Ideally, strong nonlinearities could be used to implement quantum gates for photonic qubits by well-controlled two-photon interactions. However, the dependence of the nonlinear interaction on frequency and time makes it difficult to preserve a coherent pulse shape that could justify a single-mode model for the time-frequency degree of freedom of the photons. In this paper, we analyze the problem of temporal multimode effects by considering the pulse shape of the average output field obtained from a coherent input pulse. It is shown that a significant part of the two-photon state transformation can be derived from this semiclassical description of the optical nonlinearity. The effect of a nonlinear system on a two-photon state can then be determined from the density-matrix dynamics of the coherently driven system using input-output theory. As an example, the resonant nonlinearity of a single two-level atom is characterized. The results indicate that the most efficient nonlinear effect may not be the widely studied single-mode phase shift, but the transfer of one of the photons to an orthogonal mode distinguished by its temporal and spectral properties.
Ideally, strong nonlinearities could be used to implement quantum gates for photonic qubits by well-controlled two-photon interactions. However, the dependence of the nonlinear interaction on frequency and time makes it difficult to preserve a coherent pulse shape that could justify a single-mode model for the time-frequency degree of freedom of the photons. In this paper, we analyze the problem of temporal multimode effects by considering the pulse shape of the average output field obtained from a coherent input pulse. It is shown that a significant part of the two-photon state transformation can be derived from this semiclassical description of the optical nonlinearity. The effect of a nonlinear system on a two-photon state can then be determined from the density-matrix dynamics of the coherently driven system using input-output theory. As an example, the resonant nonlinearity of a single two-level atom is characterized. The results indicate that the most efficient nonlinear effect may not be the widely studied single-mode phase shift, but the transfer of one of the photons to an orthogonal mode distinguished by its temporal and spectral properties.
Exploiting the field-amplification effect of a cavity, the possibility of optical nonlinearity by only two photons was indicated experimentally. In the present article, we review our recent analysis of the two-photon dynamics in a cavity quantum electrodynamics (QED) system. Since a cavity-QED system is highly dispersive around its resonances, the shapes of photonic pulses are significantly deformed through interaction with the system. Thus, the present analysis is based on a formalism beyond single-mode approximations. The external photon field is treated rigorously as a continuum, which enables us to handle the two-photon wavefunction in the space representation. The degree of optical nonlinearity in a two-photon state is quantified by comparing the output wavefunction with the linear output wavefunction. It is revealed that the semiclassical optical response theory can be applied for evaluation of the two-photon optical nonlinearity. The two-photon nonlinearity appears not purely as a phase shift in the output wavefunction. The degradation of the fidelity between the output wavefunction and the linear output wavefunction always occurs, which hinders the application of this nonlinear effect as a quantum phase gate. The optimum condition for maximizing the two-photon nonlinearity is clarified, suggesting that pulse shape control is more essential than the Q-value control of the cavity QED system.
The theoretical description of broadband, multimode quantum pulses undergoing a second-order χ(2)-nonlinear interaction can be quite intricate, due to the large dimensionality of the underlying phase space. However, in many cases only a few broadband (temporal) modes are relevant before and after the nonlinear interaction. Here we present an efficient framework to calculate the relation between the quantum states at the input and output of a nonlinear element in their respective relevant modes. Since the number of relevant input and output modes may differ, resulting in an open quantum system, we introduce the generalized Bloch-Messiah decomposition (GBMD), reducing the description to an equal number of input and output modes. The GBMD enables us to calculate the multimode Wigner function of the output state by convolving the rescaled Wigner function of the reduced input quantum pulse with a multivariate Gaussian phase-space function. We expand on this result by considering two examples input states: A Fock state in a single broadband mode and a two-mode squeezed vacuum, both in the THz-frequency regime, up-converted to a single output broadband mode of optical frequencies. We investigate the effect, the convolution and thermalization due to entanglement breakage have on the output Wigner function by calculating the von Neumann entropy of the output Wigner function. The methods presented here can be used to optimize the amplification or frequency conversion of broadband quantum states, opening an avenue to the generation and characterization of optical quantum states on ultrafast time scales.
