verse order, as in this case, is the real essence of the Heisenberg uncertainty principle. Besides its fundamental importance, the experimental implementation of such a sequence of basic quantum operations is an essential tool for the full-scale engineering of a quantum light state optimized for a multitude of different tasks (15), including robust quantum communication. As any quantum operation, including non-Gaussian operations, is composed of photon additions and subtractions (i.e, it can be expressed as f ð% a; % a † Þ), our experimental results constitute a step toward the full quantum control of a field and the generation of highly entangled states (16).

We review recent theoretical and experimental advances toward understanding the effects of nuclear spins in confined nanostructures. These systems, which include quantum dots, defect centers, and molecular magnets, are particularly interesting for their importance in quantum information processing devices, which aim to coherently manipulate single electron spins with high precision. On one hand, interactions between confined electron spins and a nuclear-spin environment provide a decoherence source for the electron, and on the other, a strong effective magnetic field that can be used to execute local coherent rotations. A great deal of effort has been directed toward understanding the details of the relevant decoherence processes and to find new methods to manipulate the coupled electron-nuclear system. A sequence of spectacular new results have provided understanding of spin-bath decoherence, nuclear spin diffusion, and preparation of the nuclear state through dynamic polarization and more general manipulation of the nuclear-spin density matrix through ''state narrowing.'' These results demonstrate the richness of this physical system and promise many new mysteries for the future. 1 Introduction The last several years have seen a series of breakthroughs in single-spin measurement and manipulation, motivated in large part by the potential for future quantum information processing devices [1,2]. The spin coherence times for confined electrons in semiconductor quantum dots [3][4][5][6][7][8][9][10], phosphorus donor impurities in silicon [11,12], nitrogen vacancy (NV) centers in diamond [13][14][15], and in molecular magnets [16,17] is typically limited by the interaction between the electron and nuclear spins in the host material. The coherent manipulation of electron spins therefore requires a complete understanding of the nuclear spins in these materials, typically in the presence of localized electrons.A great deal of work has been done many years ago on ensembles of electron spins at donor impurities, including experimental [18][19][20] and theoretical [21,22] studies of

We report the electrical induction and detection of dynamic nuclear polarization in the spin-blockade regime of double GaAs vertical quantum dots. The nuclear Overhauser field measurement relies on bias voltage control of the interdot spin exchange coupling and measurement of dc current at variable external magnetic fields. The largest Overhauser field observed was about 4 T, corresponding to a nuclear polarization approximately 40% for the electronic g factor typical of these devices, |g*| approximately 0.25. A phenomenological model is proposed to explain these observations.

The counter-intuitive properties of quantum mechanics have the potential to revolutionize information processing by enabling efficient algorithms with no known classical counterparts [1,2]. Harnessing this power requires developing a set of building blocks [3], one of which is a method to initialize the set of quantum bits (qubits) to a known state. Additionally, fresh ancillary qubits must be available during the course of computation to achieve fault tolerance [4,5,6,7]. In any physical system used to implement quantum computation, one must therefore be able to selectively and dynamically remove entropy from the part of the system that is to be mapped to qubits. One such method is an "open-system" cooling protocol in which a subset of qubits can be brought into contact with an external large heat-capacity system. Theoretical efforts [8,9,10] have led to an implementation-independent cooling procedure, namely heat-bath algorithmic cooling (HBAC). These efforts have culminated with the proposal of an optimal algorithm, the partner-pairing algorithm (PPA), which was used to compute the physical limits of HBAC [11]. We report here the first experimental realization of multi-step cooling of a quantum system via HBAC. The experiment was carried out using nuclear magnetic resonance (NMR) of a solid-state ensemble three-qubit system. It demonstrates the repeated repolarization of a particular qubit to an effective spin-bath temperature and alternating logical operations within the three-qubit subspace to ultimately cool a second qubit below this temperature. Demonstration of the control necessary for these operations is an important milestone in the control of solid-state NMR qubits and toward fault-tolerant quantum computing.

