Coupling of spin and orbital motion of electrons in carbon nanotubes

Electrons in atoms possess both spin and orbital degrees of freedom. In non-relativistic quantum mechanics, these are independent, resulting in large degeneracies in atomic spectra. However, relativistic effects couple the spin and orbital motion, leading to the well-known fine structure in their spectra. The electronic states in defect-free carbon nanotubes are widely believed to be four-fold degenerate, owing to independent spin and orbital symmetries, and also to possess electron-hole symmetry. Here we report measurements demonstrating that in clean nanotubes the spin and orbital motion of electrons are coupled, thereby breaking all of these symmetries. This spin-orbit coupling is directly observed as a splitting of the four-fold degeneracy of a single electron in ultra-clean quantum dots. The coupling favours parallel alignment of the orbital and spin magnetic moments for electrons and antiparallel alignment for holes. Our measurements are consistent with recent theories that predict the existence of spin-orbit coupling in curved graphene and describe it as a spin-dependent topological phase in nanotubes. Our findings have important implications for spin-based applications in carbon-based systems, entailing new design principles for the realization of quantum bits (qubits) in nanotubes and providing a mechanism for all-electrical control of spins in nanotubes.     

Allowed and forbidden transitions in artificial hydrogen and helium atoms

The strength of radiative transitions in atoms is governed by selection rules that depend on the occupation of atomic orbitals with electrons. Experiments have shown similar electron occupation of the quantized energy levels in semiconductor quantum dots--often described as artificial atoms. But unlike real atoms, the confinement potential of quantum dots is anisotropic, and the electrons can easily couple with phonons of the material. Here we report electrical pump-and-probe experiments that probe the allowed and 'forbidden' transitions between energy levels under phonon emission in quantum dots with one or two electrons (artificial hydrogen and helium atoms). The forbidden transitions are in fact allowed by higher-order processes where electrons flip their spin. We find that the relaxation time is about 200 micro s for forbidden transitions, 4 to 5 orders of magnitude longer than for allowed transitions. This indicates that the spin degree of freedom is well separated from the orbital degree of freedom, and that the total spin in the quantum dots is an excellent quantum number. This is an encouraging result for potential applications of quantum dots as basic entities for spin-based quantum information storage.     

Hybridization of electronic states in quantum dots through photon emission

The self-assembly of semiconductor quantum dots has opened up new opportunities in photonics. Quantum dots are usually described as 'artificial atoms', because electron and hole confinement gives rise to discrete energy levels. This picture can be justified from the shell structure observed as a quantum dot is filled either with excitons (bound electron-hole pairs) or with electrons. The discrete energy levels have been most spectacularly exploited in single photon sources that use a single quantum dot as emitter. At low temperatures, the artificial atom picture is strengthened by the long coherence times of excitons in quantum dots, motivating the application of quantum dots in quantum optics and quantum information processing. In this context, excitons in quantum dots have already been manipulated coherently. We show here that quantum dots can also possess electronic states that go far beyond the artificial atom model. These states are a coherent hybridization of localized quantum dot states and extended continuum states: they have no analogue in atomic physics. The states are generated by the emission of a photon from a quantum dot. We show how a new version of the Anderson model that describes interactions between localized and extended states can account for the observed hybridization.     

Optical emission from a charge-tunable quantum ring

Quantum dots or rings are artificial nanometre-sized clusters that confine electrons in all three directions. They can be fabricated in a semiconductor system by embedding an island of low-bandgap material in a sea of material with a higher bandgap. Quantum dots are often referred to as artificial atoms because, when filled sequentially with electrons, the charging energies are pronounced for particular electron numbers; this is analogous to Hund's rules in atomic physics. But semiconductors also have a valence band with strong optical transitions to the conduction band. These transitions are the basis for the application of quantum dots as laser emitters, storage devices and fluorescence markers. Here we report how the optical emission (photoluminescence) of a single quantum ring changes as electrons are added one-by-one. We find that the emission energy changes abruptly whenever an electron is added to the artificial atom, and that the sizes of the jumps reveal a shell structure.     

Single artificial-atom lasing

Solid-state superconducting circuits are versatile systems in which quantum states can be engineered and controlled. Recent progress in this area has opened up exciting possibilities for exploring fundamental physics as well as applications in quantum information technology; in a series of experiments it was shown that such circuits can be exploited to generate quantum optical phenomena, by designing superconducting elements as artificial atoms that are coupled coherently to the photon field of a resonator. Here we demonstrate a lasing effect with a single artificial atom--a Josephson-junction charge qubit--embedded in a superconducting resonator. We make use of one of the properties of solid-state artificial atoms, namely that they are strongly and controllably coupled to the resonator modes. The device is essentially different from existing lasers and masers; one and the same artificial atom excited by current injection produces many photons.     

