Quantum Tunneling of Magnetization in Single Molecular Magnets Coupled to Ferromagnetic Reservoirs

The role of spin polarized reservoirs in quantum tunneling of magnetization and relaxation processes in a single molecular magnet (SMM) is investigated theoretically. The SMM is exchange-coupled to the reservoirs and also subjected to a magnetic field varying in time, which enables the quantum tunneling of magnetization (QTM). The spin relaxation times are calculated from the Fermi golden rule. The exchange interaction with tunneling electrons is shown to affect the spin reversal due to QTM. Furthermore, it is shown that the switching is associated with transfer of a certain charge between the leads.Comment: 5 pages, 3 EPS figures, final version as publishe

Quantum Noise Interference and Back-action Cooling in Cavity Nanomechanics

We present a theoretical analysis of a novel cavity electromechanical system where a mechanical resonator directly modulates the damping rate kappa of a driven electromagnetic cavity. We show that via a destructive interference of quantum noise, the driven cavity can effectively act like a zero-temperature bath irrespective of the ratio kappa / omega_M, where omega_M is the mechanical frequency. This scheme thus allows one to cool the mechanical resonator to its ground state without requiring the cavity to be in the so-called `good cavity' limit kappa << omega_M.Comment: 4+ pages, 2 figures. Error in second last paragraph correcte

Strong and Tunable Nonlinear Optomechanical Coupling in a Low-Loss System

A major goal in optomechanics is to observe and control quantum behavior in a system consisting of a mechanical resonator coupled to an optical cavity. Work towards this goal has focused on increasing the strength of the coupling between the mechanical and optical degrees of freedom; however, the form of this coupling is crucial in determining which phenomena can be observed in such a system. Here we demonstrate that avoided crossings in the spectrum of an optical cavity containing a flexible dielectric membrane allow us to realize several different forms of the optomechanical coupling. These include cavity detunings that are (to lowest order) linear, quadratic, or quartic in the membrane's displacement, and a cavity finesse that is linear in (or independent of) the membrane's displacement. All these couplings are realized in a single device with extremely low optical loss and can be tuned over a wide range in situ; in particular, we find that the quadratic coupling can be increased three orders of magnitude beyond previous devices. As a result of these advances, the device presented here should be capable of demonstrating the quantization of the membrane's mechanical energy.Comment: 12 pages, 4 figures, 1 tabl

Signatures of Molecular Magnetism in Single-Molecule Transport Spectroscopy

Single-molecule transistors provide a unique experimental tool to investigate the coupling between charge transport and the molecular degrees of freedom in individual molecules. One interesting class of molecules for such experiments are the single-molecule magnets, since the intramolecular exchange forces present in these molecules should couple strongly to the spin of transport electrons, thereby providing both new mechanisms for modulating electron flow and also new means for probing nanoscale magnetic excitations. Here we report single-molecule transistor measurements on devices incorporating Mn12 molecules. By studying the electron-tunneling spectrum as a function of magnetic field, we are able to identify clear signatures of magnetic states and their associated magnetic anisotropy. A comparison of the data to simulations also suggests that electron flow can strongly enhance magnetic relaxation of the magnetic molecule

Green function techniques in the treatment of quantum transport at the molecular scale

The theoretical investigation of charge (and spin) transport at nanometer length scales requires the use of advanced and powerful techniques able to deal with the dynamical properties of the relevant physical systems, to explicitly include out-of-equilibrium situations typical for electrical/heat transport as well as to take into account interaction effects in a systematic way. Equilibrium Green function techniques and their extension to non-equilibrium situations via the Keldysh formalism build one of the pillars of current state-of-the-art approaches to quantum transport which have been implemented in both model Hamiltonian formulations and first-principle methodologies. We offer a tutorial overview of the applications of Green functions to deal with some fundamental aspects of charge transport at the nanoscale, mainly focusing on applications to model Hamiltonian formulations.Comment: Tutorial review, LaTeX, 129 pages, 41 figures, 300 references, submitted to Springer series "Lecture Notes in Physics

Comparison of OH reactivity measurements in the atmospheric simulation chamber SAPHIR

Hydroxyl (OH) radical reactivity (kOH) has been measured for 18 years with different measurement techniques. In order to compare the performances of instruments deployed in the field, two campaigns were conducted performing experiments in the atmospheric simulation chamber SAPHIR at Forschungszentrum Jülich in October 2015 and April 2016. Chemical conditions were chosen either to be representative of the atmosphere or to test potential limitations of instruments. All types of instruments that are currently used for atmospheric measurements were used in one of the two campaigns. The results of these campaigns demonstrate that OH reactivity can be accurately measured for a wide range of atmospherically relevant chemical conditions (e.g. water vapour, nitrogen oxides, various organic compounds) by all instruments. The precision of the measurements (limit of detection  < 1 s−1 at a time resolution of 30 s to a few minutes) is higher for instruments directly detecting hydroxyl radicals, whereas the indirect comparative reactivity method (CRM) has a higher limit of detection of 2 s−1 at a time resolution of 10 to 15 min. The performances of the instruments were systematically tested by stepwise increasing, for example, the concentrations of carbon monoxide (CO), water vapour or nitric oxide (NO). In further experiments, mixtures of organic reactants were injected into the chamber to simulate urban and forested environments. Overall, the results show that the instruments are capable of measuring OH reactivity in the presence of CO, alkanes, alkenes and aromatic compounds. The transmission efficiency in Teflon inlet lines could have introduced systematic errors in measurements for low-volatile organic compounds in some instruments. CRM instruments exhibited a larger scatter in the data compared to the other instruments. The largest differences to reference measurements or to calculated reactivity were observed by CRM instruments in the presence of terpenes and oxygenated organic compounds (mixing ratio of OH reactants were up to 10 ppbv). In some of these experiments, only a small fraction of the reactivity is detected. The accuracy of CRM measurements is most likely limited by the corrections that need to be applied to account for known effects of, for example, deviations from pseudo first-order conditions, nitrogen oxides or water vapour on the measurement. Methods used to derive these corrections vary among the different CRM instruments. Measurements taken with a flow-tube instrument combined with the direct detection of OH by chemical ionisation mass spectrometry (CIMS) show limitations in cases of high reactivity and high NO concentrations but were accurate for low reactivity (< 15 s−1) and low NO (< 5 ppbv) conditions

