We study the effects of time ordering in photon generation processes such as spontaneous parametric down-conversion (SPDC) and four wave mixing (SFWM). The results presented here are used to construct an intuitive picture that allows us to predict when time-ordering effects significantly modify the joint spectral amplitude (JSA) of the photons generated in SPDC and SFWM. These effects become important only when the photons being generated lie with the pump beam that travels through the nonlinear material for a significant amount of time. Thus sources of spectrally separable photons are ideal candidates for the observation of modifications of the JSA due to time ordering.
We study the effects of time ordering in photon generation processes such as spontaneous parametric down-conversion (SPDC) and four wave mixing (SFWM). The results presented here are used to construct an intuitive picture that allows us to predict when time-ordering effects significantly modify the joint spectral amplitude (JSA) of the photons generated in SPDC and SFWM. These effects become important only when the photons being generated lie with the pump beam that travels through the nonlinear material for a significant amount of time. Thus sources of spectrally separable photons are ideal candidates for the observation of modifications of the JSA due to time ordering.
We study time-ordering corrections to the description of spontaneous parametric down-conversion (SPDC), four-wave mixing (SFWM), and frequency conversion using the Magnus expansion. Analytic approximations to the evolution operator that are unitary are obtained. They are Gaussian preserving, and allow us to understand order-by-order the effects of time ordering. We show that the corrections due to time ordering vanish exactly if the phase-matching function is sufficiently broad. The calculation of the effects of time ordering on the joint spectral amplitude of the photons generated in SPDC and SFWM are reduced to quadrature.
This thesis presents a study of photon generation and conversion processes in nonlinear optics. Our results extend beyond the first order perturbative regime, in which only pairs of photons are generated in spontaneous parametric down-conversion or four wave mixing. They also allow us to identify the limiting factors for achieving unit efficiency frequency conversion, and to correctly account for the propagation of bright nonclassical photon states generated in the nonlinear material. This is done using the Magnus expansion, which allows us to incorporate corrections due to time-ordering effects in the time evolution of the state, while also respecting the quantum statistics associated with squeezed states (in photon generation) and single photons or coherent states (in photon conversion). We show more generally that this expansion should be the preferred strategy when dealing with any type of time-dependent Hamiltonian that is a quadratic form in the creation and annihilation operators of the fields involved. Using the Magnus expansion, simple figures of merit to estimate the relevance of these time-ordering corrections are obtained. These quantities depend on the group velocities of the modes involved in the nonlinear process and provide a very simple physical picture of the interactions between the photons at different times. These time-ordering effects are shown to be important only when the photons and pump beam overlap within the nonlinear material for a significant amount of time. We also discuss the possibility of preparing Fock states with many photons using parametric down-conversion sources and realistic photon-number-resolving detectors. After discussing photon generation processes, we study photon conversion processes in which a nonlinear material and a classical strong pump field are used modify the frequency of a second incoming low-intensity field. We show that time-ordering effects limit the efficiency of this conversion process, re-examine strategies to get around this problem, and show that it should be possible to have a clear observation of modified upconversion probabilities due to these effects, and thus have an experimental demonstration of time-ordering effects in nonlinear optics.
Summary form only given. Pairs of entangled photons display a complex quantum state that cannot be represented through a product of single-particle states. The spontaneous parametric down-conversion (SPDC) process, that takes place when a laser pulse pumps a second-order nonlinear crystal has become recently a convenient source of such nonclassical states of light in quantum optics experiments. Nonstationary effects are mainly observed when the pump pulse temporal duration is significantly shorter than the characteristic interaction time in the nonlinear crystal. We introduce a nonstationary theory of SPDC to describe the results of fourth-order quantum-interference experiments when no spectral filtering is applied to the down-converted fields. Experiments involving nonlinear SPDC crystals with three different lengths were performed. The ultraviolet laser pulses were obtained from a Ti:sapphire femtosecond laser with a second-harmonic generator. These pulses were used to pump nonlinear crystals to initiate the process of nonstationary spdc and generate orthogonally-polarized photon pairs. These pairs then went into a polarization interferometer, and the coincidence counts of the detectors at the two output ports of the interferometer were recorded.
Cavity-assisted spontaneous parametric down-conversion (SPDC) and spontaneous four-wave mixing (SFWM) in nonlinear optical materials are practical and versatile methods to generate narrowband time-energy entangled photon pairs. Time-energy entangled photons with tailored spectro-temporal properties are particularly useful for efficient quantum optical interfaces. In this work we study the generation of photon pairs in cavity-assisted SPDC and SFWM for the general case of off-resonant conversion, namely, when the frequencies of the generated photons do not match the cavity resonances. Such a frequency mismatch in particular depends on temperature and requires an additional control in the experiment. First, we propose a generic model, for description of cavity-assisted SPDC and SFWM. We show that in both processes the mismatch reduces the generation rate of photons, distorts the spectrum and the auto-correlation function of the generated fields, as well as affects the photon generation dynamics. Second, we verify the results experimentally using parametric generation of photon pairs in a nonlinear whispering gallery mode resonator (WGMR) as an experimental platform with controlled frequency mismatch. Our work reveals the role of the frequency mismatch in the photon generation process and shows a way to control it. Obtained results constitute one more step in the direction of full control over the spectro-temporal properties of entangled photon pairs and the heralded generation of single-photon pulses with a tailored temporal mode.
Pairs of entangled photons are crucial for photonic quantum technologies. The demand for integrability and multi-functionality suggests 'flat' platforms - ultrathin layers and metasurfaces - as sources of photon pairs. With the success in demonstrating spontaneous parametric down-conversion (SPDC) from such sources, an alternative process to generate photon pairs, spontaneous four-wave mixing (SFWM), also starts to attract interest. In materials with nonzero second-order nonlinear susceptibility χ(2), SFWM can generate photon pairs both directly, through the third-order nonlinear susceptibility χ(3), and in a cascaded way, through second harmonic generation (SHG) followed by SPDC. Usually, the cascaded process is more efficient. Here, we show that in a thin layer, direct SFWM dominates, because the wavevector mismatch for SFWM is much smaller than for SHG or SPDC. To demonstrate it, we implement the photon pair generation via SFWM in a second-order nonlinear material - a thin layer of lithium niobate (LN). The existence of both second- and third-order nonlinear processes offers broader opportunities for quantum state engineering.
The generation of entangled photons by spontaneous parametric down-conversion (SPDC) or spontaneous four-wave mixing (SFWM) attracted enormous interest in the field of quantum optics. Depending on applications, entangled photon sources prioritize either bandwidth (e.g. for quantum imaging) or brightness (e.g. for quantum key distribution). Layered materials offer unique advantages for both. They have already been used to realize thinnest SPDC sources [1], which, like other layered materials such as transition-metal dichalcogenides (TMDs) [2], offer nearly unlimited bandwidth thanks to relaxed phase-matching constraints. Further, their easy integration on photonic platforms is promising for bright on-chip entangled photon sources. In this context, SPDC-based solutions are limited by phase-matching, whereas SFWM would be an almost phase-matching-free process, as pump, idler, and signal photons can be generated at similar wavelengths, thus propagating at the same group velocity in integrated devices. Moreover, exploiting excitonic resonances could enhance FWM even more. However, to date, experiments with resonant FWM in TMDs have been limited to signals in the visible [3], which is unsuitable for integrated photonics and telecom systems due to reabsorption during propagation in the photonic device.