The quantum correlation of octave-spanning time–energy entangled bi-photons can be as short as a single optical cycle. Many experiments designed to explore and exploit this correlation require a uniform spectral phase (transform-limited) with very low loss. So far, transform-limited single-cycle bi-photons have not been demonstrated, primarily due to the lack of precise, broadband control of their spectral phase. Here, we demonstrate the correction of the spectral-phase of near-octave spanning bi-photons to over an octave in frequency –2600 nm). Using a prism-pair with an effectively negative separation for shaping the bi-photons' spectral phase, we obtain a tuned, very low-loss compensation of both the second and fourth dispersion orders. An essential requisite for precise tuning over such a broad bandwidth is a measure of the spectral phase that provides feedback for the tuning even when the overall dispersion is far from compensated. This is achieved by a non-classical bi-photon interference, which enables direct verification of the corrected bi-photon spectral phase.
The quantum correlation of octave-spanning time–energy entangled bi-photons can be as short as a single optical cycle. Many experiments designed to explore and exploit this correlation require a uniform spectral phase (transform-limited) with very low loss. So far, transform-limited single-cycle bi-photons have not been demonstrated, primarily due to the lack of precise, broadband control of their spectral phase. Here, we demonstrate the correction of the spectral-phase of near-octave spanning bi-photons to over an octave in frequency –2600 nm). Using a prism-pair with an effectively negative separation for shaping the bi-photons' spectral phase, we obtain a tuned, very low-loss compensation of both the second and fourth dispersion orders. An essential requisite for precise tuning over such a broad bandwidth is a measure of the spectral phase that provides feedback for the tuning even when the overall dispersion is far from compensated. This is achieved by a non-classical bi-photon interference, which enables direct verification of the corrected bi-photon spectral phase.
We demonstrate low-loss broadband tuned compensation of both the 2nd and 4th order dispersion of ultra-broad bi-photons, using a prism-pair with negative separation. The corrected spectral phase (<π/20) of the bi-photons spans nearly an octave in frequency (≈1330−2600 nm), as measured directly by a non-classical bi-photon interference effect. Due to the ultra-broad bandwidth, an ultra-high flux of bi-photons is available for quantum information experiments with extremely pronounced quantum correlations in both time and phase. Most experiments that explore these correlations require transform limited bi-photons, which are now achievable most efficiently with the prism-pair configuration.
Entangled photon spectroscopy is a nascent field that has important implications for measurement and imaging across chemical, biology, and materials fields. Entangled photon spectroscopy potentially offers improved spatial and temporal-frequency resolutions, increased cross sections for multiphoton and nonlinear measurements, and new abilities in inducing or measuring quantum correlations. A critical step in enabling entangled photon spectroscopies is the creation of high-flux entangled sources that can use conventional detectors as well as provide redundancy for the losses in realistic samples. Here, we report a periodically poled, chirped, lithium tantalate platform that generates entangled photon pairs with ∼10−7 efficiency. For a near watt level diode laser, this results in a near μW-level flux. The single photon per mode limit that is necessary to maintain non-classical photon behavior is still satisfied by distributing this power over up to an octave-spanning bandwidth. The spectral–temporal photon correlations are observed via a Michelson-type interferometer that measures the broadband Hong–Ou–Mandel two-photon interference. A coherence time of 245 fs for a 10 nm bandwidth in the collinear case and a coherence time of 62 fs for a 125 nm bandwidth in the non-collinear case are measured using a CW pump laser and, essentially, collecting the full photon cone. We outline in detail the numerical methods used for designing and tailoring the entangled photons source, such as changing center wavelength or bandwidth, with the ultimate aim of increasing the availability of high-flux UV–Vis entangled photon sources in the optical spectroscopy community.
