Periodically driven quantum systems can exhibit a plethora of intriguing nonequilibrium phenomena that can be analyzed using Floquet theory. Naturally, Floquet theory is employed to describe the dynamics of atoms interacting with intense laser fields. However, this semiclassical analysis cannot account for quantum-optical phenomena that rely on the quantized nature of light. In this paper, we take a significant step to go beyond the semiclassical description of atom-photon coupled systems by unifying Floquet theory with quantum optics using the framework of full-counting statistics. This is achieved by introducing counting fields that keep track of the photonic dynamics. This formalism, which we dub “photon-resolved Floquet theory” (PRFT), is based on two-point tomographic measurements, instead of the two-point projective measurements used in standard full-counting statistics. Strikingly, the PRFT predicts the generation of macroscopic light-matter entanglement when atoms interact with multimode electromagnetic fields, thereby leading to complete decoherence of the atomic subsystem in the basis of the Floquet states. This decoherence occurs rapidly in the optical-frequency regime, but is negligible in the radio-frequency regime. Our results thus pave the way for the design of efficient quantum memories and quantum operations. Finally, employing the PRFT, we propose a quantum-communication protocol that can significantly outperform the state-of-art few-photon protocols by two orders of magnitude or better. The PRFT potentially leads to insights in various Floquet settings including spectroscopy, thermodynamics, quantum metrology, and quantum simulations. Published by the American Physical Society 2024
Periodically driven quantum systems can exhibit a plethora of intriguing nonequilibrium phenomena that can be analyzed using Floquet theory. Naturally, Floquet theory is employed to describe the dynamics of atoms interacting with intense laser fields. However, this semiclassical analysis cannot account for quantum-optical phenomena that rely on the quantized nature of light. In this paper, we take a significant step to go beyond the semiclassical description of atom-photon coupled systems by unifying Floquet theory with quantum optics using the framework of full-counting statistics. This is achieved by introducing counting fields that keep track of the photonic dynamics. This formalism, which we dub “photon-resolved Floquet theory” (PRFT), is based on two-point tomographic measurements, instead of the two-point projective measurements used in standard full-counting statistics. Strikingly, the PRFT predicts the generation of macroscopic light-matter entanglement when atoms interact with multimode electromagnetic fields, thereby leading to complete decoherence of the atomic subsystem in the basis of the Floquet states. This decoherence occurs rapidly in the optical-frequency regime, but is negligible in the radio-frequency regime. Our results thus pave the way for the design of efficient quantum memories and quantum operations. Finally, employing the PRFT, we propose a quantum-communication protocol that can significantly outperform the state-of-art few-photon protocols by two orders of magnitude or better. The PRFT potentially leads to insights in various Floquet settings including spectroscopy, thermodynamics, quantum metrology, and quantum simulations. Published by the American Physical Society 2024
Floquet theory and other established semiclassical approaches are widely used methods to predict the state of externally driven quantum systems, yet they do not allow the prediction of the state of the photonic driving field. To overcome this shortcoming, the photon-resolved Floquet theory (PRFT) was developed recently [], which deploys concepts from full-counting statistics to predict the statistics of the photon flux between several coherent driving modes. In this paper, we study in detail the scaling properties of the PRFT in the semi-classical regime. We find that there is an ambiguity in the definition of the moment-generating function, such that different versions of this function produce the same photonic probability distribution in the semiclassical limit, and generate the same leading-order terms of the moments and cumulants. Using this ambiguity, we establish a simple expression for the Kraus operators, which describe the decoherence dynamics of the driven quantum system appearing as a consequence of the light-matter interaction. The PRFT will pave the way for improved quantum sensing methods, e.g., for spectroscopic quantum sensing protocols, reflectometry in semiconductor nanostructures, and other applications, where the detailed knowledge of the photonic probability distribution is necessary. Published by the American Physical Society 2024
Spectroscopic methods play a vital role in quantum sensing, which uses the quantized nature of atoms or molecules to reach astonishing precision for sensing of, e.g., electric or magnetic fields. In the theoretical treatment, one typically invokes semiclassical methods to describe the light-matter interaction between quantum emitters, e.g., atoms or molecules, and a strong coherent laser field. However, these semiclassical approaches struggle to predict the stochastic measurement fluctuations beyond the mean value, necessary to estimate the sensitivity of spectroscopic quantum sensing protocols. Here, we develop a theoretical framework based on the recently developed photon-resolved Floquet theory (PRFT), which is capable of predicting the measurement statistics describing higher-order cumulants of coherent quantum states of light. The PRFT constructs flow equations for the cumulants of the photonic measurement statistics utilizing only the semiclassical dynamics of the matter system. We apply the PRFT to spectroscopic quantum sensing using dissipative two-level and four-level systems (describing electric-field sensing with Rydberg atoms), and demonstrate how to calculate the Fisher information of the measurement statistics with respect to various system parameters. In doing so, we demonstrate that the PRFT is a flexible tool allowing for improving the sensitivity of spectroscopic quantum sensing devices by several orders of magnitude.
