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The results of growing multilayered nitrogen-doped nanostructures that have the form of periodically arranged nanometer-thick nitrogen-containing layers in a single-crystal CVD diamond are presented. The possibility of creating nitrogen-doped diamond layers with extremely sharp boundaries (less than 1 nm) is demonstrated. The photoluminescence study have shown that multilayered structures make it possible to obtain a higher radiation intensity of practically important NV – sites at a spin coherence time close to that for uniformly doped layers with the same concentration of nitrogen.

Integrated photonics will play a key role in quantum systems as they grow from few-qubit prototypes to tens of thousands of qubits. The underlying optical quantum technologies can only be realized through the integration of these components onto quantum photonic integrated circuits (QPICs) with accompanying electronics. In the last decade, remarkable advances in quantum photonic integration have enabled table-top experiments to be scaled down to prototype chips with improvements in efficiency, robustness, and key performance metrics. These advances have enabled integrated quantum photonic technologies combining up to 650 optical and electrical components onto a single chip that are capable of programmable quantum information processing, chip-to-chip networking, hybrid quantum system integration, and high-speed communications. In this roadmap article, we highlight the status, current and future challenges, and emerging technologies in several key research areas in integrated quantum photonics, including photonic platforms, quantum and classical light sources, quantum frequency conversion, integrated detectors, and applications in computing, communications, and sensing. With advances in materials, photonic design architectures, fabrication and integration processes, packaging, and testing and benchmarking, in the next decade we can expect a transition from single- and few-function prototypes to large-scale integration of multi-functional and reconfigurable devices that will have a transformative impact on quantum information science and engineering., JPhys Photonics, 4 (1), ISSN:2515-7647

We develop a new express methodology for modeling excited-state dynamics occurring in dense manifolds of electronic states in atomistic systems. The approach leverages a modified Landau-Zener formula, the neglect of a back-reaction approximation, and the highly efficient density functional tight-binding method. We study the hot electron dynamics in a series of H- and F-terminated silicon nanocrystals (NCs) containing up to several hundred atoms. We explain the slower electron cooling dynamics in F-terminated NCs by the larger energy gaps between the adjacent electronic states in these systems as well as their slower fluctuations. We conclude that both the mass and chemical identity of the surface termination groups equally influence the electron dynamics, on average. However, the mass effect becomes dominant for higher-energy excitations. We find that the electron decay dynamics in F-terminated NCs has a greater sensitivity to the mass of the surface ligands than do the H-terminated NCs and explain this observation by the details of the electron-phonon coupling in the systems. We find that in the H-terminated NCs, electronic transitions in the cooling process occur predominantly between the surface states, whereas in F-terminated Si NCs, both surface and NC core states are coupled to the nuclear vibrations. We find that electron energy relaxation is accelerated in larger NCs and attribute this effect to the higher densities of states and smaller energy gaps in these systems.

Accurate, high spatial resolution thermal measurements have provided fundamental insights into many fields of study; however, existing thermometer technology often suffers from one or more limitati...

Creation of localized NV center ensembles, produced by irradiation of CVD diamond with nitrogen doped delta-layer with 200 keV electron beam and the subsequent annealing is demonstrated. Results of optical measurements of activated areas at different irradiation doses are presented. Issues concerning defect formation in diamond lattice during the electron beam impact are discussed.

Recent studies demonstrated anomalous temperature shifts for some Fano-Feshbach resonances of thulium atoms. These anomalies were explained by the variation in light intensity in the optical dipole trap, which accompanied changes in temperature. In addition, a temperature-related transformation of the statistics of the inter-resonance spacing was demonstrated [Aikawa et al., Phys. Rev. Lett. 108, 210401 (2012)]. Here, we analyze the shifts of isolated $s$- and $d$-type Fano-Feshbach resonances of ultracold thulium atoms with temperature for a fixed depth of an optical dipole trap. The measurements are consistent with the three-body recombination-based theory of the temperature-related resonance shift and enable the extraction of the resonance parameters, particularly the magnetic moments of closed channel states. This parameter and the known polarizability of the open channel enable us to separate the contributions of the temperature and Stark shift to the overall shift of the resonances and show the dominant role of the Stark effect in the overall shift.

In this work, we report a new nonadiabatic molecular dynamics methodology that incorporates many-body (MB) effects in the treatment of electronic excited states in extended atomistic systems via linear-response time-dependent density functional theory (TD-DFT). The nonradiative dynamics of excited states in Si75H64 and Cd33Se33 nanocrystals is studied at the MB (TD-DFT) and single-particle (SP) levels to reveal the role of MB effects. We find that a MB description of the excited states qualitatively changes the structure of coupling between the excited states, leading to larger nonadiabatic couplings and accelerating the dynamics by a factor of 2-4. The dependence of excited state dynamics in these systems on the surface hopping/decoherence methodology and the choice of the dynamical basis is investigated and analyzed. We demonstrated that the use of special "electron-only" or "hole-only" excitation bases may be advantageous over using the full "electron-hole" basis of SP states, making the computed dynamics more consistent with the one obtained at the MB level.

