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Combining a precise sputter etching method with subsequent AlO$_x$ growth within an atomic layer deposition chamber enables fabrication of atomically flat lateral patterns of SiO$_2$ and AlO$_x$. The transfer of MoSe$_2$ monolayers onto these dielectrically modulated substrates results in formation of lateral heterojunctions, with the flat substrate topography leading to minimal strain across the junction. Kelvin probe force microscopy (KPFM) measurements show significant variations in the contact potential difference (CPD) across the interface, with AlO$_x$ regions inducing a 230~mV increase in CPD. Spatially resolved photoluminescence spectroscopy reveals shifts in spectral weight of neutral and charged exciton species across the different dielectric regions. On the AlO$_x$ side, the Fermi energy moves closer to the conduction band, leading to a higher trion-to-exciton ratio, indicating a bandgap shift consistent with CPD changes. In addition, transient reflection spectroscopy highlights the influence of the dielectric environment on carrier dynamics, with the SiO$_2$ side exhibiting rapid carrier decay typical of neutral exciton recombination. In contrast, the AlO$_x$ side shows slower, mixed decay behavior consistent with conversion of trions back into excitons. These results demonstrate how dielectric substrate engineering can tune the electronic and optical characteristics of proximal two-dimensional materials, allowing scalable fabrication of advanced junctions for novel (opto)electronics applications., Comment: 24 pages, 5 figures. SI: 2 pages, 3 figures. We welcome your feedback!

We present time-resolved and CW optical spectroscopy studies of interlayer excitons (IXs) in 2$H-$ and 3$R-$stacked MoSe$_2$/WSe$_2$ heterobilayers and obtain evidence for the strong participation of hot phonons in the underlying photo-physics. Photoluminescence excitation spectroscopy reveals that excess energy associated with optical excitation of \textit{intra}-layer excitons and relaxation to IXs affects the overall IX-PL lineshape, while the spectrally narrow emission lines conventionally associated with moir\'e IXs are unaffected. A striking uniform line-spacing of the sharp emission lines is observed together with temperature and excitation level dependent spectra suggesting an entirely new picture that photo-generated phonons lead to phonon-replicas shaping the IX-emission. Excitation power and time resolved data indicate that these features are polaronic in nature. Our experimental findings modify our current understanding of the photophysics of IXs beyond current interpretations based on moir\'e-trapped IXs.

We report temperature-dependent spectroscopy on the layered (n=4) two-dimensional (2D) Ruddlesden-Popper perovskite (BA)(MA)PbI. Helicity-resolved steady-state photoluminescence (PL) reveals no optical degree of polarization. Time-resolved PL shows a photocarrier lifetime on the order of nanoseconds. From simultaneaously recorded time-resolved differential reflectivity (TR$\Delta$R) and time-resolved Kerr ellipticity (TRKE), a photocarrier lifetime of a few nanoseconds and a spin dephasing time on the order of picoseconds was found. This stark contrast in lifetimes clearly explains the lack of spin polarization in steady-state PL. While we observe clear temperature-dependent effects on the PL dynamics that can be related to structural dynamics, the spin dephasing is nearly T-independent. Our results highlight that spin dephasing in 2D (BA)(MA)PbI occurs at time scales faster than the exciton recombination time, which poses a bottleneck for applications aimingto utilize this degree of freedom.

We report a new dark exciton in monolayer MoS$_2$ using second harmonic generation spectroscopy. Hereby, the spectrally dependent second harmonic generation intensity splits into two branches, and an anticrossing is observed at $\sim$ 25 meV blue detuned from the bright neutral exciton. These observations are indicative of coherent quantum interference arising from strong two-photon light-matter interaction with an excitonic state that is dark for single photon interaction. The existence of the dark state is supported by engineering its relaxation to bright localized excitons, mediated by vibrational modes of a proximal nanobeam cavity. We show that two-photon light-matter interaction involving dark states has the potential to control relaxation pathways induced by nanostructuring the local environment. Moreover, our results indicate that dark excitons have significant potential for nonlinear quantum devices based on their nontrivial excitonic photophysics.

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.

We report lasing of moir\'e trapped interlayer excitons (IXs) by integrating a pristine hBN-encapsulated MoSe$_2$/WSe$_2$ heterobilayer into a high-$Q$ ($>10^4$) nanophotonic cavity. We control the cavity-IX detuning using a magnetic field and measure their dipolar coupling strength 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 behavior as the transition is tuned into resonance with the cavity. 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 behaviors are pronounced at resonance while weak off-resonance. Our results show that a lasing transition can be induced in interacting moir\'e IXs with macroscopic coherence extending over the length scale of the cavity mode. Such systems raise interesting perspectives for low-power switching and synaptic nanophotonic devices using two-dimensional materials.

