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Register a new userTwo-Dimensional hybrid perovskites sustaining strong polariton interactions at room temperature
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Added by
Lorenzo Dominici dr
Publication date
2018
fields
Physics
and research's language is
English
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Polaritonic devices exploit the coherent coupling between excitonic and photonic degrees of freedom to perform highly nonlinear operations with low input powers. Most of the current results exploit excitons in epitaxially grown quantum wells and require low temperature operation, while viable alternatives have yet to be found at room temperature. Here we show that large single-crystal flakes of two-dimensional layered perovskite are able to sustain strong polariton nonlinearities at room temperature with no need to be embedded in an optical cavity. In particular, exciton-exciton interaction energies are measured to be remarkably similar to the ones known for inorganic quantum wells at cryogenic temperatures, and more than one order of magnitude larger than alternative room temperature polariton devices reported so far. Thanks to their easy fabrication, large dipolar oscillator strengths and strong nonlinearities, these materials hold great promises to realize actual polariton devices at room temperature.
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Two dimensional (2D) perovskites are promising materials for photonic applications, given their outstanding nonlinear optical properties, ease of fabrication and versatility. In particular, exploiting their high oscillator strength, the crystalline form of 2D perovskites can be used as excitonic medium in optical microcavities, allowing for the study of their optical properties in the strong light-matter coupling regime. While polariton condensation has been observed in different materials at room temperature, here we observe for the first time two distinct threshold processes in a 2D perovskite, a material that has never shown spontaneous phase transition up to now. In particular, we demonstrate lasing from the bi-exciton state which contributes to populate the lower polariton branch and, at higher excitation powers, eventually leads to the formation of a polariton condensate. The emission linewidth narrowing and a spatial coherence over 50 x 50 um2 area are the smoking gun, the formation of a quantum coherent state in 2D hybrid perovskite. Our results not only show the formation of a polariton condensate in 2D perovskites but they are also crucial for the understanding of the physical mechanisms that leads to coherent phase transition in perovskite-based polariton microcavities.
Whispering gallery modes in a microwire are characterized by a nearly equidistant energy spectrum. In the strong exciton-photon coupling regime, this system represents a bosonic cascade: a ladder of discrete energy levels that sustains stimulated transitions between neighboring steps. In this work, by using femtosecond angle-resolved spectroscopic imaging technique, the ultrafast dynamics of polaritons in a bosonic cascade based on a one-dimensional ZnO whispering gallery microcavity is explicitly visualized. Clear ladder-form build-up process from higher to lower energy branches of the polariton condensates are observed, which are well reproduced by modeling using rate equations. Moreover, the polariton parametric scattering dynamics are distinguished on a timescale of hundreds of femtoseconds. Our understanding of the femtosecond condensation and scattering dynamics paves the way towards ultrafast coherent control of polaritons at room temperature, which will make it promising for high-speed all-optical integrated applications.
The coupling of optical and electronic degrees of freedom together with quantum confinement in low-dimensional electron systems is particularly interesting for achieving exotic functionalities in strongly correlated oxide electronics. Recently, high room-temperature mobility has been achieved for a large bandgap transparent oxide - BaSnO$_3$ upon extrinsic La or Sb doping, which has excited significant research attention. In this work, we report the observation of room-temperature ferromagnetism in BaSnO$_3$ thin films and the realization of a two-dimensional electron gas (2DEG) on the surface of transparent BaSnO$_3$ via oxygen vacancy creation, which exhibits a high carrier density of $sim 7.72*10^{14} /{rm cm}^2$ and a high room-temperature mobility of ~18 cm$^2$/V/s. Such a 2DEG is rather sensitive to strain and a less than 0.1% in-plane biaxial compressive strain leads to a giant resistance enhancement of 350% (more than 540 kOhm/Square) at room temperature. Thus, this work creates a new path to exploring the physics of low-dimensional oxide electronics and devices applicable at room temperature.
Metal nanoantennas supporting localized surface plasmon resonances have become an indispensable tool in bio(chemical) sensing and nanoscale imaging applications. The high plasmon-enhanced electric field intensity in the visible or near-IR range that enables the above applications may also cause local heating of nanoantennas. We present a design of hybrid optical-thermal antennas that simultaneously enable intensity enhancement at the operating wavelength in the visible and nanoscale local temperature control. We demonstrate a possibility to reduce the hybrid antenna operating temperature via enhanced infrared thermal emission. We predict via rigorous numerical modeling that hybrid optical-thermal antennas that support high-quality-factor photonic-plasmonic modes enable up to two orders of magnitude enhancement of localized electric fields and of the optical power absorbed in the nanoscale metal volume. At the same time, the hybrid antenna temperature can be lowered by several hundred degrees with respect to its all-metal counterpart under continuous irradiance of 104-105 W/m2. The temperature reduction effect is attributed to the enhanced radiative cooling, which is mediated by the thermally-excited localized surface phonon polariton modes. We further show that temperature reduction under even higher irradiances can be achieved by a combination of enhanced radiative and convective cooling in hybrid antennas. Finally, we demonstrate how hybrid optical-thermal antennas can be used to achieve strong localized heating of nanoparticles while keeping the rest of the optical chip at low temperature.
Light-matter coupling in excitonic materials has been the subject of intense investigation due to emergence of new excitonic materials. Two-dimensional layered hybrid organic/inorganic perovskites (2D HOIPs) support strongly bound excitons at room-temperatures with some of the highest oscillator strengths and electric loss tangents among the known excitonic materials. Here, we report strong light-matter coupling in Ruddlesden-Popper phase 2D-HOIPs crystals without the necessity of an external cavity. We report concurrent occurrence of multiple-orders of hybrid light-matter states via both reflectance and luminescence spectroscopy in thick (> 100 nm) crystals and near-unity absorption in thin (< 20 nm) crystals. We observe resonances with quality factors > 250 in hybridized exciton-polaritons and identify a linear correlation between exciton-polariton mode splitting and extinction coefficient of the various 2D-HOIPs. Our work opens the door to studying polariton dynamics in self-hybridized and open cavity systems with broad applications in optoelectronics and photochemistry.
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