Recently, the transformation from random to chaotic behavior in the statistics of Fano&ndash, Feshbach resonances was observed in thulium atoms with rising ensemble temperature. We performed random matrix theory simulations of such spectra and analyzed the resulting statistics in an attempt to understand the mechanism of the transformation. Our simulations show that, when evaluated in terms of the Brody parameter, resonance statistics do not change or change insignificantly when higher temperature resonances are appended to the statistics. In the experiments evaluated, temperature was changed simultaneously with optical dipole trap depth. Thus, simulations included the Stark shift based on the known polarizability of the free atoms and assuming their polarizability remains the same in the bound state. Somewhat surprisingly, we found that, while including the Stark shift does lead to minor statistical changes, it does not change the resonance statistics and, therefore, is not responsible for the experimentally observed statistic transformation. This observation suggests that either our assumption regarding the polarizability of Feshbach molecules is poor or that an additional mechanism changes the statistics and leads to more chaotic statistical behavior.

The fine structure of the band edge exciton and the dark exciton photoluminescence (PL) are topics of significant interest in the research of semiconducting metal halide perovskite nanocrystals, with several conflicting reports on the level ordering of the bright and dark states and the accessibility of the emitting dark states. Recently, we observed the intense dark exciton PL in strongly confined CsPbBr3 nanocrystals at cryogenic temperatures, in contrast to weakly confined nanocrystals lacking dark exciton PL, which was explained by the confinement enhanced bright-dark exciton splitting. In this work, we investigated the size-dependence of the dark exciton photoluminescence properties in CsPbBr3 and CsPbI3 quantum dots in the strongly confined regime, showing the clear role of confinement in determining the bright-dark energy splitting (ΔEBD) and the dark exciton lifetime (τD). We observe the increase in both ΔEBD and τD with increasing quantum confinement in CsPbBr3 and CsPbI3 QDs, consistent with the earlier predictions on the size-dependence of ΔEBD and τD. Our results show that quantum confinement plays a crucial role in determining the accessibility to the dark exciton PL and its characteristics in metal halide perovskite nanocrystals.

A rotation sensor is one of the key elements of inertial navigation systems and compliments most cell phone sensor sets used for various applications. Currently, inexpensive and efficient solutions are mechanoelectronic devices, which nevertheless lack long-term stability. Realization of rotation sensors based on spins of fundamental particles may become a drift-free alternative to such devices. Here, we carry out a proof-of-concept experiment, demonstrating rotation measurements on a rotating setup utilizing nuclear spins of an ensemble of nitrogen vacancy centers as a sensing element with no stationary reference. The measurement is verified by a commercially available microelectromechanical system gyroscope.

Recently, the thulium atom was cooled down to the Bose-Einstein condensation temperature, thus opening a pathway to quantum simulation with this atom. However, successful simulations require instruments to control and readout states of the atom as well as the ability to control the interaction between either different species or different states of the same type of species. In this paper, we provide an experimental demonstration of high-fidelity (over 93%) manipulation of the ground state magnetic sublevels of thulium, which utilizes a simple and efficient design of a microwave (MW) antenna. The coherence time and dephasing rate of the energetically highest hyperfine level of the ground state were also examined.

The sensitivity of the nitrogen-vacancy (NV) color centers in diamond-based magnetometers strongly depends on the number of NV centers involved in the measurement. Unfortunately, an increasing concentration of NV centers leads to a decrease in their dephasing and coherence times if the nitrogen content exceeds a certain threshold level (approximately 10 17 c m - 3 or 0.6 ppm). Here, we demonstrate that this increased dephasing can be efficiently compensated for by optimizing the electron irradiation dose in postprocessing procedures in the vicinity of the threshold concentration, thus extending the range of possible useful concentrations of NV centers in diamonds with a natural carbon content.

All-optical thermometry presents a promising avenue of investigation for sensitive biological and electronic systems, with methods free of radio-frequency interference of particular importance. In this work, an all-optical scanning fiber thermometer is tested and shown to possess $5\phantom{\rule{0.2em}{0ex}}\ensuremath{\mu}\mathrm{m}$ spatial and $20\phantom{\rule{0.2em}{0ex}}\mathrm{mK}/\sqrt{\mathrm{Hz}}$ temperature resolution. This probe is then used to generate noncontact scanning thermal images of active circuit elements with microscale thermal features.

Properties of silicon-vacancy (SiV) colour centres in ultra-nanosize diamonds are studied. Nanodiamonds are obtained at a high temperature and pressure, which induced transformations in mixtures of organic and hetero-organic compounds without metal-catalysts. The size distribution of grown nanodiamonds is determined by the methods of transmission electron microscopy and atomic-force microscopy, as well as by using the model of phonon spatial localisation. In addition, Raman spectra of various nanodiamonds and luminescence properties of SiV-centres are investigated.

