Room-temperature strong coupling between CdSe nanoplatelets and a metal-DBR Fabry-Pérot cavity.

The generation of exciton-polaritons through strong light-matter interactions represents an emerging platform for exploring quantum phenomena. A significant challenge in colloidal nanocrystal-based polaritonic systems is the ability to operate at room temperature with high fidelity. Here, we demonstrate the generation of room-temperature exciton-polaritons through the coupling of CdSe nanoplatelets (NPLs) with a Fabry-Pérot optical cavity, leading to a Rabi splitting of 74.6 meV. Quantum-classical calculations accurately predict the complex dynamics between the many dark state excitons and the optically allowed polariton states, including the experimentally observed lower polariton photoluminescence emission, and the concentration of photoluminescence intensities at higher in-plane momenta as the cavity becomes more negatively detuned. The Rabi splitting measured at 5 K is similar to that at 300 K, validating the feasibility of the temperature-independent operation of this polaritonic system. Overall, these results show that CdSe NPLs are an excellent material to facilitate the development of room-temperature quantum technologies.

Quantum dynamics simulations of the 2D spectroscopy for exciton polaritons.

We develop an accurate and numerically efficient non-adiabatic path-integral approach to simulate the non-linear spectroscopy of exciton-polariton systems. This approach is based on the partial linearized density matrix approach to model the exciton dynamics with explicit propagation of the phonon bath environment, combined with a stochastic Lindblad dynamics approach to model the cavity loss dynamics. Through simulating both linear and polariton two-dimensional electronic spectra, we systematically investigate how light-matter coupling strength and cavity loss rate influence the optical response signal. Our results confirm the polaron decoupling effect, which is the reduced exciton-phonon coupling among polariton states due to the strong light-matter interactions. We further demonstrate that the polariton coherence time can be significantly prolonged compared to the electronic coherence outside the cavity.

Co-designed metaoptoelectronic deep learning.

A metaoptical system is co-designed with electronic hardware to implement deep learning image recognition. The optical convolution block includes a reflective metasurface to perform one layer of a deep neural network. The optical and digital components are jointly optimized to perform an image classification task attaining 65% accuracy, which is close to the 66% accuracy of a fully-digital network where the optical block is replaced by a digital convolution layer.

Design framework for metasurface optics-based convolutional neural networks.

Deep learning using convolutional neural networks (CNNs) has been shown to significantly outperform many conventional vision algorithms. Despite efforts to increase the CNN efficiency both algorithmically and with specialized hardware, deep learning remains difficult to deploy in resource-constrained environments. In this paper, we propose an end-to-end framework to explore how to optically compute the CNNs in free-space, much like a computational camera. Compared to existing free-space optics-based approaches that are limited to processing single-channel (i.e., gray scale) inputs, we propose the first general approach, based on nanoscale metasurface optics, that can process RGB input data. Our system achieves up to an order of magnitude energy savings and simplifies the sensor design, all the while sacrificing little network accuracy.

Molecular Polaritons Generated from Strong Coupling between CdSe Nanoplatelets and a Dielectric Optical Cavity.

We demonstrate the formation of CdSe nanoplatelet (NPL) exciton-polaritons in a distributed Bragg reflector (DBR) cavity. The molecule-cavity hybrid system is in the strong coupling regime with an 83 meV Rabi splitting, characterized from angle-resolved reflectance and photoluminescence measurements. Mixed quantum-classical dynamics simulations are used to investigate the polariton photophysics of the hybrid system by treating the electronic and photonic degrees of freedom (DOF) quantum mechanically and the nuclear phononic DOF classically. Our numerical simulations of the angle-resolved photoluminescence (PL) agree extremely well with the experimental data, providing a fundamental explanation of the asymmetric intensity distribution of the upper and lower polariton branches. Our results also provide mechanistic insights into the importance of phonon-assisted nonadiabatic transitions among polariton states, which are reflected in the various features of the PL spectra. This work proves the feasibility of coupling nanoplatelet electronic states with the photon states of a dielectric cavity to form a hybrid system and provides a new platform for investigating cavity-mediated physical and chemical processes.

Spectroscopic properties unique to nano-emitters.

The spectral position of light emission from an individual carbon nanotube is shown to depend on the location of the nanotube within the focal spot, while no such effect is present for macroscopic emitters. In addition, in contrast to macroscopic emitters, the measured line width from the nanotube emitter is independent of spectrometer entrance slit width. The effects are general for any nanoscale optical emitter with at least one dimension smaller than the optical diffraction limit.

Screening of excitons in single, suspended carbon nanotubes.

Resonant Raman spectroscopy of single carbon nanotubes suspended across trenches displays red-shifts of up to 30 meV of the electronic transition energies as a function of the surrounding dielectric environment. We develop a simple scaling relationship between the exciton binding energy and the external dielectric function and thus quantify the effect of screening. Our results imply that the underlying particle interaction energies change by hundreds of meV.