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We report resonant second harmonic generation (SHG) spectroscopy of an hBN-encapsulated monolayer of MoS$_2$. By tuning the energy of the excitation laser, we identify a dark state transition (D) that is blue detuned by +25 meV from the neutral exciton X$^0$. We observe a splitting of the SHG spectrum into two distinct peaks and a clear anticrossing between them as the SHG resonance is tuned through the energy of the dark exciton D. This observation is indicative of quantum interference arising from the strong two-photon light-matter interaction. We further probe the incoherent relaxation from the dark state to the bright excitons, including X$^0$ and localized excitons LX, by the resonant enhancement of their intensities at the SHG-D resonance. The relaxation of D to bright excitons is strongly suppressed on the bare substrate whilst enabled when the hBN/MoS$_2$/hBN heterostructure is integrated in a nanobeam cavity. The relaxation enabled by the cavity is explained by the phonon scattering enhanced by the cavity phononic effects. Our work reveals the two-photon quantum interference with long-lived dark states and enables the control through nanostructuring of the substrate. These results indicate the great potential of dark excitons in 2D-material based nonlinear quantum devices.

Two-dimensional (2D) heterostructures integrated into nanophotonic cavities have emerged as a promising approach towards novel photonic and opto-electronic devices. However, the thickness of the 2D heterostructure has a strong influence on the resonance frequency of the nanocavity. For a single cavity, the resonance frequency shifts approximately linearly with the thickness. Here, we propose to use the inherent non-linearity of the mode coupling to render the cavity mode insensitive to the thickness of the 2D heterostructure. Based on the coupled mode theory, we reveal that this goal can be achieved using either a homoatomic molecule with a filtered coupling or heteroatomic molecules. We perform numerical simulations to further demonstrate the robustness of the eigenfrequency in the proposed photonic molecules. Our results render nanophotonic structures insensitive to the thickness of 2D materials, thus owing appealing potential in energy- or detuning-sensitive applications such as cavity quantum electrodynamics.

The electron-hole exchange interaction is a fundamental mechanism that drives valley depolarization via intervalley exciton hopping in semiconductor multi-valley systems. Here, we report polarization-resolved photoluminescence spectroscopy of neutral excitons and negatively charged trions in monolayer MoSe$_2$ and WSe$_2$ under biaxial strain. We observe a marked enhancement(reduction) on the WSe$_2$ triplet trion valley polarization with compressive(tensile) strain while the trion in MoSe$_2$ is unaffected. The origin of this effect is shown to be a strain dependent tuning of the electron-hole exchange interaction. A combined analysis of the strain dependent polarization degree using ab initio calculations and rate equations shows that strain affects intervalley scattering beyond what is expected from strain dependent bandgap modulations. The results evidence how strain can be used to tune valley physics in energetically degenerate multi-valley systems.

Moir\'e trapped interlayer excitons (IXs) in heterobilayer transition metal dichalcogenides currently attract strong interest due to their potential for non-classical light generation, coherent spin-photon interfaces and exploring novel correlated phases of electrons. Here, we report lasing of moir\'e trapped IXs by integrating a pristine hBN-encapsulated MoSe$_2$/WSe$_2$ heterobilayer in a high-Q ($>10^4$) nanophotonic cavity. We control the detuning between the IX line and the cavity mode with a magnetic field and measure the dipolar coupling strength to the cavity mode to be $78 \pm 4\ \mathrm{\mu eV}$, fully consistent with the $82\ \mathrm{\mu eV}$ predicted by theory. The emission from the cavity mode shows clear threshold-like behaviour. We observe a superlinear power dependence accompanied by a narrowing of the linewidth as the distinct features of lasing. The onset and prominence of these threshold-like behaviours are significant at resonance whilst weak off-resonance. Our results show that a lasing transition can be induced in interacting moir\'e trapped IXs with macroscopic coherence extending over the lengthscale of the cavity mode. Such systems raise interesting perspectives for low-power switching and synaptic nanophotonic devices using 2D materials.