量子点人工光合成制氢研究进展

 综述了本研究组近年来量子点人工光合成制氢体系的研究进展，重点从量子点与氢化酶模拟化合物、量子点与过渡金属离子、量子点敏化光阴极3个方面分析了影响制氢效率的主要因素，指出对光生电荷（电子和空穴）的有效捕获是提高人工光合成分解水制氢效率的关键，并展望了未来人工光合成发展方向。     

量子点人工光合成制氢研究进展

 综述了本研究组近年来量子点人工光合成制氢体系的研究进展，重点从量子点与氢化酶模拟化合物、量子点与过渡金属离子、量子点敏化光阴极3个方面分析了影响制氢效率的主要因素，指出对光生电荷（电子和空穴）的有效捕获是提高人工光合成分解水制氢效率的关键，并展望了未来人工光合成发展方向。     

Optical gain in silicon nanocrystals

Adding optical functionality to a silicon microelectronic chip is one of the most challenging problems of materials research. Silicon is an indirect-bandgap semiconductor and so is an inefficient emitter of light. For this reason, integration of optically functional elements with silicon microelectronic circuitry has largely been achieved through the use of direct-bandgap compound semiconductors. For optoelectronic applications, the key device is the light source--a laser. Compound semiconductor lasers exploit low-dimensional electronic systems, such as quantum wells and quantum dots, as the active optical amplifying medium. Here we demonstrate that light amplification is possible using silicon itself, in the form of quantum dots dispersed in a silicon dioxide matrix. Net optical gain is seen in both waveguide and transmission configurations, with the material gain being of the same order as that of direct-bandgap quantum dots. We explain the observations using a model based on population inversion of radiative states associated with the Si/SiO2 interface. These findings open a route to the fabrication of a silicon laser.     

Attosecond spectroscopy in condensed matter

Comprehensive knowledge of the dynamic behaviour of electrons in condensed-matter systems is pertinent to the development of many modern technologies, such as semiconductor and molecular electronics, optoelectronics, information processing and photovoltaics. Yet it remains challenging to probe electronic processes, many of which take place in the attosecond (1 as = 10(-18) s) regime. In contrast, atomic motion occurs on the femtosecond (1 fs = 10(-15) s) timescale and has been mapped in solids in real time using femtosecond X-ray sources. Here we extend the attosecond techniques previously used to study isolated atoms in the gas phase to observe electron motion in condensed-matter systems and on surfaces in real time. We demonstrate our ability to obtain direct time-domain access to charge dynamics with attosecond resolution by probing photoelectron emission from single-crystal tungsten. Our data reveal a delay of approximately 100 attoseconds between the emission of photoelectrons that originate from localized core states of the metal, and those that are freed from delocalized conduction-band states. These results illustrate that attosecond metrology constitutes a powerful tool for exploring not only gas-phase systems, but also fundamental electronic processes occurring on the attosecond timescale in condensed-matter systems and on surfaces.     

拓扑绝缘体量子点中的磁交换相互作用

从理论上研究了拓扑绝缘体量子点中的磁交换相互作用.在拓扑绝缘体量子点中,边缘态电子数可以通过量子点的尺寸和外加电场进行调控.当量子点中掺入单个磁离子并且边缘态填充奇数电子时,电子与单个磁离子之间的交换相互作用达到最大值;而边缘态填充偶数电子时,电子与单个磁离子之间的交换相互作用消失.当量子点中掺入2个磁离子时,电子与Mn离子的sp-d相互作用会出现奇偶振荡行为,Mn离子间的相互作用取决于Mn离子间距和量子点壳层中的电子数,表现出典型的Ruderman-Kittel-Kasuya-Yosida型间接交换机制.工作澄清了拓扑绝缘体量子点壳层结构对其磁性的影响,有助于人们设计基于拓扑绝缘体量子点的自旋电子学或量子信息器件.     

Designer Dirac fermions and topological phases in molecular graphene

The observation of massless Dirac fermions in monolayer graphene has generated a new area of science and technology seeking to harness charge carriers that behave relativistically within solid-state materials. Both massless and massive Dirac fermions have been studied and proposed in a growing class of Dirac materials that includes bilayer graphene, surface states of topological insulators and iron-based high-temperature superconductors. Because the accessibility of this physics is predicated on the synthesis of new materials, the quest for Dirac quasi-particles has expanded to artificial systems such as lattices comprising ultracold atoms. Here we report the emergence of Dirac fermions in a fully tunable condensed-matter system-molecular graphene-assembled by atomic manipulation of carbon monoxide molecules over a conventional two-dimensional electron system at a copper surface. Using low-temperature scanning tunnelling microscopy and spectroscopy, we embed the symmetries underlying the two-dimensional Dirac equation into electron lattices, and then visualize and shape the resulting ground states. These experiments show the existence within the system of linearly dispersing, massless quasi-particles accompanied by a density of states characteristic of graphene. We then tune the quantum tunnelling between lattice sites locally to adjust the phase accrual of propagating electrons. Spatial texturing of lattice distortions produces atomically sharp p-n and p-n-p junction devices with two-dimensional control of Dirac fermion density and the power to endow Dirac particles with mass. Moreover, we apply scalar and vector potentials locally and globally to engender topologically distinct ground states and, ultimately, embedded gauge fields, wherein Dirac electrons react to 'pseudo' electric and magnetic fields present in their reference frame but absent from the laboratory frame. We demonstrate that Landau levels created by these gauge fields can be taken to the relativistic magnetic quantum limit, which has so far been inaccessible in natural graphene. Molecular graphene provides a versatile means of synthesizing exotic topological electronic phases in condensed matter using tailored nanostructures.     

