Rainer J. Stöhr

Optical detection of a single rare-earth ion in a crystal

Rare-earth-doped laser materials show strong prospects for quantum information storage and processing, as well as for biological imaging, due to their high-Q 4f↔4f optical transitions. However, the inability to optically detect single rare-earth dopants has prevented these materials from reaching their full potential. Here we detect a single photostable Pr3+ ion in yttrium aluminium garnet nanocrystals with high contrast photon antibunching by using optical upconversion of the excited state population of the 4f↔4f optical transition into ultraviolet fluorescence. We also demonstrate on-demand creation of Pr3+ ions in a bulk yttrium aluminium garnet crystal by patterned ion implantation. Finally, we show generation of local nanophotonic structures and cell death due to photochemical effects caused by upconverted ultraviolet fluorescence of praseodymium-doped yttrium aluminium garnet in the surrounding environment. Our study demonstrates versatile use of rare-earth atomic-size ultraviolet emitters for nanoengineering and biotechnological applications.

Fluorescence of laser-created electron-hole plasma in graphene

We present an experimental observation of nonlinear up- and down-converted optical luminescence of graphene and thin graphite subject to picosecond infrared laser pulses. We show that the excitation yields to a high-density electron-hole plasma in graphene. It is further shown that the excited charge carriers can efficiently exchange energy due to scattering in momentum space. The recombination of the resulting nonequilibrium electron-hole pairs yields to the observed white-light luminescence. Due to the scattering mechanism, the power dependence of the luminescence is quadratic until it saturates for higher laser power. Studying the luminescence intensity as a function of layer thickness gives further insight into its nature and provides a new tool for substrate independent thickness determination of multilayer flakes.

Nanoengineered diamond waveguide as a robust bright platform for nanomagnetometry using shallow nitrogen vacancy centers.

Photonic structures in diamond are key to most of its application in quantum technology. Here, we demonstrate tapered nanowaveguides structured directly onto the diamond substrate hosting shallow-implanted nitrogen vacancy (NV) centers. By optimization based on simulations and precise experimental control of the geometry of these pillar-shaped nanowaveguides, we achieve a net photon flux up to ∼ 1.7 × 10(6) s(-1). This presents the brightest monolithic bulk diamond structure based on single NV centers so far. We observe no impact on excited state lifetime and electronic spin dephasing time (T2) due to the nanofabrication process. Possessing such high brightness with low background in addition to preserved spin quality, this geometry can improve the current nanomagnetometry sensitivity ∼ 5 times. In addition, it facilitates a wide range of diamond defects-based magnetometry applications. As a demonstration, we measure the temperature dependency of T1 relaxation time of a single shallow NV center electronic spin. We observe the two-phonon Raman process to be negligible in comparison to the dominant two-phonon Orbach process.

Enhancing the spin properties of shallow implanted nitrogen vacancy centers in diamond by epitaxial overgrowth

Scaling of diamond defect center based quantum registers relies on the ability to position nitrogen vacancy (NV) centers with high spatial resolution. Using ion implantation, shallow (<10 nm) NVs can be placed with accuracy below 20 nm, but generally show reduced spin properties compared to bulk NVs. We demonstrate the enhancement of spin properties for shallow implanted NVs using a diamond overgrowth technique. An increase of coherence times up to an order of magnitude (T2 = 250 μs) was achieved, ms decoherence times were realized using dynamical decoupling. This marks a further step towards achieving strong coupling among defects positioned with nm precision.

Single defect center scanning near-field optical microscopy on graphene.

We present a scanning-probe microscope based on an atomic-size emitter, a single nitrogen-vacancy center in a nanodiamond. We employ this tool to quantitatively map the near-field coupling between the NV center and a flake of graphene in three dimensions with nanoscale resolution. Further we demonstrate universal energy transfer distance scaling between a point-like atomic emitter and a two-dimensional acceptor. Our study paves the way toward a versatile single emitter scanning microscope, which could image and excite molecular-scale light fields in photonic nanostructures or single fluorescent molecules.