Floquet engineering and cavity quantum electrodynamics represent two complementary descriptions of light-matter interaction, yet their precise connection beyond the small-coupling regime remains subtle. Here, by representing the cavity field in a large-photon-number phase basis, we show that the time-dependent Schrödinger equation of a classically driven system emerges directly from the fully quantized problem, without replacing the field by a classical trajectory or assuming a mean-field decoupling. This establishes a one-to-one correspondence between quasienergies and photon-sector-shifted quantum energies, while providing a direct quantum interpretation of the Floquet mean energy and Anandan phase. Because gauge invariance is exactly preserved at the level of the quantum Hamiltonian, the quantum-to-classical correspondence remains valid beyond perturbative and small-coupling regimes. We further show that light--matter entanglement is encoded in matter--harmonic correlations of the corresponding Floquet mode, thus identifying a semiclassical limit in which Floquet physics emerges without requiring the quantum field itself to approach a coherent classical state.
Photon-resolved Floquet theory keeps track of the photon exchange of a quantum system with a coherent driving field. It thus complements the standard full-counting statistics that counts the number of photons exchanged with incoherent photon modes giving rise to dissipation. In this paper, we introduce a unifying framework describing both situations. We develop methods suitable for an analytical evaluation of low-order cumulants of photonic probability distributions. Within this framework we analyze the two-mode Jaynes-Cummings model to demonstrate that the photon-resolved Floquet theory and the standard full-counting statistics make consistent statistical predictions. Interestingly, we find that the photon-flux fluctuations diverge for vanishing dissipation, which can be related to an entanglement effect between the driven matter system and the driving field. To substantiate our results, we use our framework to describe efficient photon up-conversion in an ac-driven lambda system, that is characterized by a high signal-to-noise ratio. Because the framework is nonperturbative and predicts fluctuations, it paves the way toward nonperturbative spectroscopy, which will assist to improve metrological methods. Published by the American Physical Society 2024
For decades, ultrafast light-matter interactions have provided a powerful means to observe electrons in motion across a wide range of physical systems. This dissertation builds new theoretical frameworks to make sense of the emergent phenomena that arise when light drives matter into the strong-field regime, spanning atomic, molecular, and condensed-matter systems. The resulting dynamics leave their fingerprints on a variety of observables, such as photoionization spectra, high-harmonic generation, and nonlinear spectroscopic signals, each of which provides a different window onto the underlying electronic motion. The work is organized into two parts.The first part focuses on the electric-field observables of nonlinear optical signals. Because both the amplitude and phase of the emitted field are experimentally accessible through techniques such as spectral interferometry and electro-optic sampling, the full field itself serves as a rich observable for characterizing nonlinear responses in atomic, molecular, and condensed-matter systems. Leveraging this, the simulations presented here uncover novel and largely unexplored physical phenomena encoded in these field observables. The second part turns to optical spectroscopy with quantum light. Although nonlinear optical processes are conventionally modeled within a semiclassical framework, treating the matter quantum mechanically while the driving ultrafast fields remain classical, the resulting signals can nonetheless exhibit intrinsically non-classical properties. Building on this insight, a framework for interpreting experimental data is introduced and used to show that four-wave mixing driven by ultrafast femtosecond laser pulses generates bright squeezed light. Beyond squeezed light, strong field-matter interactions can also produce attosecond entangled photons, a distinct form of quantum light. Several strategies are proposed to enhance the efficiency of their generation, with the developed theory predicting rates of energy-time entangled biphoton production orders of magnitude beyond those achievable with conventional spontaneous parametric down-conversion (SPDC) sources. The studies presented here are initial steps toward investigating quantum properties of these systems through quantum phynonlinear spectroscopy, which is not achievable with classical light.
We develop a general framework for the analysis of two-sided quantum interfaces, composed of collections of atoms interacting with paraxial light. Accounting for photon-mediated dipole-dipole interactions, our approach is based on the mapping of collective atom-photon interfaces onto a generic one-dimensional model of light scattering, characterized by a reflectivity parameter r 0 . This entails two key practical advantages: (i) the efficiency of the quantum interface in performing various quantum tasks, such as quantum memory or entanglement generation, is universally given by r 0 and is hence reduced to a measurement or classical calculation of a reflectivity; (ii) the efficiency can be greatly enhanced by a properly designed photon mode that spatially matches a collective-dipole eigenmode of the atoms. We demonstrate our approach for realistic cases of finite-size atomic arrays, partially filled arrays, and circular arrays. This provides a unified approach for treating collective light-matter coupling in various platforms, such as optical lattices and optical tweezers. Published by the American Physical Society 2024