Magnetic fields are one of the main tools for controlling the interaction of ultracold atoms using the so-called Feshbach resonances. However, the accurate knowledge of magnetic fields within the high-vacuum chamber is significantly complicated due to the inexact knowledge of the setup geometry, the presence of magnetic parts, and other. In this paper, we demonstrate precision calibration of magnetic fields in the high-vacuum setup using microwave spectroscopy of the ground state of ultracold thulium atoms.

A microwave antenna configuration shaped as coaxial resonant coils is proposed for exciting magnetic dipole transitions of the optical ground state of the nitrogen—vacancy color center in diamond. The field within the antenna is simulated, field amplitudes are experimentally measured.

We report a study on the non-adiabatic molecular dynamics (NA-MD) of the charge transfer (CT) process in the boron subphtalocyanine chloride (SubPc)/fullerene (C60) interface using our newly implemented Libra-X software package, which is based on an interface of the Libra NA-MD library and the GAMESS electronic structure software. In particular, we address the following aspects of the simulation protocol: (a) the choice of the potential used to treat interatomic interactions and its effect on the structures of the complex and CT rates; (b) the choice of the electronic structure methodology used; and (c) the choice of the trajectory surface hopping (TSH) methodology used. From our analysis of the electronic structure, we suggest that the distortion of the SubPc conical structure affects orbital localization and that the “breathing” motion of SubPc drives the CT process in SubPc/C60. This study illustrates that the choice of the TSH methodology and electronic decoherence are crucial for the CT simulation. We extend our analysis of CT in SubPc/(C60)n models by increasing the number of C60 molecules up to n = 4. We find that the details of the interfacial SubPc/(C60)n geometry determine the CT rate. Finally, we find the computed CT timescale to be in the range of 2.2–5.0 ps, which is in agreement with the experimentally determined timescale in the order of magnitude of ∼10 ps. The developed open-source Libra-X package is freely available on the Internet at https://github.com/Quantum-Dynamics-Hub/Libra-X.

The numerical solution to optical Bloch equations for the transition F g = 4 ⇒ F e = 5 with a wavelength of 410.6 nmin the thulium atom is presented. The absorption spectrum saturation and narrowing effects due to optical pumping are considered in detail.

Bose-Einstein condensation (BEC) is a powerful tool for a wide range of research activities, a large fraction of which is related to quantum simulations. Various problems may benefit from different atomic species, but cooling down novel species interesting for quantum simulations to BEC temperatures requires a substantial amount of optimization and is usually considered to be a difficult experimental task. In this work, we implemented the Bayesian machine learning technique to optimize the evaporative cooling of thulium atoms and achieved BEC in an optical dipole trap operating near 532 nm. The developed approach could be used to cool down other novel atomic species to quantum degeneracy without additional studies of their properties.

We present the design, fabrication and characterization of high quality factor silicon nitride nanobeam PhC cavities at visible wavelengths for coupling to diamond color centers in a cavity QED system. We demonstrate devices with a quality factor of ∼24, 000 (±250) around the zero-phonon line of the germanium-vacancy center in diamond. We also present an efficient fiber-to-waveguide coupling platform for suspended nanophotonics. By gently changing the corresponding effective indices at the fiber-waveguide interface, we achieve a coupling efficiency of ∼96% (±2%) at the cavity resonance.

Here, we report on the observation of a random to chaotic temperature transformation in the statistics of nearest-neighbor spacings of Fano-Feshbach resonances in the ultracold polarized gas of thulium-169 atoms. We associate this transformation to the appearance of so-called $d$ resonances as well as the shift of other resonances with the temperature. In addition to this statistical change, it has been observed that the characters of $s$- and $d$-resonance temperature shifts are quite different: $s$ resonances experience almost no shift or even negative shift with the temperature, while $d$ resonances experience an obvious positive shift. The sign change was attributed to the difference in polarizability of Feshbach molecules and free thulium atoms. In addition, careful analysis of the broad Fano-Feshbach resonances enabled the determination of the sign of thulium's background scattering length. A rethermalization experiment made it possible to estimate a length value of ${a}_{\mathrm{bg}}=+144\ifmmode\pm\else\textpm\fi{}38\text{ }\text{ }\mathrm{a}.\mathrm{u}.$ This indicates that thulium atoms are suitable for achieving Bose-Einstein condensation.

This review focuses on recent developments in the field of nonadiabatic molecular dynamics (NA-MD), with particular attention given to condensed-matter systems. NA-MD simulations for small molecular systems can be performed using high-level electronic structure (ES) calculations, methods accounting for the quantization of nuclear motion, and using fewer approximations in the dynamical methodology itself. Modeling condensed-matter systems imposes many limitations on various aspects of NA-MD computations, requiring approximations at various levels of theory-from the ES, to the ways in which the coupling of electrons and nuclei are accounted for. Nonetheless, the approximate treatment of NA-MD in condensed-phase materials has gained a spin lately in many applied studies. A number of advancements of the methodology and computational tools have been undertaken, including general-purpose methods, as well as those tailored to nanoscale and condensed matter systems. This review summarizes such methodological and software developments, puts them into the broader context of existing approaches, and highlights some of the challenges that remain to be solved.

