Aaron M. Jones

Electrically tunable excitonic light-emitting diodes based on monolayer WSe2 p–n junctions

The development of light-emitting diodes with improved efficiency, spectral properties, compactness and integrability is important for lighting, display, optical interconnect, logic and sensor applications. Monolayer transition-metal dichalcogenides have recently emerged as interesting candidates for optoelectronic applications due to their unique optical properties. Electroluminescence has already been observed from monolayer MoS2 devices. However, the electroluminescence efficiency was low and the linewidth broad due both to the poor optical quality of the MoS2 and to ineffective contacts. Here, we report electroluminescence from lateral p-n junctions in monolayer WSe2 induced electrostatically using a thin boron nitride support as a dielectric layer with multiple metal gates beneath. This structure allows effective injection of electrons and holes, and, combined with the high optical quality of WSe2, yields bright electroluminescence with 1,000 times smaller injection current and 10 times smaller linewidth than in MoS2 (refs 17,18). Furthermore, by increasing the injection bias we can tune the electroluminescence between regimes of impurity-bound, charged and neutral excitons. This system has the required ingredients for new types of optoelectronic device, such as spin- and valley-polarized light-emitting diodes, on-chip lasers and two-dimensional electro-optic modulators.

Electrical control of neutral and charged excitons in a monolayer semiconductor

Monolayer group-VI transition metal dichalcogenides have recently emerged as semiconducting alternatives to graphene in which the true two-dimensionality is expected to illuminate new semiconducting physics. Here we investigate excitons and trions (their singly charged counterparts), which have thus far been challenging to generate and control in the ultimate two-dimensional limit. Utilizing high-quality monolayer molybdenum diselenide, we report the unambiguous observation and electrostatic tunability of charging effects in positively charged (X(+)), neutral (X(o)) and negatively charged (X(-)) excitons in field-effect transistors via photoluminescence. The trion charging energy is large (30 meV), enhanced by strong confinement and heavy effective masses, whereas the linewidth is narrow (5 meV) at temperatures <55 K. This is greater spectral contrast than in any known quasi-two-dimensional system. We also find the charging energies for X(+) and X(-) to be nearly identical implying the same effective mass for electrons and holes.

Highly anisotropic and robust excitons in monolayer black phosphorus

Semi-metallic graphene and semiconducting monolayer transition-metal dichalcogenides are the most intensively studied two-dimensional materials of recent years. Lately, black phosphorus has emerged as a promising new two-dimensional material due to its widely tunable and direct bandgap, high carrier mobility and remarkable in-plane anisotropic electrical, optical and phonon properties. However, current progress is primarily limited to its thin-film form. Here, we reveal highly anisotropic and strongly bound excitons in monolayer black phosphorus using polarization-resolved photoluminescence measurements at room temperature. We show that, regardless of the excitation laser polarization, the emitted light from the monolayer is linearly polarized along the light effective mass direction and centres around 1.3 eV, a clear signature of emission from highly anisotropic bright excitons. Moreover, photoluminescence excitation spectroscopy suggests a quasiparticle bandgap of 2.2 eV, from which we estimate an exciton binding energy of ∼0.9 eV, consistent with theoretical results based on first principles. The experimental observation of highly anisotropic, bright excitons with large binding energy not only opens avenues for the future explorations of many-electron physics in this unusual two-dimensional material, but also suggests its promising future in optoelectronic devices.

Observation of Long-Lived Interlayer Excitons in Monolayer MoSe2-WSe2 Heterostructures

Van der Waals bound heterostructures constructed with two-dimensional materials, such as graphene, boron nitride and transition metal dichalcogenides, have sparked wide interest in device physics and technologies at the two-dimensional limit. One highly coveted heterostructure is that of differing monolayer transition metal dichalcogenides with type-II band alignment, with bound electrons and holes localized in individual monolayers, that is, interlayer excitons. Here, we report the observation of interlayer excitons in monolayer MoSe2-WSe2 heterostructures by photoluminescence and photoluminescence excitation spectroscopy. We find that their energy and luminescence intensity are highly tunable by an applied vertical gate voltage. Moreover, we measure an interlayer exciton lifetime of ~1.8 ns, an order of magnitude longer than intralayer excitons in monolayers. Our work demonstrates optical pumping of interlayer electric polarization, which may provoke further exploration of interlayer exciton condensation, as well as new applications in two-dimensional lasers, light-emitting diodes and photovoltaic devices.

Electrical tuning of valley magnetic moment through symmetry control in bilayer MoS2

Electric fields can break the structural inversion symmetry in bilayer 2D materials, providing a way of tuning the magnetic moment and Berry curvature. This effect can be probed directly in bilayer MoS2 using optical measurements.

