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arXiv:2104.06032 · The Journal of Chemical Physics

Interferometric spectroscopy with quantum light: Revealing out-of-time-ordering correlators

Shahaf Asban, Konstantin E. Dorfman, Shaul Mukamel

Published Jun 1, 2021• 17 citations
arXivHTMLPDF

Abstract

We survey the inclusion of interferometric elements in nonlinear spectroscopy performed with quantum light. Controlled interference of electromagnetic fields coupled to matter can induce constructive or destructive contributions of microscopic coupling sequences (histories) of matter. Since quantum fields do not commute, quantum light signals are sensitive to the order of light-matter coupling sequences. Matter correlation functions are thus imprinted by different field factors, which depend on that order. We identify the associated quantum information obtained by controlling the weights of different contributing pathways and offer several experimental schemes for recovering it. Nonlinear quantum response functions include out-of-time-ordering matter correlators (OTOCs), which reveal how perturbations spread throughout a quantum system (information scrambling). Their effect becomes most notable when using ultrafast pulse sequences with respect to the path difference induced by the interferometer. OTOCs appear in quantum-informatics studies in other fields, including black hole, high energy, and condensed matter physics.

DOI
10.1063/5.0047776

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We survey the inclusion of interferometric elements in nonlinear spectroscopy performed with quantum light. Controlled interference of electromagnetic fields coupled to matter can induce constructive or destructive contributions of microscopic coupling sequences (histories) of matter. Since quantum fields do not commute, quantum light signals are sensitive to the order of light-matter coupling sequences. Matter correlation functions are thus imprinted by different field factors, which depend on that order. We identify the associated quantum information obtained by controlling the weights of different contributing pathways and offer several experimental schemes for recovering it. Nonlinear quantum response functions include out-of-time-ordering matter correlators (OTOCs), which reveal how perturbations spread throughout a quantum system (information scrambling). Their effect becomes most notable when using ultrafast pulse sequences with respect to the path difference induced by the interferometer. OTOCs appear in quantum-informatics studies in other fields, including black hole, high energy, and condensed matter physics.
We develop closed expressions for a time-resolved photon counting signal induced by an entangled photon pair in an interferometric spectroscopy setup. Superoperator expressions in Liouville-space are derived that can account for relaxation and dephasing induced by coupling to a bath. Interferometric setups mix matter and light variables non-trivially, which complicates their interpretation. We provide an intuitive modular framework for this setup that simplifies its description. Based on the separation between the detection stage and the light-matter interaction processes, we show that the pair entanglement time and the interferometric time-variables control the observed physics time scale. Only a few processes contribute in the limiting case of small entanglement time with respect to the sample response, and specific contributions can be singled out.
Out-of-time-order correlators (OTOCs) are central probes of quantum scrambling, and their generalizations have recently become key primitives for both benchmarking quantum advantage and learning the structure of Hamiltonians. Yet their behavior has lacked a unified algorithmic interpretation. We show that higher-order OTOCs naturally fit within the framework of quantum signal processing (QSP): each OTOC(k)\mathrm{OTOC}^{(k)}OTOC(k) measures the 2k2k2k-th Fourier component of the phase distribution associated with the singular values of a spatially resolved truncated propagator. This explains the contrasting sensitivities of time-ordered correlators (TOCs) and higher-order OTOCs to causal-cone structure and to chaotic, integrable, or localized dynamics. Based on this understanding, we further generalize higher-order OTOCs by polynomial transformation of the singular values of the spatially resolved truncated propagator. The resultant signal allows us to construct frequency-selective filters, which we call \emph{OTOC spectroscopy}. This extends conventional OTOCs into a mode-resolved tool for probing scrambling and spectral structure of quantum many-body dynamics.
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.
This tutorial article introduces the physics of quantum information scrambling in quantum many-body systems. The goals are to understand how to precisely quantify the spreading of quantum information and how causality emerges in complex quantum systems. We introduce a general framework to study the dynamics of quantum information, including detection and decoding. We show that the dynamics of quantum information is closely related to operator dynamics in the Heisenberg picture, and, under certain circumstances, can be precisely quantified by the so-called out-of-time-ordered correlator (OTOC). The general behavior of the OTOC is discussed based on several toy models, including the Sachdev-Ye-Kitaev model, random circuit models, and Brownian models, in which the OTOC is analytically tractable. We introduce numerical methods, including exact diagonalization and tensor network methods, to calculate the OTOC for generic quantum many-body systems. We also survey current experimental schemes for measuring the OTOC in various quantum simulators. Published by the American Physical Society 2024
Out-of-time-ordered correlators (OTOCs) provide a powerful probe of quantum chaos and scrambling. While the Lindblad formalism is often used to describe OTOCs in open systems, microscopic mechanisms that give rise to the Lindblad equation at the level of time-ordered correlation functions do not necessarily justify this approach at the level of OTOCs. Starting from a microscopic model of a subsystem coupled to a random bath, we show that the resulting OTOC dynamics contains an additional contribution compared to the standard Lindblad approach. This contribution, induced by correlations between different replicas, allows key properties of the underlying unitary dynamics such as long-time freeness to be retained and information scrambling to be captured more faithfully. As an application, we show that this extended formalism can be used to numerically study OTOCs in large closed systems by replacing part of the system with a dissipative boundary, offering a way to study operator spreading and higher-order correlations beyond directly accessible system sizes.
Abstract Optical interferometry has been a long-standing setup for characterization of quantum states of light. Both linear and the nonlinear interferences can provide information regarding the light statistics and underlying detail of the light-matter interactions. Here we demonstrate how interferometric detection of nonlinear spectroscopic signals may be used to improve the measurement accuracy of matter susceptibilities. Light-matter interactions change the photon statistics of quantum light, which are encoded in the field correlation functions. Application is made to the Hong-Ou-Mandel two-photon interferometer that reveals entanglement-enhanced resolution that can be achieved with existing optical technology.