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Nonlinear optical signals and spectroscopy with quantum light (1605.06746v1)

Published 22 May 2016 in quant-ph, physics.chem-ph, and physics.optics

Abstract: Conventional nonlinear spectroscopy uses classical light to detect matter properties through the variation of its response with frequencies or time delays. Quantum light opens up new avenues for spectroscopy by utilizing parameters of the quantum state of light as novel control knobs and through the variation of photon statistics by coupling to matter. We present an intuitive diagrammatic approach for calculating ultrafast spectroscopy signals induced by quantum light, focusing on applications involving entangled photons with nonclassical bandwidth properties - known as "time-energy entanglement". Nonlinear optical signals induced by quantized light fields are expressed using time ordered multipoint correlation functions of superoperators. These are different from Glauber's g- functions for photon counting which use normally ordered products of ordinary operators. Entangled photon pairs are not subjected to the classical Fourier limitations on the joint temporal and spectral resolution. After a brief survey of properties of entangled photon pairs relevant to their spectroscopic applications, different optical signals, and photon counting setups are discussed and illustrated for simple multi-level model systems.

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Summary

  • The paper introduces a novel framework using quantum light to surpass classical spectroscopic limits.
  • It extends the Liouville space formalism to characterize nonlinear responses and time-ordered correlations.
  • Applications include enhanced resolution in entangled photon spectroscopy and probing off-resonant states.

Nonlinear Optical Signals and Spectroscopy with Quantum Light

The paper "Nonlinear Optical Signals and Spectroscopy with Quantum Light" addresses the theoretical frameworks and potential applications of using quantum light in nonlinear spectroscopic techniques. This approach leverages the unique properties of quantum light, such as entanglement and non-classical photon statistics, to enhance spectroscopic measurements and probe materials in novel ways.

The primary focus of the paper is the nonclassical features of quantum light that can be harnessed for spectroscopy. Traditional spectroscopic methods utilize classical light, often sourced from lasers, to analyze material properties. These conventional methods rely on nonlinear interactions driven by high-intensity fields. The introduction of quantum light, typically in the form of entangled photons, adds distinct advantages, notably the ability to bypass some classical limitations related to bandwidth and resolution.

Entangled photons, particularly those with time-energy entanglement, are at the forefront of this discussion. These photons are not constrained by the classical Fourier limit that dictates a trade-off between temporal and spectral resolution. The paper painstakingly details how entangled photons can maintain strong time correlations while simultaneously achieving high spectral resolution, a feat not possible with classical light sources.

The authors extend the Liouville space formalism, which operates with superoperators, to characterize these quantum light interactions. This approach allows for a systematic representation of the nonlinear processes by detailing time-ordered multi-point correlation functions, which differ significantly from the conventional Glauber theory used for photon counting in classical optics. The framework developed provides a robust theoretical backing to predict and analyze spectroscopic signals induced by quantum light.

Several key applications and phenomena are explored in the paper. Notably, it discusses entangled photon-induced transparency, where the two-photon transparency is modulated by the entanglement time, allowing selective resonance enhancement. Another highlighted application is entangled virtual-state spectroscopy, which aims to probe off-resonant states that are typically inaccessible through classical methods.

Entangled light also offers a pathway to paper collective processes in complex systems, including molecular aggregates and semiconductor materials. The use of quantum light reveals non-local properties and correlations that are otherwise hidden when using classical light, effectively increasing the detail and depth of the analysis without increasing light intensity.

From the perspective of quantum theory, the paper emphasizes the significance of entangled light in breaking the traditional nonlinear optical bounds. It explores various nonlinear optical processes such as sum-frequency generation and parametric down-conversion under the influence of quantum light, proposing that quantum-induced coherence can play a crucial role in enhancing the detection capabilities of current spectroscopic setups.

Finally, the paper contemplates the implications of these findings for future developments in spectroscopy and quantum technologies. The ability to tailor quantum states of light to interact with matter in precise ways opens new avenues in photonic quantum information processing and coherent control experiments. As the technology for generating and manipulating quantum light sources continues to evolve, the future of spectroscopy is poised to be transformed by these advancements, promising more detailed and nuanced insights into the molecular and electronic structure of materials.

In summary, the paper presents a compelling case for the integration of quantum light into nonlinear spectroscopy, supported by a comprehensive theoretical base and potential for wide-ranging applications. The utilization of quantum states and entanglement provides a novel toolkit for researchers, offering enhanced resolution and control that surpasses classical spectroscopic techniques.

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