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We demonstrate fiber-optic magnetometry using a random ensemble of nitrogen-vacancy (NV) centers in nanodiamond coupled to a tapered optical fiber, which provides a waveguide delivery of optical fields for the initialization, polarization, and readout of the electron spin in NV centers.

The trajectory surface hopping method for quantum dynamics is reformulated in the space of many-particle states to include entanglement and correlation of trajectories. Used to describe many-body correlation effects in electronic structure theories, second quantization is applied to semiclassical trajectories. The new method allows coupling between individual trajectories via energy flow and common phase evolution. It captures the properties of a wave packet, such as branching, Heisenberg uncertainty, and decoherence. Applied to a superexchange process, the method shows very accurate results, comparable to exact quantum data and improving greatly on the standard approach.

Spectra of saturated absorption of Sm atomic vapor from the ground state 7 F 0 and the first even metastable level 7 F 1, e′=292.58 cm−1 of the 4f 66s 2 configuration to the odd level 4f 6(7 F)6s6p(3 P o)9 F 1 o , e,=14863.85 cm−1 were recorded. The lines of the isotopic series were identified, and the hyperfine structure of lines in the spectra of isotopes with a nonzero nuclear spin was determined. The relative isotopic shifts and the hyperfine splitting of the even level 4f 66s 2(7 F 1) were determined.

Resonances of coherent population trapping were detected in atomic vapours of the rare-earth element samarium. The coherent population trapping was produced by two external-cavity diode lasers (672 and 686 nm) in a Λ-system formed by the three levels of 154Sm: the 4f66s2(7F0) ground state, the first fine-structure 4f66s2(7F1) sublevel of the ground state and the 4f6(7F)6s6p(3Po)9Fo1 upper level. The dependence of the spectral shapes and resonance contrasts on the polarisation of the laser beams and the direction of the applied magnetic field was studied. The obtained results were analysed.

We describe a new implementation of the molecular dynamics method aimed at simulation of the properties of biomolecular systems in which chemical reactions are possible. The quantum mechanical/molecular mechanical method based on the effective fragment potential theory is used for calculating the energies and forces along trajectories. Due to specific features of the effective fragment theory, the behavior of the molecular mechanical subsystem is described by rigid body dynamics. The method has been applied to simulation of proton transfer along the chain of water molecules inside the gramicidin channel.

Charge carrier multiplication in organic heterojunction systems, a process known as singlet fission (SF), holds promise for development of solar cells with enhanced photon-to-electron yields, and therefore it is of substantial fundamental interest. The efficiency of photovoltaic devices based on this principle is determined by complex dynamics involving key electronic states coupled to particular nuclear motions. Extensive experimental and theoretical studies are dedicated to this topic, generating multiple opinions on the nature of such states and motions, their properties, and mechanisms of the competing processes, including electron-phonon relaxation, SF, and charge separation. Using nonadiabatic molecular dynamics, we identify the key steps and mechanisms involved in the SF and subsequent charge separation, and build a comprehensive kinetic scheme that is consistent with the existing experimental and theoretical results. The ensuing model provides time scales that are in excellent agreement with the experimental observations. We demonstrate that SF competes with the traditional photoinduced electron transfer between pentacene and C60. Efficient SF relies on the presence of intermediate dark states within the pentacene subsystem. Having multiexciton and charge transfer character, these states play critical roles in the dynamics, and should be considered explicitly when explaining the entire process from the photoexcitation to the final charge separation.

We experimentally demonstrate both the lifetime reduction and the enhancement of single-photon emission from nitrogen-vacancies in nanodiamonds coupled to a TiN/Al0.6Sc0.4N superlattice. Our results pave the way towards future CMOS-compatible integrated quantum sources.

We report on accurate measurements of the scalar and tensor polarizabilities of the 5D fine structure levels 5D3/2 and 5D5/2 in Rb. The measured values show reasonable correspondence to previously published theoretical predictions, but are more accurate. We implemented laser excitation of the 5D level in a laser cooled cloud of optically polarized Rb-87 atoms placed in a constant electric field., 8 pages, 9 figures

The quantized Hamiltonian dynamics (QHD) theory provides a hierarchy of approximations to quantum dynamics in the Heisenberg representation. We apply the first-order QHD to study charge transport in molecular crystals and find that the obtained equations of motion coincide with the Ehrenfest theory, which is the most widely used mixed quantum-classical approach. Quantum initial conditions required for the QHD variables make the dynamics surpass Ehrenfest. Most importantly, the first-order QHD already captures the low-temperature regime of charge transport, as observed experimentally. We expect that simple extensions to higher-order QHDs can efficiently represent other quantum effects, such as phonon zero-point energy and loss of coherence in the electronic subsystem caused by phonons.

