Aiming to unravel the relationship between chemical configuration and electronic structure of sp 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 sp 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 via use of larger diameter SWCNTs.
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.
Two-dimensional semiconductors, including transition metal dichalcogenides, are of interest in electronics and photonics but remain nonmagnetic in their intrinsic form. Previous efforts to form two-dimensional dilute magnetic semiconductors utilized extrinsic doping techniques or bulk crystal growth, detrimentally affecting uniformity, scalability, or Curie temperature. Here, we demonstrate an in situ substitutional doping of Fe atoms into MoS 2 monolayers in the chemical vapor deposition growth. The iron atoms substitute molybdenum sites in MoS 2 crystals, as confirmed by transmission electron microscopy and Raman signatures. We uncover an Fe-related spectral transition of Fe:MoS 2 monolayers that appears at 2.28 eV above the pristine bandgap and displays pronounced ferromagnetic hysteresis. The microscopic origin is further corroborated by density functional theory calculations of dipoleallowed transitions in Fe:MoS 2. Using spatially integrating magnetization measurements and spatially resolving nitrogen-vacancy center magnetometry, we show that Fe:MoS 2 monolayers remain magnetized even at ambient conditions, manifesting ferromagnetism at room temperature.
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.
The bright and stable single-photon emission under room temperature conditions from color centers in hexagonal boron nitride (hBN) is considered as one of the most promising quantum light sources for quantum cryptography as well as spin-based qubits, similar to recent advances in nitrogen-vacancy centers in diamond. To this end, integration with cavity or waveguide modes is required to enable ideally lossless transduction of quantum light states. Here, we demonstrate a scheme to embed hBN quantum emitters into on-chip arrays of metallo-dielectric antennas that provides near unity light collection efficiencies with experimental values up to 98%, i.e. a 7fold enhancement compared to bare quantum emitters. Room-temperature quantum light emission in the 700 nm band is characterized with single-photon emission rates into the first lens up to 44 MHz under continuous excitation and up to 10 MHz under 80 MHz pulsed excitation (0.13 photons per trigger pulse) into a narrow output cone (±15°) that facilitates fiber butt-coupling. We furthermore provide here a direct measurement of the quantum yield under pulsed excitation with values of 6−12% for hBN nanoflakes. Our demonstrated scheme could enable low loss spin−photon interfaces on a chip.
Reducing the size of metal halide perovskite crystals to the nanoscale has been demonstrated to stabilize high-performance metastable polymorphs at room temperature. Cesium lead iodide (CsPbI3), for example, typically exists as the insulating δ-phase at room temperature but can adopt the narrow-bandgap γ-phase when the crystal size is reduced to the nanometer length scale. Here we advance a fundamental understanding of the role of nanoconfinement in CsPbI3 polymorph stabilization through a combination of X-ray diffraction and temperature-dependent photoluminescence. Using a wet annealing method to directly form γ-CsPbI3 from solution in the cylindrical nanopores of anodized aluminum oxide, we discovered that nanoconfinement lowers the δ−γ solid-state phase transition temperature from 448 K in the bulk to 370 K. Once formed, nanoconfined γ-CsPbI3 crystals were found to be stable across the temperature range of 4–610 K and upon an unprecedented one year of air exposure at room temperature. Taking advantage of the nanoconfinement-induced suppression of phase transitions, we report for the first time a detailed analysis of electron–phonon interactions in γ-CsPbI3 via temperature-dependent photoluminescent measurements. In-depth analysis of the temperature-dependent peak broadening revealed electron–phonon interactions to be dominated by Fröhlich scattering, similar to that observed in inorganic–organic hybrid perovskite systems. Photoluminescence mapping further confirmed that nanoconfined γ-CsPbI3 crystals exhibit spatial uniformity on the tens of micrometers length scale, suggesting nanoconfinement as a promising strategy to form stable, high-performance perovskite films from solution for light-emitting and light-harvesting applications.
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.
Isolated spins are the focus of intense scientific exploration due to their potential role as qubits for quantum information science. Optical access to single spins, demonstrated in III-V semiconducting quantum dots, has fueled research aimed at realizing quantum networks. More recently, quantum emitters in atomically thin materials such as tungsten diselenide have been demonstrated to host optically addressable single spins by means of electrostatic doping the localized excitons. Electrostatic doping is not the only route to charging localized quantum emitters and another path forward is through band structure engineering using van der Waals heterojunctions. Critical to this second approach is to interface tungsten diselenide with other van der Waals materials with relative band-alignments conducive to the phenomenon of charge transfer. In this work we show that the Type-II band-alignment between tungsten diselenide and chromium triiodide can be exploited to excite localized charged excitons in tungsten diselenide. Leveraging spin-dependent charge transfer in the device, we demonstrate spin selectivity in the preparation of the spin-valley state of localized single holes. Combined with the use of strain-inducing nanopillars to coordinate the spatial location of tungsten diselenide quantum emitters, we uncover the possibility of realizing large-scale deterministic arrays of optically addressable spin-valley holes in a solid state platform.
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