Quantum register based on individual electronic and nuclear spin qubits in diamond

The key challenge in experimental quantum information science is to identify isolated quantum mechanical systems with long coherence times that can be manipulated and coupled together in a scalable fashion. We describe the coherent manipulation of an individual electron spin and nearby individual nuclear spins to create a controllable quantum register. Using optical and microwave radiation to control an electron spin associated with the nitrogen vacancy (NV) color center in diamond, we demonstrated robust initialization of electron and nuclear spin quantum bits (qubits) and transfer of arbitrary quantum states between them at room temperature. Moreover, nuclear spin qubits could be well isolated from the electron spin, even during optical polarization and measurement of the electronic state. Finally, coherent interactions between individual nuclear spin qubits were observed and their excellent coherence properties were demonstrated. These registers can be used as a basis for scalable, optically coupled quantum information systems.     

Control and detection of singlet-triplet mixing in a random nuclear field

We observed mixing between two-electron singlet and triplet states in a double quantum dot, caused by interactions with nuclear spins in the host semiconductor. This mixing was suppressed when we applied a small magnetic field or increased the interdot tunnel coupling and thereby the singlet-triplet splitting. Electron transport involving transitions between triplets and singlets in turn polarized the nuclei, resulting in marked bistabilities. We extract from the fluctuating nuclear field a limitation on the time-averaged spin coherence time T2* of 25 nanoseconds. Control of the electron-nuclear interaction will therefore be crucial for the coherent manipulation of individual electron spins.     

Optical atomic coherence at the 1-second time scale

Highest-resolution laser spectroscopy has generally been limited to single trapped ion systems because of the rapid decoherence that plagues neutral atom ensembles. Precision spectroscopy of ultracold neutral atoms confined in a trapping potential now shows superior optical coherence without any deleterious effects from motional degrees of freedom, revealing optical resonance linewidths at the hertz level with a good signal-to-noise ratio. The resonance quality factor of 2.4 x 10(14) is the highest ever recovered in any form of coherent spectroscopy. The spectral resolution permits direct observation of the breaking of nuclear spin degeneracy for the 1S0 and 3P0 optical clock states of 87Sr under a small magnetic bias field. This optical approach for excitation of nuclear spin states allows an accurate measurement of the differential Landé g factor between 1S0 and 3P0. The optical atomic coherence demonstrated for collective excitation of a large number of atoms will have a strong impact on quantum measurement and precision frequency metrology.     

Determination of the equation of state of dense matter

Nuclear collisions can compress nuclear matter to densities achieved within neutron stars and within core-collapse supernovae. These dense states of matter exist momentarily before expanding. We analyzed the flow of matter to extract pressures in excess of 10(34) pascals, the highest recorded under laboratory-controlled conditions. Using these analyses, we rule out strongly repulsive nuclear equations of state from relativistic mean field theory and weakly repulsive equations of state with phase transitions at densities less than three times that of stable nuclei, but not equations of state softened at higher densities because of a transformation to quark matter.     

Ferromagnetic imprinting of nuclear spins in semiconductors

We examine how a ferromagnetic layer affects the coherent electron spin dynamics in a neighboring gallium arsenide semiconductor. Ultrafast optical pump-probe measurements reveal that the spin dynamics are unexpectedly dominated by hyperpolarized nuclear spins that align along the ferromagnet's magnetization. We find evidence that photoexcited carriers acquire spin-polarization from the ferromagnet, and dynamically polarize these nuclear spins. The resulting hyperfine fields are as high as 9000 gauss in small external fields (less than 1000 gauss), enabling ferromagnetic control of local electron spin coherence.     

