Rudolf Bratschitsch

Nanoscale imaging magnetometry with diamond spins under ambient conditions

Magnetic resonance imaging and optical microscopy are key technologies in the life sciences. For microbiological studies, especially of the inner workings of single cells, optical microscopy is normally used because it easily achieves resolution close to the optical wavelength. But in conventional microscopy, diffraction limits the resolution to about half the wavelength. Recently, it was shown that this limit can be partly overcome by nonlinear imaging techniques, but there is still a barrier to reaching the molecular scale. In contrast, in magnetic resonance imaging the spatial resolution is not determined by diffraction; rather, it is limited by magnetic field sensitivity, and so can in principle go well below the optical wavelength. The sensitivity of magnetic resonance imaging has recently been improved enough to image single cells, and magnetic resonance force microscopy has succeeded in detecting single electrons and small nuclear spin ensembles. However, this technique currently requires cryogenic temperatures, which limit most potential biological applications. Alternatively, single-electron spin states can be detected optically, even at room temperature in some systems. Here we show how magneto-optical spin detection can be used to determine the location of a spin associated with a single nitrogen-vacancy centre in diamond with nanometre resolution under ambient conditions. By placing these nitrogen-vacancy spins in functionalized diamond nanocrystals, biologically specific magnetofluorescent spin markers can be produced. Significantly, we show that this nanometre-scale resolution can be achieved without any probes located closer than typical cell dimensions. Furthermore, we demonstrate the use of a single diamond spin as a scanning probe magnetometer to map nanoscale magnetic field variations. The potential impact of single-spin imaging at room temperature is far-reaching. It could lead to the capability to probe biologically relevant spins in living cells.

Photoluminescence emission and Raman response of monolayer MoS 2 , MoSe 2 , and WSe 2

We mechanically exfoliate mono- and few-layers of the transition metal dichalcogenides molybdenum disulfide, molybdenum diselenide, and tungsten diselenide. The exact number of layers is unambiguously determined by atomic force microscopy and high-resolution Raman spectroscopy. Strong photoluminescence emission is caused by the transition from an indirect band gap semiconductor of bulk material to a direct band gap semiconductor in atomically thin form.

Tailoring Spatiotemporal Light Confinement in Single Plasmonic Nanoantennas

Plasmonic nanoantennas are efficient devices to concentrate light in spatial regions much smaller than the wavelength. Only recently, their ability to manipulate photons also on a femtosecond time scale has been harnessed. Nevertheless, designing the dynamical properties of optical antennas has been difficult since the relevant microscopic processes governing their ultrafast response have remained unclear. Here, we exploit frequency-resolved optical gating to directly investigate plasmon response times of different antenna geometries resonant in the near-infrared. Third-harmonic imaging is used in parallel to spatially monitor the plasmonic mode patterns. We find that the few-femtosecond dynamics of these nanodevices is dominated by radiative damping. A high efficiency for nonlinear frequency conversion is directly linked to long plasmon damping times. This single parameter explains the counterintuitive result that rod-type nanoantennas with minimum volume generate by far the strongest third-harmonic emission as compared to the more bulky geometries of bow-tie-, elliptical-, or disk-shaped specimens.

Resonant internal quantum transitions and femtosecond radiative decay of excitons in monolayer WSe2

Atomically thin two-dimensional crystals have revolutionized materials science. In particular, monolayer transition metal dichalcogenides promise novel optoelectronic applications, owing to their direct energy gaps in the optical range. Their electronic and optical properties are dominated by Coulomb-bound electron-hole pairs called excitons, whose unusual internal structure, symmetry, many-body effects and dynamics have been vividly discussed. Here we report the first direct experimental access to all 1s A excitons, regardless of momentum--inside and outside the radiative cone--in single-layer WSe2. Phase-locked mid-infrared pulses reveal the internal orbital 1s-2p resonance, which is highly sensitive to the shape of the excitonic envelope functions and provides accurate transition energies, oscillator strengths, densities and linewidths. Remarkably, the observed decay dynamics indicates an ultrafast radiative annihilation of small-momentum excitons within 150 fs, whereas Auger recombination prevails for optically dark states. The results provide a comprehensive view of excitons and introduce a new degree of freedom for quantum control, optoelectronics and valleytronics of dichalcogenide monolayers.

