Photothermal heterodyne imaging of individual nonfluorescent nanoclusters and nanocrystals

We introduce a new, highly sensitive, and simple heterodyne optical method for imaging individual nonfluorescent nanoclusters and nanocrystals. A 2 order of magnitude improvement of the signal is achieved compared to previous methods. This allows for the unprecedented detection of individual small absorptive objects such as metallic clusters (of 67 atoms) or nonluminescent semiconductor nanocrystals. The measured signals are in agreement with a calculation based on the scattering field theory from a photothermal-induced modulated index of refraction profile around the nanoparticle

Spin-flip and spin-conserving optical transitions of the nitrogen-vacancy centre in diamond

We map out the first excited state sublevel structure of single nitrogen-vacancy (NV) colour centres in diamond. The excited state is an orbital doublet where one branch supports an efficient cycling transition, while the other can simultaneously support fully allowed optical Raman spin-flip transitions. This is crucial for the success of many recently proposed quantum information applications of the NV defects. We further find that an external electric field can be used to completely control the optical properties of a single centre. Finally, a group theoretical model is developed that explains the observations and provides good physical understanding of the excited state structure

On the indistinguishability of Raman photons

We provide a theoretical framework to study the effect of dephasing on the quantum indistinguishability of single photons emitted from a coherently driven cavity QED $\Lambda$-system. We show that with a large excited-state detuning, the photon indistinguishability can be drastically improved provided that the fluctuation rate of the noise source affecting the excited state is fast compared with the photon emission rate. In some cases a spectral filter is required to realize this improvement, but the cost in efficiency can be made small.Comment: 18 pages, 3 figures, final versio

Coherent Population Trapping of Single Spins in Diamond Under Optical Excitation

Coherent population trapping is demonstrated in single nitrogen-vacancy centers in diamond under optical excitation. For sufficient excitation power, the fluorescence intensity drops almost to the background level when the laser modulation frequency matches the 2.88 GHz splitting of the ground states. The results are well described theoretically by a four-level model, allowing the relative transition strengths to be determined for individual centers. The results show that all-optical control of single spins is possible in diamond.Comment: minor correction

Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence

Single dye molecules at cryogenic temperatures display many spectroscopic phenomena known from free atoms and are thus promising candidates for fundamental quantum optical studies. However, the existing techniques for the detection of single molecules have either sacrificed the information on the coherence of the excited state or have been inefficient. Here we show that these problems can be addressed by focusing the excitation light near to the absorption cross section of a molecule. Our detection scheme allows us to explore resonance fluorescence over 9 orders of magnitude of excitation intensity and to separate its coherent and incoherent parts. In the strong excitation regime, we demonstrate the first observation of the Mollow triplet from a single solid-state emitter. Under weak excitation we report the detection of a single molecule with an incident power as faint as 150 attoWatt, paving the way for studying nonlinear effects with only a few photons.Comment: 6 figure

Low-temperature tapered-fiber probing of diamond NV ensembles coupled to GaP microcavities

In this work we present a platform for testing the device performance of a cavity-emitter system, using an ensemble of emitters and a tapered optical fiber. This method provides high-contrast spectra of the cavity modes, selective detection of emitters coupled to the cavity, and an estimate of the device performance in the single- emitter case. Using nitrogen-vacancy (NV) centers in diamond and a GaP optical microcavity, we are able to tune the cavity onto the NV resonance at 10 K, couple the cavity-coupled emission to a tapered fiber, and measure the fiber-coupled NV spontaneous emission decay. Theoretically we show that the fiber-coupled average Purcell factor is 2-3 times greater than that of free-space collection; although due to ensemble averaging it is still a factor of 3 less than the Purcell factor of a single, ideally placed center.Comment: 15 pages, 6 figure

Stark shift control of single optical centers in diamond

Lifetime limited optical excitation lines of single nitrogen vacancy (NV) defect centers in diamond have been observed at liquid helium temperature. They display unprecedented spectral stability over many seconds and excitation cycles. Spectral tuning of the spin selective optical resonances was performed via the application of an external electric field (i.e. the Stark shift). A rich variety of Stark shifts were observed including linear as well as quadratic components. The ability to tune the excitation lines of single NV centers has potential applications in quantum information processing

Single photon quantum non-demolition in the presence of inhomogeneous broadening

Electromagnetically induced transparency (EIT) has been often proposed for generating nonlinear optical effects at the single photon level; in particular, as a means to effect a quantum non-demolition measurement of a single photon field. Previous treatments have usually considered homogeneously broadened samples, but realisations in any medium will have to contend with inhomogeneous broadening. Here we reappraise an earlier scheme [Munro \textit{et al.} Phys. Rev. A \textbf{71}, 033819 (2005)] with respect to inhomogeneities and show an alternative mode of operation that is preferred in an inhomogeneous environment. We further show the implications of these results on a potential implementation in diamond containing nitrogen-vacancy colour centres. Our modelling shows that single mode waveguide structures of length $200 \mu\mathrm{m}$ in single-crystal diamond containing a dilute ensemble of NV$^-$ of only 200 centres are sufficient for quantum non-demolition measurements using EIT-based weak nonlinear interactions.Comment: 21 pages, 9 figures (some in colour) at low resolution for arXiv purpose

Properties of nitrogen-vacancy centers in diamond: group theoretic approach

We present a procedure that makes use of group theory to analyze and predict the main properties of the negatively charged nitrogen-vacancy (NV) center in diamond. We focus on the relatively low temperatures limit where both the spin-spin and spin-orbit effects are important to consider. We demonstrate that group theory may be used to clarify several aspects of the NV structure, such as ordering of the singlets in the ($e^2$) electronic configuration, the spin-spin and the spin-orbit interactions in the ($ae$) electronic configuration. We also discuss how the optical selection rules and the response of the center to electric field can be used for spin-photon entanglement schemes. Our general formalism is applicable to a broad class of local defects in solids. The present results have important implications for applications in quantum information science and nanomagnetometry.Comment: 30 pages, 6 figure