Abstract
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 dipole-allowed 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.
Abstract
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.
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
) up to F
= 180 (average F
= 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.
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 via use of larger diameter SWCNTs.
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.
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.
The realization of on-chip quantum networks requires tunable quantum states to encode information carriers on them. We show that Cr2Ge2Te6 (CGT) as a van der Waals ferromagnet can enable magnetic ...proximity coupling to site-controlled quantum emitters in WSe2, giving rise to ultrahigh exciton g factors up to 20 ± 1. By comparing the same site-controlled quantum emitter before and after ferromagnetic proximity coupling, we also demonstrate a technique to directly measure the resulting magnetic exchange field (MEF) strength. Experimentally determined values of MEF up to 1.2 ± 0.2 meV in the saturation regime approach the theoretical limit of 2.1 meV that was determined from density functional theory calculations of the CGT/WSe2 heterostructure. Our work extends the on-chip control of magneto-optical properties of excitons via van der Waals heterostructures to solid-state quantum emitters.
van der Waals ferromagnets have gained significant interest due to their unique ability to provide magnetic response even at the level of a few monolayers. Particularly in combination with 2D ...semiconductors, such as the transition metal dichalcogenide WSe2, one can create heterostructures that feature unique magneto-optical response in the exciton emission through the magnetic proximity effect. Here we use 0D quantum emitters in WSe2 to probe for the ferromagnetic response in heterostructures with Fe3GT and Fe5GT ferromagnets through an all-optical read-out technique that does not require electrodes. The spectrally narrow spin-doublet of the WSe2 quantum emitters allowed to fully resolve the hysteretic magneto-response in the exciton emission, revealing the characteristic signature of both ferro- and antiferromagnetic proximity coupling that originates from the interplay among Fe3GT or Fe5GT, a thin surface oxide, and the spin doublets of the quantum emitters. Our work highlights the utility of 0D quantum emitters for probing interface magnetic dipoles in vdW heterostructures with high precision. The observed hysteretic magneto response in the exciton emission of quantum emitters adds further new degrees of freedom for spin and g-factor manipulation of quantum states.
Metal-halide perovskites are promising candidates to advance optoelectronic devices but are known to suffer from rapid material degradation. Here we demonstrate that nanoconfinement is an effective ...strategy for the long-term stabilization of metal-halide perovskite MAPbI3 crystals against humidity-induced degradation and temperature-induced polymorph transitions. Two-dimensional X-ray diffraction patterns of MAPbI3 films reveal an unprecedented air-stability of up to 594 days in non-chemically modified, non-passivated MAPbI3 films deposited on substrates imposing complete 2D confinement on the tens of nanometers length scale. Temperature-dependent X-ray diffraction analysis and optical spectroscopy further reveal the suppression of temperature-dependent phase transitions in nanoconfined MAPbI3 crystals. Most notably, the high-temperature cubic phase of MAPbI3, typically stable at temperatures above 327 K, remains present until a temperature of 170 K when the perovskite crystals are nanoconfined within the 100 nm diameter pores of anodized aluminum oxide templates. Photoluminescence mapping confirms that nanoconfined MAPbI3 crystals exhibit spatial uniformity on the tens of microns length scale, suggesting that nanoconfinement is an effective strategy for the formation of high-quality, stable MAPbI3 crystals across large areas.
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