Trion Species-Resolved Quantum Beats in MoSe2

Monolayer photonic materials offer a tremendous potential for on-chip optoelectronic devices. Their realization requires knowledge of optical coherence properties of excitons and trions that have so far been limited to nonlinear optical experiments carried out with strongly inhomogenously broadened material. Here we employ h-BN encapsulated and electrically gated MoSe2 to reveal coherence properties of trion-species directly in the linear optical response. Autocorrelation measurements reveal long dephasing times up to T2=1.16+-0.05 ps for positively charged excitons. Gate dependent measurements provide evidence that the positively-charged trion forms via spatially localized hole states making this trion less prone to dephasing in the presence of elevated hole carrier concentrations. Quantum beat signatures demonstrate coherent coupling between excitons and trions that have a dephasing time up to 0.6 ps, a two-fold increase over those in previous reports. A key merit of the prolonged exciton/trion coherences is that they were achieved in a linear optical experiment, and thus are directly relevant to applications in nanolasers, coherent control, and on-chip quantum information processing requiring long photon coherence.Comment: 21 pages, 6 figures, 2 SOI figure

Quantum Light Signatures and Nanosecond Spectral Diffusion from Cavity-Embedded Carbon Nanotubes

Single-walled carbon nanotubes (SWCNTs) are considered for novel optoelectronic and quantum photonic devices, such as single photon sources, but methods must be developed to enhance the light extraction and spectral purity, while simultaneously preventing multiphoton emission as well as spectral diffusion and blinking in dielectric environments of a cavity. Here we demonstrate that utilization of nonpolar polystyrene as a cavity dielectric completely removes spectral diffusion and blinking in individual SWCNTs on the millisecond to multisecond time scale, despite the presence of surfactants. With these cavity-embedded SWCNT samples, providing a 50-fold enhanced exciton emission into the far field, we have been able to carry out photophysical studies for the first time with nanosecond timing resolution. We uncovered that fast spectral diffusion processes (1–3 ns) remain that make significant contributions to the spectral purity, thereby limiting the use of SWCNTs in quantum optical applications requiring indistinguishable photons. Measured quantum light signatures reveal pronounced photon antibunching (<i>g</i>²(0) = 0.15) accompanied by side-peak bunching signatures indicative of residual blinking on the submicrosecond time scale. The demonstrated enhanced single photon emission from cavity-embedded SWCNTs is promising for applications in quantum key distribution, while the demonstrated passivation effect of polystyrene with respect to the stability of the optical emission opens a novel pathway toward optoelectronic devices with enhanced performance

Strong Acoustic Phonon Localization in Copolymer-Wrapped Carbon Nanotubes

Understanding and controlling exciton–phonon interactions in carbon nanotubes has important implications for producing efficient nanophotonic devices. Here we show that laser vaporization-grown carbon nanotubes display ultranarrow luminescence line widths (120 μeV) and well-resolved acoustic phonon sidebands at low temperatures when dispersed with a polyfluorene copolymer. Remarkably, we do not observe a correlation of the zero-phonon line width with ¹³C atomic concentration, as would be expected for pure dephasing of excitons with acoustic phonons. We demonstrate that the ultranarrow and phonon sideband-resolved emission spectra can be fully described by a model assuming extrinsic acoustic phonon localization at the nanoscale, which holds down to 6-fold narrower spectral line width compared to previous work. Interestingly, both exciton and acoustic phonon wave functions are strongly spatially localized within 5 nm, possibly mediated by the copolymer backbone, opening future opportunities to engineer dephasing and optical bandwidth for applications in quantum photonics and cavity optomechanics

Nonmagnetic Quantum Emitters in Boron Nitride with Ultranarrow and Sideband-Free Emission Spectra

Hexagonal boron nitride (hBN) is an emerging material in nanophotonics and an attractive host for color centers for quantum photonic devices. Here, we show that optical emission from individual quantum emitters in hBN is spatially correlated with structural defects and can display ultranarrow zero-phonon line width down to 45 μeV if spectral diffusion is effectively eliminated by proper surface passivation. We demonstrate that undesired emission into phonon sidebands is largely absent for this type of emitter. In addition, magneto-optical characterization reveals cycling optical transitions with an upper bound for the g-factor of 0.2 ± 0.2. Spin-polarized density functional theory calculations predict possible commensurate transitions between like-spin electron states, which are in excellent agreement with the experimental nonmagnetic defect center emission. Our results constitute a step toward the realization of narrowband quantum light sources and the development of spin–photon interfaces within 2D materials for future chip-scale quantum networks

Broadband Light Collection Efficiency Enhancement of Carbon Nanotube Excitons Coupled to Metallo-Dielectric Antenna Arrays

The realization of on-chip quantum networks ideally requires lossless interfaces between photons and solid-state quantum emitters. We propose and demonstrate on-chip arrays of metallo-dielectric antennas (MDA) that are tailored toward efficient and broadband light collection from individual embedded carbon nanotube quantum emitters by trapping air gaps on chip that form cavity modes. Scalable implementation is realized by employing polymer layer dry-transfer techniques that avoid solvent incompatibility issues, as well as a planar design that avoids solid-immersion lenses. Cryogenic measurements demonstrate 7-fold enhanced exciton intensity when compared to emitters located on bare wafers, corresponding to a light collection efficiency (LCE) up to 92% in the best case (average LCE of 69%) into a narrow output cone of ±15° that enables a priori fiber-to-chip butt coupling. The demonstrated MDA arrays are directly compatible with other quantum systems, particularly 2D materials, toward enabling efficient on-chip quantum light sources or spin-photon interfaces requiring unity light collection, both at cryogenic or room temperature

Low-Temperature Single Carbon Nanotube Spectroscopy of sp³ Quantum Defects

Aiming to unravel the relationship between chemical configuration and electronic structure of sp³ defects of aryl-functionalized (6,5) single-walled carbon nanotubes (SWCNTs), we perform low-temperature single nanotube photoluminescence (PL) spectroscopy studies and correlate our observations with quantum chemistry simulations. We observe sharp emission peaks from individual defect sites that are spread over an extremely broad, 1000–1350 nm, spectral range. Our simulations allow us to attribute this spectral diversity to the occurrence of six chemically and energetically distinct defect states resulting from topological variation in the chemical binding configuration of the monovalent aryl groups. Both PL emission efficiency and spectral line width of the defect states are strongly influenced by the local dielectric environment. Wrapping the SWCNT with a polyfluorene polymer provides the best isolation from the environment and yields the brightest emission with near-resolution limited spectral line width of 270 μeV, as well as spectrally resolved emission wings associated with localized acoustic phonons. Pump-dependent studies further revealed that the defect states are capable of emitting single, sharp, isolated PL peaks over 3 orders of magnitude increase in pump power, a key characteristic of two-level systems and an important prerequisite for single-photon emission with high purity. These findings point to the tremendous potential of sp³ defects in development of room temperature quantum light sources capable of operating at telecommunication wavelengths as the emission of the defect states can readily be extended to this range <i>via</i> use of larger diameter SWCNTs