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Physical Review A

Nonlinear spectroscopy with entangled photons: Manipulating quantum pathways of matter

Oleksiy Roslyak, Christoph A. Marx, Shaul Mukamel

Published Mar 20, 2009• 73 citations
Publisher

Abstract

Optical signals obtained by the material response to classical laser fields are given by nonlinear response functions which can be expressed by sums over various quantum pathways of matter. We show that some pathways can be selected by using nonclassical fields, through the entanglement of photon and material pathways, which results in a different-power law dependence on the incoming field intensity. Spectrally overlapping stimulated Raman scattering (SRS) and two-photon-absorption (TPA) pathways in a pump probe experiment are separated by controlling the degree of entanglement of pairs of incoming photons. Pathway-selectivity opens up new avenues for mapping photon into material entanglement. New material information, otherwise erased by interferences among pathways, is revealed.

DOI
10.1103/physreva.79.033832

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Optical signals obtained by the material response to classical laser fields are given by nonlinear response functions which can be expressed by sums over various quantum pathways of matter. We show that some pathways can be selected by using nonclassical fields, through the entanglement of photon and material pathways, which results in a different-power law dependence on the incoming field intensity. Spectrally overlapping stimulated Raman scattering (SRS) and two-photon-absorption (TPA) pathways in a pump probe experiment are separated by controlling the degree of entanglement of pairs of incoming photons. Pathway-selectivity opens up new avenues for mapping photon into material entanglement. New material information, otherwise erased by interferences among pathways, is revealed.
Optical signals obtained by the material response to classical laser fields are given by nonlinear response functions which can be expressed by sums over various quantum pathways of matter. We show that some pathways can be selected by using nonclassical fields, through the entanglement of photon and material pathways, which results in a different-power law dependence on the incoming field intensity. Spectrally overlapping stimulated Raman scattering (SRS) and two-photon-absorption (TPA) pathways in a pump probe experiment are separated by controlling the degree of entanglement of pairs of incoming photons. Pathway-selectivity opens up new avenues for mapping photon into material entanglement. New material information, otherwise erased by interferences among pathways, is revealed.
The application of quantum states of light such as entangled photons, for example, created by parametric down conversion, has experienced tremendous progress in the almost 40 years since their first experimental realization. Initially, they were employed in the investigation of the foundations of quantum physics, such as the violation of Bell's inequalities and studies of quantum entanglement. They later emerged as basic platforms for quantum communication protocols and, in the recent experiments on single-photon interactions, in photonic quantum computation. These applications aim at the controlled manipulation of the photonic degrees of freedom, and therefore rely on simple models of matter, where the analysis is simpler. Furthermore, quantum imaging with entangled light can achieve enhanced resolution, and quantum metrology can overcome the shot noise limit for classical light. This Account focuses on an entirely different emerging class of applications using quantum light as a powerful spectroscopic tool to reveal novel information about complex molecules. These applications utilize two appealing properties of quantum light: its distinct intensity fluctuations and its nonclassical bandwidth properties. These give rise to new and surprising behavior of nonlinear optical signals. Nonclassical intensity fluctuations can enhance nonlinear optical signals relative to linear absorption. For instance, the two-photon absorption of entangled photon pairs scales linearly (rather than quadratically) in the photon flux, just like a single photon absorption. This enables nonlinear quantum spectroscopy of photosensitive, for example, biological, samples at low light intensities. We will discuss how the two-photon absorption cross section becomes a function of the photonic quantum state, which can be manipulated by properties of the entangled photon pairs. In addition, the quantum correlations in entangled photon states further influence the nonlinear signals in a variety of ways. Apart from affecting the signal's scaling with intensity, they also constitute an entirely new approach to shaping and controlling excitation pathways in molecular aggregates in a way that cannot be achieved with shaped classical pulses. This is because between the two absorption events in entangled two-photon absorption, the light and material system are entangled. Classical constraints for the simultaneous time and frequency resolution can thus be circumvented, since the two are not Fourier conjugates. Here we review the simplest manifestation of quantum light spectroscopy, two-photon absorption spectroscopy with entangled photons. This will allow us to discuss exemplarily the impact of quantum properties of light on a nonlinear optical signal and explore the opportunities for future applications.
