Quantum control of a nanoparticle optically levitated in cryogenic free space.

Tests of quantum mechanics on a macroscopic scale require extreme control over mechanical motion and its decoherence1-3. Quantum control of mechanical motion has been achieved by engineering the radiation-pressure coupling between a micromechanical oscillator and the electromagnetic field in a resonator4-7. Furthermore, measurement-based feedback control relying on cavity-enhanced detection schemes has been used to cool micromechanical oscillators to their quantum ground states8. In contrast to mechanically tethered systems, optically levitated nanoparticles are particularly promising candidates for matter-wave experiments with massive objects9,10, since their trapping potential is fully controllable. Here we optically levitate a femtogram (10-15 grams) dielectric particle in cryogenic free space, which suppresses thermal effects sufficiently to make the measurement backaction the dominant decoherence mechanism. With an efficient quantum measurement, we exert quantum control over the dynamics of the particle. We cool its centre-of-mass motion by measurement-based feedback to an average occupancy of 0.65 motional quanta, corresponding to a state purity of 0.43. The absence of an optical resonator and its bandwidth limitations holds promise to transfer the full quantum control available for electromagnetic fields to a mechanical system. Together with the fact that the optical trapping potential is highly controllable, our experimental platform offers a route to investigating quantum mechanics at macroscopic scales11.

Exciton-assisted electron tunnelling in van der Waals heterostructures.

The control of elastic and inelastic electron tunnelling relies on materials with well-defined interfaces. Two-dimensional van der Waals materials are an excellent platform for such studies. Signatures of acoustic phonons and defect states have been observed in current-to-voltage measurements. These features can be explained by direct electron-phonon or electron-defect interactions. Here we use a tunnelling process that involves excitons in transition metal dichalcogenides (TMDs). We study tunnel junctions consisting of graphene and gold electrodes separated by hexagonal boron nitride with an adjacent TMD monolayer and observe prominent resonant features in current-to-voltage measurements appearing at bias voltages that correspond to TMD exciton energies. By placing the TMD outside of the tunnelling pathway, we demonstrate that this tunnelling process does not require any charge injection into the TMD. The appearance of such optical modes in electrical transport introduces additional functionality towards van der Waals material-based optoelectronic devices.

State Expansion of a Levitated Nanoparticle in a Dark Harmonic Potential.

We spatially expand and subsequently contract the motional thermal state of a levitated nanoparticle using a hybrid trapping scheme. The particle's center-of-mass motion is initialized in a thermal state (temperature 155 mK) in an optical trap and then expanded by subsequent evolution in a much softer Paul trap in the absence of optical fields. We demonstrate expansion of the motional state's standard deviation in position by a factor of 24. In our system, state expansion occurs devoid of backaction from photon recoil, making this approach suitable for coherent wave function expansion.

Overbias Photon Emission from Light-Emitting Devices Based on Monolayer Transition Metal Dichalcogenides.

Tunneling light-emitting devices (LEDs) based on transition metal dichalcogenides (TMDs) and other two-dimensional (2D) materials are a new platform for on-chip optoelectronic integration. Some of the physical processes underlying this LED architecture are not fully understood, especially the emission at photon energies higher than the applied electrostatic potential, so-called overbias emission. Here we report overbias emission for potentials that are near half of the optical bandgap energy in TMD-based tunneling LEDs. We show that this emission is not thermal in nature but consistent with exciton generation via a two-electron coherent tunneling process.

Tip-Enhanced Stokes-Anti-Stokes Scattering from Carbyne.

Carbyne, a linear chain of carbon atoms, is the truly one-dimensional allotrope of carbon and the strongest known Raman scatterer. Here, we use tip-enhanced Raman scattering (TERS) to further enhance the Raman response of a single carbyne chain confined inside a double-walled carbon nanotube. We observe an increase of the anti-Stokes scattering by a factor of 3290 and a 22-fold enhancement of the anti-Stokes/Stokes ratio relative to far-field measurements. The power dependence of the anti-Stokes/Stokes ratio under TERS conditions is indicative of coherent Stokes-anti-Stokes scattering mediated by an excited phonon. The role of resonance effects and laser-induced heating are discussed and potential opportunities are outlined.