Integrating quantum emitters into nanocavities which simultaneously couple to the photonic and mechanical modes is critical for interfacing electron spins, photons and phonons in the cavity QED system. Here, we investigate the interaction between the charged boron vacancy $V_B^-$, ultra-high-Q ($\sim10^5$) cavity photonic modes and local phonon modes. A pronounced asymmetry is observed in the emission spectrum for cavities with Q-factor above a threshold of 10$^4$. Similar asymmetries are not observed for cavities without $V_B^-$ centers. To explain our findings, we model the system with phonon-induced light-matter coupling based on $V_B^-$ centers, and compare to the Jaynes-Cummings model for usual emitters. Our results reveal that the multipartite interplay arises during the light-matter coupling of $V_B^-$ centers, illustrating that it is phonon-induced, rather than being caused by thermal population of phonon modes. Such emitter-optomechanical interaction between different photon ($V_B^-$ emission, cavity photonic) and phonon ($V_B^-$ phonon, cavity mechanical) modes provides a novel system to interface spin defects, photons and phonons in condensed matters.

We report resonant Raman spectroscopy of neutral excitons X$^0$ and intravalley trions X$^-$ in hBN-encapsulated MoS$_2$ monolayer embedded in a nanobeam cavity. By temperature tuning the detuning between Raman modes of MoS$_2$ lattice phonons and X$^0$/X$^-$ emission peaks, we probe the mutual coupling of excitons, lattice phonons and cavity vibrational phonons. We observe an enhancement of X$^0$-induced Raman scattering and a suppression for X$^-$-induced, and explain our findings as arising from the tripartite exciton-phonon-phonon coupling. The cavity vibrational phonons provide intermediate replica states of X$^0$ for resonance conditions in the scattering of lattice phonons, thus enhancing the Raman intensity. In contrast, the tripartite coupling involving X$^-$ is found to be much weaker, an observation explained by the geometry-dependent polarity of the electron and hole deformation potentials. Our results indicate that phononic hybridization between lattice and nanomechanical modes plays a key role in the excitonic photophysics and light-matter interaction in 2D-material nanophotonic systems.

Negatively charged boron vacancies ($V_B^-$) in hexagonal boron nitride (hBN) exhibit a broad emission spectrum due to strong electron-phonon coupling and Jahn-Teller mixing of electronic states. As such, the direct measurement of zero-phonon line (ZPL) of $V_B^-$ has remained elusive. Here, we measure the room-temperature ZPL wavelength to be $773\pm2$ nm by coupling the hBN layer to the high-Q nanobeam cavity. As the wavelength of cavity mode is tuned, we observe a pronounced intensity resonance, indicating the coupling to $V_B^-$. Our observations are consistent with the spatial redistribution of $V_B^-$ emission. Spatially resolved measurements show a clear Purcell effect maximum at the midpoint of the nanobeam, in accord with the optical field distribution of the cavity mode. Our results are in good agreement with theoretical calculations, opening the way to using $V_B^-$ as cavity spin-photon interfaces.

Atomically thin semiconductors can be readily integrated into a wide range of nanophotonic architectures for applications in quantum photonics and novel optoelectronic devices. We report the observation of nonlocal interactions of \textit{free} trions in pristine hBN/MoS$_2$/hBN heterostructures coupled to single mode (Q $>10^4$) quasi 0D nanocavities. The high excitonic and photonic quality of the interaction system stems from our integrated nanofabrication approach simultaneously with the hBN encapsulation and the maximized local cavity field amplitude within the MoS$_2$ monolayer. We observe a nonmonotonic temperature dependence of the cavity-trion interaction strength, consistent with the nonlocal light-matter interactions in which the extent of the center-of-mass wavefunction is comparable to the cavity mode volume in space. Our approach can be generalized to other optically active 2D materials, opening the way towards harnessing novel light-matter interaction regimes for applications in quantum photonics.

