Optical control of the spin state of two Mn atoms in a quantum dot

We report on the optical spectroscopy of the spin of two magnetic atoms (Mn) embedded in an individual quantum dot interacting with either a single electron, a single exciton and single trion. As a result of their interaction to a common entity, the Mn spins become correlated. The dynamics of this process is probed by time resolved spectroscopy, that permits to determine the optical orientation time in the range of a few tens of $ns$. In addition, we show that the energy of the collective spin states of the two Mn atoms can be tuned through the optical Stark effect induced by a resonant laser field

Spin-phonon coupling in single Mn doped CdTe quantum dot

The spin dynamics of a single Mn atom in a laser driven CdTe quantum dot is addressed theoretically. Recent experimental results\cite{Le-Gall_PRL_2009,Goryca_PRL_2009,Le-Gall_PRB_2010}show that it is possible to induce Mn spin polarization by means of circularly polarized optical pumping. Pumping is made possible by the faster Mn spin relaxation in the presence of the exciton. Here we discuss different Mn spin relaxation mechanisms. First, Mn-phonon coupling, which is enhanced in the presence of the exciton. Second, phonon-induced hole spin relaxation combined with carrier-Mn spin flip coupling and photon emission results in Mn spin relaxation. We model the Mn spin dynamics under the influence of a pumping laser that injects excitons into the dot, taking into account exciton-Mn exchange and phonon induced spin relaxation of both Mn and holes. Our simulations account for the optically induced Mn spin pumping.Comment: 17 pages, 11 figures, submitted to PR

Subnanosecond spectral diffusion of a single quantum dot in a nanowire

We have studied spectral diffusion of the photoluminescence of a single CdSe quantum dot inserted in a ZnSe nanowire. We have measured the characteristic diffusion time as a function of pumping power and temperature using a recently developed technique [G. Sallen et al, Nature Photon. \textbf{4}, 696 (2010)] that offers subnanosecond resolution. These data are consistent with a model where only a \emph{single} carrier wanders around in traps located in the vicinity of the quantum dot

Polycyclic aromatic hydrocarbons (PAHs) in the atmospheres of two French alpine valleys: sources and temporal patterns

International audienceAlpine valleys represent some of the most important crossroads for international heavy-duty traffic in Europe, but the full impact of this traffic on air quality is not known due to a lack of data concerning these complex systems. As part of the program "Pollution des Vallées Alpines" (POVA), we performed two sampling surveys of polycyclic aromatic hydrocarbons (PAHs) in two sensitive valleys: the Chamonix and Maurienne Valleys, between France and Italy. Sampling campaigns were performed during the summer of 2000 and the winter of 2001, with both periods taking place during the closure of the "Tunnel du Mont-Blanc". The first objective of this paper is to describe the relations between PAH concentrations, external parameters (sampling site localization, meteorological parameters, sources), and aerosol characteristics, including its carbonaceous fraction (OC and EC). The second objective is to study the capacity of PAH profiles to accurately distinguish the different emission sources. Temporal evolution of the relative concentration of an individual PAH (CHR) and the PAH groups BghiP+COR and BbF+BkF is studied in order to differentiate wood combustion, gasoline, and diesel emissions, respectively. The results show that the total particulate PAH concentrations were higher in the Chamonix valley during both seasons, despite the cessation of international traffic. Seasonal cycles, with higher concentrations in winter, are also stronger in this valley. During winter, particulate PAH concentration can reach very high levels (up to 155 ng.m-3) in this valley during cold anticyclonic periods. The examination of sources shows the impact during summer of heavy-duty traffic in the Maurienne valley and of gasoline vehicles in the Chamonix valley. During winter, Chamonix is characterized by the strong influence of wood combustion in residential fireplaces, even if the temporal evolution of specific PAH ratios are difficult to interpret. Information on sources given by PAH profiles can only be considered in qualitative terms

Single spin optical read-out in CdTe/ZnTe quantum dot studied by photon correlation spectroscopy

Spin dynamics of a single electron and an exciton confined in CdTe/ZnTe quantum dot is investigated by polarization-resolved correlation spectroscopy. Spin memory effects extending over at least a few tens of nanoseconds have been directly observed in magnetic field and described quantitatively in terms of a simple rate equation model. We demonstrate an effective (68%) all-optical read-out of the single carrier spin state through probing the degree of circular polarization of exciton emission after capture of an oppositely charged carrier. The perturbation introduced by the pulsed optical excitation serving to study the spin dynamics has been found to be the main source of the polarization loss in the read-out process. In the limit of low laser power the read-out efficiency extrapolates to a value close to 100%. The measurements allowed us as well to determine neutral exciton spin relaxation time ranging from 3.4 +/- 0.1 ns at B = 0 T to 16 +/- 3 ns at B = 5 T.Comment: to appear in Phys. Rev.