Encoding information in the mutual coherence of spatially separated light beams.

Coherence has been used as a resource for optical communications since its earliest days. It is widely used for the multiplexing of data, but not for the encoding of data. Here we introduce a coding scheme, which we call mutual coherence coding, to encode information in the mutual coherence of spatially separated light beams. We describe its implementation and analyze its performance by deriving the relevant figures of merit (signal-to-noise ratio, maximum bit-rate, and spectral efficiency) with respect to the number of transmitted beams. Mutual coherence coding yields a quadratic scaling of the number of transmitted signals with the number of employed light beams, which might have benefits for cryptography and data security.

Ponderomotive Squeezing of Light by a Levitated Nanoparticle in Free Space.

A mechanically compliant element can be set into motion by the interaction with light. In turn, this light-driven motion can give rise to ponderomotive correlations in the electromagnetic field. In optomechanical systems, cavities are often employed to enhance these correlations up to the point where they generate quantum squeezing of light. In free-space scenarios, where no cavity is used, observation of squeezing remains possible but challenging due to the weakness of the interaction, and has not been reported so far. Here, we measure the ponderomotively squeezed state of light scattered by a nanoparticle levitated in a free-space optical tweezer. We observe a reduction of the optical fluctuations by up to 25% below the vacuum level, in a bandwidth of about 15 kHz. Our results are explained well by a linearized dipole interaction between the nanoparticle and the electromagnetic continuum. These ponderomotive correlations open the door to quantum-enhanced sensing and metrology with levitated systems, such as force measurements below the standard quantum limit.

Tip-enhanced Raman spectroscopy of confined carbon chains.

Long linear chains of carbon encapsulated in carbon nanotubes represent the finite realization of carbyne, the truly one-dimensional carbon allotrope. Driven by advances in the synthesis of such structures, carbyne has attracted significant interest in recent years, with numerous experimental studies exploring its remarkable properties. As for other carbon nanomaterials, Raman spectroscopy has played an important role in the characterization of carbyne. In particular, tip-enhanced Raman scattering (TERS) has enabled imaging and spectroscopy down to the single-chain level. In this article, we provide a general introduction to carbyne and discuss the principles and experimental implementation of TERS as a key technology for the investigation of this material system. Within this context, the development of optical nanoantennas as TERS probes is addressed. We then summarize the latest progress in the Raman spectroscopic characterization of confined carbyne, with a focus on the findings assisted by TERS. Finally, we discuss open questions in the field and outline how TERS can contribute to solving them in future studies.

Resonant Light Emission from Graphene/Hexagonal Boron Nitride/Graphene Tunnel Junctions.

Single-layer graphene has many remarkable properties but does not lend itself as a material for light-emitting devices as a result of its lack of a band gap. This limitation can be overcome by a controlled stacking of graphene layers. Exploiting the unique Dirac cone band structure of graphene, we demonstrate twist-controlled resonant light emission from graphene/hexagonal boron nitride (h-BN)/graphene tunnel junctions. We observe light emission irrespective of the crystallographic alignment between the graphene electrodes. Nearly aligned devices exhibit pronounced resonant features in both optical and electrical characteristics that vanish rapidly for twist angles θ ≳3°. These experimental findings can be well-explained by a theoretical model in which the spectral photon emission peak is attributed to photon-assisted momentum conserving electron tunneling. The resonant peak in our aligned devices can be spectrally tuned within the near-infrared range by over 0.2 eV, making graphene/h-BN/graphene tunnel junctions potential candidates for on-chip optoelectronics.

Kovacs Memory Effect with an Optically Levitated Nanoparticle.