We report an out-of-plane magnetic field induced large photoluminescence enhancement in WS${}_2$ flakes at $4$ K, in contrast to the photoluminescence enhancement provided by in-plane field in general. Two mechanisms for the enhancement are proposed. One is a larger overlap of electron and hole caused by the magnetic field induced confinement. The other is that the energy difference between $\Lambda$ and K valleys is reduced by magnetic field, and thus enhancing the corresponding indirect-transition trions. Meanwhile, the Land\'e g factor of the trion is measured as $-0.8$, whose absolute value is much smaller than normal exciton, which is around $|-4|$. A model for the trion g factor is presented, confirming that the smaller absolute value of Land\'e g factor is a behavior of this $\Lambda$-K trion. By extending the valley space, we believe this work provides a further understanding of the valleytronics in monolayer transition metal dichalcogenides., Comment: 15 pages, 4 figures

Monolayer transition metal dichalcogenides have recently attracted great interests because the quantum dots embedded in monolayer can serve as optically active single photon emitters. Here, we provide an interpretation of the recombination mechanisms of these quantum emitters through polarization-resolved and magneto-optical spectroscopy at low temperature. Three types of defect-related quantum emitters in monolayer tungsten diselenide (WSe$_2$) are observed, with different exciton g factors of 2.02, 9.36 and unobservable Zeeman shift, respectively. The various magnetic response of the spatially localized excitons strongly indicate that the radiative recombination stems from the different transitions between defect-induced energy levels, valance and conduction bands. Furthermore, the different g factors and zero-field splittings of the three types of emitters strongly show that quantum dots embedded in monolayer have various types of confining potentials for localized excitons, resulting in electron-hole exchange interaction with a range of values in the presence of anisotropy. Our work further sheds light on the recombination mechanisms of defect-related quantum emitters and paves a way toward understanding the role of defects in single photon emitters in atomically thin semiconductors., Comment: 14 pages, 4 Figures

In single microdisks, embedded active emitters intrinsically affect the cavity mode of microdisks, which results in a trivial symmetric backscattering and a low controllability. Here we propose a macroscopical control of the backscattering direction by optimizing the cavity size. The signature of positive and negative backscattering directions in each single microdisk is confirmed with two strongly coupled microdisks. Furthermore, the diabolical points are achieved at the resonance of two microdisks, which agrees well with the theoretical calculations considering backscattering directions. The diabolical points in active optical structures pave a way to implement quantum information processing with geometric phase in quantum photonic networks., Comment: 16 pages, 4 figures

Hybrid Perovskites have shown a great potential for applications in photovoltaics and light-emitting devices with high efficiency. Interaction between defect-induced trapped excitons and phonons plays an important role in understanding the emerging phenomena for such an excellent figure-of-merit. Here we demonstrate hot polarons with narrow linewidth in $\mathrm{CH_{3}NH_{3}PbBr_{3}}$ nanowires, which originate from the interaction between trapped excitons and octahedra-twist phonons. The observation of hot polarons in photoluminescence without gain methods indicates the large interaction strength between excitons and phonons. The multiple hot polarons are further confirmed by magneto-optical spectra with a Zeeman splitting of the trapped excitons and a phonon energy increase with diamagnetic effect. Furthermore, the phonons participating in the interaction are demonstrated to be the octahedra-twist vibrations which are transverse optical phonons, while the interaction between trapped excitons and longitudinal optical phonons is weak. Our work demonstrates that trapped excitons in perovskites prefer to interact with transverse rather than longitudinal optical phonons. Since bulk materials usually interact with longitudinal optical phonons, this result provides a physical explanation of the high tolerance of defects in perovskites., Comment: 16 pages, 4 figures

Crystal-phase low-dimensional structures offer great potential for the implementation of photonic devices of interest for quantum information processing. In this context, unveiling the fundamental parameters of the crystal phase structure is of much relevance for several applications. Here, we report on the anisotropy of the g-factor tensor and diamagnetic coefficient in wurtzite/zincblende (WZ/ZB) crystal-phase quantum dots (QDs) realized in single InP nanowires. The WZ and ZB alternating axial sections in the NWs are identified by high-angle annular dark-field scanning transmission electron microscopy. The electron (hole) g-factor tensor and the exciton diamagnetic coefficients in WZ/ZB crystal-phase QDs are determined through micro-photoluminescence measurements at low temperature (4.2 K) with different magnetic field configurations, and rationalized by invoking the spin-correlated orbital current model. Our work provides key parameters for band gap engineering and spin states control in crystal-phase low-dimensional structures in nanowires., Comment: 10 pages, 5 figures