We have implemented a Python-based software package within the Libra software for performing nonadiabatic molecular dynamics (NA-MD) within the neglect of back reaction approximation (NBRA). Available in the software are a wide variety of proposed hop acceptance (PHA) and decoherence methodologies. Using Libra, a comparative analysis of PHA schemes and decoherence methods is performed to examine thermal equilibrium in NA-MD simulations within the NBRA. The analysis is performed using 3 model systems, each of which highlights the effects of the different decoherence methods and PHA schemes on NA transitions. We find that the interplay between decoherence and PHA schemes is important for achieving detailed balance in the NBRA and discuss the conditions by which the detailed balance is achieved for each model. We discuss the qualitative features of NA dynamics computed using various combinations of decoherence and PHA schemes for a wide range of model and condition parameters such as temperature, energy gap magnitude, and dephasing times. Furthermore, we extend the analysis to include the Boltzmann corrected Ehrenfest methodology of Bastida and co-workers and compare the dynamics produced with it with that obtained using the surface hopping-based approach.

International audience; Ultrasmall (about 10 nm), low-strain, artificially produced diamonds with an internal, active color center have substantial potential for quantum information processing and biomedical applications. Thus, it is of great importance to be able to artificially produce such diamonds. Here, we report on the high-pressure, high-temperature synthesis of such nanodiamonds about 10 nm in size and containing an optically active, single silicon-vacancy color center. Using special sample preparation technique, we were able to prepare samples containing single nanodiamonds on the surface. By correlating atomic-force microscope images and confocal optical images, we verified the presence of optically active color centers in single nanocrystals, and using second-order correlation measurements, we proved the single-photon emission statistics of these nanodiamonds. These color centers have nonblinking, spectrally narrow emission with narrow distribution of spectral width and positions of zero-phonon line, thus proving the high quality of the nanodiamonds produced.

Silicon-doped diamond nanopillars have been produced by a microwave plasma chemical vapor deposition (CVD) on a single crystal diamond substrate through holes in a Si mask perforated with a focused ion beam. Arrays of 400 nm diameter pillars with aspect ratio up to 2.8 are grown epitaxially being confined by channels in the mask, the latter serving also as the Si doping source. Strong photoluminescent (PL) emission of the SiV centers at 738.7 nm wavelength, localized within the pillars, has been detected and imaged with a fluorescence microscope. The SiV PL decay time of 1.1 ns has been deduced from PL kinetics measurements. An increase of specific PL intensity (intensity per unit volume of the pillar) with the aspect ratio is noted.

Developed 25 years ago, Tully's fewest switches surface hopping (FSSH) has proven to be the most popular approach for simulating quantum-classical dynamics in a broad variety of systems, ranging from the gas phase, to the liquid and solid phases, to biological and nanoscale materials. FSSH is widely adopted as the fundamental platform to introduce modifications as needed. Significant progress has been made recently to enhance the accuracy and efficiency of the surface hopping technique. Various limitations of the standard FSSH-associated with quantum nuclear effects, interference and decoherence, trivial or "unavoided" crossings, superexchange, and representation dependence-have been lifted. These advances are needed to allow one to treat many important phenomena in chemistry, physics, materials, and related disciplines. Examples include charge transport in extended systems such as organic solids, singlet fission in molecular aggregates, Auger-type exciton multiplication, recombination and relaxation in quantum dots and other nanoscale materials, Auger-assisted charge transfer, nonradiative luminescence quenching, and electron-hole recombination. This Perspective summarizes recent advances in the surface hopping formulation of nonadiabatic dynamics and provides an outlook on the future of surface hopping.

The "methodology discovery" library for quantum and classical dynamics simulations is presented. One of the major foci of the code is on nonadiabatic molecular dynamics simulations with model and atomistic Hamiltonians treated on the same footing. The essential aspects of the methodology, design philosophy, and implementation are discussed. The code capabilities are demonstrated on a number of model and atomistic test cases. It is demonstrated how the library can be used to study methodologies for quantum and classical dynamics, as well as a tool for performing detailed atomistic studies of nonadiabatic processes in molecular systems. The source code and additional information are available on the Web at http://www.acsu.buffalo.edu/~alexeyak/libra/index.html. © 2016 Wiley Periodicals, Inc.