The valley Zeeman physics of excitons in monolayer transition metal dichalcogenides provides valuable insight into the spin and orbital degrees of freedom inherent to these materials. Being atomically-thin materials, these degrees of freedom can be influenced by the presence of adjacent layers, due to proximity interactions that arise from wave function overlap across the 2D interface. Here, we report 60 T magnetoreflection spectroscopy of the A- and B- excitons in monolayer WS$_2$, systematically encapsulated in monolayer graphene. While the observed variations of the valley Zeeman effect for the A- exciton are qualitatively in accord with expectations from the bandgap reduction and modification of the exciton binding energy due to the graphene-induced dielectric screening, the valley Zeeman effect for the B- exciton behaves markedly different. We investigate prototypical WS$_2$/graphene stacks employing first-principles calculations and find that the lower conduction band of WS$_2$ at the $K/K'$ valleys (the $CB^-$ band) is strongly influenced by the graphene layer on the orbital level. This leads to variations in the valley Zeeman physics of the B- exciton, consistent with the experimental observations. Our detailed microscopic analysis reveals that the conduction band at the $Q$ point of WS$_2$ mediates the coupling between $CB^-$ and graphene due to resonant energy conditions and strong coupling to the Dirac cone. Our results therefore expand the consequences of proximity effects in multilayer semiconductor stacks, showing that wave function hybridization can be a multi-step process with different bands mediating the interlayer interactions. Such effects can be exploited to resonantly engineer the spin-valley degrees of freedom in van der Waals and moir\'e heterostructures., Comment: 14 pages, 6 figures, 3 tables

Spin defects in hexagonal Boron Nitride (hBN) attract increasing interest for quantum technology since they represent optically-addressable qubits in a van der Waals material. In particular, negatively-charged boron vacancy centers (${V_B}^-$) in hBN have shown promise as sensors of temperature, pressure, and static magnetic fields. However, the short spin coherence time of this defect currently limits its scope for quantum technology. Here, we apply dynamical decoupling techniques to suppress magnetic noise and extend the spin coherence time by nearly two orders of magnitude, approaching the fundamental $T_1$ relaxation limit. Based on this improvement, we demonstrate advanced spin control and a set of quantum sensing protocols to detect electromagnetic signals in the MHz range with sub-Hz resolution. This work lays the foundation for nanoscale sensing using spin defects in an exfoliable material and opens a promising path to quantum sensors and quantum networks integrated into ultra-thin structures.

Optoelectronic properties of van der Waals homostructures can be selectively engineered by the relative twist angle between layers. Here, we study the twist-dependent moire coupling in MoSe2 homobilayers. For small angles, we find a pronounced redshift of the K-K and {\Gamma}-K excitons accompanied by a transition from K-K to {\Gamma}-K emission. Both effects can be traced back to the underlying moire pattern in the MoSe2 homobilayers, as confirmed by our low-energy continuum model for different moire excitons. We identify two distinct intralayer moire excitons for R-stacking, while H-stacking yields two degenerate intralayer excitons due to inversion symmetry. In both cases, bright interlayer excitons are found at higher energies. The performed calculations are in excellent agreement with experiment and allow us to characterize the observed exciton resonances, providing insight about the layer composition and relevant stacking configuration of different moire exciton species.

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.

Magnetic resonance imaging of spin systems combines scientific applications in medicine, chemistry and physics. Here, we investigate the pixel-wise coherent quantum dynamics of spins consisting of a 40 by 40 micron sized region of interest implanted with nitrogen vacancy centers (NV) coupled to a nano-magnetic flake of $\mathrm{CrTe_2}$. $\mathrm{CrTe_2}$ is an in-plane van der Waals ferromagnet, which we can probe quantitatively by the NV electron's spin signal even at room temperature. First, we combine the nano-scale sample shapes measured by atomic force microscope with the magnetic resonance imaging data. We then map out the coherent dynamics of the colour centers coupled to the van der Waals ferromagnet using pixel-wise coherent Rabi and Ramsey imaging of the NV sensor layer. Next, we fit the pixel-wise solution of the Hamiltonian to the quantum sensor data. Combining data and model, we can explore the detuning range of the spin oscillation with a quantum dynamic range of over $\left|\Delta_{max}\right|= 60 { }\mathrm{MHz} $ in the Ramsey interferometry mode. Finally, we show the effect of the $\mathrm{CrTe_2}$ van der Waals magnet on the coherence of the NV sensor layer and measure a 70 times increase in the maximum frequency of the quantum oscillation going from the Rabi to the Ramsey imaging mode.