All-Optical High-Resolution Nanopatterning and 3D Suspending of Graphene

We introduce a laser-based technique capable of both imaging and patterning graphene with high spatial resolution. Both tasks are performed in situ using the same confocal microscope. Imaging graphene is based on the recombination of a laser-created electron-hole plasma yielding to a broadband up- and down-converted fluorescence. Patterning is due to burning graphene by local heating causing oxidation and conversion into CO(2). By shaping the laser beam profile using 1D phase-shifting plates and 2D vortex plates we can produce graphene dots below 100 nm in diameter and graphene nanoribbons down to 20 nm in width. Additionally, we demonstrate that this technique can also be applied to freely suspended graphene resulting in freely suspended graphene nanoribbons. We further present a way of freely hanging graphene vertically and imaging it in 3D. Taking advantage of having vertically hanging graphene for the first time, we measure the out-of-plane anisotropy of the upconversion fluorescence.

Mapping spin coherence of a single rare-earth ion in a crystal onto a single photon polarization state.

We report on optical detection of a single photostable Ce(3+) ion in an yttrium aluminium garnet (YAG) crystal and on its magneto-optical properties at room temperature. The spin quantum state of the emitting level of a single cerium ion in YAG can be initialized by a circularly polarized laser pulse. Coherent precession of the electron spin is read out by observing temporal behavior of circularly polarized fluorescence of the ion. This implies direct mapping of the spin quantum state of Ce(3+) ion onto the polarization state of the emitted photon and represents the quantum interface between a single spin and a single photon.

Single spin optically detected magnetic resonance with 60–90 GHz (E-band) microwave resonators

Magnetic resonance with ensembles of electron spins is commonly performed around 10 GHz, but also at frequencies above 240 GHz and in corresponding magnetic fields of over 9 T. However, experiments with single electron and nuclear spins so far only reach into frequency ranges of several 10 GHz, where existing coplanar waveguide structures for microwave (MW) delivery are compatible with single spin readout techniques (e.g., electrical or optical readout). Here, we explore the frequency range up to 90 GHz, with magnetic fields of up to ≈3 T for single spin magnetic resonance in conjunction with optical spin readout. To this end, we develop MW resonators with optical single spin access. In our case, rectangular 60-90 GHz (E-band) waveguides guarantee low-loss supply of microwaves to the resonators. Three dimensional cavities, as well as coplanar waveguide resonators, enhance MW fields by spatial and spectral confinement with a MW efficiency of 1.36 mT/√W. We utilize single nitrogen vacancy (NV) centers as hosts for optically accessible spins and show that their properties regarding optical spin readout known from smaller fields (<0.65 T) are retained up to fields of 3 T. In addition, we demonstrate coherent control of single nuclear spins under these conditions. Furthermore, our results extend the applicable magnetic field range of a single spin magnetic field sensor. Regarding spin based quantum registers, high fields lead to a purer product basis of electron and nuclear spins, which promises improved spin lifetimes. For example, during continuous single-shot readout, the (14)N nuclear spin shows second-long longitudinal relaxation times.

Production yield of rare-earth ions implanted into an optical crystal

Rare-earth ions doped into desired locations of optical crystals might enable a range of novel integrated photonic devices for quantum applications. With this aim, we have investigated the production yield of cerium and praseodymium by means of ion implantation. As a measure, the collected fluorescence intensity from both, implanted samples and single centers was used. With a tailored annealing procedure for cerium, a yield up to 53% was estimated. Praseodymium yield amounts up to 91%.

Enhanced photoluminescence from self-organized rubrene single crystal surface structures

The exciton dynamics on flat (001) rubrene crystal surfaces have been compared with those under confined pyramidal geometry by time-resolved photoluminescence with micrometer spatial resolution. The luminescence spectra can be interpreted in terms of generation of a free and a self-trapped exciton. Their ratio depends significantly on the structural size which we explain by the optical absorption profile of the pyramids in combination with the exciton diffusion constant. For the latter a lower limit of 0.2 cm2/s at 4 K has been estimated. Temperature-dependent decay times reveal activation barriers between free and self-trapped exciton of 3 meV and 14 meV.We report on crystalline pyramidal structures grown via self-organization on the rubrene (001) surface. The analysis of their spectral response by means of photoluminescence with micrometer lateral resolution reveals an intensity enhancement on-top of the surface structures. As we demonstrate this intensity increase can be related to the excitation processes at the molecular level in combination with exciton confinement within the pyramids.