Intermolecular dipole-dipole interactions were once thought to average to zero in gases and liquids as a result of rapid molecular motion that leads to sharp nuclear magnetic resonance lines. Recent papers have shown that small residual couplings survive the motional averaging if the magnetization is nonuniform or nonspherical. Here, we show that a much larger, qualitatively different intermolecular dipolar interaction remains in nanogases and nanoliquids as an effect of confinement. The dipolar coupling that characterizes such interactions is identical for all spin pairs and depends on the shape, orientation (with respect to the external magnetic field), and volume of the gas/liquid container. This nanoscale effect is useful in the determination of nanostructures and could have unique applications in the exploration of quantum space.

Off-resonant charge transport through molecular junctions has been extensively studied since the advent of single-molecule electronics and is now well understood within the framework of the non-interacting Landauer approach. Conversely, gaining a qualitative and quantitative understanding of the resonant transport regime has proven more elusive. Here, we study resonant charge transport through graphene-based zinc-porphyrin junctions. We experimentally demonstrate an inadequacy of non-interacting Landauer theory as well as the conventional single-mode Franck–Condon model. Instead, we model overall charge transport as a sequence of non-adiabatic electron transfers, with rates depending on both outer and inner-sphere vibrational interactions. We show that the transport properties of our molecular junctions are determined by a combination of electron–electron and electron-vibrational coupling, and are sensitive to interactions with the wider local environment. Furthermore, we assess the importance of nuclear tunnelling and examine the suitability of semi-classical Marcus theory as a description of charge transport in molecular devices.

Given its importance to many other areas of physics, from condensed-matter physics to thermodynamics, time-reversal symmetry has had relatively little influence on quantum information science. Here we develop a network-based picture of time-reversal theory, classifying Hamiltonians and quantum circuits as time symmetric or not in terms of the elements and geometries of their underlying networks. Many of the typical circuits of quantum information science are found to exhibit time asymmetry. Moreover, we show that time asymmetry in circuits can be controlled using local gates only and can simulate time asymmetry in Hamiltonian evolution. We experimentally implement a fundamental example in which controlled time-reversal asymmetry in a palindromic quantum circuit leads to near-perfect transport. Our results pave the way for using time-symmetry breaking to control coherent transport and imply that time asymmetry represents an omnipresent yet poorly understood effect in quantum information science.

Advanced large-scale electrochemical energy storage requires cost-effective battery systems with high energy densities. Aprotic sodium-oxygen (Na-O2) batteries offer advantages, being comprised of low-cost elements and possessing much lower charge overpotential and higher reversibility compared to their lithium-oxygen battery cousins. Although such differences have been explained by solution-mediated superoxide transport, the underlying nature of this mechanism is not fully understood. Water has been suggested to solubilize superoxide via formation of hydroperoxyl (HO2), but direct evidence of these HO2 radical species in cells has proven elusive. Here, we use ESR spectroscopy at 210 K to identify and quantify soluble HO2 radicals in the electrolyte-cold-trapped in situ to prolong their lifetime-in a Na-O2 cell. These investigations are coupled to parallel SEM studies that image crystalline sodium superoxide (NaO2) on the carbon cathode. The superoxide radicals were spin-trapped via reaction with 5,5-dimethyl-pyrroline N-oxide at different electrochemical stages, allowing monitoring of their production and consumption during cycling. Our results conclusively demonstrate that transport of superoxide from cathode to electrolyte leads to the nucleation and growth of NaO2, which follows classical mechanisms based on the variation of superoxide content in the electrolyte and its correlation with the crystallization of cubic NaO2. The changes in superoxide content upon charge show that charge proceeds through the reverse solution process. Furthermore, we identify the carbon-centered/oxygen-centered alkyl radicals arising from attack of these solubilized HO2 species on the diglyme solvent. This is the first direct evidence of such species, which are likely responsible for electrolyte degradation.