Interferometric Imaging Using Shared Quantum Entanglement.

Quantum entanglement-based imaging promises significantly increased resolution by extending the spatial separation of optical collection apertures used in very-long-baseline interferometry for astronomy and geodesy. We report a tabletop entanglement-based interferometric imaging technique that utilizes two entangled field modes serving as a phase reference between two apertures. The spatial distribution of a simulated thermal light source is determined by interfering light collected at each aperture with one of the entangled fields and performing joint measurements. This experiment demonstrates the ability of entanglement to implement interferometric imaging.

Quantifying the enhancement of two-photon absorption due to spectral-temporal entanglement.

When a low flux of time-frequency-entangled photon pairs (EPP) illuminates a two-photon transition, the rate of two-photon absorption (TPA) can be enhanced considerably by the quantum nature of photon number correlations and frequency correlations. We use a quantum-theoretic derivation of entangled TPA (ETPA) and calculate an upper bound on the amount of quantum enhancement that is possible in such systems. The derived bounds indicate that in order to observe ETPA the experiments would need to operate at a combination of significantly higher rates of EPP illumination, molecular concentrations, and conventional TPA cross sections than are achieved in typical experiments.

Entangled two-photon absorption by atoms and molecules: A quantum optics tutorial.

Two-photon absorption (TPA) and other nonlinear interactions of molecules with time-frequency-entangled photon pairs have been predicted to display a variety of fascinating effects. Therefore, their potential use in practical quantum-enhanced molecular spectroscopy requires close examination. This Tutorial presents a detailed theoretical study of one- and two-photon absorption by molecules, focusing on how to treat the quantum nature of light. We review some basic quantum optics theory and then we review the density-matrix (Liouville) derivation of molecular optical response, emphasizing how to incorporate quantum states of light into the treatment. For illustration, we treat in detail the TPA of photon pairs created by spontaneous parametric down conversion, with an emphasis on how quantum light TPA differs from that with classical light. In particular, we treat the question of how much enhancement of the TPA rate can be achieved using entangled states. This Tutorial includes a review of known theoretical methods and results as well as some extensions, especially the comparison of TPA processes that occur via far-off-resonant intermediate states only and those that involve off-resonant intermediate states by virtue of dephasing processes. A brief discussion of the main challenges facing experimental studies of entangled two-photon absorption is also given.

Time-frequency optical filtering: efficiency vs. temporal-mode discrimination in incoherent and coherent implementations.

Time-frequency (TF) filtering of analog signals has played a crucial role in the development of radio-frequency communications and is currently being recognized as an essential capability for communications, both classical and quantum, in the optical frequency domain. How best to design optical time-frequency (TF) filters to pass a targeted temporal mode (TM), and to reject background (noise) photons in the TF detection window? The solution for 'coherent' TF filtering is known-the quantum pulse gate-whereas the conventional, more common method is implemented by a sequence of incoherent spectral filtering and temporal gating operations. To compare these two methods, we derive a general formalism for two-stage incoherent time-frequency filtering, finding expressions for signal pulse transmission efficiency, and for the ability to discriminate TMs, which allows the blocking of unwanted background light. We derive the tradeoff between efficiency and TM discrimination ability, and find a remarkably concise relation between these two quantities and the time-bandwidth product of the combined filters. We apply the formalism to two examples-rectangular filters or Gaussian filters-both of which have known orthogonal-function decompositions. The formalism can be applied to any state of light occupying the input temporal mode, e.g., 'classical' coherent-state signals or pulsed single-photon states of light. In contrast to the radio-frequency domain, where coherent detection is standard and one can use coherent matched filtering to reject noise, in the optical domain direct detection is optimal in a number of scenarios where the signal flux is extremely small. Our analysis shows how the insertion loss and SNR change when one uses incoherent optical filters to reject background noise, followed by direct detection, e.g. photon counting. We point out implications in classical and quantum optical communications. As an example, we study quantum key distribution, wherein strong rejection of background noise is necessary to maintain a high quality of entanglement, while high signal transmission is needed to ensure a useful key generation rate.

Fluorescence-detected Fourier transform electronic spectroscopy by phase-tagged photon counting.