We investigate the single-mode operation of a quantum optical nonlinear $\ensuremath{\pi}$ phase-shift gate implemented by a single two-level atom in one-dimensional free space. Since the single-mode property of the input photons at the atom is not preserved in the interaction at the atom, we analyze the efficiency of single-mode operation that can still be achieved. We show how the input pulse shape can be optimized to obtain high efficiencies for the nonlinear single-mode operation. With this analysis, we obtain an optimal single-mode transmittance per photon of 78% for the successful nonlinear $\ensuremath{\pi}$ phase-shift operation.
The problem of photon-photon interaction controlled by a two-level system is studied in this paper. Specifically, we have proposed two scenarios: Case 1, how a two-level system changes the pulse shapes of two initially uncorrelated input photons in a single input channel; and Case 2, how a two-level system entangles two counter-propagating photons, one in each input channel. The steady-state output field states for both cases are derived explicitly. For Case 1, the Wigner spectrum is used to exhibit the interesting properties of the output field state. For Case 2, the nonlinear property of the interaction between the two-level system and the two input photons has been revealed by the probabilities of observing photons in the output channels. In addition, two-photon interference, similar to Hong-Ou-Mandel effect, occurs when the two input photons are chosen with the same pulse shape.
Quantum nonlinearity is an essential ingredient for many quantum technologies, but often the nonlinearity is too weak to be exploited at the few-photon level. However, few photons interacting strongly with single quantum emitters in a waveguide environment can impact a significant nonlinear response, opening up a wide range of photon-photon correlations. Using a waveguide-QED system containing a single atom (treated as a two-level system) chirally coupled to a waveguide, we theoretically investigate two-photon nonlinearities with delay-controlled temporal correlations. We use both matrix product states (MPS) and a frequency-dependent scattering theory approach to analyze the exact population dynamics, as well as the first-order and second-order photon correlation functions in transmission of the system, when pumped by a two-photon Fock-state pulse with a bimodal temporal pulse envelope. The two-photon Fock-state pulses are considered to be either two single photons localized to each peak of the pulse, or both photons delocalized (but correlated) between the two peaks. We consider the regimes of a short, moderate, and (relatively) long distance between the two pulse peaks, comparing the important differences in the temporal correlations with the two types of two-photon pulses. We demonstrate the strikingly different nonlinear features and quantum correlations that occur for uncorrelated and correlated two-photon pairs in experimentally accessible regimes.
We present a detailed quantum theory and simulations of few-photon Fock state pulses interacting with a two-level system (TLS) in an open waveguide-QED system. For a rectangular pulse shape, we present an exact temporal scattering theory to derive analytical expressions for the TLS population, using one-photon and two-photon pulses, for both chiral and symmetric emitters. We also derive the stationary (long-time) and time-dependent spectra for one-photon excitation, and show how these differ at a fundamental level when considering TLS population effects. Numerically, we also present matrix product state (MPS) simulations, which allow us to compute more general photon correlation functions for arbitrary quantum pulses, and we use this approach to also show results for Gaussian quantum pulses and to confirm the accuracy of our analytical solutions. In the case of a chiral TLS, we show how a one-photon pulse, of any temporal shape, yields a transmitted long-time spectrum that is identical to the input pulse, despite significant TLS population effects. However, the dynamical spectra and spectral intensity show rich population effects, allowing for their detection in spectroscopic experiments. We also show the striking differences between one-photon and two-photon excitation, where the latter shows clear signatures of nonlinear saturation effects. In addition, we demonstrate how significant population TLS dynamics also occur for pulses that are relatively long compared to the radiative decay time (showing that a weak excitation approximation, which neglects finite TLS population effects, cannot be made) and investigate the population signatures, nonlinear features and dynamical behavior as a function of quantum pulse length.