Engineering the Impact of Phonon Dephasing on the Coherence of a WSe_{2} Single-Photon Source via Cavity Quantum Electrodynamics.

Emitter dephasing is one of the key issues in the performance of solid-state single-photon sources. Among the various sources of dephasing, acoustic phonons play a central role in adding decoherence to the single-photon emission. Here, we demonstrate that it is possible to tune and engineer the coherence of photons emitted from a single WSe_{2} monolayer quantum dot via selectively coupling it to a spectral cavity resonance. We utilize an open cavity to demonstrate spectral enhancement, leveling, and suppression of the highly asymmetric phonon sideband, finding excellent agreement with a microscopic description of the exciton-phonon dephasing in a truly two-dimensional system. Moreover, the impact of cavity tuning on the dephasing is directly assessed via optical interferometry, which points out the capability to utilize light-matter coupling to steer and design dephasing and coherence of quantum emitters in atomically thin crystals.

Monolayer-Based Single-Photon Source in a Liquid-Helium-Free Open Cavity Featuring 65% Brightness and Quantum Coherence.

Solid-state single-photon sources are central building blocks in quantum information processing. Atomically thin crystals have emerged as sources of nonclassical light; however, they perform below the state-of-the-art devices based on volume crystals. Here, we implement a bright single-photon source based on an atomically thin sheet of WSe2 coupled to a tunable optical cavity in a liquid-helium-free cryostat without the further need for active stabilization. Its performance is characterized by high single-photon purity (g(2)(0) = 4.7 ± 0.7%) and record-high, first-lens brightness of linearly polarized photons of 65 ± 4%, representing a decisive step toward real-world quantum applications. The high performance of our devices allows us to observe two-photon interference in a Hong-Ou-Mandel experiment with 2% visibility limited by the emitter coherence time and setup resolution. Our results thus demonstrate that the combination of the unique properties of two-dimensional materials and versatile open cavities emerges as an inspiring avenue for novel quantum optoelectronic devices.

Second-Order Temporal Coherence of Polariton Lasers Based on an Atomically Thin Crystal in a Microcavity.

Bosonic condensation and lasing of exciton polaritons in microcavities is a fascinating solid-state phenomenon. It provides a versatile platform to study out-of-equilibrium many-body physics and has recently appeared at the forefront of quantum technologies. Here, we study the photon statistics via the second-order temporal correlation function of polariton lasing emerging from an optical microcavity with an embedded atomically thin MoSe_{2} crystal. Furthermore, we investigate the macroscopic polariton phase transition for varying excitation powers and temperatures. The lower-polariton exhibits photon bunching below the threshold, implying a dominant thermal distribution of the emission, while above the threshold, the second-order correlation transits towards unity, which evidences the formation of a coherent state. Our findings are in agreement with a microscopic numerical model, which explicitly includes scattering with phonons on the quantum level.

Hybridized Exciton-Photon-Phonon States in a Transition Metal Dichalcogenide van der Waals Heterostructure Microcavity.

Excitons in atomically thin transition-metal dichalcogenides (TMDs) have been established as an attractive platform to explore polaritonic physics, owing to their enormous binding energies and giant oscillator strength. Basic spectral features of exciton polaritons in TMD microcavities, thus far, were conventionally explained via two-coupled-oscillator models. This ignores, however, the impact of phonons on the polariton energy structure. Here we establish and quantify the threefold coupling between excitons, cavity photons, and phonons. For this purpose, we employ energy-momentum-resolved photoluminescence and spatially resolved coherent two-dimensional spectroscopy to investigate the spectral properties of a high-quality-factor microcavity with an embedded WSe_{2} van der Waals heterostructure at room temperature. Our approach reveals a rich multibranch structure which thus far has not been captured in previous experiments. Simulation of the data reveals hybridized exciton-photon-phonon states, providing new physical insight into the exciton polariton system based on layered TMDs.

Improving the Water Oxidation Efficiency with a Light-Induced Electric Field in Nanograting Photoanodes.

Severe charge recombination in solar water-splitting devices significantly limits their performance. To address this issue, we design a frustum of a cone nanograting configuration by taking the hematite and Au-based thin-film photoanode as a model system, which greatly improves the photoelectrochemical water oxidation activity, affording an approximately 10-fold increase in the photocurrent density at 1.23 V versus the reversible hydrogen electrode compared to the planar counterpart. The surface plasmon polariton-induced electric field in hematite plays a dominant role in efficiency enhancement by facilitating charge separation, thus dramatically increasing the incident photon-to-current efficiency (IPCE) by more than 2 orders of magnitude in the near band gap of hematite. And the relatively weak electric field caused by light scattering in the nanograting structure is responsible for the approximate maximum 20-fold increase in IPCE within a broadband wavelength range. Our scalable strategy can be generalized to other solar energy conversion systems.