Time-frequency entangled photons ("biphotons") exhibit joint spectral and temporal correlations that are unattainable with classical light. Besides being deployed for tests of quantum nonlocality, these photonic states are desirable for a unique range of applications that can significantly impact communications and computation. In this dissertation, we describe novel schemes based on spectral and temporal domain processing for manipulating and characterizing broadband biphotons. Implementing frequency-dependent filters, first, we present and demonstrate a technique for controlling the relative delay between a pair of entangled photons, relying on pump frequency tuning and the quantum concept of nonlocal dispersion cancellation. Next, we demonstrate near-field frequency-to-time mapping, a technique adopted from classical photonics, for arbitrary control of biphoton temporal correlations. Subsequently, we generate temporal correlation trains by creating biphoton frequency combs through programmable spectral amplitude shaping and demonstrate the temporal Talbot effect with entangled photons for the first time. Moreover, in the absence of fast single-photon detectors, we show how electro-optic phase modulation (originally a time-dependent operation) can be used to examine the coherence of biphoton frequency combs. Lastly, we introduce a scheme based on electro-optic intensity modulation, another time-domain operation, for improving the resolution in biphoton temporal correlation measurements. Overall, our body of work could provide additional insight into the manipulation and characterization of biphoton states, as well as contribute towards the improvement of quantum technologies.
Single photons provide a natural platform for quantum communication and quantum networking, as they can be entangled in many degrees of freedom and maintain coherence over long-distance links. However, while their minimal interactions with the environment isolate them from detrimental noise, it can make them difficult to measure and manipulate. In particular, manipulation on the ultrafast timescale is necessary to fully exploit the energy-time (or spectral) photonic degree of freedom. Full control over the spectral properties of single photons is key to many quantum technologies and opens the door to natural high-dimensional quantum encodings. \n \nIn this thesis, we theoretically and experimentally examine the use of nonlinear optical processes mediated by strong laser pulses as a method to control the spectral properties of ultrafast single photons. By mixing single-photon pulses with strong escort pulses that have been shaped through dispersion in a nonlinear crystal, the shape of the escort is imprinted on the photon, resulting in a custom-tailored upconverted pulse. We theoretically examine this process for quadratic spectral phases and show that it has the potential to be simultaneously effective and efficient for the customization of single-photon spectral waveforms, and can be performed in an entanglement-conserving manner. \n \nWe then experimentally demonstrate the range of this technique through three applications. First, we show that sum-frequency generation with shaped pulses can be used to coherently measure time-bin encoded photons with bin separations on the order of picoseconds, well below the timing resolution of our detectors. Secondly, we show that this technique can be adapted to convert a train of pulses to a frequency comb, which can be read out in a straightforward manner using diffraction-based spectrometry. We also show here that this process can be performed in a polarization-maintaining fashion, and demonstrate that entanglement with a partner photon is conserved with high fidelity. Finally, we show that this process can be viewed as a time lens, which modulates a temporal waveform in an analogous fashion to a lens focusing a beam of light. We apply the time lens to a photon from an energy-time entangled pair, and show negative magnification of the joint spectrum through a reversal of the spectral correlations. Such processes could find application in quantum state engineering and high-speed single-photon measurement.
The visibility of nonlinear SU(1,1) interference directly reflects the nonclassical properties of entangled bi-photons and squeezed light with practically unlimited bandwidth, high efficiency and ultra-high photon flux, orders of magnitude beyond the abilities of standard photo-detectors. We study experimentally the dependence of the SU(1,1) visibility on the phase matching conditions and beam parameters in a free-space configuration, and show that maximal SU(1,1) visibility requires extreme collinear conditions, which deviate from the conditions for maximal nonlinear conversion. We demonstrate near-ideal visibility of ∼95% (limited only by internal loss) in an ultra-broadband SU(1,1), interferometer with over 120 THz of squeezed light bandwidth. Utilizing this analysis we demonstrate efficient detection of the spectral phase of single-cycle bi-photons and precise compensation of the dispersion over a full octave of bandwidth.
We demonstrate a technique that allows full control of the bandwidth of entangled photons independently of the frequency band of interest and of the nonlinear crystal. We theoretically show that this technique allows generating nearly transform-limited biphotons with almost one octave of bandwidth (hundreds of terahertz) which corresponds to correlation times of just a few femtoseconds. The presented method becomes an enabling tool for attosecond entangled-photons quantum optics. The technique can also be used to generate paired photons with a very high degree of entanglement.