We introduce a new method, called entangled photon-pair two-dimensional fluorescence spectroscopy (EPP-2DFS), to sensitively probe the nonlinear electronic response of molecular systems. The method incorporates a separated two-photon ('Franson') interferometer, which generates time-frequency-entangled photon pairs, into the framework of a fluorescence-detected 2D optical spectroscopic experiment. The entangled photons are temporally shaped and phase-modulated in the interferometer, and are used to excite a two-photon-absorbing (TPA) sample, whose excited-state population is selectively detected by simultaneously monitoring the sample fluorescence and the exciting fields. In comparison to 'classical' 2DFS techniques, major advantages of this scheme are the suppression of uncorrelated background signals, the enhancement of simultaneous time-and-frequency resolution, the suppression of diagonal 2D spectral features, and the enhancement and narrowing of off-diagonal spectral cross-peaks that contain information about electronic couplings. These effects are a consequence of the pure-state field properties unique to a parametric down-conversion light source, which must be included in the quantum mechanical description of the composite field-molecule system. We numerically simulate the EPP-2DFS observable for the case of an electronically coupled molecular dimer. The EPP-2DFS spectrum is greatly simplified in comparison to its classical 2D counterpart. Our results indicate that EPP-2DFS can provide previously unattainable resolution to extract model Hamiltonian parameters from electronically coupled molecular dimers.

Interaction of spin and intrinsic orbital angular momentum of light is observed, as evidenced by length-dependent rotations of both spatial patterns and optical polarization in a cylindricallysymmetric isotropic optical fiber. Such rotations occur in straight few-mode fiber when superpositions of two modes with parallel and anti-parallel orientation of spin and intrinsic orbital angular momentum (IOAM=2 ) are excited, resulting from a degeneracy splitting of the propagation constants of the modes.

Sensing with optical whispering gallery modes (WGMs) is a rapidly developing detection method in modern microfluidics research. This method explores the perturbations of spectra of WGMs propagating along the wall of an optical microcapillary to characterize the liquid medium inside it. Here we show that WGMs in a silica microcapillary can be fully localized (rather than perturbed) by evanescent coupling to a water droplet and, thus, form a high quality-factor microresonator. The spectra of this resonator, measured with a microfiber translated along the capillary, present a hierarchy of resonances which allow us to determine the size of the droplet and variation of its length due to the evaporation. The resolution of our measurements of this variation equal to 4.5 nm is only limited by the resolution of the optical spectrum analyzer used. The discovered phenomenon of complete localization of light in liquid-filled optical microcapillaries suggests a new type of microfluidic photonic devices as well as an ultraprecise method for microfluidic characterization.

Coupling between optical microresonators and waveguides is a critical characteristic of resonant photonic devices that has complex behavior that is not well understood. When the characteristic variation length of the microresonator modes is much larger than the waveguide width, local coupling parameters emerge that are independent of the resonator mode distributions and offer a simplified description of coupling behavior. We develop a robust numerical-fitting-based methodology for experimental determination of the local coupling parameters in all coupling regimes and demonstrate their characterization along a microfiber waveguide coupled to an elongated bottle microresonator.

We present an experimental method for creating and verifying photon-number states created by non-degenerate, third-order nonlinear-optical photon-pair sources. By using spatially multiplexed, thresholding single-photon detectors and inverting a conditional probability matrix, we determine the photon-number probabilities created through heralded spontaneous four-wave-mixing. The deleterious effects of noise photons on reliable heralding are investigated and shown to degrade the conditional preparation of two-photon number states more than they degrade conditional single-photon states. We derive the equivalence between the presence of unwanted noise in the herald channel and loss in the signal channel of heralded experiments. A procedure for characterizing the noise-photon contributions, and a means of estimating the herald noise-free photon-number distribution is demonstrated.