Excited state dynamics at the nanoscale requires treatment of systems involving hundreds and thousands of atoms. In the majority of cases, depending on the process under investigation, the electronic structure component of the calculation constitutes the computation bottleneck. We developed an efficient approach for simulating nonadiabatic molecular dynamics (NA-MD) of large systems in the framework of the self-consistent charge density functional tight binding (SCC-DFTB) method. SCC-DFTB is combined with the fewest switches surface hopping (FSSH) and decoherence induced surface hopping (DISH) techniques for NA-MD. The approach is implemented within the Python extension for the ab initio dynamics (PYXAID) simulation package, which is an open source NA-MD program designed to handle nanoscale materials. The accuracy of the developed approach is tested with ab initio DFT and experimental data, by considering intraband electron and hole relaxation, and nonradiative electron-hole recombination in a CdSe quantum dot and the (10,5) semiconducting carbon nanotube. The technique is capable of treating accurately and efficiently excitation dynamics in large, realistic nanoscale materials, employing modest computational resources.

In this work we had developed optical structures from silicon nitride for further integration of the nanodiamonds containing NV-centers with them. We have introduced method of the nanodiamonds solution application on the substrates. The work has practical meaning in nanophotonics sphere and in development of optical devices with single-photon sources.

Dipolar atoms have unique properties, making them interesting for laser cooling and quantum simulations. But, due to relatively large orbital momentum in the ground state these atoms may have large dynamic tensor and vector polarizabilities in the ground state. This enables the formation of spin-dependent optical traps. In this paper the real part of tensor and vector dynamic polarizability was experimentally measured and compared to a theoretical simulation. For an optical dipole trap operating around 532.07 nm, tensor polarizability was found to be $\ensuremath{-}145\ifmmode\pm\else\textpm\fi{}53\phantom{\rule{0.16em}{0ex}}\phantom{\rule{0.16em}{0ex}}\mathrm{a}.\mathrm{u}.$ and vector polarizability was $680\ifmmode\pm\else\textpm\fi{}240\phantom{\rule{0.16em}{0ex}}\phantom{\rule{0.16em}{0ex}}\mathrm{a}.\mathrm{u}.$ The measurements were compared with simulations, which were done based on the known set of levels from a thulium atom. The simulations are in good agreement with experimental results. In addition, losses of atoms from the dipole trap were measured for different trap configurations and compared to the calculated imaginary part of vector and tensor polarizabilities.

The sensing applications of nitrogen-vacancy color centers in a diamond require an efficient manipulation of the color center ground state over the whole volume of an ensemble. Thus, it is necessary to produce strong uniform magnetic fields of a well-defined circular polarization at microwave frequencies. In this paper, we develop a circularly polarized microwave antenna based on the excitation of hybrid electromagnetic modes in a high-permittivity dielectric resonator. The influence of the geometrical parameters of the antenna on the reflection coefficient and magnetic field magnitude is studied numerically and discussed. The Rabi frequencies and their inhomogeneity over the volume of a commercially available diamond sample are calculated. With respect to the numerical predictions, a Rabi frequency as high as 34 MHz with an inhomogeneity of 4% over a 1.2 mm × ∅2.5 mm (5.9 mm3 in volume) diamond sample can be achieved for 10 W of input power at room temperature. The antenna prototype is fabricated, and experimental investigations of its characteristics are performed in microwave and optical frequency domains. The circular polarization of the microwave magnetic field with an ellipticity of 0.94 is demonstrated experimentally. The Rabi oscillation frequency and its inhomogeneity are measured, and the results demonstrate a good agreement with the numerically predicted results.

The outcomes of nonadiabatic molecular dynamics (NA-MD) calculations are modulated by the parameters entering the time-dependent Schrodinger equation (TD-SE). The adiabatic states are commonly used as the basis in which the TD-SE is integrated. However, the phase inconsistencies of such states along the nuclear trajectories obtained in NA-MD simulations may render the wave function and other relevant properties ill-behaving, adversely affecting the dynamics. This work illustrates the consequence of adiabatic state phase inconsistencies in nonadiabatic Ehrenfest dynamics. A simple phase-correction approach is proposed and is demonstrated to alter the dynamics to make it consistent with the reference calculations done in the phase-consistent diabatic representation.

Ensembles of nitrogen-vacancy color centers in diamond hold promise for ultra-precise magnetometery, competing with superconducting quantum interference device detectors. Sensor and metrology applications for situations involving high sensitivity require efficient manipulation of the nitrogen-vacancy color centers electronic spins within large volume. Thus, the design of microwave antennas providing a uniform and strong microwave magnetic field over a relatively large volume is on a high demand. In this paper we report different antenna designs based on low loss high permittivity dielectric materials for coherent manipulation of a large ensemble of nitrogen-vacancy color centers in diamond. The operational principle of the proposed antennas is based on excitation of transverse electric (TE) or hybrid electromagnetic (HEM) modes of dielectric resonators. The first antenna design is based on TE01 mode excited inside the resonator made on a ceramic with permittivity of 80. The uniformity of the microwave magnetic field generated by the antenna was verified by measurement of the optically detected magnetic resonance and Rabi frequency in a high-density ensemble of nitrogen-vacancy color centers placed in the center bore of the antenna. Rabi frequency of 10 MHz in a volume of 7 cubic millimeters with a standard deviation of less than 1% at 5 W pump power has been measured at the room temperature. This is enough to coherently excite all color centers in commercially available diamond plates at room temperature. The second antenna design is based on HEM11δ mode excited in the ceramic resonator characterized by the permittivity of 235. The numerical simulations predict the Rabi frequency value of 34.85 MHz in a volume of 6 cubic millimeters with a standard deviation of less than 5% at 5 W pump power. The obtained result paves the way to improve the sensitivity of cutting-edge nitrogen-vacancy color centers based magnetometers by several orders of magnitude, practically reaching superconducting quantum interference device detectors level of sensitivity.

