Revealing Giant Exciton Fine-Structure Splitting in Two-Dimensional Perovskites Using van der Waals Passivation.

Organic-inorganic layered perovskites are currently some of the most promising 2D van der Waals materials. Low crystal quality usually broadens the exciton line width, obscuring the fine structure of the exciton in conventional photoluminescence experiments. Here, we propose a mechanical approach to reducing the effect of spectral diffusion by means of hBN capping on layered perovskites, revealing the exciton fine structure. We used a stochastic model to link the reduction of the spectral line width with the population of charge fluctuation centers present in the organic spacer. van der Waals forces between both lattices cause the partial clamping of the perovskite organic spacer molecules, and hence the amplitude of the overall spectral diffusion effect is reduced. Our work provides a low-cost solution to the problem of accessing important fine-structure excitonic state information, along with an explanation of the important carrier dynamics present in the organic spacer that affect the quality of the optical emission.

Extrinsic Effects on the Optical Properties of Surface Color Defects Generated in Hexagonal Boron Nitride Nanosheets.

Hexagonal boron nitride (hBN) is a wide-band gap van der Waals material able to host light-emitting centers behaving as single photon sources. Here, we report the generation of color defects in hBN nanosheets dispersed on different kinds of substrates by thermal treatment processes. The optical properties of these defects have been studied using microspectroscopy techniques and far-field simulations of their light emission. Using these techniques, we have found that subsequent ozone treatments of the deposited hBN nanosheets improve the optical emission properties of created defects, as revealed by their zero-phonon linewidth narrowing and reduction of background emission. Microlocalized color defects deposited on dielectric substrates show bright (≈1 MHz) and stable room-temperature light emission with zero-phonon line peak energy varying from 1.56 to 2.27 eV, being the most probable value 2.16 eV. In addition to this, we have observed a substrate dependence of the optical performance of the generated color defects. The energy range of the emitters prepared on gold substrates is strongly reduced, as compared to that observed in dielectric substrates or even alumina. We attribute this effect to the quenching of low-energy color defects (these of energies lower than 1.9 eV) when gold substrates are used, which reveals the surface nature of the defects created in hBN nanosheets. Results described here are important for future quantum light experiments and their integration in photonic chips.

Emergence of quantum correlations from interacting fibre-cavity polaritons.

Over the past decade, exciton-polaritons in semiconductor microcavities have revealed themselves as one of the richest realizations of a light-based quantum fluid1, subject to fascinating new physics and potential applications2-6. For instance, in the regime of large two-body interactions, polaritons can be used to manipulate the quantum properties of a light field7-9. In this work, we report on the emergence of quantum correlations in laser light transmitted through a fibre-cavity polariton system. We observe a dispersive shape of the autocorrelation function around the polariton resonance that indicates the onset of this regime. The weak amplitude of these correlations indicates a state that still remains far from a low-photon-number state. Nonetheless, given the underlying physical mechanism7, our work opens up the prospect of eventually using polaritons to turn laser light into single photons.

A fluorescent layered oxalato-based canted antiferromagnet.

We report the synthesis and characterization of the first fluorescent oxalato-based canted antiferromagnet. Compound [DOC][MnFe(C2O4)3] (1) (DOC = 3,3'-diethyloxacarbocyanine) combines the well-known canted antiferromagnetic [MnFe(C2O4)3]- honeycomb layers with a fluorescent cationic cyanine-type fluorescent dye. Besides the expected spin canted antiferromagnetic order in the oxalato layer at ca. 29 K, we show the key role played by the anionic oxalato lattice in the optical properties of the cation since it provides isolation of dye cations in the hexagonal cavities of the oxalato-based matrix. The emission of the DOC+ dye shows a redshift and a broadening of the emission as well as an increase in the lifetime compared to the emission of the DOC+ cations in solution. These facts are attributed to the isolation effect of the oxalato-based matrix.

Tunable light emission by exciplex state formation between hybrid halide perovskite and core/shell quantum dots: Implications in advanced LEDs and photovoltaics.

We report the first observation of exciplex state electroluminescence due to carrier injection between the hybrid lead halide perovskite (MAPbI3-xClx) and quantum dots (core/shell PbS/CdS). Single layers of perovskite (PS) and quantum dots (QDs) have been produced by solution processing methods, and their photoluminescent properties are compared to those of bilayer samples in both PS/QD and QD/PS configurations. Exciplex emission at lower energies than the band gap of both PS and QD has been detected. The exciplex emission wavelength of this mixed system can be simply tuned by controlling the QD size. Light-emitting diodes (LEDs) have been fabricated using those configurations, which provide light emission with considerably low turn-on potential. The "color" of the LED can also be tuned by controlling the applied bias. The presence of the exciplex state PS and QDs opens up a broad range of possibilities with important implications not only in tunable LEDs but also in the preparation of intermediate band gap photovoltaic devices with the potentiality of surpassing the Shockley-Queisser limit.

Two-color single-photon emission from InAs quantum dots: toward logic information management using quantum light.

In this work, we propose the use of the Hanbury-Brown and Twiss interferometric technique and a switchable two-color excitation method for evaluating the exciton and noncorrelated electron-hole dynamics associated with single photon emission from indium arsenide (InAs) self-assembled quantum dots (QDs). Using a microstate master equation model we demonstrate that our single QDs are described by nonlinear exciton dynamics. The simultaneous detection of two-color, single photon emission from InAs QDs using these nonlinear dynamics was used to design a NOT AND logic transference function. This computational functionality combines the advantages of working with light/photons as input/output device parameters (all-optical system) and that of a nanodevice (QD size of ∼ 20 nm) while also providing high optical sensitivity (ultralow optical power operational requirements). These system features represent an important and interesting step toward the development of new prototypes for the incoming quantum information technologies.

Purcell effect in photonic crystal microcavities embedding InAs/InP quantum wires.

The spontaneous emission rate and Purcell factor of self-assembled quantum wires embedded in photonic crystal micro-cavities are measured at 80 K by using micro-photoluminescence, under transient and steady state excitation conditions. The Purcell factors fall in the range 1.1 - 2 despite the theoretical prediction of ≈15.5 for the figure of merit. We explain this difference by introducing a polarization dependence on the cavity orientation, parallel or perpendicular with respect to the wire axis, plus spectral and spatial detuning factors for the emitters and the cavity modes, taking in account the finite size of the quantum wires.

Selective optical pumping of charged excitons in unintentionally doped InAs quantum dots.

We have investigated the selective optical pumping of charged excitonic species in a sample containing quantum dots of different sizes and low areal density by photoluminescence and excitation of the photoluminescence microspectroscopy. We study the selective optical excitation of negatively charged excitons as an alternative to commonly used electrical methods. We demonstrate that under resonant excitation in impurity related bands, the selective pumping efficiency can be as high as 85% in small quantum dots having one electron shell and emitting at around 930 nm, and around 65% in big quantum dots having four electron shells and emitting at 1160 nm.