We demonstrate an all-optical method for magnetic sensing of individual molecules in ambient conditions at room temperature. Our approach is based on shallow nitrogen-vacancy (NV) centers near the surface of a diamond crystal, which we use to detect single paramagnetic molecules covalently attached to the diamond surface. The manipulation and readout of the NV centers is all-optical and provides a sensitive probe of the magnetic field fluctuations stemming from the dynamics of the electronic spins of the attached molecules. As a specific example, we demonstrate detection of a single paramagnetic molecule containing a gadolinium (Gd$^{3+}$) ion. We confirm single-molecule resolution using optical fluorescence and atomic force microscopy to co-localize one NV center and one Gd$^{3+}$-containing molecule. Possible applications include nanoscale and in vivo magnetic spectroscopy and imaging of individual molecules.

Review: emphasis on processes that are essential in terms of photovoltaic and photocatlytic cells; 655 refs.

Photochemical water splitting is a promising avenue to sustainable, clean energy and fuel production. Gallium nitride (GaN) and its solid solutions are excellent photocatalytic materials; however, the efficiency of the process is low on pure GaN, and cocatalysts are required to increase the yields. We present the first time-domain theoretical study of the initial steps of photocatalytic water splitting on a GaN surface. Our state-of-the-art simulation technique, combining nonadiabatic molecular dynamics and time-dependent density functional theory, allows us to characterize the mechanisms and time scales of the evolution of the photogenerated positive charge (hole) and the subsequent proton transfer at the GaN/water interface. The calculations show that the hole loses its excess energy within 100 fs and localizes primarily on the nitrogen atoms of the GaN surface, initiating a sequence of proton-transfer events from the surface N-H group to the nearby OH groups and bulk water molecules. Water splitting requires hole localization on oxygen rather than nitrogen, necessitating nonadiabatic transitions uphill in energy on pure GaN. Such transitions happen rarely, resulting in low yields of the photocatalytic water splitting observed experimentally. We conclude that efficient cocatalysts should favor localization of the photogenerated hole on oxygen-containing species at the semiconductor/water interface.

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.

We propose a numerical algorithm for calculation of quantized directed motion of a stochastic system of interacting particles induced by periodic changes of control parameters on the graph of microstates. As a main application, we consider models of catenane molecular motors, which demonstrated the possibility of a similar control of directed motion of molecular components. We show that our algorithm allows one to calculate the motion of a system in the space of its microstates even when the considered phase space is combinatorially large (~1 × 10(6) microscopic states). Several general observations are made about the structure of the phase diagram of the systems studied, which may be used for rational design and efficient control of new generations of molecular motors.

We propose and demonstrate a new approach for achieving strong light-matter interactions with quantum emitters. Our approach makes use of a plasmon resonator composed of defect-free, highly crystalline silver nanowires surrounded by patterned dielectric distributed Bragg reflectors (DBRs). These resonators have an effective mode volume (Veff) two orders of magnitude below the diffraction limit and quality factor (Q) approaching 100, enabling enhancement of spontaneous emission rates by a factor exceeding 75 at the cavity resonance. We also show that these resonators can be used to convert a broadband quantum emitter to a narrowband single-photon source with color-selective emission enhancement.

We propose a numerical approach to quantify the control of a nonautonomous molecular rotor motion. Unlike straightforward molecular dynamics simulations in an explicitly time-dependent framework, our method is based on the theory of geometric phases. This theory allows us to define a sensitivity field (SF) in control parameter space that characterizes average motion of a molecule induced by a cyclic perturbation. We show that the SF can be obtained using only equilibrium free energy sampling techniques. A density plot of the SF quantifies response of a molecule to an arbitrary cyclic adiabatic evolution of parameters. For demonstration, we numerically find the SFs for two surface mounted molecular rotor molecules that can be driven, in practice, by strong time-dependent electric fields of a STM tip.

