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.
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.
Single photons are a natural platform for quantum technologies as they support entanglement in many degrees of freedom and are inherently well protected from a detrimental type of noise called decoherence. In order to fully exploit photons for quantum technologies, it will be necessary to be able to shape, control, and measure their properties in all degrees of freedom: space, time, frequency, and polarization. \n \n The time-frequency degree of freedom of light is of particular interest for quantum information tasks as it supports various encodings, including frequency bins and time bins, and is intrinsically robust for propagation through long-distance fibre links. Applications which harness quantum correlations in this degree of freedom, referred to as energy-time entanglement, include dispersion cancellation and high-dimensional quantum key distribution. However, detection of this entanglement and observation of these effects requires time resolution beyond the capabilities of current photon detectors. Thus, for operations on ultrafast time scales, more powerful and complex methods are required. \n \n In this thesis, we use a nonlinear technique known as optical gating to surpass the limitations in current detectors and measure single photon pairs, improving the time resolution by two orders of magnitude. When a single photon enters a nonlinear medium at the same time as a strong laser pulse, it may upconvert to a higher energy photon. The strong laser pulse effectively acts as an ultrafast shutter or gate and this creates a high resolution snapshot of the photon in time. Optical gating in conjunction with single photon spectrometers then allow us to measure both the spectral and temporal features of photons on subpicosecond time scales. \n \n These high resolution measurements enable us to explore a host of quantum effects which remained previously inaccessible. First, we directly observe energy-time entanglement, analogous to Einstein-Rosen-Podolsky correlations but \\emph{in frequency and time}. Then, with full control over the dispersion of each photon, we observe nonlocal dispersion cancellation on femtosecond time scales. We also explore ultrafast interferometry in the quantum domain by temporally resolving two-photon interference from a Franson interferometer and observe a violation of the CHSH-Bell inequality. Finally, we show that, using these measurements, it is possible to reconstruct a two-photon energy-time entangled state. Such measurement capabilities will be essential to precisely control both the spectral and temporal shape of entangled photons and to develop new applications in quantum state engineering.
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.
Spectral-temporal manipulation of optical pulses has enabled numerous developments within a broad range of research topics, ranging from fundamental science to practical applications. Within quantum optics spectral-temporal degree of freedom of light offers a promising platform for integrated photonic quantum information processing. An important challenge in experimentally realizing spectral-temporal manipulation of quantum states of light is the need for highly efficient manipulation tools. In this context the intrinsically deterministic electro-optic methods show great promise for quantum applications. We experimentally demonstrate application of electro-optic platform for spectral-temporal manipulation of ultrashort pulsed quantum light. Using techniques analogous to serrodyne frequency shifting we show active spectral translation of few-picosecond single photon pulses by up to 0.5 THz. By employing an approach based on an electro-optic time lens we demonstrate up to 6-fold spectral compression of heralded single photon pulses with efficiency that enables us to significantly increase single photon flux through a narrow bandpass filter. We realize the required temporal phase manipulation by driving a lithium niobate waveguided electrooptic modulator with 33 dBm sinusoidal RF field at the frequency of either 10 GHz or 40 GHz. We use a phase lock loop to temporally lock the RF field to the 80 MHz repetition rate of approximately 1 ps long optical pulses. Heralded single photon wavepackets are generated by means of spontaneous parametric down-conversion in potassium dihydrogen phosphate (KDP) crystal, which enables preparation of spectrally pure single photon wavepackets without the need for spectral filtering. Spectral shifting is achieved by locking single-photon pulses to the linear slope of sinusoidal 40 GHz RF phase modulation. We verify the spectral shift by performing spectrally resolved heralded single photon counting, using frequency-to-time conversion by means of a highly dispersive chirped fiber Bragg grating. We verify the non-classicality of spectrally shifted single photons by measuring high-visibility Hong-Ou-Mandel interference using a reference single photon pulse. Spectral compression is based on the time lens principle, which requires locking optical pulses to approximately quadratic region of sinusoidal phase modulation. We utilize both 10 GHz and 40 GHz RF driving frequencies. Bandwidth compression is achieved by chirping the single photon pulse using an appropriate length of single-mode fibre and subsequently subjecting it to the action of the time lens. We verify spectral compression directly using the aforementioned spectrally-resolved heralded single photon counting method. We achieve 3-fold spectral compression of 2 nm bandwidth single photon pulses using 40 GHZ modulation frequency, and 6-fold spectral compression of 0.9 nm bandwidth single photon pulses using 10 GHz modulation frequency. Overall transmission of our set-up exceeding 30% enables practical usability of our spectral compression method which we demonstrate experimentally by showing an increased photon flux through a narrowband filter. Our results present an important contribution towards implementing quantum information processing in the spectral-temporal degree of freedom of a photon. In the context of quantum networks they present an enabling tool towards efficient photonic interfacing of different quantum information processing platforms.
A fiber-integrated spectrometer for single-photon pulses outside the telecommunications wavelength range based upon frequency-to-time mapping, implemented by chromatic group delay dispersion (GDD), and precise temporally-resolved single-photon counting, is presented. A chirped fiber Bragg grating provides low-loss GDD, mapping the frequency distribution of an input pulse onto the temporal envelope of the output pulse. Time-resolved detection with fast single-photon-counting modules enables monitoring of a wavelength range from 825 nm to 835 nm with nearly uniform efficiency at 55 pm resolution (24 GHz at 830 nm). To demonstrate the versatility of this technique, spectral interference of heralded single photons and the joint spectral intensity distribution of a photon-pair source are measured. This approach to single-photon-level spectral measurements provides a route to realize applications of time-frequency quantum optics at visible and near-infrared wavelengths, where multiple spectral channels must be simultaneously monitored.