Photovoltaic and Photothermoelectric Effect in a Double-Gated WSe2 Device

Tungsten diselenide (WSe2), a semiconducting transition metal dichalcogenide (TMDC), shows great potential as active material in optoelectronic devices due to its ambipolarity and direct bandgap in its single-layer form. Recently, different groups have exploited the ambipolarity of WSe2 to realize electrically tunable PN junctions, demonstrating its potential for digital electronics and solar cell applications. In this Letter, we focus on the different photocurrent generation mechanisms in a double-gated WSe2 device by measuring the photocurrent (and photovoltage) as the local gate voltages are varied independently in combination with above- and below-bandgap illumination. This enables us to distinguish between two main photocurrent generation mechanisms, the photovoltaic and photothermoelectric effect. We find that the dominant mechanism depends on the defined gate configuration. In the PN and NP configurations, photocurrent is mainly generated by the photovoltaic effect and the device displays a maximum responsivity of 0.70 mA/W at 532 nm illumination and rise and fall times close to 10 ms. Photocurrent generated by the photothermoelectric effect emerges in the PP configuration and is a factor of 2 larger than the current generated by the photovoltaic effect (in PN and NP configurations). This demonstrates that the photothermoelectric effect can play a significant role in devices based on WSe2 where a region of strong optical absorption, caused by, for example, an asymmetry in flake thickness or optical absorption of the electrodes, generates a sizable thermal gradient upon illumination.

Single defect centers in diamond nanocrystals as quantum probes for plasmonic nanostructures

We present two applications of a single nitrogen vacancy center in a nanodiamond as quantum probe for plasmonic nanostructures. Coupling to the nanostructures is achieved in a highly controlled manner by picking up a pre-characterized nanocrystal with an atomic force microscope and placing it at the desired position. Local launching of single excitations into a nanowire with a spatial control of few nanometers is demonstrated. Further, a two dimensional map of the electromagnetic environment of a plasmonic bowtie antenna was derived, resembling an ultimate limit of fluorescence lifetime nanoscopy.

Trion fine structure and coupled spin–valley dynamics in monolayer tungsten disulfide

Monolayer transition-metal dichalcogenides have recently emerged as possible candidates for valleytronic applications, as the spin and valley pseudospin are directly coupled and stabilized by a large spin splitting. The optical properties of these two-dimensional crystals are dominated by tightly bound electron–hole pairs (excitons) and more complex quasiparticles such as charged excitons (trions). Here we investigate monolayer WS2 samples via photoluminescence and time-resolved Kerr rotation. In photoluminescence and in energy-dependent Kerr rotation measurements, we are able to resolve two different trion states, which we interpret as intravalley and intervalley trions. Using time-resolved Kerr rotation, we observe a rapid initial valley polarization decay for the A exciton and the trion states. Subsequently, we observe a crossover towards exciton–exciton interaction-related dynamics, consistent with the formation and decay of optically dark A excitons. By contrast, resonant excitation of the B exciton transition leads to a very slow decay of the Kerr signal.

Thermally Assisted All‐Optical Helicity Dependent Magnetic Switching in Amorphous Fe100–xTbx Alloy Films

All-optical switching (AOS) in ferrimagnetic Fe(100-x)Tb(x) alloys is presented. AOS is witnessed below, above, and in samples without a magnetic compensation point. It is found that AOS is associated with laser heating up to the Curie temperature and intimately linked to a low remanent sample magnetization. Above a threshold magnetization of 220 emu/cc helicity dependent AOS is replaced by pure thermal demagnetization.

Bow-tie nano-antenna assisted generation of extreme ultraviolet radiation

We report on the generation of extreme ultraviolet radiation utilizing the plasmonic field enhancement in arrays of bow-tie gold optical antennae. Furthermore, their suitability to support high-order harmonic generation is examined by means of finite-difference time-domain calculations and experiments. Particular emphasis is paid to the thermal properties, which become significant at the employed peak intensities. A damage threshold depending on the antenna length is predicted and confirmed by our experimental findings. Moreover, the gas density in the vicinity of the antennae is characterized experimentally to determine the number of atoms contributing to the measured radiation, which is almost an order of magnitude larger than previously reported.

Enhancement of the magnetic modulation of surface plasmon polaritons in Au/Co/Au films

The deposition of a dielectric overlayer on top of Au/Co/Au multilayer films can significantly enhance the magnetic field induced modulation of the surface plasmon polariton (SPP) wave vector. This enhancement is analyzed as a function of the thickness of the dielectric overlayer and the associated SPP electromagnetic field confinement and redistribution. The decrease in SPP propagation distance is taken into account by analyzing an adequate figure of merit.