Single spin defects in 2D transition-metal dichalcogenides are natural spin-photon interfaces for quantum applications. Here we report high-field magneto-photoluminescence spectroscopy from three emission lines (Q1, Q2 and Q*) of He-ion induced sulfur vacancies in monolayer $\text{MoS}_2$. Analysis of the asymmetric PL lineshapes in combination with the diamagnetic shift of Q1 and Q2 yields a consistent picture of localized emitters with a wavefunction extent of $\sim$ 3.5 nm. The distinct valley-Zeeman splitting in out-of-plane $B$-fields and the brightening of dark states through in-plane $B$-fields necessitates spin-valley selectivity of the defect states and lifted spin-degeneracy at zero field. Comparing our results to ab-initio calculations identifies the nature of Q1 and Q2 and suggests that Q* is the emission from a chemically functionalized defect. Analysis of the optical degree of circular polarization reveals that the Fermi level is a parameter that enables the tunability of the emitter. These results show that defects in 2D semiconductors may be utilized for quantum technologies.

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.

We present a novel transparent conductive support structure for two-dimensional (2D) materials that provides an electronically passive 2D/3D interface while also enabling facile interfacial charge transport. This structure, which comprises an evaporated nanocrystalline carbon (nc-C) film beneath an atomic layer deposited alumina (ALD AlOx) layer, is thermally stable and allows direct chemical vapor deposition (CVD) of 2D materials onto the surface. When the nc-C/AlOx is deposited onto a 270 nm SiO2 layer on Si, strong optical contrast for monolayer flakes is retained. Raman spectroscopy reveals good crystal quality for MoS2 and we observe a ten-fold photoluminescence intensity enhancement compared to flakes on conventional Si/SiO2. Tunneling across the ultrathin AlOx enables interfacial charge injection, which we demonstrate by artifact-free scanning electron microscopy and photoemission electron microscopy. Thus, this combination of scalable fabrication and electronic conductivity across a weakly interacting 2D/3D interface opens up new application and characterization opportunities for 2D materials., Comment: 28 pages, 9 figures

We report magneto-photoluminescence spectroscopy of gated MoS$_2$ monolayers in high magnetic fields to 28 T. At B = 0T and electron density $n_s\sim 10^{12}cm^-2$, we observe three trion resonances that cannot be explained within a single-particle picture. Employing ab initio calculations that take into account three-particle correlation effects as well as local and non-local electron-hole exchange interaction, we identify those features as quantum superpositions of inter- and intravalley spin states. We experimentally investigate the mixed character of the trion wave function via the filling factor dependent valley Zeeman shift in positive and negative magnetic fields. Our results highlight the importance of exchange interactions for exciton physics in monolayer MoS$_2$ and provide new insights into the microscopic understanding of trion physics in 2D multi-valley semiconductors for low excess carrier densities., Comment: Main manuscript: 7 pages, 3 figures ; Supplemental material: 16 pages, 4 figures

Nanoplasmonic systems combined with optically-active two-dimensional materials provide intriguing opportunities to explore and control light-matter interactions at extreme sub-wavelength lengthscales approaching the exciton Bohr radius. Here, we present room- and cryogenic-temperature investigations of light-matter interactions between an MoSe$_2$ monolayer and individual lithographically defined gold dipole nanoantennas having sub-10 nm feed gaps. By progressively tuning the nanoantenna size, their dipolar resonance is tuned relative to the A-exciton transition in a proximal MoSe$_2$ monolayer achieving a total tuning of $\sim 130\;\mathrm{meV}$. Differential reflectance measurements performed on $> 100$ structures reveal an apparent avoided crossing between exciton and dipolar mode and an exciton-plasmon coupling constant of $g= 55\;\mathrm{meV}$, representing $g/(\hbar\omega_X)\geq3\%$ of the transition energy. This places our hybrid system in the intermediate-coupling regime where spectra exhibit a characteristic Fano-like shape, indicative of the interplay between pronounced light-matter coupling and significant damping. We also demonstrate active control of the optical response by varying the polarization of the excitation light to programmably suppress coupling to the dipole mode. We further study the emerging optical signatures of the monolayer localized at dipole nanoantennas at $10\;\mathrm{K}$. Our findings represent a key step towards realizing non-linear photonic devices based on 2D materials with potential for low-energy and ultrafast performance., Comment: 17 pages, 12 figures, https://pubs.acs.org/doi/10.1021/acs.nanolett.1c02676

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.