The understanding of the dynamics of nonequilibrium cooling and heating processes at the nanoscale is still an open problem. These processes can follow surprising relaxation paths due to, e.g., memory effects, which significantly alter the expected equilibration routes. The Kovacs effect can take place when a thermalization process is suddenly interrupted by a change of the bath temperature, leading to a nonmonotonic evolution of the energy of the system. Here, we demonstrate that the Kovacs effect can be observed in the thermalization of the center of mass motion of a levitated nanoparticle. The temperature is controlled during the experiment through an external source of white Gaussian noise that mimics an effective thermal bath at a temperature that can be changed faster than any relaxation time of the system. We describe our experiments in terms of the dynamics of a Brownian particle in a harmonic trap without any fitting parameter, suggesting that the Kovacs effect can appear in a large variety of systems.

Sub-Kelvin Feedback Cooling and Heating Dynamics of an Optically Levitated Librator.

Rotational optomechanics strives to gain quantum control over mechanical rotors by harnessing the interaction of light and matter. We optically trap a dielectric nanodumbbell in a linearly polarized laser field, where the dumbbell represents a nanomechanical librator. Using measurement-based parametric feedback control in high vacuum, we cool this librator from room temperature to 240 mK and investigate its heating dynamics when released from feedback. We exclude collisions with residual gas molecules as well as classical laser noise as sources of heating. Our findings indicate that we observe the torque fluctuations arising from the zero-point fluctuations of the electromagnetic field.

Erratum: GHz Rotation of an Optically Trapped Nanoparticle in Vacuum [Phys. Rev. Lett. 121, 033602 (2018)].

This corrects the article DOI: 10.1103/PhysRevLett.121.033602.

Coupling Interlayer Excitons to Whispering Gallery Modes in van der Waals Heterostructures.

Van der Waals heterostructures assembled from two-dimensional materials offer a promising platform to engineer structures with desired optoelectronic characteristics. Here we use waveguide-coupled disk resonators made of hexagonal boron nitride (h-BN) to demonstrate cavity-coupled emission from interlayer excitons of a heterobilayer of two monolayer transition metal dichalcogenides. We sandwich a MoSe2-WSe2 heterobilayer between two slabs of h-BN and directly pattern the resulting stack into waveguide-coupled disk resonators. This enables us to position the active materials into regions of highest optical field intensity, thereby maximizing the mode overlap and the coupling strength. Since the interlayer exciton emission energy is lower than the optical band gaps of the individual monolayers and since the interlayer transition itself has a weak oscillator strength, the circulating light is only weakly reabsorbed, which results in an unaffected quality factor. Our devices are fully waveguide-coupled and represent a promising platform for on-chip van der Waals photonics.

Raman Scattering Cross Section of Confined Carbyne.

We experimentally quantify the Raman scattering from individual carbyne chains confined in double-walled carbon nanotubes. We find that the resonant differential Raman cross section of confined carbyne is on the order of 10-22 cm2 sr-1 per atom, making it the strongest Raman scatterer ever reported.

Resonant Optical Antennas with Atomic-Sized Tips and Tunable Gaps Achieved by Mechanical Actuation and Electrical Control.

Enhanced electromagnetic fields in nanometer gaps of plasmonic structures increase the optical interaction with matter, including Raman scattering and optical absorption. Quantum electron tunneling across sub-1 nm gaps, however, lowers these effects again. Understanding these phenomena requires controlled variation of gap sizes. Mechanically actuated plasmonic antennas enable repeatable tuning of gap sizes from the weak-coupling over the quantum-electron-tunneling to the direct-electrical-contact regime. Gap sizes are controlled electrically via leads that only weakly disturb plasmonic modes. Conductance signals show a near-continuous transition from electron tunneling to metallic contact. As the antenna's absorption cross-section is reduced, thermal expansion effects are negligible, in contrast to conventional break-junctions. Optical scattering spectra reveal first continuous red shifts for decreasing gap sizes and then blue shifts below gaps of 0.3 nm. The approach provides pathways to study opto- and electromolecular processes at the limit of plasmonic sensing.

Motional Sideband Asymmetry of a Nanoparticle Optically Levitated in Free Space.