Minimization of internal degrees of freedom is an important step in the cooling of atomic species to degeneracy temperature. Here, we report on the loading of 6*10^5 thulium atoms optically polarized at maximum possible magnetic quantum number mf=-4 state into dipole trap operating at 532 nm. The purity of polarizations of the atoms was experimentally verified using a Stern-Gerlach-type experiment. Experimental measured polarization of the state is 3.91(26).

Ensembles of nitrogen-vacancy color centers in diamond hold promise for ultra-precise magnetometry, competing with superconducting quantum interference device detectors. By utilizing the advantages of dielectric materials, such as very low losses for electromagnetic field, with the potential for creating high Q-factor resonators with strong concentration of the field within it, we implemented a dielectric resonator antenna for coherent manipulation of a large ensemble of nitrogen-vacancy centers in diamond. We reached average Rabi frequency of 10 MHz in a volume of 7 mm3 with a standard deviation of less than 1% at a moderate pump power. The obtained result enables use of large volume low nitrogen-vacancy concentration diamond plates in modern nitrogen-vacancy magnetometers thus improving sensitivity via larger coherence time and higher optical detected magnetic resonance contrast.

In the condensed-matter environments, the vibronic Hamiltonian that describes nonadiabatic dynamics often appears as an erratic entity, and one may assume it can be generated stochastically. This property is utilized to formulate novel stochastic and quasi-stochastic vibronic Hamiltonian methodologies, which open a new route to long-time excited state dynamics in atomistic solid-state systems at negligible computational cost. Using a model mimicking a typical solid-state material in noisy environment, general conclusions regarding the simulation of nonadiabatic dynamics are obtained: (1) including bath is critical to complete excited state relaxation; (2) a totally stochastic modulation of energies and couplings has a net effect of no bath and inhibits relaxation; (3) including a single or several dominant electron-phonon modes may be insufficient to complete the excited state relaxation; (4) only the multiple modes, even those that have negligible weights, can represent both the deterministic modulation of system's Hamiltonian and stochastic effects of bath.

NV centers ensemble have proven to be sensitive and versatile sensor platform for many applications such as magnetometry [1, 2], electric field sensing [3], thermometry [4] and rotation sensing [5]. The tradeoff between concentration of NVs and coherence lifetime of the electronic spin limits the maximum sensitivity of such devices. Recently usage of quantum memory associated with nuclear spins nearby NV center was shown to dramatically increase the sensitivity via accumulation of the sensed signal in memory [6]. This way sensing on single NV center can benefit a lot from nearby environment, but extension of this technique on atomic ensemble is still quite challenging. Here we present a versatile platform for quantum manipulation with a highly dense NV ensemble in HPHT diamond plates. In our work, we demonstrate several approaches to initialize quantum memory in regular magnetic fields, manipulation of quantum memory, and reading the quantum information from it. Also, we carefully study decoherence rate in our sample using “Echo” and “FID” techniques. We believe the key sources of decoherence in our samples are natural abundance of 13C isotopes and P1 centers. To better understand and clarify contribution of each component we studied number of samples with different defect concentrations. Besides, multifrequency resonances were investigated in NV ensembles both experimentally and theoretically. Previously multifrequency resonances were studied in single NV center system at various combinations of transverse and longitudinal MW and RF field allowing to detect many-photon transitions in electron spin subshell[7]. Here we provide study of additional series of resonances achieved in NV ensemble configuration with a close look to the many-photon transitions both in electron and nuclear eigen states. This resonances could be utilized to hyperpolarize the nuclear spin environment in diamond.

Single NV centers in HPHT IIa diamond are fabricated by helium implantation through lithographic masks. The concentrations of created NV centers in different growth sectors of HPHT are compared quantitatively. It is shown that the purest {001} growth sector (GS) of HPHT diamond allows to create groups of single NV centers in predetermined locations. The {001} GS HPHT diamond is thus considered a good material for applications that involve single NV centers.

A design for an ultrahigh Q/V nanobeam cavity engineered to interact with Germanium-vacancy (GeV) centers is presented. The nanobeam cavity supports a mode with Q/V>108 with transmission over 70%. The proposed design is based on a new scalable approach developed to reduce the footprint of nanobeam cavities by more than 50% without losing the cavity Q/V value and transmission. Cavity quantum electrodynamics analysis reveals that strong coupling between the zero-phonon line transition of GeV centers and the cavity mode can be achieved for a range of nanobeam dimensions.