Emerging local Kondo screening and spatial coherence in the heavy-fermion metal YbRh2Si2

The entanglement of quantum states is both a central concept in fundamental physics and a potential tool for realizing advanced materials and applications. The quantum superpositions underlying entanglement are at the heart of the intricate interplay of localized spin states and itinerant electronic states that gives rise to the Kondo effect in certain dilute magnetic alloys. In systems where the density of localized spin states is sufficiently high, they can no longer be treated as non-interacting; if they form a dense periodic array, a Kondo lattice may be established. Such a Kondo lattice gives rise to the emergence of charge carriers with enhanced effective masses, but the precise nature of the coherent Kondo state responsible for the generation of these heavy fermions remains highly debated. Here we use atomic-resolution tunnelling spectroscopy to investigate the low-energy excitations of a generic Kondo lattice system, YbRh(2)Si(2). We find that the hybridization of the conduction electrons with the localized 4f electrons results in a decrease in the tunnelling conductance at the Fermi energy. In addition, we observe unambiguously the crystal-field excitations of the Yb(3+) ions. A strongly temperature-dependent peak in the tunnelling conductance is attributed to the Fano resonance resulting from tunnelling into the coherent heavy-fermion states that emerge at low temperature. Taken together, these features reveal how quantum coherence develops in heavy 4f-electron Kondo lattices. Our results demonstrate the efficiency of real-space electronic structure imaging for the investigation of strong electronic correlations, specifically with respect to coherence phenomena, phase coexistence and quantum criticality.     

Kondo effect in an integer-spin quantum dot

The Kondo effect--a many-body phenomenon in condensed-matter physics involving the interaction between a localized spin and free electrons--was discovered in metals containing small amounts of magnetic impurities, although it is now recognized to be of fundamental importance in a wide class of correlated electron systems. In fabricated structures, the control of single, localized spins is of technological relevance for nanoscale electronics. Experiments have already demonstrated artificial realizations of isolated magnetic impurities at metallic surfaces, nanoscale magnets, controlled transitions between two-electron singlet and triplet states, and a tunable Kondo effect in semiconductor quantum dots. Here we report an unexpected Kondo effect in a few-electron quantum dot containing singlet and triplet spin states, whose energy difference can be tuned with a magnetic field. We observe the effect for an even number of electrons, when the singlet and triplet states are degenerate. The characteristic energy scale is much larger than in the ordinary spin-1/2 case.     

Continuous generation of single photons with controlled waveform in an ion-trap cavity system

The controlled production of single photons is of fundamental and practical interest; they represent the lowest excited quantum states of the radiation field, and have applications in quantum cryptography and quantum information processing. Common approaches use the fluorescence of single ions, single molecules, colour centres and semiconductor quantum dots. However, the lack of control over such irreversible emission processes precludes the use of these sources in applications (such as quantum networks) that require coherent exchange of quantum states between atoms and photons. The necessary control may be achieved in principle in cavity quantum electrodynamics. Although this approach has been used for the production of single photons from atoms, such experiments are compromised by limited trapping times, fluctuating atom-field coupling and multi-atom effects. Here we demonstrate a single-photon source based on a strongly localized single ion in an optical cavity. The ion is optimally coupled to a well-defined field mode, resulting in the generation of single-photon pulses with precisely defined shape and timing. We have confirmed the suppression of two-photon events up to the limit imposed by fluctuations in the rate of detector dark counts. The stream of emitted photons is uninterrupted over the storage time of the ion, as demonstrated by a measurement of photon correlations over 90 min.     

硅量子点表面掺氮的电子结构计算

本文在量子点表面掺入氮原子,用第一性原理方法模拟计算硅量子点（111）面上的电子结构.本文主要解决两个问题：（1）比较研究六种不同大小的量子点结构掺杂和未掺杂氮原子情况下的带隙宽度和电子态密度变化;（2）分别用广义梯度近似（GGA）和局域密度近似（LDA）两种不同的算法计算六种量子点结构的带隙宽度和态密度,并比较GGA和LDA算法的特点.计算结果发现：带隙随着量子点的尺度变小而展宽,这符合量子受限规律;在量子点表面掺杂氮原子会减小带隙宽度;重要的是发现LDA算法对局域态更加敏感.     

Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots

Photoluminescence blinking--random switching between states of high (ON) and low (OFF) emissivities--is a universal property of molecular emitters found in dyes, polymers, biological molecules and artificial nanostructures such as nanocrystal quantum dots, carbon nanotubes and nanowires. For the past 15 years, colloidal nanocrystals have been used as a model system to study this phenomenon. The occurrence of OFF periods in nanocrystal emission has been commonly attributed to the presence of an additional charge, which leads to photoluminescence quenching by non-radiative recombination (the Auger mechanism). However, this 'charging' model was recently challenged in several reports. Here we report time-resolved photoluminescence studies of individual nanocrystal quantum dots performed while electrochemically controlling the degree of their charging, with the goal of clarifying the role of charging in blinking. We find that two distinct types of blinking are possible: conventional (A-type) blinking due to charging and discharging of the nanocrystal core, in which lower photoluminescence intensities correlate with shorter photoluminescence lifetimes; and a second sort (B-type), in which large changes in the emission intensity are not accompanied by significant changes in emission dynamics. We attribute B-type blinking to charge fluctuations in the electron-accepting surface sites. When unoccupied, these sites intercept 'hot' electrons before they relax into emitting core states. Both blinking mechanisms can be electrochemically controlled and completely suppressed by application of an appropriate potential.     

Orbital Kondo effect in carbon nanotubes

Progress in the fabrication of nanometre-scale electronic devices is opening new opportunities to uncover deeper aspects of the Kondo effect--a characteristic phenomenon in the physics of strongly correlated electrons. Artificial single-impurity Kondo systems have been realized in various nanostructures, including semiconductor quantum dots, carbon nanotubes and individual molecules. The Kondo effect is usually regarded as a spin-related phenomenon, namely the coherent exchange of the spin between a localized state and a Fermi sea of delocalized electrons. In principle, however, the role of the spin could be replaced by other degrees of freedom, such as an orbital quantum number. Here we show that the unique electronic structure of carbon nanotubes enables the observation of a purely orbital Kondo effect. We use a magnetic field to tune spin-polarized states into orbital degeneracy and conclude that the orbital quantum number is conserved during tunnelling. When orbital and spin degeneracies are present simultaneously, we observe a strongly enhanced Kondo effect, with a multiple splitting of the Kondo resonance at finite field and predicted to obey a so-called SU4 symmetry.     

Macroscopically ordered state in an exciton system

There is a rich variety of quantum liquids -- such as superconductors, liquid helium and atom Bose-Einstein condensates -- that exhibit macroscopic coherence in the form of ordered arrays of vortices. Experimental observation of a macroscopically ordered electronic state in semiconductors has, however, remained a challenging and relatively unexplored problem. A promising approach for the realization of such a state is to use excitons, bound pairs of electrons and holes that can form in semiconductor systems. At low densities, excitons are Bose-particles, and at low temperatures, of the order of a few kelvin, excitons can form a quantum liquid -- that is, a statistically degenerate Bose gas or even a Bose-Einstein condensate. Here we report photoluminescence measurements of a quasi-two-dimensional exciton gas in GaAs/AlGaAs coupled quantum wells and the observation of a macroscopically ordered exciton state. Our spatially resolved measurements reveal fragmentation of the ring-shaped emission pattern into circular structures that form periodic arrays over lengths up to 1 mm.     

Spin-orbit qubit in a semiconductor nanowire

Motion of electrons can influence their spins through a fundamental effect called spin-orbit interaction. This interaction provides a way to control spins electrically and thus lies at the foundation of spintronics. Even at the level of single electrons, the spin-orbit interaction has proven promising for coherent spin rotations. Here we implement a spin-orbit quantum bit (qubit) in an indium arsenide nanowire, where the spin-orbit interaction is so strong that spin and motion can no longer be separated. In this regime, we realize fast qubit rotations and universal single-qubit control using only electric fields; the qubits are hosted in single-electron quantum dots that are individually addressable. We enhance coherence by dynamically decoupling the qubits from the environment. Nanowires offer various advantages for quantum computing: they can serve as one-dimensional templates for scalable qubit registers, and it is possible to vary the material even during wire growth. Such flexibility can be used to design wires with suppressed decoherence and to push semiconductor qubit fidelities towards error correction levels. Furthermore, electrical dots can be integrated with optical dots in p-n junction nanowires. The coherence times achieved here are sufficient for the conversion of an electronic qubit into a photon, which can serve as a flying qubit for long-distance quantum communication.