Manipulating electronic interlayer coupling in layered van der Waals (vdW) materials is essential for designing opto-electronic devices. Here, we control vibrational and electronic interlayer coupling in bi- and trilayer 2H-MoS$_2$ using large external electric fields in a micro-capacitor device. The electric field lifts Raman selection rules and activates phonon modes in excellent agreement with ab-initio calculations. Through polarization resolved photoluminescence spectroscopy in the same device, we observe a strongly tunable valley dichroism with maximum circular polarization degree of $\sim 60\%$ in bilayer and $\sim 35\%$ in trilayer MoS$_2$ that are fully consistent with a rate equation model which includes input from electronic band structure calculations. We identify the highly delocalized electron wave function between the layers close to the high symmetry $Q$ points as the origin of the tunable circular dichroism. Our results demonstrate the possibility of electric field tunable interlayer coupling for controlling emergent spin-valley physics and hybridization driven effects in vdW materials and their heterostructures., Comment: Main manuscript: 10 pages, 4 figures ; Supplemental material: 14 pages, 9 figures

Monolayers of semiconducting transition metal dichalcogenides are a strongly emergent platform for exploring quantum phenomena in condensed matter, building novel opto-electronic devices with enhanced functionalities. Due to their atomic thickness, their excitonic optical response is highly sensitive to their dielectric environment. In this work, we explore the optical properties of monolayer thick MoSe$_2$ straddling domain wall boundaries in periodically poled LiNbO$_3$. Spatially-resolved photoluminescence experiments reveal spatial sorting of charge and photo-generated neutral and charged excitons across the boundary. Our results reveal evidence for extremely large in-plane electric fields of 3000\,kV/cm at the domain wall whose effect is manifested in exciton dissociation and routing of free charges and trions toward oppositely poled domains and a non-intuitive spatial intensity dependence. By modeling our result using drift-diffusion and continuity equations, we obtain excellent qualitative agreement with our observations and have explained the observed spatial luminescence modulation using realistic material parameters., Comment: 29 pages, 6 figures, submetted material

Materials combining the optoelectronic functionalities of semiconductors with control of the spin degree of freedom are highly sought after for the advancement of quantum technology devices. Here, we report the paramagnetic Ruddlesden-Popper hybrid perovskite Mn:(PEA)2PbI4 (PEA = phenethylammonium) in which the interaction of isolated Mn2+ ions with magnetically brightened excitons leads to circularly polarized photoluminescence. Using a combination of superconducting quantum interference device (SQUID) magnetometry and magneto-optical experiments, we find that the Brillouin-shaped polarization curve of the photoluminescence follows the magnetization of the material. This indicates coupling between localized manganese magnetic moments and exciton spins via a magnetic proximity effect. The saturation polarization of 15% at 4 K and 6 T indicates a highly imbalanced spin population and demonstrates that manganese doping enables efficient control of excitonic spin states in Ruddlesden-Popper perovskites. Our finding constitutes the first example of polarization control in magnetically doped hybrid perovskites and will stimulate research on this highly tuneable material platform that promises tailored interactions between magnetic moments and electronic states.

We report magneto-absorption spectroscopy of gated WSe$_2$ monolayers in high magnetic fields up to 60~T. When doped with a 2D Fermi sea of mobile holes, well-resolved sequences of optical transitions are observed in both $\sigma^\pm$ circular polarizations, which unambiguously and separately indicate the number of filled Landau levels (LLs) in both $K$ and $K'$ valleys. This reveals the interaction-enhanced valley Zeeman energy, which is found to be highly tunable with hole density $p$. We exploit this tunability to align the LLs in $K$ and $K'$, and find that the 2D hole gas becomes unstable against small changes in LL filling and can spontaneously valley-polarize. These results cannot be understood within a single-particle picture, highlighting the importance of exchange interactions in determining the ground state of 2D carriers in monolayer semiconductors., Comment: 8 pages, 4 figures + 3 supplementary figures