Stellar and 0ther high-temperature molecules

Optical spectroscopy of stellar molecules trapped at 4 degrees K is particularly valuable when the data can be used to complement the corresponding gas data. The ground state is then directly established by measurement of the absorption spectrum at the low temperature, since all transitions beginning from excited states are eliminated. Isotopic substitution establishes the (0,0) bands of transitions to excited electronic states, and when these data are combined with infrared and fluorescence measurements at 4 degrees K, most of the vibrational properties of the ground and excited states can be obtained. Of the many examples cited and discussed here, C(3) is perhaps the most outstanding. Because the various molecules trapped in matrices are usually identified through prior mass spectrometric work, the optical observations often lead to the discovery of band systems of molecules whose spectra have not previously been observed-for example, those of Si(2)C(3), TaO(2), and WO(2). In these cases the location of the spectral regions in which molecular transitions appear may also serve to encourage the gas spectroscopist to further exploration with high-dispersion spectrographs. I share Ramsay's view (4, p. 204) that further investigation of f-number determinations from matrix spectra should be encouraged, particularly because of the lack of such data for molecules in stars. The principal source of error probably lies in the estimation of the number of molecules per square centimeter in the matrix, but no real test of this has been made. The only existing f values from matrix spectra are those for the C(3) (43, 44) and C(2) (51) molecules, and these are not ideal for test purposes. Because of the anomalous nature of the matrix results discussed above, the rather good agreement between f values for the solid and gas phases of C(2) (51) cannot be considered as support for the matrix determinations. What is needed is a matrix determination of several f(v'v") values (that is, determinations for specific bands) for molecules such as CN and NO or, preferably, for a gas vaporized at high temperature, for which these f values are relatively well established in the gas phase. In this connection the possibility of determining other molecular properties in matrices comes to mind. However, it has been clearly shown that the shape of the potential energy function in the electronic states of molecules can be affected when molecules are trapped in matrices. Brewer, Brabson, and Meyer, in work on S(2) (55), and Schnepp and Dressler, in work on O(2) (56), have examined the anharmonicity in matrices over many vibrational levels. Distortion of the gas potential energy curves occurs in the heavier matrices and sometimes at high vibrational levels in the light ones. Recently work has been begun on comparing the Franck-Condon factors connecting the ground state and two excited states of ScF trapped in a neon matrix (57) with factors calculated from the gas-spectrum data of R. F. Barrow et al. (58) (Deltar(e), the change in interatomic distance upon excitation, has a relatively large value of ~ 0.1 A in these systems). As is well known, such factors are particularly sensitive to the value of Deltar(e), but differences in anharmonicity do not, however, have as significant an effect upon the Franck-Condon factors. Hence a comparison of the matrix and gas factors will lead to further information about matrix effects and will indicate whether Franck-Condon factors can be obtained from matrix spectra. One of the important problems in the study of stellar molecules is the determination of the low-lying electronically excited states, similar to the (1)Delta <--> X(3)Delta difference (~ 580 cm(-1)) in TiO measured by Phillips. Most of the transition-metal oxides have such low-lying levels, and they must be taken into consideration in any calculation of thermodynamic effects at high temperature. It appears that the study of emission spectra in the infrared at 4 degrees K may be one approach to this problem, and an attempt is now being made to confirm the TiO value in order to test the method. Perhaps the greatest advantage of matrix-isolation is the fact that it allows study of these molecules-or of any molecules difficult to produce in a microwave cavity-by electron-paramagnetic-resonance spectroscopy. Study of molecules by this means can provide information about ground state wave functions that is not obtainable by optical spectroscopy, as illustrated by the investigation of ScO, YO, and LaO. Also, it seems likely that the preferential orientation of molecules in matrices, which is probably achievable in most cases, will be a valuable asset in the study of the magnetic properties of molecules by electron-paramagneticresonance spectroscopy, regardless of whether the molecules are "hot" or "cold" (60).     

Coherent dynamics of coupled electron and nuclear spin qubits in diamond

Understanding and controlling the complex environment of solid-state quantum bits is a central challenge in spintronics and quantum information science. Coherent manipulation of an individual electron spin associated with a nitrogen-vacancy center in diamond was used to gain insight into its local environment. We show that this environment is effectively separated into a set of individual proximal 13C nuclear spins, which are coupled coherently to the electron spin, and the remainder of the 13C nuclear spins, which cause the loss of coherence. The proximal nuclear spins can be addressed and coupled individually because of quantum back-action from the electron, which modifies their energy levels and magnetic moments, effectively distinguishing them from the rest of the nuclei. These results open the door to coherent manipulation of individual isolated nuclear spins in a solid-state environment even at room temperature.     