Optical nanocavities for coherent interfaces usually have their electric field maximum at the center point, which normally benefits interactions with small local quantum emitters. Here, we propose a partial thickness modulation on 2D slab photonic crystal cavities for a cratered cavity mode function to improve nonlocal interactions. The thickness modulation is applied around the central region, and has little effect on the fringe electric field, which determines the coupling to waveguides or other cavities. Furthermore, the partial modulation enhances the cratered electric field at positions that are distant from the center point. Therefore, interactions with multiple separated emitters are simultaneously enhanced, and the interaction with a large emitter beyond the dipole approximation is also doubled. The improvement of the nonlocal interactions demonstrates a great potential for the cratered cavity mode profile for applications in quantum photonic networks., Comment: 14 pages, 5 figures

Transition metal dichalcogenide monolayers provide an emerging material system to implement quantum photonics with intrinsic two-dimensional excitons or embedded zero-dimensional localized states. Here we demonstrate the mesoscopic localized states between two- and zero- dimensions, which is a many-body system with electron-electron Coulomb interactions. A fine structure splitting is observed, which is similar to quantum dots. Meanwhile the polarization is changed by the magnetic field, due to the nature of two-dimensional monolayers. Furthermore, a large quadratic diamagnetism with a coefficient of around $100\ \mathrm{\mu eV/T^2}$ is observed, as a unique consequence of the mesoscopic scale. The many-body effect also results in the emission energy variation and linewidth narrowing in the spectrum, which corresponds well to the theoretical analysis. These unique properties indicate the great potential of mesoscopic localized states in many-body physics and quantum photonics., Comment: 14 pages, 4 figures

The valley of transition metal dichalcogenides provides an additional platform to manipulate spin due to its unique selection rule. Normally, intralayer optical transitions in magnetic field show a Zeeman splitting with g factor of about $-4$. Here we report remarkable valley Zeeman effect exhibited by splitting of excitonic emission in a bilayer WS$_{2}$, with a value of g factor as large as $-16.5$. The observed large g factor results from the interlayer recombination, as the conduction band and valence band are modified in opposite directions by magnetic field in different layers. The interlayer recombination is due to the defect induced inversion symmetry breaking, which is theoretically not accessible in ideal bilayer WS$_{2}$ with inversion symmetry. Large g factor of interlayer emission offers potential benefits for future optical spin control and detection., Comment: 12 pages, 4 figures

We report on an increase in the carrier tunneling time in a single quantum dot (QD) with a magnetic field in Faraday geometry using photocurrent spectroscopy. A nearly 60\% increase in hole tunneling time is observed with an applied magnetic field equal to 9 T. For a truncated pyramid QD, hole tunnels out faster at the lateral edge of the QD due to the reduced barrier height. The magnetic field in Faraday geometry shrinks the hole wave function at the center of QD plane, which weakens the tunneling at lateral edge and increases the average tunneling time. This mechanism also works for electron but the effect is smaller. The electron wave function is more localized at the center of the QD due to the uniform confining potential, therefore the relatively weak shrinkage caused by the magnetic field does not reduce the tunneling rate significantly., Comment: 13 pages, 4 figures

Large coupling strengths in exciton-photon interactions are important for quantum photonic network, while strong cavity-quantum-dot interactions have been focused on s-shell excitons with small coupling strengths. Here we demonstrate strong interactions between cavities and p-shell excitons with a great enhancement by the \textit{in situ} wave-function control. The p-shell excitons are demonstrated with much larger wave-function extents and nonlocal interactions beyond the dipole approximation. Then the interaction is tuned from the nonlocal to local regime by the wave-function shrinking, during which the enhancement is obtained. A large coupling strength of $210\ \mu\mathrm{eV}$ has been achieved, indicating the great potential of p-shell excitons for coherent information exchange. Furthermore, we propose a distributed delay model to quantitatively explain the coupling strength variation, revealing the intertwining of excitons and photons beyond the dipole approximation., Comment: 12 pages, 5 figures