Magnetic control of valley pseudospin in monolayer WSe2

Supplementary Text S1. Computing the valley Zeeman effect in multiple samples. The peak splitting due to the valley Zeeman effect is small compared to the width of the photoluminescence (PL) peaks so care must be taken in determining the Zeeman splitting. The peaks are slightly asymmetric, with shape varying somewhat with magnetic field, and do not conform well to a Gaussian or Lorentzian peak shape. We use two methods to determine the peak position and hence the Zeeman splitting, both of which make no assumptions about the peak shape. As shown in Figure 1c, they agree very well. The first, “max point”, simply finds the 15 points in each spectrum with the most counts and assigns the peak position to the median value of these points. This method is insensitive to the trion peak, which is too far away to influence these points; however, it is more sensitive to noise as it only considers a few points. The second method, “weighted average”, computes the “center of mass” of the peak, , where is the PL spectral density and E is photon energy. In this method the effect of noise is greatly reduced because it makes use of all the several hundred points that make up the spectrum, but on the other hand it is more sensitive to the trion peak, which will tend to over-weight the low-energy side of the peak. However, since the valley exciton Zeeman splitting is small and we are interested in the difference between the σ+ and σpeaks, the weak trion effects on both peaks tend to balance each other out. The data in Fig. 1c and Fig. S1a are from two different samples. We can see that the splitting as a function of magnetic field obtained by these two different methods has little difference. Eight samples were measured and all were observed to have a splitting linear in the applied field. In Figure S1b we plot the fitted slope of the splittings from all the samples, in units of Bohr magnetons. The data presented in the main text is from the fifth sample. We see that the data can be split into two groups with mean values of 1.57 μB and 2.86 μB. The origin of this bimodal distribution in the g-factors is unclear due to the lack of understanding of what external factors can affect the g-factors in these new materials. Future studies will be necessary to quantitatively determine the effect of variables such as strain, doping, and substrate on the magnetic properties. However, all samples show similar behavior in their valley polarization as a function of the applied field (i.e., the “X” and “V” patterns).

Spin-layer locking effects in optical orientation of exciton spin in bilayer WSe2

Monolayer and few-layer materials present interesting spin and pseudospin states. A study of the coupling between spin, valley and layer degrees of freedom in bilayer WSe2 reveals coherent superpositions of distinct valley configurations and suggests the possibility of electrical control of the spin states.

Electrical control of second-harmonic generation in a WSe2 monolayer transistor

Nonlinear optical frequency conversion, in which optical fields interact with a nonlinear medium to produce new field frequencies, is ubiquitous in modern photonic systems. However, the nonlinear electric susceptibilities that give rise to such phenomena are often challenging to tune in a given material and, so far, dynamical control of optical nonlinearities remains confined to research laboratories as a spectroscopic tool. Here, we report a mechanism to electrically control second-order optical nonlinearities in monolayer WSe₂, an atomically thin semiconductor. We show that the intensity of second-harmonic generation at the A-exciton resonance is tunable by over an order of magnitude at low temperature and nearly a factor of four at room temperature through electrostatic doping in a field-effect transistor. Such tunability arises from the strong exciton charging effects in monolayer semiconductors, which allow for exceptional control over the oscillator strengths at the exciton and trion resonances. The exciton-enhanced second-harmonic generation is counter-circularly polarized to the excitation laser due to the combination of the two-photon and one-photon valley selection rules, which have opposite helicity in the monolayer. Our study paves the way towards a new platform for chip-scale, electrically tunable nonlinear optical devices based on two-dimensional semiconductors.

Control of two-dimensional excitonic light emission via photonic crystal

Monolayers of transition metal dichalcogenides (TMDCs) have emerged as new optoelectronic materials in the two dimensional (2D) limit, exhibiting rich spin-valley interplays, tunable excitonic effects, and strong light–matter interactions. An essential yet undeveloped ingredient for many photonic applications is the manipulation of its light emission. Here we demonstrate the control of excitonic light emission from monolayer tungsten diselenide (WSe2) in an integrated photonic structure, achieved by transferring one monolayer onto a photonic crystal (PhC) with a cavity. In addition to the observation of an effectively coupled cavity-mode emission, the suspension effects on PhC not only result in a greatly enhanced (~60 times) photoluminescence but also strongly pattern the emission in the subwavelength spatial scale, contrasting on and off the holes. Such an effect leads to a significant diffraction grating effect, which allows us to redistribute the emitted photons both polarly and azimuthally in the far field through designing PhC structures, as revealed by momentum-resolved microscopy. A 2D optical antenna is thus constructed. Our work suggests a new way of manipulating photons in hybrid 2D photonics, important for future energy efficient optoelectronics and 2D nano-lasers.

Quantum-Enhanced Tunable Second-Order Optical Nonlinearity in Bilayer Graphene

Second order optical nonlinear processes involve the coherent mixing of two electromagnetic waves to generate a new optical frequency, which plays a central role in a variety of applications, such as ultrafast laser systems, rectifiers, modulators, and optical imaging. However, progress is limited in the mid-infrared (MIR) region due to the lack of suitable nonlinear materials. It is desirable to develop a robust system with a strong, electrically tunable second order optical nonlinearity. Here, we demonstrate theoretically that AB-stacked bilayer graphene (BLG) can exhibit a giant and tunable second order nonlinear susceptibility χ((2)) once an in-plane electric field is applied. χ((2)) can be electrically tuned from 0 to ~10(5) pm/V, 3 orders of magnitude larger than the widely used nonlinear crystal AgGaSe(2). We show that the unusually large χ((2)) arise from two different quantum enhanced two-photon processes thanks to the unique electronic spectrum of BLG. The tunable electronic bandgap of BLG adds additional tunability on the resonance of χ((2)), which corresponds to a tunable wavelength ranging from ~2.6 to ~3.1 μm for the up-converted photon. Combined with the high electron mobility and optical transparency of the atomically thin BLG, our scheme suggests a new regime of nonlinear photonics based on BLG.