Nonlinear optical signals and spectroscopy with quantum light

Dorfman, Konstantin E.; Schlawin, Frank; Mukamel, Shaul

doi:10.1103/revmodphys.88.045008

Cited by 318 publications

(294 citation statements)

References 303 publications

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“…For polarization entangled photonic states, adding random phase has been shown to be a useful tool to generate in a controlled way mixed states required to test quantum protocols [16][17][18][19][20][21][22]. In the present work, the possibility to control the amount of classical versus quantum energy correlations opens the way for practical demonstration of the genuine advantage of entanglement, for instance as in quantum spectroscopy schemes [11].…”

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confidence: 99%

“…However, classical thermal light also shows photon bunching, and thus, can be exploited to enhance two-photon absorption as well [7]. The quantum nature of dispersion cancellation was also subject to debate [8,9].Energy entangled biphoton states are an essential tool in the prospect of experimentally realizing quantum spectroscopy experiments [10,11], and more generally for any energy-time two-photon metrology scheme, as for example quantum optical coherence tomography [12]. Here the relevance of entanglement can also be misleading.…”

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confidence: 99%

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Observing the transition from quantum to classical energy correlations with photon pairs

Stefanov¹,

Lerch²

2017

Quantum Information and Measurement (QIM) 2017

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We experimentally demonstrate a method to control the relative amount of quantum and classical energy correlations between two photons from a pair emitted by spontaneous parametric downconversion. Decoherence in the energy basis is achieved by applying random spectral phases on the photons. As a consequence a diverging temporal second order correlation function is observed and is explained by a mixture between an energy entangled pure state and a fully classically correlated mixte state.Quantum entanglement implies correlations beyond those allowed by classical models and plays a fundamental role in quantum metrology [1]. In optical metrology, photon pairs generated by spontaneous parametric downconversion (SPDC) [2] are the most practical realization of correlated light beams. Because the process is coherent, the emitted photons are in essence entangled, but it is of interest to experimentally be able to tune the correlations of quantum states, from purely quantum to classical. In particular since it is not always obvious to distinguish between advantages in metrology originating from genuine entanglement and effects due to classical correlations [3]. Indeed, while some schemes where previously thought to be based on entanglement, they actually only rely on classical correlations. For instance in ghost imaging [4], coincidence measurements from a thermal source allow to reproduce the image of an object, without the need of non-classical transverse correlations as originating from an SPDC source [5]. Another example can be found in photon number correlations. In SPDC, the down-converted photons are created pairwise, leading to a linear absorption rate for two-photon absorption processes [6]. However, classical thermal light also shows photon bunching, and thus, can be exploited to enhance two-photon absorption as well [7]. The quantum nature of dispersion cancellation was also subject to debate [8,9].Energy entangled biphoton states are an essential tool in the prospect of experimentally realizing quantum spectroscopy experiments [10,11], and more generally for any energy-time two-photon metrology scheme, as for example quantum optical coherence tomography [12]. Here the relevance of entanglement can also be misleading. For instance, in the case of two independent atoms, each of them excited by a single photon, a predicted enhanced absorption rate was first attributed to energy-time entanglement between the photons [13]. Yet it was later shown, that only classical frequency anticorrelations are actually enhancing the absorption rate [14]. Similarly in [15] a pump-probe scheme is proposed, where a sample is excited by a classical pulse and probed by a photon from an entangled pair. Again, such scheme rely fun- * andre.stefanov@iap.unibe.ch damentally on energy correlations and not on genuine entanglement.In this paper we propose and experimentally realize a scheme to control transition from quantum to classical correlations with energy correlated photons. A characteristic of such entangled photon pairs is to show...