Understanding the carrier excitation and transport processes at the single-charge level plays a key role in quantum-dot-based solar cells and photodetectors. Here, we report on Coulomb-induced giant photocurrent enhancement of positive charged trions (\emph{X$^+$}) in a single self-assembled InAs/GaAs quantum dot embedded in an \emph{n-i-}Schottky device by high-resolution photocurrent (PC) spectroscopy. The Coulomb repulsion between the two holes in the \emph{X$^+$} increases the tunneling rate of the hole, and the remaining hole can be reused as the initial state to regenerate \emph{X$^+$} again. This process brings the PC amplitude of \emph{X$^+$} up to 30 times larger than that of the neutral exciton. The analysis of the hole tunneling time gives the equivalent change of hole tunnel barriers caused by Coulomb interaction between two holes with a value of 8.05 meV during the tunneling process. Our work brings a fundamental understanding of energy conversion for solar cells in nanoscale to improve internal quantum efficiency for energy harvesting., Comment: 17 pages, 4 figures

Two-photon Rabi splitting in a cavity-dot system provides a basis for multi-qubit coherent control in quantum photonic network. Here we report on two-photon Rabi splitting in a strongly coupled cavity-dot system. The quantum dot was grown intentionally large in size for large oscillation strength and small biexciton binding energy. Both exciton and biexciton transitions couple to a high quality factor photonic crystal cavity with large coupling strengths over 130 $\mu$eV. Furthermore, the small binding energy enables the cavity to simultaneously couple with two exciton states. Thereby two-photon Rabi splitting between biexciton and cavity is achieved, which can be well reproduced by theoretical calculations with quantum master equations., Comment: 12 pages, 4 figures

Defects are detrimental for optoelectronics devices, such as stacking faults can form carrier-transportation barriers, and foreign impurities (Au) with deep-energy levels can form carrier traps and non-radiative recombination centers. Here, we first developed self-catalyzed p-type GaAs nanowires (NWs) with pure zinc blende (ZB) structure, and then fabricated photodetector made by these NWs. Due to absence of stacking faults and suppression of large amount of defects with deep energy levels, the photodetector exhibits room-temperature high photo responsivity of 1.45 x 105 A W^-1 and excellent specific detectivity (D*) up to 1.48 x 10^14 Jones for low-intensity light signal of wavelength 632.8 nm, which outperforms previously reported NW-based photodetectors. These results demonstrate that these self-catalyzed pure-ZB GaAs NWs to be promising candidates for optoelectronics applications., Comment: 22 pages,6 figures

We report on high-resolution photoluminescence (PL) and photocurrent (PC) spectroscopies of a single self-assembled InAs/GaAs quantum dot (QD) embedded in an n-i-Schottky device with an applied magnetic field in Faraday and Voigt geometries. The single-QD PC spectrum of neutral exciton (X$^0$) is obtained by sweeping the bias-dependent X$^0$ transition energy to achieve resonance with a fixed narrow-bandwidth laser through quantum-confined Stark effect. With a magnetic field applied in Faraday geometry, the diamagnetic effect and the Zeeman splitting of X$^0$ are observed both in PL and PC spectra. When the magnetic field is applied in Voigt geometry, the mixture of bright and dark states results in an observation of dark exciton states, which are confirmed by the polarization-resolved PL and PC spectra., Comment: 13 pages, 4 figures

We report on a temporal evolution of photoluminescence (PL) spectroscopy of CuInS$_{2}$/ZnS colloidal quantum dots (QDs) by drop-casting on SiO$_{2}$/Si substrates and high quality factor microdisks (MDs) under different atmospheric conditions. Fast PL decay, peak blueshift and linewidth broadening due to photooxidation have been observed at low excitation power. With further increasing of the excitation power, the PL peak position shows a redshift and linewidth becomes narrow, which is ascribed to the enhanced F$\ddot{o}$rster resonant energy transfer between different QDs by photoinduced agglomeration. The oxygen plays an important role in optically induced PL decay which is verified by reduced photobleaching effect in vacuum. When the QDs drop-casted on MDs, photooxidation and photobleaching are accelerated because the excitation efficiency is greatly enhanced with coupling the pumping laser with the cavity modes. However, when the emitted photons couple with cavity modes, a PL enhancement by more than 20 times is achieved because of the increased extraction efficiency and Purcell effects of MDs at room temperature (RT), and 35 times at 20 K. The photobleaching can be avoided with a small excitation power but with a strong PL intensity by taking advantages of high quality factor cavities. The high efficient PL emission without photodegradation is very promising for using CuInS$_{2}$ QDs as high efficient photon emitters at RT, where the photodegradation has always been limiting the practical applications of colloidal quantum dots., Comment: 23 pages, 8 figures in ACS Photonics, 2017