The fascinating nature of light has driven many discoveries in physics, from the theory of special relativity to quantum mechanics. As a carrier of information, light is at the core of high-speed communication over the internet and facilitates the study of numerous physical properties of materials by the interaction of light and matter. Advances in generating and detecting ultrashort light pulses enabled the spectroscopic investigation of matter with unprecedented detail. Meanwhile, the development of more precise and sensitive measurements, leveraging quantum properties of light, has expanded the experimental frontiers of the physical world. Naturally, the question arises: Could the combination of these two breakthroughs push the frontiers even further? A promising candidate to achieve this combination is electro-optic sampling, an electromagnetic-field measurement comprising an up-conversion and a phase-space measurement based on homodyne detection. While it is predominantly used in classical terahertz time-domain spectroscopy, the high sensitivity and spatio-temporal resolution of electro-optic sampling recently enabled the detection of vacuum fluctuations in the ground state of the electromagnetic field by probing an adjustable space-time volume. Yet, the generation and characterization of more intricate quantum pulses on ultrafast timescales is still challenging, especially in the terahertz frequencies. Exploiting the quantum properties of a light pulse over a broad frequency range requires sophisticated knowledge about the prepared quantum pulse as well as the measurement setup at use. However, Heisenberg's uncertainty relation fundamentally prevents the complete determination of an arbitrary quantum state from a single measurement. Instead, the quantum state has to be reconstructed from the statistics of many measurements — a process known as quantum state tomography. In this thesis, we establish the theoretical foundations for a comprehensive tomographic reconstruction of pulsed quantum states of light, encompassing both the statistics and dynamics of the state. Additionally, we introduce tools to simplify the description of the nonlinear interaction underlying electro-optic sampling and in turn the tomography setups presented here. As a first step, we investigate the application of electro-optic sampling to the time-local reconstruction of various pulsed quantum states of light on ultrafast timescales. We identify two types of noise, which impact the quality of the reconstruction: shot noise, arising from the nonlinear interaction in electro-optic sampling, and thermal noise, due to the localization of the (correlated) quantum state within a small space-time volume during the measurement. To improve the reconstruction, we propose to use a strong probe pulse, suppressing the shot noise, and to select an appropriate detection frequency band, reducing thermal noise. Thus, the proposed tomography enables the characterization of quantum states in terahertz frequency range on ultrafast timescales. However, the time-local nature of the measurement imposes a trade-off between the reconstruction of the quantum state in phase space and the time domain. In a second step, we propose a reconstruction method based on two-time field-correlation measurement, which we call correlation tomography, able to overcome the restriction to time-local states. While the tomography of quantum states in an optimal pulse basis has been demonstrated, it requires prior knowledge about the temporal structure of the quantum state. We introduce an algorithm for reconstructing high-dimensional multimode Gaussian quantum states, which are completely characterized by the covariance matrix of the quadratures of fully distinguishable pulses. The reconstruction is achieved by orthogonalizing the overlapping time windows of the correlation measurement in post-processing. We compare a homodyne-based implementation to electro-optic sampling and develop an optimization scheme for the latter, to mitigate the shot noise in the non-perturbative regime of strong nonlinear interactions. Furthermore, we derive the full-counting statistics of the field-correlation measurement and theoretically demonstrate the reconstruction of pulsed Fock states. This opens an avenue to the full tomography of highly multimode non-Gaussian states. In the third and last step, we derive a formalism to simplify the description of the up-conversion required in electro-optic sampling. If a pulsed quantum states is up-converted and localized in a small space-time region, the transformation of the localized modes during the nonlinear interaction corresponds to an open quantum system, rendering the standard tools of quantum optics inapplicable. By introducing the generalized Bloch-Messiah decomposition, we simplify the input-output relation of the nonlinear interaction to a set of effective modes relevant for subsequent processing, such as detection. Using this framework, we derive an analytic phase-space input-output relation for the nonlinear interaction of pulsed quantum states, applicable to open quantum systems. We study the resulting dynamics using two example input states: a Fock state and a two-mode squeezed state. Based on the von Neumann entropy of the output state, we develop an intuitive understanding of the generalized Bloch-Messiah decomposition. The rich structure of pulsed quantum states of light can be a powerful resource, but also challenging to operate with, in theory as well as in experiment. The characterization methods and theoretical tools developed in this thesis, tailored to pulsed quantum light and the nonlinear interaction thereof, can pave the way to the application of this resource to fundamental research as well as quantum technologies.
Temporal-spectral modes of light provide a fundamental window into the nature of quantum systems and offer a robust means for information encoding. Methods to precisely characterize the temporal-spectral state of light at the single-photon level thus play a central role in understanding single-photon sources and their applications in emerging optical quantum technologies. Here we demonstrate an optical reference-free method, which melds techniques from ultrafast metrology and single-photon spectral detection, to characterize the pulse-mode structure of heralded single photons.