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confidence: 99%

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confidence: 99%

Observing the transition from quantum to classical energy correlations with photon pairs

Stefanov¹,

Lerch²

2017

Quantum Information and Measurement (QIM) 2017

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“…Quantum light sources are realized for many different material platforms in semiconductor, atom and molecular systems [1][2][3][4][5] and offer an exciting testbed for nonlinear quantum dynamics [6], including quantum ghost imaging, two-photon-spectroscopy [7][8][9] and quantum light spectroscopy [10][11][12]. Prototypical single photon emitters based on semiconductor nanostructures are produced [13][14][15] and used in quantum cryptography protocols [16][17][18] and quantum sensing [19].…”

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confidence: 99%

Quantum cascade driving: Dissipatively mediated coherences

et al. 2017

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Quantum cascaded systems offer the possibility to manipulate a target system with the quantum state of a source system. Here, we study in detail the differences between a direct quantum cascade and coherent/incoherent driving for the case of two coupled cavity-QED systems. We discuss qualitative differences between these excitations scenarios, which are particular strong for higherorder photon-photon correlations: g (n) (0) with n > 2. Quantum cascaded systems show a behavior differing from the idealized cases of individual coherent/incoherent driving and allow to produce qualitatively different quantum statistics. Furthermore, the quantum cascaded driving exhibits an interesting mixture of quantum coherent and incoherent excitation dynamics. We develop a measure, where the two regimes intermix and quantify these differences via experimentally accessible higher-order photon correlations.PACS numbers: Valid PACS appear here * shahab@ut.ee 1 arXiv:1706.05273v1 [quant-ph]

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“…However, the quantum nature of light may be used for the manipulation and spectroscopic studies of molecules in many other ways that not necessarily involve cavities (19). Conventional nonlinear spectroscopy uses classical light to detect matter properties through the variation of its response with frequencies or time delays.…”

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confidence: 99%

“…The quantum nature of light manifests in collective effects in many-body systems by its ability to project entanglement back and forth between field and matter. Higher excited states in molecular aggregates may then be prepared and controlled by placing a sample into the beam line of one of the two entangled photons and recording the change of the coincidence count rate (19) with the other photon. It is possible to achieve higher spectral and temporal resolutions and improve spatial resolution by ghost imaging of X-ray photons.…”

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Manipulating molecules with quantum light

Kowalewski

Mukamel

2017

Proc. Natl. Acad. Sci. U.S.A.

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It was first realized by Purcell (1) that the spontaneous emission rate of a quantum system can be enhanced or suppressed by placing it in a resonant radiofrequency cavity. Spontaneous emission as it was first theoretically described by Einstein (2) is not a pure property of matter. It is described by matter coupled to quantized radiation field modes, which can be manipulated in an artificial structure such as a cavity. Cavity quantum electrodynamics (QED) is used to describe such effects that intimately depend on the fact that light is made of photons. Cavity QED has been extensively studied in atoms and the experi-A B D C mental proof was awarded with the Nobel Prize in 2012 (3). It has been applied to cooling of single atoms and for the detection of single atoms and creating and studying states with few photons and few atoms (4). In more recent developments these ideas have been extended to manipulate electronic states (5) and vibrations in molecules (6, 7). In PNAS, Flick et al. (8) introduce recent theoretical developments for the application of cavity QED to molecules and suggest possible novel applications to photochemistry. These include nonadiabatic dynamics of molecules in cavities, the modification of molecular properties, and the integration of QED with density functional theory.A quantized electromagnetic field mode can be described as a harmonic oscillator whose coordinate is the electric field displacement (Fig. 1A). The zero point energy translates into a nonvanishing field intensity ε 2 in the ground state |0 (vacuum fluctuations). The electric vacuum field increases for a small cavity volumewhere V is the cavity mode volume and ω c its frequency. Cavity QED is based on the JaynesCummings (JC) model (9), which describes the interaction of a two-level atom with a single quantized field mode:where a and σ are the annihilation operators of the field mode and the molecular excitation, respectively, and ω 0 is the excitation energy of the molecule. The atom-cavity coupling g = µε c /2 represents the interaction of the cavity field with the molecular dipole µ. The combined states of matter and field obtained from Eq. 2, known as dressed states (3) [or polaritons (10)], are shown in Fig. 1B. The new eigenvalues are split up by 2g √ n + 1, where n in the number of photons initially in the cavity and the corresponding eigenfunctions may not be solely attributed to atomic or photonic degrees of freedom

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Nonlinear optical signals and spectroscopy with quantum light

Cited by 318 publications

References 303 publications

Observing the transition from quantum to classical energy correlations with photon pairs

Observing the transition from quantum to classical energy correlations with photon pairs

Quantum cascade driving: Dissipatively mediated coherences

Manipulating molecules with quantum light

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