Layered metals as polarized transparent conductors.

The quest to improve transparent conductors balances two key goals: increasing electrical conductivity and increasing optical transparency. To improve both simultaneously is hindered by the physical limitation that good metals with high electrical conductivity have large carrier densities that push the plasma edge into the ultra-violet range. Technological solutions reflect this trade-off, achieving the desired transparencies only by reducing the conductor thickness or carrier density at the expense of a lower conductance. Here we demonstrate that highly anisotropic crystalline conductors offer an alternative solution, avoiding this compromise by separating the directions of conduction and transmission. We demonstrate that slabs of the layered oxides Sr2RuO4 and Tl2Ba2CuO6+δ are optically transparent even at macroscopic thicknesses >2 µm for c-axis polarized light. Underlying this observation is the fabrication of out-of-plane slabs by focused ion beam milling. This work provides a glimpse into future technologies, such as highly polarized and addressable optical screens.

Erratum: Observation of Magnetic Proximity Effect Using Resonant Optical Spectroscopy of an Electrically Tunable MoSe_{2}/CrBr_{3} Heterostructure [Phys. Rev. Lett. 124, 197401 (2020)].

This corrects the article DOI: 10.1103/PhysRevLett.124.197401.

Optical Sensing of Fractional Quantum Hall Effect in Graphene.

Graphene and its heterostructures provide a unique and versatile playground for explorations of strongly correlated electronic phases, ranging from unconventional fractional quantum Hall (FQH) states in a monolayer system to a plethora of superconducting and insulating states in twisted bilayers. However, the access to those fascinating phases has been thus far entirely restricted to transport techniques, due to the lack of a robust energy bandgap that makes graphene hard to access optically. Here we demonstrate an all-optical, noninvasive spectroscopic tool for probing electronic correlations in graphene using excited Rydberg excitons in an adjacent transition metal dichalcogenide monolayer. These excitons are highly susceptible to the compressibility of graphene electrons, allowing us to detect the formation of odd-denominator FQH states at high magnetic fields. Owing to its submicron spatial resolution, the technique we demonstrate circumvents spatial inhomogeneities and paves the way for optical studies of correlated states in optically inactive atomically thin materials.

Electrically tunable quantum confinement of neutral excitons.

Confining particles to distances below their de Broglie wavelength discretizes their motional state. This fundamental effect is observed in many physical systems, ranging from electrons confined in atoms or quantum dots1,2 to ultracold atoms trapped in optical tweezers3,4. In solid-state photonics, a long-standing goal has been to achieve fully tunable quantum confinement of optically active electron-hole pairs, known as excitons. To confine excitons, existing approaches mainly rely on material modulation5, which suffers from poor control over the energy and position of trapping potentials. This has severely impeded the engineering of large-scale quantum photonic systems. Here we demonstrate electrically controlled quantum confinement of neutral excitons in 2D semiconductors. By combining gate-defined in-plane electric fields with inherent interactions between excitons and free charges in a lateral p-i-n junction, we achieve exciton confinement below 10 nm. Quantization of excitonic motion manifests in the measured optical response as a ladder of discrete voltage-dependent states below the continuum. Furthermore, we observe that our confining potentials lead to a strong modification of the relative wave function of excitons. Our technique provides an experimental route towards creating scalable arrays of identical single-photon sources and has wide-ranging implications for realizing strongly correlated photonic phases6,7 and on-chip optical quantum information processors8,9.

Electrically tunable Feshbach resonances in twisted bilayer semiconductors.

Moiré superlattices in transition metal dichalcogenide bilayers provide a platform for exploring strong correlations with optical spectroscopy. Despite the observation of rich Mott-Wigner physics stemming from an interplay between the periodic potential and Coulomb interactions, the absence of tunnel coupling­induced hybridization of electronic states has ensured a classical layer degree of freedom. We investigated a MoSe2 homobilayer structure where interlayer coherent tunneling allows for electric field­controlled manipulation and measurement of the ground-state hole-layer pseudospin. We observed an electrically tunable two-dimensional Feshbach resonance in exciton-hole scattering, which allowed us to control the strength of interactions between excitons and holes located in different layers. Our results may enable the realization of degenerate Bose-Fermi mixtures with tunable interactions.

Signatures of Wigner crystal of electrons in a monolayer semiconductor.

