Scaffold-Guided Crystallization of Oriented α-FAPbI Nanowire Arrays for Solar Cells.

Perovskite nanowire arrays with large surface areas for efficient charge transfer and continuous highly crystalline domains for efficient charge transport exhibit ideal morphologies for solar-cell active layers. Here, we introduce a room temperature two-step method to grow dense, vertical nanowire arrays of formamidinium lead iodide (FAPbI). PbI nanocrystals embedded in the cylindrical nanopores of anodized titanium dioxide scaffolds were converted to FAPbI by immersion in a FAI solution for a period of 0.

High-Purity Generation and Switching of Twisted Single Photons.

Quantum technologies, if scaled into a high-dimensional Hilbert space, can dramatically enhance connection capabilities with supporting higher bit rates and ultrasecure information transfer. Twisted single photons, carrying orbital angular momentum (OAM) as an unbounded dimension, could address the growing demand for high-dimensional quantum information encoding and transmission. By hybrid integration of two-dimensional semiconductor WSe_{2} with a spin-orbit-coupled microring resonator, we demonstrate an integrated tunable twisted single photon source with the ability to precisely define and switch between highly pure spin-OAM states.

Free Trions with Near-Unity Quantum Yield in Monolayer MoSe.

Trions, quasiparticles composed of an electron-hole pair bound to a second electron and/or hole, are many-body states with potential applications in optoelectronics. Trions in monolayer transition metal dichalcogenide (TMD) semiconductors have attracted recent interest due to their valley/spin polarization, strong binding energy, and tunability through external gate control. However, low materials quality (, high defect density) has hindered efforts to understand the intrinsic properties of trions.

Enhanced Emission from Interlayer Excitons Coupled to Plasmonic Gap Cavities.

The emergence of interlayer excitons (IEs) from atomic layered transition metal dichalcogenides (TMDCs) heterostructures has drawn tremendous attention due to their unique and exotic optoelectronic properties. Coupling the IEs into optical cavities provides distinctive electromagnetic environments which plays an important role in controlling multiple optical processes such as optical nonlinear generation or photoluminescence enhancement. Here, the integration of IEs in TMDCs into plasmonic nanocavities based on a nanocube on a metallic mirror is reported.

Coupling Spin Defects in a Layered Material to Nanoscale Plasmonic Cavities.

Spin defects in hexagonal boron nitride, and specifically the negatively charged boron vacancy (V ) centers, are emerging candidates for quantum sensing. However, the V defects suffer from low quantum efficiency and, as a result, exhibit weak photoluminescence. In this work, a scalable approach is demonstrated to dramatically enhance the V emission by coupling to a plasmonic gap cavity.

Antiferromagnetic proximity coupling between semiconductor quantum emitters in WSe and van der Waals ferromagnets.

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 effects of substitutional Fe-doping on magnetism in MoSand WSmonolayers.

Doping of two-dimensional (2D) semiconductors has been intensively studied toward modulating their electrical, optical, and magnetic properties. While ferromagnetic 2D semiconductors hold promise for future spintronics and valleytronics, the origin of ferromagnetism in 2D materials remains unclear. Here, we show that substitutional Fe-doping of MoSand WSmonolayers induce different magnetic properties.

Exciton Dipole Orientation of Strain-Induced Quantum Emitters in WSe.

Transition metal dichalcogenides are promising semiconductors to enable advances in photonics and electronics and have also been considered as a host for quantum emitters. Particularly, recent advances demonstrate site-controlled quantum emitters in WSe through strain deformation. Albeit essential for device integration, the dipole orientation of these strain-induced quantum emitters remains unknown.

Enabling room temperature ferromagnetism in monolayer MoS via in situ iron-doping.

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 monolayers in the chemical vapor deposition growth.

Carbon Nanotube Color Centers in Plasmonic Nanocavities: A Path to Photon Indistinguishability at Telecom Bands.

Indistinguishable single photon generation at telecom wavelengths from solid-state quantum emitters remains a significant challenge to scalable quantum information processing. Here we demonstrate efficient generation of "indistinguishable" single photons directly in the telecom O-band from aryl-functionalized carbon nanotubes by overcoming the emitter quantum decoherence with plasmonic nanocavities. With an unprecedented single-photon spontaneous emission time down to 10 ps (from initially 0.