Rotating surface-mounted molecules have attracted attention of many research groups as a way to develop new nanoscale devices and materials. However, mechanisms of motion of these rotors at the single-molecule level are still not well understood. Theoretical and experimental studies on thioether molecular rotors on gold surfaces suggest that the size of the molecules, their flexibility and steric repulsions with the surface are important for dynamics of the system. A complex combination of these factors leads to the observation that the rotation speeds have not been hindered by increasing the length of the alkyl chains. However, experiments on diferrocene derivatives indicated that a significant increase in the rotational barriers for longer molecules. We present here a comprehensive theoretical study that combines molecular dynamics simulations and simple models to investigate what factors influence single-molecule rotations on the surfaces. Our results suggest that rotational dynamics is determined by the size and by the symmetry of the molecules and surfaces, and by interactions with surfaces. Our theoretical predictions are in excellent agreement with current experimental observations.

We have experimentally studied sub-Doppler laser cooling in a magneto-optical trap for thulium atoms working at the wavelength of 410.6\,nm. Without any dedicated molasses period of sub-Doppler cooling, the cloud of $3\times 10^6$ atoms at the temperature of 25(5)\,$\mu$K was observed. The measured temperature is significantly lower than the Doppler limit of 240$\mu$K for the cooling transition at 410.6\,nm. High efficiency of the sub-Doppler cooling process is due to a near-degeneracy of the Land\'e-$g$ factors of the lower $4f^{13}6s^{2}\, (J\,=\,{7}/{2})$ and the upper $4f^{12}5d_{3/2}6s^{2}\, (J\,=\,{9}/{2})$ cooling levels.}, Comment: 4 pages, 4 figures

We demonstrate supersymmetry in the counting statistics of stochastic particle currents and use it to derive exact nonperturbative relations for the statistics of currents induced by arbitrarily fast time-dependent protocols., 4 pages, 2 figures

Thulium atoms are trapped in a magneto-optical trap using a strong transition at 410 nm with a small branching ratio. We trap up to $7\times10^{4}$ atoms at a temperature of 0.8(2) mK after deceleration in a 40 cm long Zeeman slower. Optical leaks from the cooling cycle influence the lifetime of atoms in the MOT which varies between 0.3 -1.5 s in our experiments. The lower limit for the leaking rate from the upper cooling level is measured to be 22(6) s$^{-1}$. The repumping laser transferring the atomic population out of the F=3 hyperfine ground-state sublevel gives a 30% increase for the lifetime and the number of atoms in the trap., Comment: 4 pages, 6 figures

The results of frequency-modulation (FM) spectroscopy of coherent dark resonances from the Zeeman sublevelsof the transition F =2 $ F =1 of D 1 line in absorption of 87 Rb atoms are presented and discussed in detail.By contrast with the conventional spectroscopy of coherent dark resonances employing two laser beams, relativefrequency of which can be varied, these data has been obtained with the help of a single frequency-modulatedlaser ¯eld. Variation of the modulation frequency plays then similar role with variation the relative frequencyin conventional spectroscopy. Experimental data are ¯t to the theoretical calculations, which are based onthe theory of FM spectroscopy of coherent dark resonances recently developed by us. Feasibility of using suchexperimental technique for accurate measurements of magnetic ¯elds is also discussed.Keywords: Coherent population trapping, absorption, dark resonance, magnetometry, metrology 1. INTRODUCTION The coherent population trapping (CPT) is one of the most intriguing quantum interference phenomena thatcan be most vividly seen in a three-level system in ¤-con¯guration. In this system, if two monochromaticpumping ¯elds are tuned into the resonance with the respective transitions, all the population is captured in thecoherent superposition of two low-lying levels, which gives the name of the phenomenon|coherent populationtrapping [1]. This means that the media of such three-level atoms under CPT will not emit °uorescence and donot absorb photons. In absorption spectra it is revealed as a narrow sharp dip in the absorption pro¯le whilescanning frequency of one of the pumping laser ¯elds. These resonances are called the coherent dark resonances.Due to the rather small spectral width of the dark resonances they found applications in precision spectroscopicapplications, such as metrology

We demonstrate laser slowing of a hot thulium atomic beam using the nearly closed cycling transition $4\textrm{f}^{13}6\textrm{s}^2(^2\textrm{F}^\circ)(J=7/2)\leftrightarrow4\textrm{f}^{12}(^3\textrm{H}_5)5\textrm{d}_{3/2}6\textrm{s}^2(J=9/2)$ at 410.6 nm. Atoms are decelerated to velocities around 25 m/s by a 40 cm Zeeman slower. The flux of slowed atoms is evaluated as $10^7 \textrm{s}^{-1}\textrm{cm}^{-2}$. The experiment explicitly indicates the possibility of trapping Tm atoms in a magneto-optical trap., Comment: 3 pages, 4 figures