Control of thickness and orientation of solution-grown silicon nanowires

Bulk quantities of defect-free silicon (Si) nanowires with nearly uniform diameters ranging from 40 to 50 angstroms were grown to a length of several micrometers with a supercritical fluid solution-phase approach. Alkanethiol-coated gold nanocrystals (25 angstroms in diameter) were used as uniform seeds to direct one-dimensional Si crystallization in a solvent heated and pressurized above its critical point. The orientation of the Si nanowires produced with this method could be controlled with reaction pressure. Visible photoluminescence due to quantum confinement effects was observed, as were discrete optical transitions in the ultraviolet-visible absorbance spectra.     

Generation of spatially coherent light at extreme ultraviolet wavelengths

We present spatial coherence measurements of extreme ultraviolet (EUV) light generated through the process of high-harmonic up-conversion of a femtosecond laser. With a phase-matched hollow-fiber geometry, the generated beam was found to exhibit essentially full spatial coherence. The coherence of this laser-like EUV source was shown by recording Gabor holograms of small objects. This work demonstrates the capability to perform EUV holography with a tabletop experimental setup. Such an EUV source, with low divergence and high spatial coherence, can be used for experiments involving high-precision metrology, inspection of optical components for EUV lithography, and microscopy and holography with nanometer resolution. Furthermore, the short time duration of the EUV radiation (a few femtoseconds) will enable EUV microscopy and holography to be performed with ultrahigh time resolution.     

Universal signatures of fractionalized quantum critical points

Ground states of certain materials can support exotic excitations with a charge equal to a fraction of the fundamental electron charge. The condensation of these fractionalized particles has been predicted to drive unusual quantum phase transitions. Through numerical and theoretical analysis of a physical model of interacting lattice bosons, we establish the existence of such an exotic critical point, called XY*. We measure a highly nonclassical critical exponent η = 1.493 and construct a universal scaling function of winding number distributions that directly demonstrates the distinct topological sectors of an emergent Z(2) gauge field. The universal quantities used to establish this exotic transition can be used to detect other fractionalized quantum critical points in future model and material systems.     

The (Me5C5)Si+ cation: a stable derivative of HSi+

The reaction of decamethylsilicocene, (Me5C5)2Si, with the proton-transfer reagent Me5C5H2+B(C6F5)4- produces the salt (Me5C5)Si+ B(C6F5)4(2), which can be isolated as a colorless solid that is stable in the absence of air and moisture. The crystal structure reveals the presence of a cationic pi complex with an eta5-pentamethylcyclopentadienyl ligand bound to a bare silicon center. The 29Si nuclear magnetic resonance at very high field (delta = - 400.2 parts per million) is typical of a pi complex of divalent silicon. The (eta5-Me5C5)Si+ cation in 2 can be regarded as the "resting state" of a silyliumylidene-type (eta1-Me5C5)Si+ cation. The availability of 2 opens new synthetic avenues in organosilicon chemistry. For example, 2 reacted with lithium bis(trimethylsilyl)amide to give the disilene E-[(eta1-Me5C5)[N(SiMe3)2]Si]2(3).     

Quantum state engineering and precision metrology using state-insensitive light traps

Precision metrology and quantum measurement often demand that matter be prepared in well-defined quantum states for both internal and external degrees of freedom. Laser-cooled neutral atoms localized in a deeply confining optical potential satisfy this requirement. With an appropriate choice of wavelength and polarization for the optical trap, two electronic states of an atom can experience the same trapping potential, permitting coherent control of electronic transitions independent of the atomic center-of-mass motion. Here, we review a number of recent experiments that use this approach to investigate precision quantum metrology for optical atomic clocks and coherent control of optical interactions of single atoms and photons within the context of cavity quantum electrodynamics. We also provide a brief survey of promising prospects for future work.     