Brightening of a dark monolayer semiconductor via strong light-matter coupling in a cavity.

Engineering the properties of quantum materials via strong light-matter coupling is a compelling research direction with a multiplicity of modern applications. Those range from modifying charge transport in organic molecules, steering particle correlation and interactions, and even controlling chemical reactions. Here, we study the modification of the material properties via strong coupling and demonstrate an effective inversion of the excitonic band-ordering in a monolayer of WSe2 with spin-forbidden, optically dark ground state. In our experiments, we harness the strong light-matter coupling between cavity photon and the high energy, spin-allowed bright exciton, and thus creating two bright polaritonic modes in the optical bandgap with the lower polariton mode pushed below the WSe2 dark state. We demonstrate that in this regime the commonly observed luminescence quenching stemming from the fast relaxation to the dark ground state is prevented, which results in the brightening of this intrinsically dark material. We probe this effective brightening by temperature-dependent photoluminescence, and we find an excellent agreement with a theoretical model accounting for the inversion of the band ordering and phonon-assisted polariton relaxation.

Valley-exchange coupling probed by angle-resolved photoluminescence.

The optical properties of monolayer transition metal dichalcogenides are dominated by tightly-bound excitons. They form at distinct valleys in reciprocal space, and can interact via the valley-exchange coupling, modifying their dispersion considerably. Here, we predict that angle-resolved photoluminescence can be used to probe the changes of the excitonic dispersion. The exchange-coupling leads to a unique angle dependence of the emission intensity for both circularly and linearly-polarised light. We show that these emission characteristics can be strongly tuned by an external magnetic field due to the valley-specific Zeeman-shift. We propose that angle-dependent photoluminescence measurements involving both circular and linear optical polarisation as well as magnetic fields should act as strong verification of the role of valley-exchange coupling on excitonic dispersion and its signatures in optical spectra.

Spatial coherence of room-temperature monolayer WSe2 exciton-polaritons in a trap.

The emergence of spatial and temporal coherence of light emitted from solid-state systems is a fundamental phenomenon intrinsically aligned with the control of light-matter coupling. It is canonical for laser oscillation, emerges in the superradiance of collective emitters, and has been investigated in bosonic condensates of thermalized light, as well as exciton-polaritons. Our room temperature experiments show the strong light-matter coupling between microcavity photons and excitons in atomically thin WSe2. We evidence the density-dependent expansion of spatial and temporal coherence of the emitted light from the spatially confined system ground-state, which is accompanied by a threshold-like response of the emitted light intensity. Additionally, valley-physics is manifested in the presence of an external magnetic field, which allows us to manipulate K and K' polaritons via the valley-Zeeman-effect. Our findings validate the potential of atomically thin crystals as versatile components of coherent light-sources, and in valleytronic applications at room temperature.

Remote Lightening and Ultrafast Transition: Intrinsic Modulation of Exciton Spatiotemporal Dynamics in Monolayer MoS2.

Devices operating with excitons have promising prospects for overcoming the dilemma of response time and integration in current generation of electron- or/and photon-based elements and devices. Although the intrinsic properties including edges, grain boundaries, and defects of atomically thin semiconductors have been demonstrated as a powerful tool to adjust the bandgap and exciton energy, investigating the intrinsic modulation of spatiotemporal dynamics still remains challenging on account of the short exciton diffusion length. Here, we achieve the attractive remote lightening phenomenon, in which the emission region could be far away (up to 14.6 µm) from the excitation center, by utilizing a femtosecond laser with ultrahigh peak power as excitation source and the edge region with high photoluminescence efficiency as a bright emitter. Furthermore, the ultrafast transition between exciton and trion is demonstrated, which provides insight into the intrinsic modulation on populations of exciton and trion states. The complete cascaded physical scenario of exciton spatiotemporal dynamics is eventually established. This work can refresh our perspective on the spatial nonuniformities of CVD-grown atomically thin semiconductors and provide important implications for developing durable and stable excitonic devices in the future.

Photoluminescence enhancement of MoS2/CdSe quantum rod heterostructures induced by energy transfer and exciton-exciton annihilation suppression.