We discuss recent experiments involving a new, broadband approach for engineering photon-emitter interactions via subwavelength confinement of guided optical fields in metallic nanowires [1–2]. The tight confinement of guided excitations in these nanostructures, known as surface plasmons [3–5], results in large interactions between single photons and single optical emitters without the use of a cavity, which can further be manipulated using quantum optical techniques.

Control over the interaction between single photons and individual optical emitters is an outstanding problem in quantum science and engineering. It is of interest for ultimate control over light quanta, as well as for potential applications such as efficient photon collection, single-photon switching and transistors, and long-range optical coupling of quantum bits. Recently, substantial advances have been made towards these goals, based on modifying photon fields around an emitter using high-finesse optical cavities. Here we demonstrate a cavity-free, broadband approach for engineering photon-emitter interactions via subwavelength confinement of optical fields near metallic nanostructures. When a single CdSe quantum dot is optically excited in close proximity to a silver nanowire, emission from the quantum dot couples directly to guided surface plasmons in the nanowire, causing the wire's ends to light up. Non-classical photon correlations between the emission from the quantum dot and the ends of the nanowire demonstrate that the latter stems from the generation of single, quantized plasmons. Results from a large number of devices show that efficient coupling is accompanied by more than 2.5-fold enhancement of the quantum dot spontaneous emission, in good agreement with theoretical predictions.

We have studied possible candidates for laser cooling transitions in $^{169}$Tm in the spectral region 410 -- 420 nm. By means of saturation absorption spectroscopy we have measured the hyperfine structure and rates of two nearly closed cycling transitions from the ground state $4\textrm{f}^{13}6\textrm{s}^2(^2\textrm{F}_0)(J_g=7/2)$ to upper states $4\textrm{f}^{12}(^3\textrm{H}_5)5\textrm{d}_{3/2}6\textrm{s}^2(J_e=9/2)$ at 410.6 nm and $4\textrm{f}^{12}(^3\textrm{F}_4)5\textrm{d}_{5/2}6\textrm{s}^2(J_e=9/2)$ at 420.4 nm and evaluated the life times of the excited levels as 15.9(8) ns and 48(6) ns respectively. Decay rates from these levels to neighboring opposite-parity levels are evaluated by means of Hartree-Fock calculations. We conclude, that the strong transition at 410.6 nm has an optical leak rate of less then $2\cdot10^{-5}$ and can be used for efficient laser cooling of $^{169}$Tm from a thermal atomic beam. The hyperfine structure of two other even-parity levels which can be excited from the ground state at 409.5 nm and 418.9 nm is also measured by the same technique. In addition we give a calculated value of $7(2)$ s$^{-1}$ for the rate of magnetic-dipole transition at 1.14 $\mu$m between the fine structure levels $(J_g=7/2)\leftrightarrow(J'_g=5/2)$ of the ground state which can be considered as a candidate for applications in atomic clocks., Comment: 8 pages, 5 figures

We analyze the applicability of the seminal fewest switches surface hopping (FSSH) method of Tully to modeling quantum transitions between electronic states that are not coupled directly, in the processes such as Auger recombination. We address the known deficiency of the method to describe such transitions by introducing an alternative definition for the surface hopping probabilities, as derived from the Markov state model perspective. We show that the resulting transition probabilities simplify to the quantum state populations derived from the time-dependent Schrodinger equation, reducing to the rapidly switching surface hopping approach of Tully and Preston. The resulting surface hopping scheme is simple and appeals to the fundamentals of quantum mechanics. The computational approach is similar to the FSSH method of Tully, yet it leads to a notably different performance. We demonstrate that the method is particularly accurate when applied to superexchange modeling. We further show improved accuracy of ...

We report on accurate measurements of the scalar αS and tensor αT polarizabilities of the 5D fine structure levels 5D3/2 and 5D5/2 in Rb.

