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arXiv:2603.20463 · Optica Quantum

Pulsed two-photon scattering from a single atom in a waveguide with delay-modified temporal correlations

Matthew Kozma, Sofia Arranz Regidor, Stephen Hughes

quant-phSubmitted Mar 20, 2026• Announced Mar 24, 2026• 0 citations• Revised Jul 19, 2026 (v2)
v1 · Mar 20, 2026v2 · Jul 19, 2026
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Abstract

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.

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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.
We present a quantum dynamical study of pulsed few-photon scattering from a single artificial atom, consisting of a two-level system (TLS) or qubit, in a waveguide QED system, directly comparing and contrasting two different quantum theoretical simulation methods: (i) an input-output scattering approach that uses frequency-dependent scattering matrices, and (ii) a matrix product states (MPS) approach, which uses quantum noise operators in time bins and a tensor network technique to solve the time-dependent waveguide function for the entire system. Beginning with pulsed excitation using one-photon and two-photon Fock state pulses, we first show how to compute time-dependent observables with the scattering matrix approach, in terms of frequency integrals that encode the pulse spectrum, including how to extract the population dynamics of the excited quantum emitter, as well as the linear and nonlinear contributions. We present solutions for both symmetric and chiral TLS coupling. We then show how to compute the qubit and field observables in a more direct way using MPS, and obtain the characteristic bird-like shape for the two-photon correlation function at two times, which has been observed in recent experiments. We compare and contrast both of these methods, for one and two-photon excitation pulses, and show excellent agreement. We also present a study of the linear and nonlinear contributions, which can easily be calculated using scattering theory, and show the important role of pulse duration. Finally, we demonstrate the clear advantages of MPS by easily going to higher N-photon excitations, and show selected example population dynamics of up to eight-photon Fock-state pulses, manifesting in clear nonlinear population oscillations during the pulse interaction, similar to classical Rabi oscillations, but with quantum input fields that have a vanishing electric field expectation value.
Squeezed light states have a special place in quantum optics with potentially profound applications in emerging quantum technologies. We present a numerically-exact matrix product states (MPS) approach to model quantum pulses of squeezed light, at the few-photon level, interacting with a two-level system in a waveguide environment. We represent the squeezed state as a coherent superposition of Fock states and explore the nonlinear population dynamics as well as multi-photon correlation functions that emerge. We show how the squeezed pulse can create quantum correlations that are unique to squeezed pulses, including ⟨b(t)b(t+t′)⟩\langle b(t) b(t+t')\rangle⟨b(t)b(t+t′)⟩ for transmitted fields as well as ⟨b†(t)b†(t+t′)b(t+t′)b(t)⟩\langle b^\dagger(t) b^\dagger(t+t') b(t+t') b(t) \rangle⟨b†(t)b†(t+t′)b(t+t′)b(t)⟩. We also demonstrate how ⟨b(t)b(t+t′)⟩\langle b(t) b(t+t') \rangle⟨b(t)b(t+t′)⟩, a first-order correlation function, shows nonlinear photon correlations that are similar to those known and measured for two-photon scattering states. Finally, we also study the squeezed spectra of the pulse before and after interacting with the two-level system, and highlight the role of the spectral bandwidth of the incident pulse. The MPS theory allows the modeling of arbitrary bandwidth squeezing without making any Markov and Born approximations for the light-matter interaction processes, and can easily be extended to waveguide systems with multiple emitters and time-delayed feedback.
The study of waveguide-QED systems, where a continuum of quantum field modes is coupled to qubits or two-level systems, has improved our ability to manipulate quantum light-matter interactions on chip. In the typical theoretical approaches to waveguide QED, there are a few necessary approximations, e.g., considering the system in the weak excitation regime, or treating the waveguide as a bath. However, these inherent approximations can break down with short pulse excitation. Here, we investigate the few-photon quantum nonlinear response of chiral qubits, when excited with one and two-photon Fock states. Our theory uses a numerically exact approach, based on Matrix Product States, avoiding the limitations of the usual waveguide-QED approximations. Using a chiral-emitter waveguide system, we show explicitly the breakdown of the weak excitation approximation, and study the single and two-photon nonlinear responses. We demonstrate the impact on the qubit population, and discuss how the phase change can be examined from the photon quantum correlation functions, seeing a radical departure from scattering theory solutions.
We study the dynamical light emission from few-photon Fock states in waveguide-QED with a chiral two-level system. We first investigate the time dynamics of the system by calculating the emitter population and illustrate the breakdown of the weak excitation approximation, for both 1-photon and 2-photon excitation. We show how a 1-photon pulse yields a transmitted long-time spectrum that is identical to the input pulse, despite significant population effects. However, the dynamical spectra and spectral intensity show rich population effects. We also show the differences between 1-photon and 2-photon excitation, where the latter shows clear signatures of nonlinear saturation effects. Analytical and numerically exact matrix product state solutions are shown.
We theoretically study the few-and many-body dynamics of photons in chiral waveguides.In particular, we examine pulse propagation through an ensemble of N two-level systems chirally coupled to a waveguide.We show that the system supports correlated multiphoton bound states, which have a welldefined photon number n and propagate through the system with a group delay scaling as 1=n 2 .This has the interesting consequence that, during propagation, an incident coherent-state pulse breaks up into different bound-state components that can become spatially separated at the output in a sufficiently long system.For sufficiently many photons and sufficiently short systems, we show that linear combinations of n-body bound states recover the well-known phenomenon of mean-field solitons in self-induced transparency.Our work thus covers the entire spectrum from few-photon quantum propagation, to genuine quantum many-body (atom and photon) phenomena, and ultimately the quantum-to-classical transition.Finally, we demonstrate that the bound states can undergo elastic scattering with additional photons.Together, our results demonstrate that photon bound states are truly distinct physical objects emerging from the most elementary light-matter interaction between photons and two-level emitters.Our work opens the door to studying quantum many-body physics and soliton physics with photons in chiral waveguide QED.