Single-walled carbon nanotubes (SWCNTs) are promising absorbers and emitters to enable novel photonic applications and devices but are also known to suffer from low optical quantum yields. Here we demonstrate SWCNT excitons coupled to plasmonic nanocavity arrays reaching deeply into the Purcell regime with Purcell factors (F P) up to F P = 180 (average F P = 57), Purcell-enhanced quantum yields of 62% (average 42%), and a photon emission rate of 15 MHz into the first lens. The cavity coupling is quasi-deterministic since the photophysical properties of every SWCNT are enhanced by at least one order of magnitude. Furthermore, the measured ultra-narrow exciton linewidth (18 μeV) reaches the radiative lifetime limit, which is promising towards generation of transform-limited single photons. To demonstrate utility beyond quantum light sources we show that nanocavity-coupled SWCNTs perform as single-molecule thermometers detecting plasmonically induced heat at cryogenic temperatures in a unique interplay of excitons, phonons, and plasmons at the nanoscale.

Control over the out-of-plane molecular orientation of solution-processed organic semiconductors is a long-standing challenge in the organic electronics community. Here, a generalizable strategy using nanoconfinement to direct the nucleation of small-molecule organic semiconductors during solution-phase deposition is presented. Using a facile dip-coating process, triisopropylsilylethynylderivatized acene molecules were deposited onto nanoporous anodized aluminum oxide (AAO) scaffolds with average pore diameters ranging from 60 to 200 nm. Preferentially oriented nuclei were found to form within the cylindrical AAO nanopores such that the fast growth direction (i.e., the π-stack direction) aligned with the long axes of the pores. Crystal growth then propagated above the scaffold, resulting in the formation of vertical crystal arrays with the high surface energy π-planes exposed at the crystal tips. The diameters and heights of these crystals were tunable over ranges of 100−600 nm and 0.8−6.7 μm, respectively, by varying the dip-coating speed and scaffold pore diameters. Photoluminescence (PL) experiments further revealed an 8-fold enhancement of the PL signal from vertical crystal arrays compared to horizontal crystals deposited on flat SiO 2 substrates due to waveguiding along the crystal length. Critically, this strategy is compatible with continuous deposition techniques that will enable the high-throughput, large-area manufacturing of flexible and inexpensive optoelectronic devices.

The low-frequency Raman spectra of metal-halide perovskites are reported using a combination of a 976 nm laser and nanoconfinement to stabilize the crystals against temperature-induced polymorph transitions and humidity-induced degradation.

Light carries both spin angular momentum (SAM) and orbital angular momentum (OAM), which can be used as potential degrees of freedom for quantum information processing. Quantum emitters are ideal candidates towards on-chip control and manipulation of the full SAM–OAM state space. Here, we show coupling of a spin-polarized quantum emitter in a monolayer W S e 2 with the whispering gallery mode of a S i 3 N 4 ring resonator. The cavity mode carries a transverse SAM of σ = ± 1 in the evanescent regions, with the sign depending on the orbital power flow direction of the light. By tailoring the cavity–emitter interaction, we couple the intrinsic spin state of the quantum emitter to the SAM and propagation direction of the cavity mode, which leads to spin–orbit locking and subsequent chiral single-photon emission. Furthermore, by engineering how light is scattered from the WGM, we create a high-order Bessel beam which opens up the possibility to generate optical vortex carrying OAM states.