Subnanosecond spectral diffusion measurement using photon correlation

Spectral diffusion is a result of random spectral jumps of a narrow line as a result of a fluctuating environment. It is an important issue in spectroscopy, because the observed spectral broadening prevents access to the intrinsic line properties. However, its characteristic parameters provide local information on the environment of a light emitter embedded in a solid matrix, or moving within a fluid, leading to numerous applications in physics and biology. We present a new experimental technique for measuring spectral diffusion based on photon correlations within a spectral line. Autocorrelation on half of the line and cross-correlation between the two halves give a quantitative value of the spectral diffusion time, with a resolution only limited by the correlation set-up. We have measured spectral diffusion of the photoluminescence of a single light emitter with a time resolution of 90 ps, exceeding by four orders of magnitude the best resolution reported to date

Unconventional motional narrowing in the optical spectrum of a semiconductor quantum dot

Motional narrowing refers to the striking phenomenon where the resonance line of a system coupled to a reservoir becomes narrower when increasing the reservoir fluctuation. A textbook example is found in nuclear magnetic resonance, where the fluctuating local magnetic fields created by randomly oriented nuclear spins are averaged when the motion of the nuclei is thermally activated. The existence of a motional narrowing effect in the optical response of semiconductor quantum dots remains so far unexplored. This effect may be important in this instance since the decoherence dynamics is a central issue for the implementation of quantum information processing based on quantum dots. Here we report on the experimental evidence of motional narrowing in the optical spectrum of a semiconductor quantum dot broadened by the spectral diffusion phenomenon. Surprisingly, motional narrowing is achieved when decreasing incident power or temperature, in contrast with the standard phenomenology observed for nuclear magnetic resonance

Insights into the secondary fraction of the organic aerosol in a Mediterranean urban area: Marseille

A comprehensive aerosol characterization was conducted at Marseille during summer, including organic (OC) and elemental carbon (EC), major ionic species, radiocarbon (¹⁴C), water-soluble OC and HULIS (HUmic LIke Substances), elemental composition and primary and secondary organic markers. This paper is the second paper of a two-part series that uses this dataset to investigate the sources of Organic Aerosol (OA). While the first paper investigates the primary sources (El Haddad et al., 2010), this second paper focuses on the secondary fraction of the organic aerosol. <br><br> In the context of overall OC mass balance, primary OC (POC) contributes on average for only 22% and was dominated by vehicular emissions accounting on average for 17% of OC. As a result, 78% of OC mass cannot be attributed to the major primary sources and remains un-apportioned. Radiocarbon measurements suggest that more than 70% of this fraction is of non-fossil origin, assigned predominantly to biogenic secondary organic carbon (BSOC). Therefore, contributions from three traditional BSOC precursors, isoprene, $\alpha$-pinene and &beta;-caryophyllene, were considered. These were estimated using the ambient concentrations of Secondary Organic Aerosol (SOA) markers from each precursor and laboratory-derived marker mass fraction factors. <br><br> Secondary organic markers derived from isoprene photo-oxidation (ie: 2-methylglyceric acid and 2-methyltetrols) do not exhibit the same temporal trends. This variability was assigned to the influence of NO_x concentration on their formation pathways and to their potential decay by further processing in the atmosphere. The influence of changes in isoprene chemistry on assessment of isoprene SOC contribution was evaluated explicitly. The results suggest a 60-fold variation between the different estimates computed using different isoprene SOC markers, implying that the available profiles do not reflect the actual isoprene SOC composition observed in Marseille. <br><br> Using the marker-based approach, the aggregate contribution from traditional BSOC was estimated at only 4.2% of total OC and was dominated by α-pinene SOC accounting on average for 3.4% of OC. As a result, these estimates underpredict the inexplicably high loadings of OC. This underestimation can be associated with (1) uncertainties underlying the marker-based approach, (2) presence of other SOC precursors and (3) further processing of fresh SOC, as indicated by organosulfates (RSO₄H) and HUmic LIke Substances (HULIS) measurements

Optical probing of spin fluctuations of a single magnetic atom

We analyzed the photoluminescence intermittency generated by a single paramagnetic spin localized in an individual semiconductor quantum dot. The statistics of the photons emitted by the quantum dot reflect the quantum fluctuations of the localized spin interacting with the injected carriers. Photon correlation measurements which are reported here reveal unique signatures of these fluctuations. A phenomenological model is proposed to quantitatively describe these observations, allowing a measurement of the spin dynamics of an individual magnetic atom at zero magnetic field. These results demonstrate the existence of an efficient spin relaxation channel arising from a spin-exchange with individual carriers surrounding the quantum dot. A theoretical description of a spin-flip mechanism involving spin exchange with surrounding carriers gives relaxation times in good agreement with the measured dynamics