Tobias Hanke

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.

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.

Compact coherent anti-Stokes Raman scattering microscope based on a picosecond two-color Er:fiber laser system

We present a compact coherent anti-Stokes Raman scattering microscope based on a widely tunable picosecond Er:fiber laser. Intense and bandwidth-limited 1 ps pump pulses at a center wavelength of 775 nm are generated via frequency mixing within the broadband fundamental at 1.55 microm. Narrowband Stokes pulses are obtained by frequency shifting of solitons in a highly nonlinear bulk fiber and subsequent second-harmonic generation. The tuning range from 850 nm to 1100 nm gives access to vibrational resonances between 1150 cm(-1) and 3800 cm(-1). A first imaging application in the spectral region of CH stretch vibrations is demonstrated.

Ultrabroadband background-free coherent anti-Stokes Raman scattering microscopy based on a compact Er:fiber laser system

We demonstrate a scheme for efficient coherent anti-Stokes Raman scattering (CARS) microscopy free of nonresonant background. Our method is based on a compact Er:fiber laser source. Impulsive excitation of molecular resonances is achieved by an 11 fs pulse at 1210 nm. Broadband excitation gives access to molecular resonances from 0 cm(-1) up to 4000 cm(-1). Time-delayed narrowband probing at 775 nm enables sensitive and high-speed spectral detection of the CARS signal free of nonresonant background with a resolution of 10 cm(-1).

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.

Ultrafast spin dynamics in colloidal ZnO quantum dots

We perform time-resolved Faraday rotation measurements on colloidal ZnO quantum dots. A biexponential decay of the dephasing time T2* of the electron spins governed by competing recombination processes is observed.

Colloidal ZnO quantum dots in ultraviolet pillar microcavities

Three dimensional light confinement and distinct pillar microcavity modes in the ultraviolet have been observed in pillar resonators with embedded colloidal ZnO quantum dots fabricated by focused ion beam milling. Results from a waveguide model for the mode patterns and their spectral positions are in excellent agreement with the experimental data.

Single-cycle light pulses from a compact Er:fiber laser

We demonstrate a setup based entirely on compact Er:fiber technology which synthesizes pulses of a duration of 4.3 fs. This value corresponds to a single cycle of light in the telecom wavelength region.

Coherent anti-Stokes Raman scattering microspectroscopy based on a compact Er:fiber laser

A two branch Er:fiber laser was developed for coherent anti-Stokes Raman scattering (CARS) microspectroscopy. The compact and highly stable light source allows for fast single-frequency CARS microspectroscopy with a wide tuning range from 1150 cm-1 up to 3800 cm-1. Single-pass frequency conversion enables easy tunability. The spectral selectivity of the system is shown using polymer beads. Imaging of biological samples is demonstrated on C. elegans and yeast cells. Modification of the light source allows for broadband background-free CARS microspectroscopy. Impulsive excitation of molecular resonances is achieved using an 11 fs pulse at 1210 nm. Broadband excitation gives access to molecular resonances from 0 cm-1 up to 4000 cm-1. Time-delayed narrowband probing at 775 nm enables sensitive and high-speed spectral detection of the CARS signal, free of nonresonant background with a resolution of 10 cm-1.

Femtosecond probing of few-fermion dynamics and deterministic single-photon gain in a single semiconductor quantum dot

We report on femtosecond readout of the optical properties of a single CdSe/ZnSe quantum dot. Owing to the uncertainty principle, this timescale represents the ultimate limit for coherent quantum manipulation of such an artificial atom. After resonant excitation of a hot electron-hole pair the absorption of the fundamental exciton resonance is switched off via instantaneous Coulomb renormalization. Subsequently, optical gain builds up after ultrafast intraband relaxation. The speed of thermalization is dominated by the electron spin, since our system is charged permanently with one excess electron. When operating in the nonlinear regime, the number of quanta in a femtosecond light pulse may be changed by exactly ±1. We demonstrate that this deterministic single photon amplifier is characterized by a flat gain spectrum.