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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.

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.

We present a theoretical proof that the “quantum enhancement” of two-photon absorption, thought to be a means to improve molecular spectroscopy and imaging, is tightly bounded by the physics of photonic entanglement and nonlinear response.

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.