Room-temperature quantum emission from interface excitons in mixed-dimensional heterostructures.

The development of van der Waals heterostructures has introduced unconventional phenomena that emerge at atomically precise interfaces. For example, interlayer excitons in two-dimensional transition metal dichalcogenides show intriguing optical properties at low temperatures. Here we report on room-temperature observation of interface excitons in mixed-dimensional heterostructures consisting of two-dimensional tungsten diselenide and one-dimensional carbon nanotubes. Bright emission peaks originating from the interface are identified, spanning a broad energy range within the telecommunication wavelengths. The effect of band alignment is investigated by systematically varying the nanotube bandgap, and we assign the new peaks to interface excitons as they only appear in type-II heterostructures. Room-temperature localization of low-energy interface excitons is indicated by extended lifetimes as well as small excitation saturation powers, and photon correlation measurements confirm antibunching. With mixed-dimensional van der Waals heterostructures where band alignment can be engineered, new opportunities for quantum photonics are envisioned.

Resonant exciton transfer in mixed-dimensional heterostructures for overcoming dimensional restrictions in optical processes.

Nanomaterials exhibit unique optical phenomena, in particular excitonic quantum processes occurring at room temperature. The low dimensionality, however, imposes strict requirements for conventional optical excitation, and an approach for bypassing such restrictions is desirable. Here we report on exciton transfer in carbon-nanotube/tungsten-diselenide heterostructures, where band alignment can be systematically varied. The mixed-dimensional heterostructures display a pronounced exciton reservoir effect where the longer-lifetime excitons within the two-dimensional semiconductor are funneled into carbon nanotubes through diffusion. This new excitation pathway presents several advantages, including larger absorption areas, broadband spectral response, and polarization-independent efficiency. When band alignment is resonant, we observe substantially more efficient excitation via tungsten diselenide compared to direct excitation of the nanotube. We further demonstrate simultaneous bright emission from an array of carbon nanotubes with varied chiralities and orientations. Our findings show the potential of mixed-dimensional heterostructures and band alignment engineering for energy harvesting and quantum applications through exciton manipulation.

Electric-Field Induced Activation of Dark Excitonic States in Carbon Nanotubes.

Electrical activation of optical transitions to parity-forbidden dark excitonic states in individual carbon nanotubes is reported. We examine electric-field effects on various excitonic states by simultaneously measuring photocurrent and photoluminescence. As the applied field increases, we observe an emergence of new absorption peaks in the excitation spectra. From the diameter dependence of the energy separation between the new peaks and the ground state of E11 excitons, we attribute the peaks to the dark excited states which became optically active due to the applied field. Field-induced exciton dissociation can explain the photocurrent threshold field, and the edge of the E11 continuum states has been identified by extrapolating to zero threshold.

Gate-controlled generation of optical pulse trains using individual carbon nanotubes.

In single-walled carbon nanotubes, electron-hole pairs form tightly bound excitons because of limited screening. These excitons display a variety of interactions and processes that could be exploited for applications in nanoscale photonics and optoelectronics. Here we report on optical pulse-train generation from individual air-suspended carbon nanotubes under an application of square-wave gate voltages. Electrostatically induced carrier accumulation quenches photoluminescence, while a voltage sign reversal purges those carriers, resetting the nanotubes to become luminescent temporarily. Frequency-domain measurements reveal photoluminescence recovery with characteristic frequencies that increase with excitation laser power, showing that photoexcited carriers provide a self-limiting mechanism for pulsed emission. Time-resolved measurements directly confirm the presence of an optical pulse train synchronized to the gate voltage signal, and flexible control over pulse timing and duration is also demonstrated. These results identify an unconventional route for optical pulse generation and electrical-to-optical signal conversion, opening up new prospects for controlling light at the nanoscale.

Illuminating the future of silicon photonics: optical coupling of carbon nanotubes to microrings.

Advances in carbon nanotube material quality and processing techniques have led to an increased interest in nanotube photonics. In particular, emission in the telecommunication wavelengths makes nanotubes compatible with silicon photonics. Noury et al (2014 Nanotechnology 25 215201) have reported on carbon nanotube photoluminescence coupled to silicon microring resonators, underscoring the advantage of combining carbon nanotube emitters with silicon photonics. Their results open up the possibility of using nanotubes in other waveguide-based devices, taking advantage of well-established technologies.

Ultralow mode-volume photonic crystal nanobeam cavities for high-efficiency coupling to individual carbon nanotube emitters.

The unique emission properties of single-walled carbon nanotubes are attractive for achieving increased functionality in integrated photonics. In addition to being room-temperature telecom-band emitters that can be directly grown on silicon, they are ideal for coupling to nanoscale photonic structures. Here we report on high-efficiency coupling of individual air-suspended carbon nanotubes to silicon photonic crystal nanobeam cavities. Photoluminescence images of dielectric- and air-mode cavities reflect their distinctly different mode profiles and show that fields in the air are important for coupling. We find that the air-mode cavities couple more efficiently, and estimated spontaneous emission coupling factors reach a value as high as 0.85. Our results demonstrate advantages of ultralow mode-volumes in air-mode cavities for coupling to low-dimensional nanoscale emitters.

Spontaneous exciton dissociation in carbon nanotubes.

Simultaneous photoluminescence and photocurrent measurements on individual single-walled carbon nanotubes reveal spontaneous dissociation of excitons into free electron-hole pairs. The correlation of luminescence intensity and photocurrent shows that a significant fraction of excitons are dissociating before recombination. Furthermore, the combination of optical and electrical signals also allows for extraction of the absorption cross section and the oscillator strength. Our observations explain the reasons why photoconductivity measurements in single-walled carbon nanotubes are straightforward despite the large exciton binding energies.

Exciton diffusion in air-suspended single-walled carbon nanotubes.

Direct measurements of the diffusion length of excitons in air-suspended single-walled carbon nanotubes are reported. Photoluminescence microscopy is used to identify individual nanotubes and to determine their lengths and chiral indices. Exciton diffusion length is obtained by comparing the dependence of photoluminescence intensity on the nanotube length to numerical solutions of diffusion equations. We find that the diffusion length in these clean, as-grown nanotubes is significantly longer than those reported for micelle-encapsulated nanotubes.

Current-induced spin polarization in strained semiconductors.

The polarization of conduction electron spins due to an electrical current is observed in strained nonmagnetic semiconductors using static and time-resolved Faraday rotation. The density, lifetime, and orientation rate of the electrically polarized spins are characterized by a combination of optical and electrical methods. In addition, the dynamics of the current-induced spins are investigated by utilizing electrical pulses generated from a photoconductive switch. These results demonstrate the possibility of a spin source for semiconductor spintronic devices without the use of magnetic materials.

Observation of the spin Hall effect in semiconductors.

Electrically induced electron-spin polarization near the edges of a semiconductor channel was detected and imaged with the use of Kerr rotation microscopy. The polarization is out-of-plane and has opposite sign for the two edges, consistent with the predictions of the spin Hall effect. Measurements of unstrained gallium arsenide and strained indium gallium arsenide samples reveal that strain modifies spin accumulation at zero magnetic field. A weak dependence on crystal orientation for the strained samples suggests that the mechanism is the extrinsic spin Hall effect.