Energy transfer in heterostructures is an essential interface interaction for extraordinary energy conversion properties, which promote promising applications in light-emitting and photovoltaic devices. However, when atomic-layered transition metal dichalcogenides (TMDCs) act as the energy acceptor because of strong Coulomb interactions, the transferred energy can be consumed by nonradiative exciton annihilations, which hampers the development of light-emitting devices. Hence, revealing the mechanism of energy transfer and the related relaxation processes from the aspect of the acceptor in the heterostructure is key to reducing nonradiative loss and optimizing luminescence. Here, we study the exciton dynamics from the standpoint of the acceptor in MoS2/CdSe quantum rod (QR) heterostructures and realize efficiently enhanced photoluminescence (PL). Through femtosecond pump-probe measurements, it is directly observed that energy transfer from CdSe QRs largely raises the exciton population of the acceptor, MoS2, providing a larger emission "source". In addition, the dielectric environment introduced by CdSe QRs efficiently enhances the PL by suppressing exciton-exciton annihilation (EEA). This study provides new insights for on-chip applications such as light-emitting diodes and optical conversion devices based on low dimensional semiconductor heterostructures.

Self-Healing Originated van der Waals Homojunctions with Strong Interlayer Coupling for High-Performance Photodiodes.

The dangling-bond-free surfaces of van der Waals (vdW) materials make it possible to build ultrathin junctions. Fundamentally, the interfacial phenomena and related optoelectronic properties of vdW junctions are modulated by the interlayer coupling effect. However, the weak interlayer coupling of vdW heterostructures limits the interlayer charge transfer efficiency, resulting in low photoresponsivity. Here, a bilayer MoS2 homogeneous junction is constructed by stacking the as-grown onto the self-healed monolayer MoS2. The homojunction barrier of ∼165 meV is obtained by the electronic structure modulation of defect self-healing. This homojunction reveals the stronger interlayer coupling effect in comparison with vdW heterostructures. This ultrastrong interlayer coupling effect is experimentally verified by Raman spectra and angle-resolved photoemission spectroscopy. The ultrafast interlayer charge transfer takes place within ∼447 fs, which is faster than those of most vdW heterostructures. Furthermore, the homojunction photodiode manifests outstanding rectifying behavior with an ideal factor of ∼1.6, perfect air stability over 12 months, and high responsivity of ∼54.6 mA/W. Moreover, the interlayer exciton peak of ∼1.66 eV is found in vdW homojunctions. This work offers an uncommon vdW junction with strong interlayer coupling and perfects the relevance of interlayer coupling and interlayer charge transfer.

Direct observation of ultrafast plasmonic hot electron transfer in the strong coupling regime.

Achieving strong coupling between plasmonic oscillators can significantly modulate their intrinsic optical properties. Here, we report the direct observation of ultrafast plasmonic hot electron transfer from an Au grating array to an MoS2 monolayer in the strong coupling regime between localized surface plasmons (LSPs) and surface plasmon polaritons (SPPs). By means of femtosecond pump-probe spectroscopy, the measured hot electron transfer time is approximately 40 fs with a maximum external quantum yield of 1.65%. Our results suggest that strong coupling between LSPs and SPPs has synergetic effects on the generation of plasmonic hot carriers, where SPPs with a unique nonradiative feature can act as an 'energy recycle bin' to reuse the radiative energy of LSPs and contribute to hot carrier generation. Coherent energy exchange between plasmonic modes in the strong coupling regime can further enhance the vertical electric field and promote the transfer of hot electrons between the Au grating and the MoS2 monolayer. Our proposed plasmonic strong coupling configuration overcomes the challenge associated with utilizing hot carriers and is instructive in terms of improving the performance of plasmonic opto-electronic devices.

Plasmonics of 2D Nanomaterials: Properties and Applications.

Plasmonics has developed for decades in the field of condensed matter physics and optics. Based on the classical Maxwell theory, collective excitations exhibit profound light-matter interaction properties beyond classical physics in lots of material systems. With the development of nanofabrication and characterization technology, ultra-thin two-dimensional (2D) nanomaterials attract tremendous interest and show exceptional plasmonic properties. Here, we elaborate the advanced optical properties of 2D materials especially graphene and monolayer molybdenum disulfide (MoS2), review the plasmonic properties of graphene, and discuss the coupling effect in hybrid 2D nanomaterials. Then, the plasmonic tuning methods of 2D nanomaterials are presented from theoretical models to experimental investigations. Furthermore, we reveal the potential applications in photocatalysis, photovoltaics and photodetections, based on the development of 2D nanomaterials, we make a prospect for the future theoretical physics and practical applications.

Controlled growth and shape-directed self-assembly of gold nanoarrows.