We report magneto-optical spectroscopy of gated monolayer MoS$_2$ in high magnetic fields up to 28T and obtain new insights on the many-body interaction of neutral and charged excitons with the resident charges of distinct spin and valley texture. For neutral excitons at low electron doping, we observe a nonlinear valley Zeeman shift due to dipolar spin-interactions that depends sensitively on the local carrier concentration. As the Fermi energy increases to dominate over the other relevant energy scales in the system, the magneto-optical response depends on the occupation of the fully spin-polarized Landau levels in both $K/K^{\prime}$ valleys. This manifests itself in a many-body state. Our experiments demonstrate that the exciton in monolayer semiconductors is only a single particle boson close to charge neutrality. We find that away from charge neutrality it smoothly transitions into polaronic states with a distinct spin-valley flavour that is defined by the Landau level quantized spin and valley texture., Comment: Main manuscript: 7 pages, 4 figures ; Supplemental material: 20 pages, 8 figures

Interlayer excitons (IXs) in hetero-bilayers of transition metal dichalcogenides (TMDs) represent an exciting emergent class of long-lived dipolar composite bosons in an atomically thin, near-ideal two-dimensional (2D) system. The long-range interactions that arise from the spatial separation of electrons and holes can give rise to novel quantum, as well as classical multi-particle correlation effects. In order to acquire a detailed understanding of the possible many-body effects, the fundamental interactions between individual IXs have to be studied. Here, we trap a tunable number of dipolar within a nanoscale confinement potential induced by placing a MoSe$_2$-WSe$_2$ hetero-bilayer (HBL) onto an array of SiO$_2$ nanopillars. We control the mean occupation of the IX trap via the optical excitation level and observe discrete sharp-line emission from different configurations of interacting IXs. We identify these features as different multiparticle states with $N_{IX}\sim1-5$ via their power dependencies and directly measure the hierarchy of dipolar and exchange interactions as $N_{IX}$ increases. The interlayer biexciton ($N_{IX}=2$) is found to be an emission doublet that is blue-shifted from the single exciton by $\Delta E=(8.4\pm0.6)$ meV and split by $2J=(1.2\pm0.5)$ meV. The blueshift is even more pronounced for triexcitons ($(12.4\pm0.4)$ meV), quadexcitons ($(15.5\pm0.6)$ meV) and quintexcitons ($(18.2\pm0.8)$ meV). These values are shown to be mutually consistent with numerical modelling of dipolar excitons confined to a harmonic trapping potential having a confinement lengthscale in the range $\ell\approx 3$ nm. Our results contribute to the understanding of interactions between IXs in TMD HBLs at the discrete limit of only a few excitations and represent a key step towards exploring quantum correlations between them., Comment: 15 pages, 3 figures plus Supplementary Information (19 pages, 11 pages)

We experimentally study the radii of excitons in hBN-encapsulated WS2 monolayers by means of magneto-optical reflectance spectroscopy at cryogenic temperatures in magnetic fields up to 29 T. We observe field-induced energy shifts of the exciton ground and excited states due to valley Zeeman and diamagnetic effects. We find the g factor of the first excited state of $-4.2(+/-0.1) to be essentially equal to that of the ground state of -4.35(+/-0.1). From diamagnetic shifts we determine the root mean square radii of the excitons. The radius of the first excited state is found to be 5-8 nm and that of the ground state around 2 nm. Our results further confirm the Wannier-Mott nature of the exciton quasiparticles in monolayer semiconductors and the assignment of the optical resonances in absorption-type measurements. They also provide additional support for the applicability of the effective mass hydrogenlike models in these systems., Comment: accepted for publication in Phys. Rev. B

Topological insulators have been predicted to exhibit a variety of interesting phenomena including a quantized magnetoelectric response and novel spintronics effects due to spin textures on their surfaces. However, experimental observation of these phenomena has proved difficult due to the finite bulk carrier density which may overwhelm the intrinsic topological responses that are expressed at the surface. Here, we demonstrate a novel ionic gel gating technique to tune the chemical potential of Bi$_{2}$Se$_{3}$ thin films while simultaneously performing THz spectroscopy. We can tune the carrier concentration by an order of magnitude and shift the Fermi energy, E$_{F} $ to as low as $\simeq$ 10 meV above the Dirac point. At high bias voltage and magnetic field, we observe a quantized Faraday angle consistent with the topological magnetoelectric effect that can be tuned by ionic gel gating through a number of plateau states