We report the observation of influence of homogeneous magnetic field on an optical lattice losses of ultracold thulium atoms. The atomic cloud temperature was T = 15 mK. The dependence of trap population on a value of magnetic field has a broad resonance in the low-field region with a center at B = 0.4 G. We also have measured a decrease of optical lattice lifetime in a presence of resonance magnetic field. The observed magnetically-induced trap losses are assumed to be Feshbach resonance which is a dependence of an atomic scattering length on magnetic field.

A theoretical model of the coherent population trapping (CPT) in multilevel samarium atom and its comparison with experimental spectroscopic data are presented. Theoretical model describes a degenerated (Lambda) -system in Sm atom formed of the transitions 4f66s2(7F0) mutually implies 4f6(7F)6s6p(3Po)9Fo1 mutually implies 4f66s2(7F1) and includes also a fourth level 4f66s2(7F2), which complements the model making it an open system. An open character of the system reduces the contrast of the resonance curves in the CPT- spectra, but does not change the width of the CPT resonance. Numerical modeling of the CPT resonances in Sm atom was carried out for the case of applied longitudinal and transverse magnetic fields in 7- and 12-level models, as well.

We propose to use the magnetic-dipole transition at λ = 1.14 μm coupling two ground state fine-structure components of thulium (Tm), as a 'clock transition' in optical clocks. We have demonstrated first stage laser cooling of Tm atoms down to a temperature of 25 μK using a strong transition at λ = 410.6 nm and we have also shown preliminary results for second stage cooling using a weaker transition at λ = 530.7 nm (natural linewidth γG = 350 kHz). Laser cooled atoms have been trapped in an optical dipole trap and in a 1D optical lattice operating near 532 nm.

We present a formulation of quantized Hamiltonian dynamics (QHD) using variables that arise naturally from the Heisenberg equation of motion. The QHD equations are obtained and solved either directly in terms of these generalized variables, or by employing a wavefunction ansatz. The approach avoids a Taylor expansion and other approximations to the potential, leading to more stable dynamics and a higher precision of the calculated quantities. The proposed formulation is also amenable to for analytic and numerical implementations, thus facilitating its use in molecular dynamics simulation.

We studied light-assisted collisions of Tm atoms in a magneto-optical trap (MOT), working on a weak cooling transition at 530.7 nm [$4{f}^{13}(^{2}F^{o})6{s}^{2},\phantom{\rule{0.16em}{0ex}}J=7/2,\phantom{\rule{0.16em}{0ex}}F=4$ to $4{f}^{12}(^{3}H_{6})5{d}_{5/2}6{s}^{2},\phantom{\rule{0.16em}{0ex}}J=9/2,\phantom{\rule{0.16em}{0ex}}F=5$]. We observed a strong influence from radiation trapping and light-assisted collisions on the dynamics of this trap. We carefully separated these two contributions and measured the binary loss rate constant at different laser powers and detuning frequencies near the cooling transition. Analyzing losses from the MOT, we found the light-assisted inelastic binary loss rate constant to reach values of up to $\ensuremath{\beta}={10}^{\ensuremath{-}9}\phantom{\rule{0.16em}{0ex}}\mathrm{c}{\mathrm{m}}^{3}/\mathrm{s}$ and gave the upper bound on a branching ratio $kl0.8\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}6}$ for the 530.7 nm transition.

Photonic circuits can be much faster than their electronic counterparts, but they are difficult to miniaturize below the optical wavelength scale. Nanoscale photonic circuits based on surface plasmon polaritons (SPs) are a promising solution to this problem because they can localize light below the diffraction limit. However, there is a general tradeoff between the localization of an SP and the efficiency with which it can be detected with conventional far-field optics. Here we describe a new all-electrical SP detection technique based on the near-field coupling between guided plasmons and a nanowire field-effect transistor. We use the technique to electrically detect the plasmon emission from an individual colloidal quantum dot coupled to an SP waveguide. Our detectors are both nanoscale and highly efficient (0.1 electrons/plasmon), and a plasmonic gating effect can be used to amplify the signal even higher (up to 50 electrons/plasmon). These results enable new on-chip optical sensing applications and are a key step towards "dark" optoplasmonic nanocircuits in which SPs can be generated, manipulated, and detected without involving far-field radiation., manuscript followed by supplementary information

In this paper, we experimentally investigate optical and spin properties of NV centers in aggregates of detonation nanodiamonds. We show that despite the small size of nanodiamonds forming the aggregate, the NV centers in these aggregates exhibit spin properties comparable to similar size nanodiamonds grown by other methods, but with brightness enhanced by a factor of 2.