Fluorescence-detected Fourier transform (FT) spectroscopy is a technique in which the relative paths of an optical interferometer are controlled to excite a material sample, and the ensuing fluorescence is detected as a function of the interferometer path delay and relative phase. A common approach to enhance the signal-to-noise ratio in these experiments is to apply a continuous phase sweep to the relative optical path, and to detect the resulting modulated fluorescence using a phase-sensitive lock-in amplifier. In many important situations, the fluorescence signal is too weak to be measured using a lock-in amplifier, so that photon counting techniques are preferred. Here we introduce an approach to low-signal fluorescence-detected FT spectroscopy, in which individual photon counts are assigned to a modulated interferometer phase ('phase-tagged photon counting,' or PTPC), and the resulting data are processed to construct optical spectra. We studied the fluorescence signals of a molecular sample excited resonantly by a pulsed coherent laser over a range of photon flux and visibility levels. We compare the performance of PTPC to standard lock-in detection methods and establish the range of signal parameters over which meaningful measurements can be carried out. We find that PTPC generally outperforms the lock-in detection method, with the dominant source of measurement uncertainty being associated with the statistics of the finite number of samples of the photon detection rate.

Photonic temporal-mode multiplexing by quantum frequency conversion in a dichroic-finesse cavity.

Photonic temporal modes (TMs) form a field-orthogonal basis set representing a continuous-variable degree of freedom that is in principle infinite dimensional, and create a promising resource for quantum information science and technology. The ideal quantum pulse gate (QPG) is a device that multiplexes and demultiplexes temporally orthogonal optical pulses that have the same carrier frequency, spatial mode, and polarization. The QPG is the chief enabling technology for usage of orthogonal temporal modes as a basis for high-dimensional quantum information storage and processing. The greatest hurdle for QPG implementation using nonlinear-optical, parametric processes with time-varying pump or control fields is the limitation on achievable temporal mode selectivity, defined as perfect TM discrimination combined with unity efficiency. We propose the use of pulsed nonlinear frequency conversion in an optical cavity having greatly different finesses for different frequencies to implement a nearly perfectly TM-selective QPG in a low-loss integrated-optics platform.

Temperature-dependent conformations of exciton-coupled Cy3 dimers in double-stranded DNA.

Understanding the properties of electronically interacting molecular chromophores, which involve internally coupled electronic-vibrational motions, is important to the spectroscopy of many biologically relevant systems. Here we apply linear absorption, circular dichroism, and two-dimensional fluorescence spectroscopy to study the polarized collective excitations of excitonically coupled cyanine dimers (Cy3)2 that are rigidly positioned within the opposing sugar-phosphate backbones of the double-stranded region of a double-stranded (ds)-single-stranded (ss) DNA fork construct. We show that the exciton-coupling strength of the (Cy3)2-DNA construct can be systematically varied with temperature below the ds-ss DNA denaturation transition. We interpret spectroscopic measurements in terms of the Holstein vibronic dimer model, from which we obtain information about the local conformation of the (Cy3)2 dimer, as well as the degree of static disorder experienced by the Cy3 monomer and the (Cy3)2 dimer probe locally within their respective DNA duplex environments. The properties of the (Cy3)2-DNA construct we determine suggest that it may be employed as a useful model system to test fundamental concepts of protein-DNA interactions and the role of electronic-vibrational coherence in electronic energy migration within exciton-coupled bio-molecular arrays.

Engineering temporal-mode-selective frequency conversion in nonlinear optical waveguides: from theory to experiment.

Quantum frequency conversion (FC) in nonlinear optical media is a powerful tool for temporal-mode selective manipulation of light. Recent attempts at achieving high mode selectivities and/or fidelities have had to resort to multi-dimensional optimization schemes to determine the system's natural Schmidt modes. Certain combinations of relative-group velocities between the relevant frequency bands, medium length, and temporal pulse widths have been known to achieve good selectivities (exceeding 80%) for temporal modes that are nearly identical to pump pulse shapes, even for high conversion efficiencies. Working in this parameter regime using an off-the-shelf, second-harmonic generation, MgO:PPLN waveguide, and with pulses on the order of 500 fs at wavelengths around 800 nm, we verify experimentally that model-predicted Schmidt modes provide the high temporal-mode selectivity expected. The good agreement between experiment and theory paves the way to the implementation of a proposed two-stage FC scheme that is predicted by the present theory to reach near-perfect (100%) selectivity.

Observation of Interaction of Spin and Intrinsic Orbital Angular Momentum of Light.

The 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 cylindrically symmetric isotropic optical fiber. Such rotations occur in a straight few-mode fiber when superpositions of two modes with parallel and antiparallel orientation of spin and intrinsic orbital angular momentum (IOAM=2ℏ) are excited, resulting from a degeneracy splitting of the propagation constants of the modes.

Four-wave-mixing cascades near the zero-dispersion frequency.

Exact formulas are obtained for the amplitudes of light waves involved in four-wave-mixing cascades near the zero-dispersion frequency of a fiber. The cascade that is initiated by two strong pump waves is phase insensitive, whereas the cascade that is initiated by two strong pump waves and a weak signal wave is phase sensitive. In both cascades, the number of waves that have significant power increases with distance.