Single molecule photon counting statistics for quantum mechanical chromophore dynamics

We extend the generating function technique for calculation of single molecule photon emission statistics [Y. Zheng and F. L. H. Brown, Phys. Rev. Lett., 90,238305 (2003)] to systems governed by multi-level quantum dynamics. This opens up the possibility to study phenomena that are outside the realm of purely stochastic and mixed quantum-stochastic models. In particular, the present methodology allows for calculation of photon statistics that are spectrally resolved and subject to quantum coherence. Several model calculations illustrate the generality of the technique and highlight quantitative and qualitative differences between quantum mechanical models and related stochastic approximations. Calculations suggest that studying photon statistics as a function of photon frequency has the potential to reveal more about system dynamics than the usual broadband detection schemes.Comment: Submitted to the Journal of Physical Chemistr

The Efimov effect for three interacting bosonic dipoles

Three oriented bosonic dipoles are treated using the hyperspherical adiabatic representation, providing numerical evidence that the Efimov effect persists near a two-dipole resonance and in a system where angular momentum is not conserved. Our results further show that the Efimov features in scattering observables become universal, with a known three-body parameter, i.e. the resonance energies depend only on the two-body physics, which also has implications for the universal spectrum of the four-dipole problem. Moreover, the Efimov states should be long-lived, which is favorable for their creation and manipulation in ultracold dipolar gases. Finally, deeply-bound two-dipole states are shown to be relatively stable against collisions with a third dipole, owing to the emergence of a repulsive interaction originating in the angular momentum nonconservation for this system.Comment: 4 pages, 2 figures, 1 tabl

Prediction of the Size Distributions of Methanol-Ethanol Clusters Detected in VUV Laser/Time-of-flight Mass Spectrometry

The size distributions and geometries of vapor clusters equilibrated with methanol−ethanol (Me−Et) liquid mixtures were recently studied by vacuum ultraviolet (VUV) laser time-of-flight (TOF) mass spectrometry and density functional theory (DFT) calculations (Liu, Y.; Consta, S.; Ogeer, F.; Shi, Y. J.; Lipson, R. H. Can. J. Chem. 2007, 85, 843−852). On the basis of the mass spectra recorded, it was concluded that the formation of neutral tetramers is particularly prominent. Here we develop grand canonical Monte Carlo (GCMC) and molecular dynamics (MD) frameworks to compute cluster size distributions in vapor mixtures that allow a direct comparison with experimental mass spectra. Using the all-atom optimized potential for liquid simulations (OPLS-AA) force field, we systematically examined the neutral cluster size distributions as functions of pressure and temperature. These neutral cluster distributions were then used to derive ionized cluster distributions to compare directly with the experiments. The simulations suggest that supersaturation at 12 to 16 times the equilibrium vapor pressure at 298 K or supercooling at temperature 240 to 260 K at the equilibrium vapor pressure can lead to the relatively abundant tetramer population observed in the experiments. Our simulations capture the most distinct features observed in the experimental TOF mass spectra: Et3H+ at m/z = 139 in the vapor corresponding to 10:90% Me−Et liquid mixture and Me3H+ at m/z = 97 in the vapors corresponding to 50:50% and 90:10% Me−Et liquid mixtures. The hybrid GCMC scheme developed in this work extends the capability of studying the size distributions of neat clusters to mixed species and provides a useful tool for studying environmentally important systems such as atmospheric aerosols

Universal three-body physics for fermionic dipoles

A study of the universal physics for three oriented fermionic dipoles in the hyperspherical adiabatic representation predicts a single long-lived three-dipole state, which exists in only one three-body symmetry, should form near a two-dipole resonance. Our analysis reveals the spatial configuration of the universal state, and the scaling of its binding energy and lifetime with the strength of the dipolar interaction. In addition, three-body recombination of fermionic dipoles is found to be important even at ultracold energies. An additional finding is that an effective long-range repulsion arises between a dipole and a dipolar dimer that is tunable via dipolar interactions.Comment: 4 pages, 3 figures, 1 tabl

Berry phase manipulation in ultrathin SrRuO3_3 films

A notion of the Berry phase is a powerful means to unravel the non-trivial role of topology in various novel phenomena observed in chiral magnetic materials and structures. A celebrated example is the intrinsic anomalous Hall effect (AHE) driven by the non-vanishing Berry phase in the momentum space. As the AHE is highly dependent on details of the band structure near the Fermi edge, the Berry phase and AHE can be altered in thin films whose chemical potential is tunable by dimensionality and disorder. Here, we demonstrate that in ultrathin SrRuO$_3$ films the Berry phase can be effectively manipulated by the effects of disorder on the intrinsic Berry phase contribution to the AHE, which is corroborated by our numerically exact calculations. In addition, our findings provide ample experimental evidence for the superficial nature of the topological Hall effect attribution to the protected spin texture and instead lend strong support to the multi-channel AHE scenario in ultrathin SrRuO$_3$