaritons in the presence of electron drift

Traveling-wave interaction between optical phonons and electrons drifting in diatomic semiconductors has potential for amplification and generation of terahertz radiation. Existing models of this interaction were developed for infinite materials. As a more practically relevant configuration, we studied theoretically a finite semiconductor slab surrounded by a dielectric. This paper analyzes the optical-phonon instability in the slab including the Lorentz force and compares it to the instability in an infinite material. As the analysis shows, the slab instability occurs because of the interaction of surface optical-phonon polaritons with surface plasmon polaritons in the presence of electron drift. The properties of the instability depend on the slab thickness when the thickness is comparable to the wavelength. For large slab thicknesses, however, the dispersion relation of the slab is similar to that of an infinite material, although the coupling is weaker. The results could be used for the design of practical terahertz traveling-wave oscillators and amplifiers.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Coupling between gap plasmon polariton and magnetic polariton in a metallic-dielectric multilayer structure

The excitation of plasmons in a metallic nanostructure represents a feasible and practical approach for manipulating the propagation and absorption of light at the subwavelength scale. Of particular interest is the coupling between plasmons, which can be used to facilitate the spectral tunability and tailor the optical response of the structure. In this paper, we study the coupling between two highly localized plasmonic modes: gap plasmon polariton mode and magnetic polariton mode, supported by a metallic-dielectric multilayer structure. The strong coupling gives rise to the formation of hybrid plasmon modes and large mode splitting. These hybrid modes result in unique spectral-directional absorption characteristics in the structure. The findings hold promise in applications such as photonic and energy conversion systems as well as the design of plasmonic nanodevices.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