Trapped and Coupled Trapped single atoms are ideal for storing and manipulating quantum information. Thompson et al. (p. 1202 , published online 25 April; see the Perspective by Keller ) were able to control single atoms interacting coherently with a field mode of a photonic crystal cavity. An optical tweezer was used to trap the single atom, which enabled positioning of the atom in close proximity to the photonic crystal waveguide, coupling the atom to the optical mode of the cavity. Such coupling should prove useful in quantum measurement, sensing, and information processing.

This work presents a nonadiabatic molecular dynamics methodology that relies on the use of fragment molecular orbitals computed using tight-binding Hamiltonians. The approach aims to model charge and energy transfer in large systems via quantum-classical trajectory-based approaches. The technique relies on a chemically motivated fragmentation of the overall system into arbitrary fragments. Several types of fragment molecular orbitals (FMO) can be constructed and used in nonadiabatic simulations, comprising quasidiabatic, adiabatic, and Lowdin-transformed ones. The adiabatic FMOs are found to be most suitable for modeling nonadiabatic dynamics in complex molecular systems. The overall algorithm shows advantageous scaling properties, making it possible to model long time scale charge transfer processes in large systems with many hundreds of atoms. The approach is applied to study charge transfer in subphtalocyanine(SubPc)/C60 heterojunction. The computational results emphasize the importance of decoherence ...

Understanding the dynamics of electron–ion energy transfer in warm dense (WD) matter is important to the measurement of equation of state (EOS) properties and for understanding the energy balance in dynamic simulations. In this work, we present a comprehensive investigation of nonadiabatic electron relaxation and thermal excitation dynamics in aluminum under high pressure and temperature. Using quantum–classical trajectory surface hopping approaches, we examine the role of nonadiabatic couplings and electronic decoherence in electron-nuclear energy transfer in WD aluminum. The computed timescales range from 400 fs to 4.0 ps and are consistent with existing experimental studies. We have derived general scaling relationships between macroscopic parameters of WD systems such as temperature or mass density and the timescales of energy redistribution between quantum and classical degrees of freedom. The scaling laws are supported by computational results. We show that electronic decoherence plays essential role and can change the functional dependencies qualitatively. The established scaling relationships can be of use in modelling of WD matter.

Nonadiabatic molecular dynamics (NA-MD) is an extremely useful approach to model electron transfer dynamics in molecular and solid state systems. The performance of NA-MD simulations depends critically on the accuracy of the underlying electronic structure properties, such as state energies and nonadiabatic couplings (NAC). Practical NA-MD modeling relies extensively on computationally efficient pure density functionals, despite the known intrinsic problems of the latter. A reliable solution to the problems presented by the use of pure density functionals, is the use of hybrid functionals, however hybrid functionals are significantly more expensive. In this work, we investigate how the choice of the density functional can affect the NAC magnitudes for small silicon clusters and silicon hydrides. We find that pure functionals can significantly overestimate NAC magnitudes in comparison to those obtained with hybrid functionals. The ratio of the two magnitudes increases with the system size and differs by an order of magnitude even for small Si

Integration of solid-state quantum emitters such as NV center in diamond with tapered optical fiber is demanded by number of applications ranging from sensing and imaging to quantum communications and computations. Nevertheless, utilization of a single NV center coupled with an optical fiber meets significant challenge of fiber fluorescence that can considerably mask emission of the quantum object. In this paper, we analyze main sources of such fluorescence for the case of NV center coupled to tapered single mode optical fiber and discuss possible ways of improving signal to noise ratio in this case.

NV center in diamond is attracting a lot of attention in quantum information processing community [1]. Been spin system in clean and well-controlled environment of diamond it shows outstanding performance as quantum memory even at room temperature, spin control with single shot optical readout and possibility to build up quantum registers even on single NV center. Moreover, NV centers could be used as high-resolution sensitive elements of detectors of magnetic or electric field, temperature, tension, force or rotation. For all of these applications collection of the light emitted by NV center is crucial point. There were number of approaches suggested to address this issue, proposing use of surface plasmoms [2], manufacturing structures in diamond [3] etc. One of the key feature of any practically important interface is compatibility with the fiber technology. Several groups attacking this problem using various approaches. One of them is placing of nanodiamonds in the holes of photonic crystal fiber [4], another is utilization of AFM to pick and place nanodiamond on the tapered fiber[5]. We have developed a novel technique of placing a nanodiamond with single NV center on the tapered fiber by controlled transfer of a nanodiamond from one “donor” tapered fiber to the “target” clean tapered fiber. We verify our ability to transfer only single color centers by means of measurement of second order correlation function. With this technique, we were able to double collection efficiency of confocal microscope. The majority of the factors limiting the collection of photons via optical fiber are technical and may be removed allowing order of magnitude improved in collection. We also discuss number of extensions of this technique to all fiber excitation and integration with nanostructures. References: [1] Marcus W. Doherty, Neil B. Manson, Paul Delaney, Fedor Jelezko, Jorg Wrachtrup, Lloyd C.L. Hollenberg , " The nitrogen-vacancy colour centre in diamond," Physics Reports, vol. 528, no. 1, p. 1–45, 2013. [2] A.V. Akimov, A. Mukherjee, C.L. Yu, D.E. Chang, A.S. Zibrov, P.R. Hemmer, H. Park and M.D. Lukin, "Generation of single optical plasmons in metallic nanowires coupled to quantum dots," Nature, vol. 450, p. 402–406, 2007. [3] Michael J. Burek , Yiwen Chu, Madelaine S.Z. Liddy, Parth Patel, Jake Rochman , Srujan Meesala, Wooyoung Hong, Qimin Quan, Mikhail D. Lukin and Marko Loncar High quality-factor optical nanocavities in bulk single-crystal diamond, Nature communications 6718 (2014) [4] Tim Schroder, Andreas W. Schell, Gunter Kewes, Thomas Aichele, and Oliver Benson Fiber-Integrated Diamond-Based Single Photon Source, Nano Lett. 2011, 11, 198-202 [5]Lars Liebermeister, et. al. “Tapered fiber coupling of single photons emitted by a deterministically positioned single nitrogen vacancy center”, Appl. Phys. Lett. 104, 031101 (2014)

