The nonclassical light sources, such as frequency-time entangled photons, are anticipated to offer significant benefits for emerging quantum optical sensing or spectroscopic measurements and manifest on ultrafast time scales (sub-ps to fs). However, the constrained time resolution (ns to ps) of photon-counting detectors poses challenges in comprehensively characterizing their detailed properties on ultrafast time scales. Therefore, we present a novel asynchronous optical sampling (ASOPS) technique utilizing two-color optical frequency combs to demonstrate highly precise and sensitive ultrafast time-resolved cross-correlation measurements at the single-photon level. By employing photon counting statistics, this method successfully reconstructed the picosecond pulse width cross-correlation waveforms at extremely low power level (<1 photon per pulse), while effectively suppressing the residual temporal jitter between the two combs via optically triggered averaging using asynchronous optical sampling of combs. The use of repetition frequency stabilized distinct-wavelength pulses allowed for the effective suppression of strong background light from the pump through spectral filtering, achieving single-photon sensitivity. Subsequently, we parametrically down converted the frequency doubled light from the Er comb in the nonlinear ppKTP waveguide to generate quantum entangled photons at telecom band. A 9.04% Klyshko efficiency with a photon pair generation rate of 0.98 MHz/mW was obtained using heralding detection. Employing the established ASOPS technique to the generated photon pairs enabled the realization of ultrafast time-resolved and quantum mechanical correlation measurements. This paves the way for a versatile and comprehensive manipulation of quantum-entangled photon pairs in the time-domain, with potential applications in ultrafast optical quantum technology and ultrashort fluorescence measurements.
The nonclassical light sources, such as frequency-time entangled photons, are anticipated to offer significant benefits for emerging quantum optical sensing or spectroscopic measurements and manifest on ultrafast time scales (sub-ps to fs). However, the constrained time resolution (ns to ps) of photon-counting detectors poses challenges in comprehensively characterizing their detailed properties on ultrafast time scales. Therefore, we present a novel asynchronous optical sampling (ASOPS) technique utilizing two-color optical frequency combs to demonstrate highly precise and sensitive ultrafast time-resolved cross-correlation measurements at the single-photon level. By employing photon counting statistics, this method successfully reconstructed the picosecond pulse width cross-correlation waveforms at extremely low power level (<1 photon per pulse), while effectively suppressing the residual temporal jitter between the two combs via optically triggered averaging using asynchronous optical sampling of combs. The use of repetition frequency stabilized distinct-wavelength pulses allowed for the effective suppression of strong background light from the pump through spectral filtering, achieving single-photon sensitivity. Subsequently, we parametrically down converted the frequency doubled light from the Er comb in the nonlinear ppKTP waveguide to generate quantum entangled photons at telecom band. A 9.04% Klyshko efficiency with a photon pair generation rate of 0.98 MHz/mW was obtained using heralding detection. Employing the established ASOPS technique to the generated photon pairs enabled the realization of ultrafast time-resolved and quantum mechanical correlation measurements. This paves the way for a versatile and comprehensive manipulation of quantum-entangled photon pairs in the time-domain, with potential applications in ultrafast optical quantum technology and ultrashort fluorescence measurements.
Abstract We demonstrated an ultrafast time-resolved measurement method operating at the single-photon level and employing a two-color comb-based asynchronous optical sampling (ASOPS) setup. We harnessed the two-color ASOPS photon counting approach to achieve long-term averaging of the ultralow intensity signal with a synchronized optical trigger signal, which minimizes residual timing jitter between the two combs. A pulse-width limited picosecond cross-correlation signal was successfully obtained with a power level of <1 photon/pulse. This approach enables the thorough study of ultrafast time-resolved detection of entangled photon pairs, quantum mechanical correlations in the time-frequency domain and finds wide use in optical quantum technology.
Quantum correlations of ultrafast quantum optical states in the time–frequency domain manifest prominently on femtosecond time scales, an elusive challenging regime. We develop a new method to probe the time–frequency mode structure of ultrafast two-photon states utilizing dual-comb-based asynchronously overlapping pulses with single-photon frequency upconversion through femtosecond optical sampling. This method enables quick, highly precise joint temporal intensity measurements over a broad temporal dynamic range with only a single linear scanning stage. We demonstrate full characterization of time–frequency entangled two-photon states in both time and frequency domains. We quantified the time–frequency mode structure in both time and frequency domains through Schmidt decomposition, resulting in temporal and spectral purities of 87.7% and 76.9%, respectively, for heralded single-photons without any spectral filtering. Furthermore, through the simple control of pump spectral bandwidth, we demonstrate the ability to tailor time–frequency entanglement, verifying the two-dimensional Fourier duality. This method paves the way for a substantial upgrade to ultrafast quantum optical techniques, enabling a rapid, detailed, and multi-dimensional characterization of entangled states with potential applications in quantum metrology and photon-deficient fluorescence imaging.