Electrochromic nanocrystal quantum dots

Incorporating nanocrystals into future electronic or optoelectronic devices will require a means of controlling charge-injection processes and an understanding of how the injected charges affect the properties of nanocrystals. We show that the optical properties of colloidal semiconductor nanocrystal quantum dots can be tuned by an electrochemical potential. The injection of electrons into the quantum-confined states of the nanocrystal leads to an electrochromic response, including a strong, size-tunable, midinfrared absorption corresponding to an intraband transition, a bleach of the visible interband exciton transitions, and a quench of the narrow band-edge photoluminescence.     

Near-field coherent spectroscopy and microscopy of a quantum dot system

We combined coherent nonlinear optical spectroscopy with nano-electron volt energy resolution and low-temperature near-field microscopy with subwavelength resolution (相似文献   

Structure-assigned optical spectra of single-walled carbon nanotubes

Spectrofluorimetric measurements on single-walled carbon nanotubes (SWNTs) isolated in aqueous surfactant suspensions have revealed distinct electronic absorption and emission transitions for more than 30 different semiconducting nanotube species. By combining these fluorimetric results with resonance Raman data, each optical transition has been mapped to a specific (n,m) nanotube structure. Optical spectroscopy can thereby be used to rapidly determine the detailed composition of bulk SWNT samples, providing distributions in both tube diameter and chiral angle. The measured transition frequencies differ substantially from simple theoretical predictions. These deviations may reflect combinations of trigonal warping and excitonic effects.     

Metastable oxygen emission bands

Recombination of ground-state oxygen atoms populates six different bound electronic states of molecular oxygen. Of the six optical transitions expected between the three upper states at 4 to 4.5 electron volts and the two lowest states, five have been observed in the afterglow of a conventional helium-oxygen microwave discharge in both 16O(2) and (18)O(2), three of them for the first time in gas-phase spectra. Generation of these emissions from oxygen atoms in a system free of molecular oxygen establishes that atom recombination is the production mechanism.     

Optical spectroscopy of individual single-walled carbon nanotubes of defined chiral structure

We simultaneously determined the physical structure and optical transition energies of individual single-walled carbon nanotubes by combining electron diffraction with Rayleigh scattering spectroscopy. These results test fundamental features of the excited electronic states of carbon nanotubes. We directly verified the systematic changes in transition energies of semiconducting nanotubes as a function of their chirality and observed predicted energy splittings of optical transitions in metallic nanotubes.     

Optical coherence tomography

A technique called optical coherence tomography (OCT) has been developed for noninvasive cross-sectional imaging in biological systems. OCT uses low-coherence interferometry to produce a two-dimensional image of optical scattering from internal tissue microstructures in a way that is analogous to ultrasonic pulse-echo imaging. OCT has longitudinal and lateral spatial resolutions of a few micrometers and can detect reflected signals as small as approximately 10(-10) of the incident optical power. Tomographic imaging is demonstrated in vitro in the peripapillary area of the retina and in the coronary artery, two clinically relevant examples that are representative of transparent and turbid media, respectively.     

The dynamic energy landscape of dihydrofolate reductase catalysis

We used nuclear magnetic resonance relaxation dispersion to characterize higher energy conformational substates of Escherichia coli dihydrofolate reductase. Each intermediate in the catalytic cycle samples low-lying excited states whose conformations resemble the ground-state structures of preceding and following intermediates. Substrate and cofactor exchange occurs through these excited substates. The maximum hydride transfer and steady-state turnover rates are governed by the dynamics of transitions between ground and excited states of the intermediates. Thus, the modulation of the energy landscape by the bound ligands funnels the enzyme through its reaction cycle along a preferred kinetic path.     

Coherence dynamics in photosynthesis: protein protection of excitonic coherence

The role of quantum coherence in promoting the efficiency of the initial stages of photosynthesis is an open and intriguing question. We performed a two-color photon echo experiment on a bacterial reaction center that enabled direct visualization of the coherence dynamics in the reaction center. The data revealed long-lasting coherence between two electronic states that are formed by mixing of the bacteriopheophytin and accessory bacteriochlorophyll excited states. This coherence can only be explained by strong correlation between the protein-induced fluctuations in the transition energy of neighboring chromophores. Our results suggest that correlated protein environments preserve electronic coherence in photosynthetic complexes and allow the excitation to move coherently in space, enabling highly efficient energy harvesting and trapping in photosynthesis.