Self-assembly of colloidal nanocrystals into complex superstructures offers notable opportunities to create functional devices and artificial materials with unusual properties. Anisotropic nanoparticles with nonspherical shapes, such as rods, plates, polyhedra, and multipods, enable the formation of a diverse range of ordered superlattices. However, the structural complexity and tunability of nanocrystal superlattices are restricted by the limited geometries of the anisotropic nanoparticles available for supercrystal self-assembly. We show that uniform gold nanoarrows (GNAs) consisting of two pyramidal heads connected by a four-wing shaft are readily synthesized through controlled overgrowth of gold nanorods. The distinct concave geometry endows the GNAs with unique packing and interlocking ability and allows for the shape-directed assembly of sophisticated two-dimensional (2D) and 3D supercrystals with unprecedented architectures. Net-like 2D supercrystals are assembled through the face-to-face contact of the GNAs lying on the pyramidal edges, whereas zipper-like and weave-like 2D supercrystals are constructed by the interlocked GNAs lying on the pyramidal {111} facets. Furthermore, multilayer packing of net-like and weave-like 2D assemblies of GNAs leads to non-close-packed 3D supercrystals with varied packing efficiencies and pore structures. Electromagnetic simulation of the diverse nanoarrow supercrystals exhibits exotic patterns of nanoscale electromagnetic field confinement. This study may open new avenues toward tunable self-assembly of nanoparticle superstructures with increased complexity and unusual functionality and may advance the design of novel plasmonic metamaterials for nanophotonics and reconfigurable architectured materials.

Single-Nanoparticle Plasmonic Electro-optic Modulator Based on MoS2 Monolayers.

The manipulation of light in an integrated circuit is crucial for the development of high-speed electro-optic devices. Recently, molybdenum disulfide (MoS2) monolayers generated broad interest for the optoelectronics because of their huge exciton binding energy, tunable optical emission, direct electronic band-gap structure, etc. Miniaturization and multifunctionality of electro-optic devices further require the manipulation of light-matter interaction at the single-nanoparticle level. The strong exciton-plasmon interaction that is generated between the MoS2 monolayers and metallic nanostructures may be a possible solution for compact electro-optic devices at the nanoscale. Here, we demonstrate a nanoplasmonic modulator in the visible spectral region by combining the MoS2 monolayers with a single Au nanodisk. The narrow MoS2 excitons coupled with broad Au plasmons result in a deep Fano resonance, which can be switched on and off by applying different gate voltages on the MoS2 monolayers. A reversible display device that is based on this single-nanoparticle modulator is demonstrated with a heptamer pattern that is actively controlled by the external gates. Our work provides a potential application for electro-optic modulation on the nanoscale and promotes the development of gate-tunable nanoplasmonic devices in the future.

How To Light Special Hot Spots in Multiparticle-Film Configurations.

The precise control over the locations of hot spots in a nanostructured ensemble is of great importance in plasmon-enhanced spectroscopy, chemical sensing, and super-resolution optical imaging. However, for multiparticle configurations over metal films that involve localized and propagating surface plasmon modes, the locations of hot spots are difficult to predict due to complex plasmon competition and synergistic effects. In this work, theoretical simulations based on multiparticle-film configurations predict that the locations of hot spots can be efficiently controlled in the particle-particle gaps, the particle-film junctions, or in both, by suppressing or promoting specific plasmonic coupling effects in specific wavelength ranges. These findings offer an avenue to obtain strong Raman signals from molecules situated on single crystal surfaces and simultaneously avoid signal interference from particle-particle gaps.

Internal-Modified Dithiol DNA-Directed Au Nanoassemblies: Geometrically Controlled Self-Assembly and Quantitative Surface-Enhanced Raman Scattering Properties.

In this work, a hierarchical DNA-directed self-assembly strategy to construct structure-controlled Au nanoassemblies (NAs) has been demonstrated by conjugating Au nanoparticles (NPs) with internal-modified dithiol single-strand DNA (ssDNA) (Au-B-A or A-B-Au-B-A). It is found that the dithiol-ssDNA-modified Au NPs and molecule quantity of thiol-modified ssDNA grafted to Au NPs play critical roles in the assembly of geometrically controlled Au NAs. Through matching Au-DNA self-assembly units, geometrical structures of the Au NAs can be tailored from one-dimensional (1D) to quasi-2D and 2D. Au-B-A conjugates readily give 1D and quasi-2D Au NAs while 2D Au NAs can be formed by A-B-Au-B-A building blocks. Surface-enhanced Raman scattering (SERS) measurements and 3D finite-difference time domain (3D-FDTD) calculation results indicate that the geometrically controllable Au NAs have regular and linearly "hot spots"-number-depended SERS properties. For a certain number of NPs, the number of "hot spots" and accordingly enhancement factor of Au NAs can be quantitatively evaluated, which open a new avenue for quantitative analysis based on SERS technique.