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.
Quantum physics holds promise to revolutionise a number of technologies by enabling performance beyond what is feasible with classical resources, such as secure communications, precision measurement and high-speed simulation and computation. To realise this, quantum information must be encoded into one of the physical degrees of freedom of light. The time-frequency (TF) domain provides a infinite-dimensional space which is naturally compatible with integrated optical platforms. Additionally, future quantum networks will require coherent coupling of quantum systems that do not necessarily exhibit TF mode overlap. The ability to generate, coherently control and measure a variety of TF states of quantum light is therefore a necessary step towards implementing optical quantum technologies. Developing the building blocks for future optical quantum applications calls for an assortment of methods for measuring the properties of TF states of quantum light. Whilst much progress has been made towards this goal recently, deficiencies with existing methods remain. Efficient spectrally-resolved detection away from the telecoms wavelength range and a robust approach to single-photon state characterisation that is sensitive to the spectral phase have so far proven challenging. Additionally, accessing quantum advantages requires measurements that are sensitive to the nonclassical correlations that can exist between separate subsystems. However, until now a flexible approach to determining the full quantum state of systems of multiple time/frequency entangled photons has been lacking. Here we develop a toolbox of techniques for the measurement of TF quantum states of light for few-photon systems, and apply these to the task of precision measurement. Firstly, we propose, construct and demonstrate efficient single-photon spectrometers based on dispersive time-to-frequency mapping, using chirped fibre Bragg gratings to apply the necessary group delay dispersion. We use two such devices operating in coincidence to realise a full phase-sensitive reconstruction of the TF state of a single photon, by spectrally resolving the output of a nonclassical interference process with an external reference. We also demonstrate a complementary, optical reference-free method. This characterisation tool, an implementation of electro-optic spectral shearing interferometry with coincident spectrally-resolved single-photon detection, melds techniques from ultrafast metrology and quantum optics. We proceed to demonstrate the flexibility of this device by reconstructing a wide range of test pulses generated with a pulse shaper. By implementing this technique in conjunction with spectrally-resolved detection of a second photon, we realise complete characterisation of the TF wave function of a spectrally-entangled broadband photon pair. This method is robust to a wide range of inputs and is generalisable to spectrally mixed states and across a wide range of wavelengths, including to spectrally non-degenerate photon pairs. To demonstrate, we generate an entangled photon pair with controllable TF entanglement and perform a full reconstruction. Lastly, we present a new technique for using TF entangled photon pairs to realise quantum-enhanced measurement of a time delay in a quantum channel in the presence of environmental noise. This scheme is based on entanglement-enhanced rejection of background light. A simple experiment demonstrating the feasibility of such a measurement is presented.
Ultrafast quantum optics with time-frequency entangled photons is at the forefront of progress towards future quantum technologies. However, to unravel the time domain structure of entangled photons and exploit fully their rich dimensionality, a single-photon detector with sub-picosecond temporal resolution is required. Here, we present ultrafast single-photon detection using an optical Kerr gate composed of a photonic crystal fiber (PCF) placed inside a Sagnac interferometer. A near-rectangle temporal waveform of a heralded single-photon generated via spontaneous parametric down-conversion is measured with temporal resolution as high as 224 ± 9 fs. The large nonlinearity and long effective interaction length of the PCF enables maximum detection efficiency to be achieved with only 30.5 mW gating pulse average power, demonstrating an order-of-magnitude improvement compared to optical gating with sum-frequency generation. Also, we discuss the trade-off relationship between detection efficiency and temporal resolution.
Classical time-resolved optical spectroscopy experiments are performed using sequences of ultrashort light pulses, with photon fluxes incident on the sample which are many orders of magnitude higher than real-world conditions corresponding to sunlight illumination. Here we overcome this paradigm by exploiting quantum correlations to perform time-resolved spectroscopy with entangled photons. Starting from spontaneous parametric down-conversion driven by a continuous-wave laser, we exploit the temporal entanglement between randomly generated signal/idler pairs to obtain temporal resolution, and their spectral entanglement to select the excitation frequency. We also add spectral resolution in detection, using a Fourier transform approach which employs a common-path interferometer. We demonstrate the potential of our entangled-photon streak camera by resolving, at the single-photon level, excitation energy transfer cascades from LH2 to LH1 in the photosynthetic membrane and disentangling the lifetimes of two dyes in a mixture. We show that time-resolved spectroscopy with quantum light can be performed without compromising measurement time, recording a fluorescence time trace in less than a minute even for samples with low quantum yield, which can be reduced to sub-second times with acceptable signal-to-noise ratio. Our results provide a new approach to ultrafast optical spectroscopy, where experiments are performed under conditions comparable to real-world sunlight illumination.