Tunneling Spectra of Individual Magnetic Endofullerene Molecules

The manipulation of single magnetic molecules may enable new strategies for high-density information storage and quantum-state control. However, progress in these areas depends on developing techniques for addressing individual molecules and controlling their spin. Here we report success in making electrical contact to individual magnetic N@C60 molecules and measuring spin excitations in their electron tunneling spectra. We verify that the molecules remain magnetic by observing a transition as a function of magnetic field which changes the spin quantum number and also the existence of nonequilibrium tunneling originating from low-energy excited states. From the tunneling spectra, we identify the charge and spin states of the molecule. The measured spectra can be reproduced theoretically by accounting for the exchange interaction between the nitrogen spin and electron(s) on the C60 cage.Comment: 7 pages, 4 figures. Typeset in LaTeX, updated text of previous versio

Nano-Opto-Electro-Mechanical Systems

A new class of hybrid systems that couple optical, electrical and mechanical degrees of freedom in nanoscale devices is under development in laboratories worldwide. These nano-opto-electro-mechanical systems (NOEMS) offer unprecedented opportunities to dynamically control the flow of light in nanophotonic structures, at high speed and low power consumption. Drawing on conceptual and technological advances from cavity optomechanics, they also bear the potential for highly efficient, low-noise transducers between microwave and optical signals, both in the classical and quantum domains. This Progress Article discusses the fundamental physical limits of NOEMS, reviews the recent progress in their implementation, and suggests potential avenues for further developments in this field.Comment: 27 pages, 3 figures, 2 boxe

OH in the coastal boundary layer of Crete during MINOS : measurements and relationship with ozone photolysis

Hydroxyl radical (OH) concentrations were measured in August 2001 at Finokalia Station on the northeastern coast of Crete during the Mediterranean Intensive Oxidant Study (MINOS). OH was measured based on selected ion chemical ionization mass spectrometry (SI/CIMS) with a time resolution of 30 sec and signal integration of 5 min. The corresponding accuracy, precision, and detection limit were 20% (1sigma), 11% (1sigma), and 2.4 x 10(5) molecules cm(-3) (2sigma), respectively. OH levels showed a strong diurnal variability with high maxima (approximately 2 x 10(7) molecules cm(-3)) occurring around 13:30 LT (10:30 UTC) and nighttime values below the detection limit. Daily 24-hour average concentrations varied between 3.6-6.7 x 10(6) cm(-3). For the total measurement period (6-21 August) the mean and standard deviation were 4.5 +/- 1.1 x 10(6) cm(-3). The OH data set is analyzed based on a classification into three periods: I: Aug 6-8, II: Aug 9-11, III: Aug 13-18. For each of the three periods the measured OH concentrations are described by the empirical function [OH] = a J((OD)-D-1)(b), with J((OD)-D-1) being the ozone photolysis frequency and a = 1.4 x 10(10) s cm(-3), 1.7 x 10(10) s cm(-3), 2.2 x 10(10) s cm(-3), and b = 0.68, respectively. Taking into account the estimated precision of the OH measurements this empirical function using three values for a and one value for b explains 99% of the observed variance of OH. A detailed sensitivity analysis using a CH4-CO box model was performed to interpret this relationship, in particular the meanings of the pre-exponential factor a and the exponent b. It was found that the value of b which represents the total logarithmic dependence of [OH] on J((OD)-D-1) includes the individual contributions from the photolysis of O-3, NO2, HCHO, HONO, and H2O2 which could be determined using the box model. For the conditions prevailing during the MINOS campaign the exponent b was found to be dominated by the contributions from O-3- and NO2-photolysis. For the in-dividual functional dependences between [OH] and J((OD)-D-1), [OH] and J(NO2), and J(NO2) and J((OD)-D-1) the partial logarithmic derivatives were determined to be 0.5, 0.6, and 0.3, respectively. Overall, the box model yields a value of 0.70 for the exponent b in very good agreement with the corresponding value derived from the empirical analysis of the measurements. This empirical approach in which the chemical air mass characteristics influencing the OH radical balance and thereby, the self-cleansing efficiency of the atmosphere, are represented by only two parameters which are constant over quite substantial time periods may be used in future experiments to test and compare OH measurements made in different atmospheric environments