When the Coulomb repulsion between electrons dominates over their kinetic energy, electrons in two-dimensional systems are predicted to spontaneously break continuous-translation symmetry and form a quantum crystal1. Efforts to observe2-12 this elusive state of matter, termed a Wigner crystal, in two-dimensional extended systems have primarily focused on conductivity measurements on electrons confined to a single Landau level at high magnetic fields. Here we use optical spectroscopy to demonstrate that electrons in a monolayer semiconductor with density lower than 3 × 1011 per centimetre squared form a Wigner crystal. The combination of a high electron effective mass and reduced dielectric screening enables us to observe electronic charge order even in the absence of a moiré potential or an external magnetic field. The interactions between a resonantly injected exciton and electrons arranged in a periodic lattice modify the exciton bandstructure so that an umklapp resonance arises in the optical reflection spectrum, heralding the presence of charge order13. Our findings demonstrate that charge-tunable transition metal dichalcogenide monolayers14 enable the investigation of previously uncharted territory for many-body physics where interaction energy dominates over kinetic energy.

Observation of Magnetic Proximity Effect Using Resonant Optical Spectroscopy of an Electrically Tunable MoSe_{2}/CrBr_{3} Heterostructure.

van der Waals heterostructures combining two-dimensional magnetic and semiconducting layers constitute a promising platform for interfacing magnetism, electronics, and optics. Here, we use resonant optical reflection spectroscopy to observe the magnetic proximity effect in a gate-tunable MoSe_{2}/CrBr_{3} heterostructure. The high quality of the interface leads to a giant zero-field splitting of the K and K^{'} valley excitons in MoSe_{2}, equivalent to an external magnetic field of 12 T, with a weak but distinct electric field dependence that hints at potential for electrical control of magnetization. The magnetic proximity effect allows us to use resonant optical spectroscopy to fully characterize the CrBr_{3} magnet, determining the easy-axis coercive field, the magnetic anisotropy energy, and critical exponents associated with spin susceptibility and magnetization.

Strongly correlated electrons and hybrid excitons in a moiré heterostructure.

Two-dimensional materials and their heterostructures constitute a promising platform to study correlated electronic states, as well as the many-body physics of excitons. Transport measurements on twisted graphene bilayers have revealed a plethora of intertwined electronic phases, including Mott insulators, strange metals and superconductors1-5. However, signatures of such strong electronic correlations in optical spectroscopy have hitherto remained unexplored. Here we present experiments showing how excitons that are dynamically screened by itinerant electrons to form exciton-polarons6,7 can be used as a spectroscopic tool to investigate interaction-induced incompressible states of electrons. We study a molybdenum diselenide/hexagonal boron nitride/molybdenum diselenide heterostructure that exhibits a long-period moiré superlattice, as evidenced by coherent hole-tunnelling-mediated avoided crossings of an intralayer exciton with three interlayer exciton resonances separated by about five millielectronvolts. For electron densities corresponding to half-filling of the lowest moiré subband, we observe strong layer pseudospin paramagnetism, demonstrated by an abrupt transfer of all the (roughly 1,500) electrons from one molybdenum diselenide layer to the other on application of a small perpendicular electric field. Remarkably, the electronic state at half-filling of each molybdenum diselenide layer is resilient towards charge redistribution by the applied electric field, demonstrating an incompressible Mott-like state of electrons. Our experiments demonstrate that optical spectroscopy provides a powerful tool for investigating strongly correlated electron physics in the bulk and paves the way for investigating Bose-Fermi mixtures of degenerate electrons and dipolar excitons.

Nonlinear optics in the fractional quantum Hall regime.

Engineering strong interactions between optical photons is a challenge for quantum science. Polaritonics, which is based on the strong coupling of photons to atomic or electronic excitations in an optical resonator, has emerged as a promising approach to address this challenge, paving the way for applications such as photonic gates for quantum information processing1 and photonic quantum materials for the investigation of strongly correlated driven-dissipative systems2,3. Recent experiments have demonstrated the onset of quantum correlations in exciton-polariton systems4,5, showing that strong polariton blockade6-the prevention of resonant injection of additional polaritons in a well delimited region by the presence of a single polariton-could be achieved if interactions were an order of magnitude stronger. Here we report time-resolved four-wave-mixing experiments on a two-dimensional electron system embedded in an optical cavity7, demonstrating that polariton-polariton interactions are strongly enhanced when the electrons are initially in the fractional quantum Hall regime. Our experiments indicate that, in addition to strong correlations in the electronic ground state, exciton-electron interactions leading to the formation of polaron-polaritons8-11 have a key role in enhancing the nonlinear optical response of the system. Our findings could facilitate the realization of strongly interacting photonic systems, and suggest that nonlinear optical measurements could provide information about fractional quantum Hall states that is not accessible through their linear optical response.