The sensitivity of magnetic and electric field sensors based on nitrogen-vacancy (NV) center in diamond strongly depends on the available concentration of NV and their coherence properties. Achieving high coherence times simultaneously with high concentration is a challenging experimental task. Here, we demonstrate that by using a temperature gradient method of high-pressure, high-temperature growing technique, one can achieve nearly maximally possible dephasing times, limited only by carbon nuclear spins at low nitrogen concentrations or nitrogen electron spin at high nitrogen concentrations. Hahn-echo T 2 coherence times were also investigated and found to demonstrate reasonable values. Thus, the high-pressure, high-temperature technique is a strong contender to the popular chemical vapor deposition method in the development of high-sensitivity, diamond-based sensors.

Color centers in diamonds have shown promising potential for luminescent thermometry. So far, the nitrogen-vacancy (NV) color center has demonstrated a high sensitivity for optical temperature monitoring in biological systems. However, the NV center requires microwave excitation which can cause unwanted heating, and the NV is also sensitive to non-axial magnetic fields, both of which can result in inaccurate temperature measurements. To overcome this drawback, the silicon-vacancy (SiV) and germanium-vacancy (GeV) color centers in diamonds have recently been explored and have shown good optical temperature sensitivity owing to the temperature dependent wavelength optical zero-phonon line. Here, we report optical temperature measurements using the recently discovered tin-vacancy (SnV) color center in diamond and show sensitivity better than 0.2 K in 10 s integration time. Also, we compare the relative merits of SnV with respect to SiV and GeV for luminescent thermometry. These results illustrate that there are likely to be many future options for nanoscale thermometry using diamonds.

A simple and robust methodology, dubbed Entangled Trajectories Hamiltonian Dynamics (ETHD), is developed to capture quantum nuclear effects such as tunneling and zero-point energy through the coupling of multiple classical trajectories. The approach reformulates the classically mapped second-order Quantized Hamiltonian Dynamics (QHD-2) in terms of coupled classical trajectories. The method partially enforces the uncertainty principle and facilitates tunneling. The applicability of the method is demonstrated by studying the dynamics in symmetric double well and cubic metastable state potentials. The methodology is validated using exact quantum simulations and is compared to QHD-2. We illustrate its relationship to the rigorous Bohmian quantum potential approach, from which ETHD can be derived. Our simulations show a remarkable agreement of the ETHD calculation with the quantum results, suggesting that ETHD may be a simple and inexpensive way of including quantum nuclear effects in molecular dynamics simulations.

We demonstrated a simple and reliable technique of coupling diamond nanocrystal containing NV center to tapered optical fiber. The NV center emission was collected by the fiber via nearfield interaction between NV center and the tapered portion of the fiber. Single photon statistics was demonstrated at the fiber end as well as up to 3 times improvement in collection efficiency with respect to our confocal microscope. Also, we carefully studied fluorescence of the fiber itself and were able to suppress it to the level lower than single photon emission from the NV center.

Further development of quantum emitter based communication and sensing applications intrinsically depends on the availability of robust single-photon detectors. Here, we demonstrate a new generation of superconducting single-photon detectors specifically optimized for the 500–1100 nm wavelength range, which overlaps with the emission spectrum of many interesting solid-state atom-like systems, such as nitrogen-vacancy and silicon-vacancy centers in diamond. The fabricated detectors have a wide dynamic range (up to 350 million counts per second), low dark count rate (down to 0.1 counts per second), excellent jitter (62 ps), and the possibility of on-chip integration with a quantum emitter. In addition to performance characterization, we tested the detectors in real experimental conditions involving nanodiamond nitrogen-vacancy emitters enhanced by a hyperbolic metamaterial.