Quantum entanglement offers an incredible resource for enhancing the sensing and spectroscopic probes. Here we develop a microscopic theory for the stimulated Raman scattering (SRS) using entangled photons. We demonstrate that the time-energy correlation of the photon pairs can optimize the signal for polyatomic molecules. Our results show that the spectral-line intensity of the entangled-photon SRS (ESRS) is of the same order of magnitude as the one for the entangled two-photon absorption (ETPA); the parameter window is thus identified to do so. Moreover, the vibrational coherence is found to play an important role for enhancing the ESRS against the ETPA intensity. Our work paves a firm road for extending the schemes of molecular spectroscopy with quantum light, based on the observation of the ETPA in experiments.
Quantum entanglement offers an incredible resource for quantum-enhanced sensing, imaging, and spectroscopy. Here we evaluate the enhancement of stimulated Raman scattering (SRS) signal by entangled photons. We demonstrate that the time-energy correlation of the photon pairs can optimize the signal for polyatomic molecules. Our results show that the spectral-line intensity of the entangled-photon SRS (ESRS) is of the same order of magnitude as the one for the entangled two-photon absorption (ETPA); the parameter window is thus identified to do so. Moreover, the vibrational coherence is found to play an important role for enhancing the ESRS against the ETPA intensity. Our work paves a firm road for extending the schemes of molecular spectroscopy with quantum light, based on the observation of the ETPA in experiments.
Quantum light is increasingly recognized as a promising resource for developing optical measurement techniques. Particular attention has been paid to enhancing the precision of the measurements beyond classical techniques by using nonclassical correlations between quantum entangled photons. Recent advances in the quantum optics technology have made it possible to manipulate spectral and temporal properties of entangled photons, and photon correlations can facilitate the extraction of matter information with relatively simple optical systems compared to conventional schemes. In these respects, the applications of entangled photons to time-resolved spectroscopy can open new avenues for unambiguously extracting information on dynamical processes in complex molecular and materials systems. Here, we propose time-resolved spectroscopy in which specific signal contributions are selectively enhanced by harnessing nonclassical correlations of entangled photons. The entanglement time characterizes the mutual delay between an entangled twin and determines the spectral distribution of photon correlations. The entanglement time plays a dual role as the knob for controlling the accessible time region of dynamical processes and the degrees of spectral selectivity. In this sense, the role of the entanglement time is substantially equivalent to the temporal width of the classical laser pulse. The results demonstrate that the application of quantum entangled photons to time-resolved spectroscopy leads to monitoring dynamical processes in complex molecular and materials systems by selectively extracting desired signal contributions from congested spectra. We anticipate that more elaborately engineered photon states would broaden the availability of quantum light spectroscopy.
Classical light such as lasers and thermal radiation has long been utilized for spectroscopy to explore material structures and dynamics. However, quantum states of light open new avenues for ultrafast optics and spectroscopy, by the variation of their unique properties, e.g., entanglement and photon statistics, after interacting with materials. Quantum light possesses unique characteristics that distinguish it from classical light, particularly the phase-space distribution which reflects its fundamental quantum statistics and the quantum control protocol that may take advantage of noise reduction. This Review will focus on spectroscopic applications using entangled photons and squeezed light, in conjunction with quantum coherent control. We provide a brief introduction to the generation of the entangled and squeezed light, discussing their fundamental properties and connections to the control protocol that may enhance spectroscopic techniques. A microscopic theory for the spectroscopy and corresponding signals induced by certain transition processes is developed. Nonlinear optical signals induced by entangled photons for the coherent anti-Stokes Raman spectra (CARS) and the stimulated Raman spectra (SRS) are investigated. We further extend our efforts to the transient absorption process that enables real-time monitoring of the exciton transfer in the transition metal dichalcogenides (TMDs), namely, using the WS 2 monolayer. This series of works on nonlinear optical spectroscopy using quantum light explicitly demonstrates the quantum supremacy in ultrafast spectroscopy through jointly enhancing the time and energy scales beyond the classical bound.