Very large tunneling magnetoresistance in layered magnetic semiconductor CrI3.

Magnetic layered van der Waals crystals are an emerging class of materials giving access to new physical phenomena, as illustrated by the recent observation of 2D ferromagnetism in Cr2Ge2Te6 and CrI3. Of particular interest in semiconductors is the interplay between magnetism and transport, which has remained unexplored. Here we report magneto-transport measurements on exfoliated CrI3 crystals. We find that tunneling conduction in the direction perpendicular to the crystalline planes exhibits a magnetoresistance as large as 10,000%. The evolution of the magnetoresistance with magnetic field and temperature reveals that the phenomenon originates from multiple transitions to different magnetic states, whose possible microscopic nature is discussed on the basis of all existing experimental observations. This observed dependence of the conductance of a tunnel barrier on its magnetic state is a phenomenon that demonstrates the presence of a strong coupling between transport and magnetism in magnetic van der Waals semiconductors.

Polaron Polaritons in the Integer and Fractional Quantum Hall Regimes.

Elementary quasiparticles in a two-dimensional electron system can be described as exciton polarons since electron-exciton interactions ensures dressing of excitons by Fermi-sea electron-hole pair excitations. A relevant open question is the modification of this description when the electrons occupy flat bands and electron-electron interactions become prominent. Here, we perform cavity spectroscopy of a two-dimensional electron system in the strong coupling regime, where polariton resonances carry signatures of strongly correlated quantum Hall phases. By measuring the evolution of the polariton splitting under an external magnetic field, we demonstrate the modification of polaron dressing that we associate with filling factor dependent electron-exciton interactions.

Realization of an Electrically Tunable Narrow-Bandwidth Atomically Thin Mirror Using Monolayer MoSe_{2}.

The advent of two-dimensional semiconductors, such as van der Waals heterostructures, propels new research directions in condensed matter physics and enables development of novel devices with unique functionalities. Here, we show experimentally that a monolayer of MoSe_{2} embedded in a charge controlled heterostructure can be used to realize an electrically tunable atomically thin mirror, which effects 87% extinction of an incident field that is resonant with its exciton transition. The corresponding maximum reflection coefficient of 41% is only limited by the ratio of the radiative decay rate to the nonradiative linewidth of exciton transition and is independent of incident light intensity up to 400 W/cm^{2}. We demonstrate that the reflectivity of the mirror can be drastically modified by applying a gate voltage that modifies the monolayer charge density. Our findings could find applications ranging from fast programable spatial light modulators to suspended ultralight mirrors for optomechanical devices.

Giant Paramagnetism-Induced Valley Polarization of Electrons in Charge-Tunable Monolayer MoSe_{2}.

For applications exploiting the valley pseudospin degree of freedom in transition metal dichalcogenide monolayers, efficient preparation of electrons or holes in a single valley is essential. Here, we show that a magnetic field of 7 T leads to a near-complete valley polarization of electrons in a MoSe_{2} monolayer with a density 1.6×10^{12} cm^{-2}; in the absence of exchange interactions favoring single-valley occupancy, a similar degree of valley polarization would have required a pseudospin g factor of 38. To investigate the magnetic response, we use polarization resolved photoluminescence as well as resonant reflection measurements. In the latter, we observe gate voltage dependent transfer of oscillator strength from the exciton to the attractive Fermi polaron: stark differences in the spectrum of the two light helicities provide a confirmation of valley polarization. Our findings suggest an interaction induced giant paramagnetic response of MoSe_{2}, which paves the way for valleytronics applications.

Electrically tunable artificial gauge potential for polaritons.

Neutral particles subject to artificial gauge potentials can behave as charged particles in magnetic fields. This fascinating premise has led to demonstrations of one-way waveguides, topologically protected edge states and Landau levels for photons. In ultracold neutral atoms, effective gauge fields have allowed the emulation of matter under strong magnetic fields leading to realization of Harper-Hofstadter and Haldane models. Here we show that application of perpendicular electric and magnetic fields effects a tunable artificial gauge potential for two-dimensional microcavity exciton polaritons. For verification, we perform interferometric measurements of the associated phase accumulated during coherent polariton transport. Since the gauge potential originates from the magnetoelectric Stark effect, it can be realized for photons strongly coupled to excitations in any polarizable medium. Together with strong polariton-polariton interactions and engineered polariton lattices, artificial gauge fields could play a key role in investigation of non-equilibrium dynamics of strongly correlated photons.