Magnetic Proximity Coupling of Quantum Emitters in WSe to van der Waals Ferromagnets.

The realization of on-chip quantum networks requires tunable quantum states to encode information carriers on them. We show that CrGeTe (CGT) as a van der Waals ferromagnet can enable magnetic proximity coupling to site-controlled quantum emitters in WSe, giving rise to ultrahigh exciton 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.

Near-Unity Light Collection Efficiency from Quantum Emitters in Boron Nitride by Coupling to Metallo-Dielectric Antennas.

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.

Deterministic coupling of site-controlled quantum emitters in monolayer WSe to plasmonic nanocavities.

Solid-state single-quantum emitters are crucial resources for on-chip photonic quantum technologies and require efficient cavity-emitter coupling to realize quantum networks beyond the single-node level. Monolayer WSe, a transition metal dichalcogenide semiconductor, can host randomly located quantum emitters, while nanobubbles as well as lithographically defined arrays of pillars in contact with the transition metal dichalcogenide act as spatially controlled stressors. The induced strain can then create excitons at defined locations.

Suppression of exciton dephasing in sidewall-functionalized carbon nanotubes embedded into metallo-dielectric antennas.

Covalent functionalization of single-walled carbon nanotubes (SWCNTs) is a promising route to enhance the quantum yield of exciton emission and can lead to single-photon emission at room temperature. However, the spectral linewidth of the defect-related E11* emission remains rather broad. Here, we systematically investigate the low-temperature exciton emission of individual SWCNTs that have been dispersed with sodium-deoxycholate (DOC) and polyfluorene (PFO-BPy), are grown by laser vaporization (LV) or by CoMoCat techniques and are functionalized with oxygen as well as 3,5-dichlorobenzene groups.

Remarkable long-term stability of nanoconfined metal-halide perovskite crystals against degradation and polymorph transitions.

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.

Purcell-enhanced quantum yield from carbon nanotube excitons coupled to plasmonic nanocavities.

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.

Trion-Species-Resolved Quantum Beats in MoSe.

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 inhomogeneously broadened material. Here we employ h-BN-encapsulated and electrically gated MoSe to reveal coherence properties of trion species directly in the linear optical response.

Low-Temperature Single Carbon Nanotube Spectroscopy of sp Quantum Defects.

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.

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.

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 (13)C atomic concentration, as would be expected for pure dephasing of excitons with acoustic phonons.

Improved photoresponse with enhanced photoelectric contribution in fully suspended graphene photodetectors.

Graphene's unique optoelectronic properties are promising to realize photodetectors with ultrafast photoresponse over a wide spectral range from far-infrared to ultraviolet radiation. The underlying mechanism of the photoresponse has been a particular focus of recent work and was found to be either photoelectric or photo-thermoelectric in nature and enhanced by hot carrier effects. Graphene supported by a substrate was found to be dominated by the photo-thermoelectric effect, which is known to be an order of magnitude slower than the photoelectric effect.

Prolonged spontaneous emission and dephasing of localized excitons in air-bridged carbon nanotubes.

The bright exciton emission of carbon nanotubes is appealing for optoelectronic devices and fundamental studies of light-matter interaction in one-dimensional nanostructures. However, to date, the photophysics of excitons in carbon nanotubes is largely affected by extrinsic effects. Here we perform time-resolved photoluminescence measurements over 14 orders of magnitude for ultra-clean carbon nanotubes bridging an air gap over pillar posts.

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.

Optical control of edge chirality in graphene.

We performed optical annealing experiments at the edges of nanopatterned graphene to study the resultant edge reconstruction. The lithographic patterning direction was orthogonal to a zigzag edge. μ-Raman spectroscopy shows an increase in the polarization contrast of the G band as a function of annealing time.

Holographic control of motive shape in plasmonic nanogap arrays.

Here we demonstrate that 4-beam holographic lithography can be utilized to create plasmonic nanogaps that are 70 times smaller than the laser wavelength (488 nm). This was achieved by controlling phase, polarization, and laser beam intensity in order to tune the relative spacing of the two sublattices in the interference pattern of a compound-lattice in combination with the nonlinear resist response. Exemplarily, twin and triplet motive features were designed and patterned into polymer in a single exposure step and then transferred into gold nanogap arrays resulting in an average gap size of 22 nm and smallest features down to 7 nm.