Role of the spectral shape of quantum correlations in two-photon virtual-state spectroscopy

León‐Montiel, Roberto de J.; Svozilík, Jiří; Salazar-Serrano, Luis José; Torres, Juan P.

doi:10.1088/1367-2630/15/5/053023

Cited by 52 publications

(98 citation statements)

References 37 publications

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“…However, it turns out that the effect depends crucially on the tails of the spectral distribution in Eq. (49) (de J Leon- Montiel et al, 2013). The sinc-function in the two-photon wavefunction (51) has a long Lorentzian tail ∼ 1/ω, which covers extremely far off-resonant intermediate states.…”

Section: Two-photon Absorption Vs Two-photon-induced Fluorescencementioning

confidence: 99%

Nonlinear optical signals and spectroscopy with quantum light

2016

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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 in the joint field plus matter phase space. These are distinct from Glauber's photon counting formalism which use normally ordered products of ordinary operators in the field space. One notable advantage for spectroscopy applications is that 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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Section: Two-photon Absorption Vs Two-photon-induced Fluorescencementioning

confidence: 99%

Nonlinear optical signals and spectroscopy with quantum light

2016

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“…Applications to spectroscopy received considerable attention in experiments [6][7][8][9] as well as in theoretical works [10][11][12][13][14][15][16]. These prospects necessitate the adaption of quantum information concepts to spectroscopic applications.…”

Section: Introductionmentioning

confidence: 99%

Photon statistics of intense entangled photon pulses

Schlawin

Mukamel

2013

J. Phys. B: At. Mol. Opt. Phys.

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Time-and frequency-gated two-photon counting is given by a four-time correlation function of the electric field. This reduces to two times with purely time gating. We calculate this function for entangled photon pulses generated by parametric down-conversion. At low intensity, the pulses consist of well-separated photon pairs, and crossover to squeezed light as the intensity is increased. This is illustrated by the two-photon absorption signal of a three-level model, which scales linearly for a weak pump intensity where both photons come from the same pair, and gradually becomes nonlinear as the intensity is increased. We find that the strong frequency correlations of entangled photon pairs persist even for higher photon numbers. This could help facilitate the application of these pulses to nonlinear spectroscopy, where these correlations can be used to manipulate congested signals.

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“…This is possibly due to the fact that TPA is a third order nonlinear process in which four light fields are intertwined in complicated ways with various time intervals. Some proposed mathematical models in the literature primarily deal with the case of monochromatic excitation [10][11][12], while current studies of TPA use ultra-short laser pulse possessing with very broad spectral bandwidth. It is also necessary to consider the effect of higher order spectral phase for short pulses.…”

Section: Introductionmentioning

confidence: 99%

Spectral intensity and phase changes of short laser pulses by two-photon absorption

Tsogvoo

Myung-Whun

Munkhbaatar

2019

Journal of Modern Optics

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We calculated third order non-linear polarization to estimate the two-photon absorption of non-interacting two-level molecules in the transmission-type degenerate pump-probe geometry. The spectral intensity and the phase changes of the laser pulses when passing through a thin dielectric slab composed of the molecules were considered. We also investigated the effect of the decay rate of the molecules and the chirp of the pulses on their spectral intensity and phase changes.Since the slab is thin, we can approximate / ≈ ∆ /∆ and / ≈ ∆ /∆ .Here, ∆ (∆ ) corresponds to change of the signal intensity (phase) before the pump pulse. ∆ can be considered as the thin slab thickness . A conventional pump-probe experiments uses the self-heterodyne detection method, which measures the difference between the probe field and the reference field (or local oscillator). We are interested in obtaining the difference or change of the signals (i.e. ∆ and ∆ ). Therefore, we ignore the z-dependence of the polarization and collect the third order terms:By considering pulse -band widths much smaller than the pulse -center frequency, the intensity change ∆ and phase change (∆ ) are proportional to:∆ ( , ) ∝ [ ( ) ( , )/ * ( )]. (9)Here, the third order polarization ( ) ( , ) is depending on , the frequency of transmitted light through the material and , the time delay between pump and probe pulses. We can estimate ∆ ( , ) and ∆ ( , ) by using the Eqs. (2), (8), and (9) if the laser pulse field is known. RESULTS AND DISCUSSIONWe simulated the TPA signal of a thin dielectric slab in the conventional laser pulse pump-probe experiment. For the simulation, we used a Gaussian-shape electric field for both the pump and probe fields of which the spectrum has the following functional form:( ) = − ( − ) − ( ) . (10)

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Role of the spectral shape of quantum correlations in two-photon virtual-state spectroscopy

Cited by 52 publications

References 37 publications

Nonlinear optical signals and spectroscopy with quantum light

Nonlinear optical signals and spectroscopy with quantum light

Photon statistics of intense entangled photon pulses

Spectral intensity and phase changes of short laser pulses by two-photon absorption

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