We report 65 tesla magneto-absorption spectroscopy of exciton Rydberg states in the archetypal monolayer semiconductor WSe$_2$. The strongly field-dependent and distinct energy shifts of the 2s, 3s, and 4s excited neutral excitons permits their unambiguous identification and allows for quantitative comparison with leading theoretical models. Both the sizes (via low-field diamagnetic shifts) and the energies of the $ns$ exciton states agree remarkably well with detailed numerical simulations using the non-hydrogenic screened Keldysh potential for 2D semiconductors. Moreover, at the highest magnetic fields the nearly-linear diamagnetic shifts of the weakly-bound 3s and 4s excitons provide a direct experimental measure of the exciton's reduced mass, $m_r = 0.20 \pm 0.01~m_0$., Comment: To appear in Phys. Rev. Lett. Updated version (25 jan 2018) now includes detailed supplemental discussion of Landau levels, Rydberg exciton energies, exciton mass, Dirac Hamiltonian, nonparabolicity, and dielectric effects

Excitons in atomically-thin semiconductors necessarily lie close to a surface, and therefore their properties are expected to be strongly influenced by the surrounding dielectric environment. However, systematic studies exploring this role are challenging, in part because the most readily accessible exciton parameter -- the exciton's optical transition energy -- is largely \textit{un}affected by the surrounding medium. Here we show that the role of the dielectric environment is revealed through its systematic influence on the \textit{size} of the exciton, which can be directly measured via the diamagnetic shift of the exciton transition in high magnetic fields. Using exfoliated WSe$_2$ monolayers affixed to single-mode optical fibers, we tune the surrounding dielectric environment by encapsulating the flakes with different materials, and perform polarized low-temperature magneto-absorption studies to 65~T. The systematic increase of the exciton's size with dielectric screening, and concurrent reduction in binding energy (also inferred from these measurements), is quantitatively compared with leading theoretical models. These results demonstrate how exciton properties can be tuned in future 2D optoelectronic devices., Comment: 7 pages, 4 figures

We describe recent experimental efforts to perform polarization-resolved optical spectroscopy of monolayer transition-metal dichalcogenide semiconductors in very large pulsed magnetic fields to 65 tesla. The experimental setup and technical challenges are discussed in detail, and temperature-dependent magneto-reflection spectra from atomically thin tungsten disulphide (WS$_2$) are presented. The data clearly reveal not only the valley Zeeman effect in these 2D semiconductors, but also the small quadratic exciton diamagnetic shift from which the very small exciton size can be directly inferred. Finally, we present model calculations that demonstrate how the measured diamagnetic shifts can be used to constrain estimates of the exciton binding energy in this new family of monolayer semiconductors., Comment: PCSI-43 conference (Jan. 2016; Palm Springs, CA)

We report circularly-polarized optical reflection spectroscopy of monolayer WS$_2$ and MoS$_2$ at low temperatures (4~K) and in high magnetic fields to 65~T. Both the A and the B exciton transitions exhibit a clear and very similar Zeeman splitting of approximately $-$230~$\mu$eV/T ($g\simeq -4$), providing the first measurements of the valley Zeeman effect and associated $g$-factors in monolayer transition-metal disulphides. These results complement and are compared with recent low-field photoluminescence measurements of valley degeneracy breaking in the monolayer diselenides MoSe$_2$ and WSe$_2$. Further, the very large magnetic fields used in our studies allows us to observe the small quadratic diamagnetic shifts of the A and B excitons in monolayer WS$_2$ (0.32 and 0.11~$\mu$eV/T$^2$, respectively), from which we calculate exciton radii of 1.53~nm and 1.16~nm. When analyzed within a model of non-local dielectric screening in monolayer semiconductors, these diamagnetic shifts also constrain and provide estimates of the exciton binding energies (410~meV and 470~meV for the A and B excitons, respectively), further highlighting the utility of high magnetic fields for understanding new 2D materials., Comment: 9 pages, 5 figures

Based on specific heat and magnetoresistance measurements, we report that a "heavy" electronic state exists below $T \approx$ 20 K in KNi$_2$Se$_2$, with an increased carrier mobility and enhanced effective electronic band mass, $m$* = 6$m_b$ to 18$m_b$. This "heavy" state evolves into superconductivity at $T_c$ = 0.80(1) K. These properties resemble that of a many-body heavy-fermion state, which derives from the hybridization between localized magnetic states and conduction electrons. Yet, no evidence for localized magnetism or magnetic order is found in KNi$_2$Se$_2$ from magnetization measurements or neutron diffraction. Instead, neutron pair-distribution-function analysis reveals the presence of local charge-density-wave distortions that disappear on cooling, an effect opposite to what is typically observed, suggesting that the low-temperature electronic state of KNi$_2$Se$_2$ arises from cooperative Coulomb interactions and proximity to, but avoidance of, charge order.