The hallmark of quantum physics is Planck's constant h, whose finite value entails the quantization that gave the theory its name. The finite value of h gives rise to inevitable zero-point fluctuations even at vanishing temperature. The zero-point fluctuation of mechanical motion becomes smaller with growing mass of an object, making it challenging to observe at macroscopic scales. Here, we transition a dielectric particle with a diameter of 136 nm from the classical realm to the regime where its zero-point motion emerges as a sizable contribution to its energy. To this end, we optically trap the particle at ambient temperature in ultrahigh vacuum and apply active feedback cooling to its center-of-mass motion. We measure an asymmetry between the Stokes and anti-Stokes sidebands of photons scattered by the levitated particle, which is a signature of the particle's quantum ground state of motion.

Electron Transport through Metal/MoS2 Interfaces: Edge- or Area-Dependent Process?

In ultrathin two-dimensional (2-D) materials, the formation of ohmic contacts with top metallic layers is a challenging task that involves different processes than in bulk-like structures. Besides the Schottky barrier height, the transfer length of electrons between metals and 2-D monolayers is a highly relevant parameter. For MoS2, both short (≤30 nm) and long (≥0.5 µm) values have been reported, corresponding to either an abrupt carrier injection at the contact edge or a more gradual transfer of electrons over a large contact area. Here we use ab initio quantum transport simulations to demonstrate that the presence of an oxide layer between a metallic contact and a MoS2 monolayer, for example, TiO2 in the case of titanium electrodes, favors an area-dependent process with a long transfer length, while a perfectly clean metal-semiconductor interface would lead to an edge process. These findings reconcile several theories that have been postulated about the physics of metal/MoS2 interfaces and provide a framework to design future devices with lower contact resistances.

Beam Steering with a Nonlinear Optical Phased Array Antenna.

Transition metal dichalcogenides (TMDCs) exhibit high second harmonic (SH) generation in the visible due to their noncentrosymmetric crystal structure in odd-layered form and direct bandgap transition when thinned down to a monolayer. In order to emit the SH radiation into a desired direction, one requires a means to control the phase of the in-plane nonlinear polarization. Here, we couple the SH response of a monolayer MoS2 to an optical phased array antenna and demonstrate controllable steering of the nonlinear emission. By exploiting the intrinsic SH generation by the phased array antenna we achieve uniform emission efficiency into a broad angular range. Our work has relevance for novel optoelectronic applications, such as programmable optical interconnects and on-chip LIDAR.

One-Dimensional Edge Contacts to a Monolayer Semiconductor.

Integration of electrical contacts into van der Waals (vdW) heterostructures is critical for realizing electronic and optoelectronic functionalities. However, to date no scalable methodology for gaining electrical access to buried monolayer two-dimensional (2D) semiconductors exists. Here we report viable edge contact formation to hexagonal boron nitride (hBN) encapsulated monolayer MoS2. By combining reactive ion etching, in situ Ar+ sputtering and annealing, we achieve a relatively low edge contact resistance, high mobility (up to ∼30 cm2 V-1 s-1) and high on-current density (>50 µA/µm at VDS = 3V), comparable to top contacts. Furthermore, the atomically smooth hBN environment also preserves the intrinsic MoS2 channel quality during fabrication, leading to a steep subthreshold swing of 116 mV/dec with a negligible hysteresis. Hence, edge contacts are highly promising for large-scale practical implementation of encapsulated heterostructure devices, especially those involving air sensitive materials, and can be arbitrarily narrow, which opens the door to further shrinkage of 2D device footprint.

Optical antennas driven by quantum tunneling: a key issues review.

Analogous to radio- and microwave antennas, optical nanoantennas are devices that receive and emit radiation at optical frequencies. Until recently, the realization of electrically driven optical antennas was an outstanding challenge in nanophotonics. In this review we discuss and analyze recent reports in which quantum tunneling-specifically inelastic electron tunneling-is harnessed as a means to convert electrical energy into photons, mediated by optical antennas. To aid this analysis we introduce the fundamentals of optical antennas and inelastic electron tunneling. Our discussion is focused on recent progress in the field and on future directions and opportunities.