The ability to resolve molecules individually has many potential applications. These include understanding the local environments of single molecules including details of their interactions with surroundings. The ability to individually address and manipulate the spin states is also required for spin based quantum information processing. Although optical detection techniques, such as optically detected electron spin resonance (ESR) seem very powerful in these contexts, multiple molecules in the focal volume of a diffraction limited confocal microscope spot cannot in general be resolved individually. Here we propose to solve this problem using optically detected ESR imaging based on the use of high field gradients. In the present research, subwavelength single molecule imaging is demonstrated by using the optically detected ESR technique and the optically detected electron spin echo envelope modulation (ESEEM) technique. Ultra fast Rabi nutation experiments are also performed to demonstrate the feasibility of fast spin manipulations at a low microwave power. Micrometer sized gradient coils, together with micrometer sized co-planar microstrip transmission lines, are designed and fabricated by optical lithography in order to produce the necessary high magnetic field gradients. These fabricated devices are used to demonstrate this subwavelength imaging technique by imaging single electron spins of the nitrogen-vacancy (NV) defect in diamond. In this demonstration, multiple NV defects, unresolved in a single focal volume of a diffraction limited microscope are successfully resolved by the optically detected ESR techniques. Specifically, two neighboring NV defects separated by about 170nm are resolved. Ultra Fast electron spin nutation with an oscillation period of 1.33ns is also achieved by the high microwave magnetic field induced by the current flowing through the fabricated co-planar microstrip lines. These optically detected ESR and ESEEM techniques combined with the micrometer sized gradient coil may find many applications, including single molecule imaging and quantum information processing.

A novel experimental setup has been realized to measure weak magnetic moments which can be modulated at radio frequencies (~1–5 MHz). Using an optimized radio-frequency (RF) pickup coil and lock-in amplifier, an experimental sensitivity of 10 -15 Am2 corresponding to 10 -18 emu has been demonstrated with a one second time constant. The detection limit at room temperature is 9.3 10 -16 Am2/√Hz limited by Johnson noise of the coil. In order to demonstrate the sensitivity of this technique it was used to electrically detect the polarized spins in semiconductors in zero applied magnetic fields. For example in GaAs, the magnetic moment due to a small number (~ 7 x 108) of spin polarized electrons generated by polarization modulated optical radiation was detected. Spin polarization was generated by optical injection using circularly polarized light which is modulated rapidly using an electro-optic cell. The modulated spin polarization generates a weak time-varying magnetic field which is detected by the sensitive radio-frequency coil. Using a radio-frequency lock-in amplifier, clear signals were obtained for bulk GaAs and Ge samples from which an optical spin orientation efficiency of ~ 10–20% could be determined for Ge at 1342 nm excitation wavelength at 127 K. In the presence of a small external magnetic field, the signal decayed according to the Hanle Effect, from which a spin lifetime of 4.6 ± 1.0 ns for electrons in bulk Ge at 127 K was extracted. The spin dynamics in n-Ge was further explored and the temperature dependence of the spin lifetime was plotted for a temperature range of about 90 K to 180 K. The temperature dependence of the optical pumping efficiency was also measured though no quantitative conclusions could be derived. The signals observed for semi-insulating GaAs, n-GaAs, GaSb and CdTe which are direct gap semiconductors are much larger than expected (almost two orders of magnitude). An attempt was made to explain this unexpected behavior of these direct gap semiconductors using the spin hall effect.

Das Co2FeSi/GaAs-Hybridsystem wurde hinsichtlich seiner Eignung für Anwendungen in der Spintronik untersucht. Die Heusler-Legierung Co2FeSi ist ein aussichtsreicher Kandidat für derartige Anwendungen, weil der vollständig geordneten Kristallphase Halbmetallizität, d. h. eine Spinpolarisation von 100% an der Fermi-Energie, vorhergesagt wird. Zunächst wurde im Rahmen dieser Arbeit die elektrische Spininjektion und Spindetektion in lateralen Transportstrukturen in der sogenannten nicht-lokalen Konfiguration sowohl für die vollständig geordnete, als auch für eine teilweise ungeordnete Kristallphase mittels Spinventil- und Hanle-Messungen nachgewiesen. Die Abhängigkeiten der Spinsignale vom Strom und von der Temperatur konnten erklärt werden und eine Spininjektionsefizienz von 16 bzw. 9% wurde ermittelt. Für den praktischen Einsatz werden allerdings lokale Spinventile benötigt, deren Funktionsfähigkeit für beide kristallinen Ordnungen demonstriert wurde. Der Magnetowiderstand, der ein Maß für die Güte der lokalen Spinventile darstellt, beträgt 0.03% und liegt im Bereich des theoretisch zu erwartenden Wertes. Anhand des sogenannten Fert-Kriteriums konnten die Gründe für diesen niedrigen Wert aufgezeigt werden. Des Weiteren ließ ein Vergleich der lokalen und nicht-lokalen Spinsignale auf eine hohe Spinpolarisation des Co2FeSi schließen. Die Spinextraktion bietet neben der Spininjektion eine weitere Möglichkeit zur Erzeugung einer Spinakkumulation in einem Halbleiter. Die Stromabhängigkeiten von Spininjektion und Spinextraktion unterscheiden sich für beide kristallinen Phasen des Co2FeSi. Das stark unterschiedliche Verhalten konnte anhand des Einflusses der jeweiligen Bandstruktur auf die Spinerzeugung erklärt werden. Des Weiteren konnte aus dem Vergleich zwischen der Messungen und der theoretisch vorhergesagten Bandstruktur der halbmetallische Charakter der vollständig geordneten Kristallphase nachgewiesen werden. / The Co2FeSi/GaAs hybrid system was investigated regarding its suitability for spintronic applications. The Heusler-compound Co2FeSi is a promissing canditate for these kind of applications due to the predicted half-metallicity, i. e. a 100% spin polarisation at the Fermi energy, for its fully ordered crystall phase. The electrical spin injection and detection was demonstrated in lateral tranpost structures in the so called non-local geometry for the fully ordered and for a partly disordered crystall phase by observing spin valve signatures and Hanle characteristics. The current and temperature dependence of the spin signals was explained and a respective spin injection efficiencies of 16 and 9% determined. For practical use one needs local spin valves, which where demonstrated for both crystalline phases. The magnetoresistance, a measure of the goodness of a local spin valve, was 0.03%, i. e. in the theoretically expected range. Making use of the so-called Fert criterion the reasons for this low value could be pointed out. Further the quotient of the local and non-local spin signals implied a high spin polarisation of the Co2FeSi. Spin extraction is another method to create a spin accumulation in a semiconductor. The current dependece of the spin injection and the spin extraction signals strongly depends on the degree of ordering in the Co2FeSi lattice. The different behavior is explanied by the crucial influence of the respective electronic band structure on the spin generation processes. Further, the comparison between the measured signals and the theoretically calculated electronic band structure hints towards the half-metalicity of the fully ordered crystall phase of Co2FeSi.