Plasmonic nanoantennas are versatile tools for coherently controlling and directing light on the nanoscale. For these antennas, current fabrication techniques such as electron beam lithography (EBL) or focused ion beam (FIB) milling with Ga(+)-ions routinely achieve feature sizes in the 10 nm range. However, they suffer increasingly from inherent limitations when a precision of single nanometers down to atomic length scales is required, where exciting quantum mechanical effects are expected to affect the nanoantenna optics. Here, we demonstrate that a combined approach of Ga(+)-FIB and milling-based He(+)-ion lithography (HIL) for the fabrication of nanoantennas offers to readily overcome some of these limitations. Gold bowtie antennas with 6 nm gap size were fabricated with single-nanometer accuracy and high reproducibility. Using third harmonic (TH) spectroscopy, we find a substantial enhancement of the nonlinear emission intensity of single HIL-antennas compared to those produced by state-of-the-art gallium-based milling. Moreover, HIL-antennas show a vastly improved polarization contrast. This superior nonlinear performance of HIL-derived plasmonic structures is an excellent testimonial to the application of He(+)-ion beam milling for ultrahigh precision nanofabrication, which in turn can be viewed as a stepping stone to mastering quantum optical investigations in the near-field.

We investigate the optical modes in three-dimensional single-crystalline gold tapers by means of electron energy-loss spectroscopy. At the very proximity to the apex, a broad-band excitation at all photon energies from 0.75 to 2 eV, which is the onset for interband transitions, is detected. At large distances from the apex, though, we observe distinct resonances with energy dispersions roughly proportional to the inverse local radius. The nature of these phenomena is unraveled by finite difference time-domain simulations of the taper and an analytical treatment of the energy loss in fibers. Our calculations and the perfect agreement with our experimental results demonstrate the importance of phase-matching between electron field and radiative taper modes in mesoscopic structures. The local taper radius at the electron impact location determines the selective excitation of radiative modes with discrete angular momenta.

Light states composed of multiple entangled photons—such as cluster states—are essential for developing and scaling-up quantum computing networks. Photonic cluster states can be obtained from single-photon sources and entangling gates, but so far this has only been done with probabilistic sources constrained to intrinsically low efficiencies, and an increasing hardware overhead. Here, we report the resource-efficient generation of polarization-encoded, individually-addressable photons in linear cluster states occupying a single spatial mode. We employ a single entangling-gate in a fiber loop configuration to sequentially entangle an ever-growing stream of photons originating from the currently most efficient single-photon source technology—a semiconductor quantum dot. With this apparatus, we demonstrate the generation of linear cluster states up to four photons in a single-mode fiber. The reported architecture can be programmed for linear-cluster states of any number of photons, that are required for photonic one-way quantum computing schemes.

We report the observation of coherent light scattering from nanometer-sized gap regions in a nanofocusing scanning near-field optical microscope. When approaching a nanofocusing gold taper to the surface of a thin semitransparent gold film and detecting in transmission, we find a steep increase in scattering intensity over the last 5 nm in a near-field signal selected in k-space. This is confirmed as a signature of highly confined gap plasmons by detailed comparisons to finite element method simulations. The simulations reveal that the confinement is adjustable via the underlying probe–sample distance control scheme even to levels well below the taper apex radius. This controlled experimental realization of gap plasmons and the extraction of their signature in a scanning probe microscope pave the way toward broadband spectroscopy at and below single-nanometer length scales, using parallel detection at multiple wavelengths, for instance, in transient absorption or two-dimensional spectroscopy.

Nanophononics is essential for the engineering of thermal transport in nanostructured electronic devices, it greatly facilitates the manipulation of mechanical resonators in the quantum regime, and it could unveil a new route in quantum communications using phonons as carriers of information. Acoustic phonons also constitute a versatile platform for the study of fundamental wave dynamics, including Bloch oscillations, Wannier-Stark ladders, and other localization phenomena. Many of the phenomena studied in nanophononics were inspired by their counterparts in optics and electronics. In these fields, the consideration of topological invariants to control wave dynamics has already had a great impact for the generation of robust confined states. Interestingly, the use of topological phases to engineer nanophononic devices remains an unexplored and promising field. Conversely, the use of acoustic phonons could constitute a rich platform to study topological states. Here, we introduce the concept of topological invariants to nanophononics and experimentally implement a nanophononic system supporting a robust topological interface state at 350 GHz. The state is constructed through band inversion, i.e., by concatenating two semiconductor superlattices with inverted spatial mode symmetries. The existence of this state is purely determined by the Zak phases of the constituent superlattices, i.e., the one-dimensional Berry phase. We experimentally evidenced the mode through Raman spectroscopy. The reported robust topological interface states could become part of nanophononic devices requiring resonant structures such as sensors or phonon lasers.

SummaryWe investigate the radiation patterns of sharp conical gold tapers, which were designed as adiabatic nanofocusing probes for scanning near-field optical microscopy (SNOM). Field calculations show that only the lowest order eigenmode of such a taper can reach the very apex and thus induce the generation of strongly enhanced near-field signals. Higher-order modes are coupled into the far field at finite distances from the apex. Here, we demonstrate experimentally how to distinguish and separate between the lowest and higher-order eigenmodes of such a metallic taper by filtering in the spatial frequency domain. Our approach has the potential to considerably improve the signal-to-background ratio in spectroscopic experiments at the nanoscale.

The coherent exchange of optical near fields between two neighboring dipoles 1, 2, 3 plays an essential role for the optical properties, quantum dynamics and thus for the function of many naturally occurring 4, 5 and artificial 3,6,7,8,9 nanosystems. These interactions are inherently short-ranged, extending over a few nanometers only, and depend sensitively on relative orientation, detuning and dephasing, i.e., on the vectorial properties of the coupled dipolar near fields. This makes it challenging to analyze them experimentally.Here, we introduce plasmonic nanofocusing spectroscopy to record coherent light scattering spectra with 5-nm spatial resolution from a small dipole antenna, excited solely by evanescent fields 10,11,12 , and coupled to plasmon resonances in a single gold nanorod 13,14,15 . We resolve mode couplings, resonance energy shifts and Purcell effects as a function of dipole distance and relative orientation, and show how they arise from different vectorial components of the interacting optical near-fields.Our results pave the way for using dipolar alignment to control the optical properties and function of nanoscale systems.

Half-integer photon-resonances in a periodically shaken double well are investigated on the level of the N -particle quantum dynamics. Contrary to non-linear mean-field equations, the linear Nparticle Schrödinger equation does not contain any non-linearity which could be the origin of such resonances. Nevertheless, analytic calculations on the N -particle level explain why such resonances can be observed even for particle numbers as low as N = 2. These calculations also demonstrate why fractional photon resonances are not restricted to half-integer values.