No Arabic abstract
We investigate the effect of intercombination transitions in excitation hopping processes such as those found in Forster resonance energy transfer. Taking strontium Rydberg states as our model system, the breakdown of $LS$-coupling leads to weakly allowed transitions between Rydberg states of different spin quantum number. We show that the long-range interactions between two Rydberg atoms can be affected by these weakly allowed spin transitions, and the effect is greatest when there is a near-degeneracy between the initial state and a state with a different spin quantum number. We also consider a case of four atoms in a spin chain, and show that a spin impurity can resonantly hop along the chain. By engineering the many-body energy levels of the spin-chain, the breakdown of $LS$ coupling due to inter-electronic effects in individual atoms can be mapped onto a spatial separation of the total spin and the total orbital angular momentum along the spin chain.
We investigate the quantum dynamics of energy and charge transfer in a wheel-shaped artificial photosynthetic antenna-reaction center complex.This complex consists of six light-harvesting chromophores and an electron-acceptor fullerene. To describe quantum effects on a femtosecond time scale, we derive the set of exact non-Markovian equations for the Heisenberg operators of this photosynthetic complex in contact with a Gaussian heat bath. With these equations we can analyze the regime of strong system-bath interactions, where reorganization energies are of the order of the intersite exciton couplings. We show that the energy of the initially-excited antenna chromophores is efficiently funneled to the porphyrin-fullerene reaction center, where a charge-separated state is set up in a few picoseconds, with a quantum yield of the order of 95%. In the single-exciton regime, with one antenna chromophore being initially excited, we observe quantum beatings of energy between two resonant antenna chromophores with a decoherence time of $sim$ 100 fs. We also analyze the double-exciton regime, when two porphyrin molecules involved in the reaction center are initially excited. In this regime we obtain pronounced quantum oscillations of the charge on the fullerene molecule with a decoherence time of about 20 fs (at liquid nitrogen temperatures). These results show a way to directly detect quantum effects in artificial photosynthetic systems.
We study resonant energy transfer in a one-dimensional chain of two to five atoms by analyzing time-dependent probabilities as function of their interatomic distances. The dynamics of the system are first investigated by including the nearest-neighbour interactions and then accounting for all next-neighbour interactions. We find that inclusion of nearest-neighbour interactions in the Hamiltonian for three atoms chain exhibits perdiocity during the energy transfer dynamics, however this behavior displays aperiodicity with the all-neighbour interactions. It shows for the equidistant chains of four and five atoms the peaks are always irregular but regular peaks are retrieved when the inner atoms are placed closer than the atoms at both the ends. In this arrangement, the energy transfer swings between the atoms at both ends with very low probability of finding an atom at the center. This phenomenon resembles with quantum notion of Newtons cradle. We also find out the maximum distance up to which energy could be transferred within the typical lifetimes of the Rydberg states.
We report the observation of a novel nonlinear effect in the hard x-ray range. Upon illuminating Fe and Cu metal foils with intense x-ray pulses tuned near their respective K edges, photons at nearly twice the incoming photon energy are emitted. The signal rises quadratically with the incoming intensity, consistent with two-photon excitation. The spectrum of emitted high-energy photons comprises multiple Raman lines that disperse with the incident photon energy. Upon reaching the double K-shell ionization threshold, the signal strength undergoes a marked rise. Above this threshold, the lines cease dispersing, turning into orescence lines with energies much greater than obtainable by single electron transitions, and additional Raman lines appear. We attribute these processes to electron-correlation mediated multielectron transitions involving double-core hole excitation and various two-electron de-excitation processes to a final state involving one or more L and M core-holes.
We present a spectroscopy scheme for the 7-kHz-wide 689-nm intercombination line of strontium. We rely on shelving detection, where electrons are first excited to a metastable state by the spectroscopy laser before their state is probed using the broad transition at 461 nm. As in the similar setting of calcium beam clocks, this enhances dramatically the signal strength as compared to direct saturated fluorescence or absorption spectroscopy of the narrow line. We implement shelving spectroscopy both in directed atomic beams and hot vapor cells with isotropic atomic velocities. We measure a fractional frequency instability $sim 2 times 10^{-12}$ at 1 s limited by technical noise - about one order of magnitude above shot noise limitations for our experimental parameters. Our work illustrates the robustness and flexibility of a scheme that can be very easily implemented in the reference cells or ovens of most existing strontium experiments, and may find applications for low-complexity clocks.
We consider hyperfine-mediated effects for clock transitions in $^{176}$Lu$^+$. Mixing of fine structure levels due to the hyperfine interaction bring about modifications to Lande $g$-factors and the quadrupole moment for a given state. Explicit expressions are derived for both $g$-factor and quadrupole corrections, for which leading order terms arise from the nuclear magnetic dipole coupling. High accuracy measurements of the $g$-factors for the $^1S_0$ and $^3D_1$ hyperfine levels are carried out, which provide an experimental determination of the leading order correction terms.