Systems with coupled cavities and waveguides have been demonstrated as optical switches and optical sensors. To optimize the functionalities of these optical devices, Fano resonance with asymmetric and steep spectral line shape has been used. We theoretically propose a coupled photonic crystal cavity-waveguide structure to achieve Fano resonance by placing partially reflecting elements in waveguide. To enhance Fano resonance, optical gain material is introduced into the cavity. As the gain increases, the transmission line shape becomes steepened and the transmissivity can be six times enhanced, giving a large contrast by a small frequency shift. It is prospected that the gain enhanced Fano resonance is very useful for optical switches and optical sensors., Comment: 16 pages, 5 figures

We report on temperature- and excitation-power-dependent photoluminescence (PL) study of CuInS$_{2}$/ZnS nanocrystals dispersed on a SiO$_{2}$/Si substrate with a confocal micro-PL system. With increasing the excitation power at 22 K and room temperature, the PL spectra are blue-shifted because of the state filling. At low temperature, a small peak is observed at the low energy side of the spectrum, which could be due to the F$\ddot{o}$rster resonance energy transfer between different nanocrystals. The integrated PL intensity increases sublinearly as a function of excitation power with a power factor of around 2/3, which demonstrates the Auger recombination dominated process in the nanocrystals, especially under the high excitation power., Comment: 12 pages, 3 figures

We report the direct observation of coupling between a single self-assembled InAs quantum dot and a wetting layer, based on strong diamagnetic shifts of many-body exciton states using magneto-photoluminescence spectroscopy. An extremely large positive diamagnetic coefficient is observed when an electron in the wetting layer combines with a hole in the quantum dot; the coefficient is nearly one order of magnitude larger than that of the exciton states confined in the quantum dots. Recombination of electrons with holes in a quantum dot of the coupled system leads to an unusual negative diamagnetic effect, which is five times stronger than that in a pure quantum dot system. This effect can be attributed to the expansion of the wavefunction of remaining electrons in the wetting layer or the spread of electrons in the excited states of the quantum dot to the wetting layer after recombination. In this case, the wavefunction extent of the final states in the quantum dot plane is much larger than that of the initial states because of the absence of holes in the quantum dot to attract electrons. The properties of emitted photons that depend on the large electron wavefunction extents in the wetting layer indicate that the coupling occurs between systems of different dimensionality, which is also verified from the results obtained by applying a magnetic field in different configurations. This study paves a new way to observe hybrid states with zero- and two-dimensional structures, which could be useful for investigating the Kondo physics and implementing spin-based solid-state quantum information processing., Comment: 20 pages, 7 figures in Nano Research, 2015

We study the coupling between photonic molecules and waveguides in photonic crystal slab structures using finite-difference time-domain method and coupled mode theory. In a photonic molecule with two cavities, the coupling of cavity modes results in two super-modes with symmetric and anti-symmetric field distributions. When two super-modes are excited simultaneously, the energy of electric field oscillates between the two cavities. To excite and probe the energy oscillation, we integrate photonic molecule with two photonic crystal waveguides. In coupled structure, we find that the quality factors of two super-modes might be different because of different field distributions of super-modes. After optimizing the radii of air holes between two cavities of photonic molecule, nearly equal quality factors of two super-modes are achieved, and coupling strengths between the waveguide modes and two super-modes are almost the same. In this case, complete energy oscillations between two cavities can be obtained with a pumping source in one waveguide, which can be read out by another waveguide. Finally, we demonstrate that the designed structure can be used for ultrafast optical switching with a time scale of a few picoseconds., Comment: 18 pages, 6 figures