Continuous-wave pumping of multiexciton bands in the photoluminescence spectrum of a single CdTe-CdSe core-shell colloidal quantum dot.

Single-exciton, biexciton, triexciton, and quadraexciton bands were resolved in the microphotoluminescence spectrum of a single CdTe/CdSe core-shell colloidal quantum dot, revealing nearly blinking-free behavior. Multiexcitons were generated by a sequential filling of electronic shells with the increase of a continuous-wave excitation power, and their probability was evaluated under steady-state conditions. A partial carriers' delocalization was determined at the core-shell interface, and an exciton binding energy was estimated by a second-order perturbation theory.

Optical detection of single-electron spin resonance in a quantum dot.

We demonstrate optically detected spin resonance of a single electron confined to a self-assembled quantum dot. The dot is rendered dark by resonant optical pumping of the spin with a laser. Contrast is restored by applying a radio frequency (rf) magnetic field at the spin resonance. The scheme is sensitive even to rf fields of just a few microT. In one case, the spin resonance behaves as a driven 3-level lambda system with weak damping; in another one, the dot exhibits remarkably strong (67% signal recovery) and narrow (0.34 MHz) spin resonances with fluctuating resonant positions, evidence of unusual dynamic processes.

Fiber-based confocal microscope for cryogenic spectroscopy.

We describe the design and performance of a fiber-based confocal microscope for cryogenic operation. The microscope combines positioning at low temperatures along three space coordinates of millimeter translation and nanometer precision with high stability and optical performance at the diffraction limit. It was successfully tested under ambient conditions as well as at liquid nitrogen (77 K) and liquid helium (4 K) temperatures. The compact nonmagnetic design provides for long term position stability against helium refilling transfers, temperature sweeps, as well as magnetic field variation between -9 and 9 T. As a demonstration of the microscope performance, applications in the spectroscopy of single semiconductor quantum dots are presented.

Optical pumping of a single hole spin in a quantum dot.

The spin of an electron is a natural two-level system for realizing a quantum bit in the solid state. For an electron trapped in a semiconductor quantum dot, strong quantum confinement highly suppresses the detrimental effect of phonon-related spin relaxation. However, this advantage is offset by the hyperfine interaction between the electron spin and the 10(4) to 10(6) spins of the host nuclei in the quantum dot. Random fluctuations in the nuclear spin ensemble lead to fast spin decoherence in about ten nanoseconds. Spin-echo techniques have been used to mitigate the hyperfine interaction, but completely cancelling the effect is more attractive. In principle, polarizing all the nuclear spins can achieve this but is very difficult to realize in practice. Exploring materials with zero-spin nuclei is another option, and carbon nanotubes, graphene quantum dots and silicon have been proposed. An alternative is to use a semiconductor hole. Unlike an electron, a valence hole in a quantum dot has an atomic p orbital which conveniently goes to zero at the location of all the nuclei, massively suppressing the interaction with the nuclear spins. Furthermore, in a quantum dot with strong strain and strong quantization, the heavy hole with spin-3/2 behaves as a spin-1/2 system and spin decoherence mechanisms are weak. We demonstrate here high fidelity (about 99 per cent) initialization of a single hole spin confined to a self-assembled quantum dot by optical pumping. Our scheme works even at zero magnetic field, demonstrating a negligible hole spin hyperfine interaction. We determine a hole spin relaxation time at low field of about one millisecond. These results suggest a route to the realization of solid-state quantum networks that can intra-convert the spin state with the polarization of a photon.

Voltage-controlled optics of a quantum dot.

We show how the optical properties of a single semiconductor quantum dot can be controlled with a small dc voltage applied to a gate electrode. We find that the transmission spectrum of the neutral exciton exhibits two narrow lines with approximately 2 mueV linewidth. The splitting into two linearly polarized components arises through an exchange interaction within the exciton. The exchange interaction can be turned off by choosing a gate voltage where the dot is occupied with an additional electron. Saturation spectroscopy demonstrates that the neutral exciton behaves as a two-level system. Our experiments show that the remaining problem for manipulating excitonic quantum states in this system is spectral fluctuation on a mueV energy scale.