Nonlinear spectroscopy with time- and frequency-gated photon counting: A superoperator diagrammatic approach

Dorfman, Konstantin E.; Mukamel, Shaul

doi:10.1103/physreva.86.013810

Cited by 29 publications

(47 citation statements)

References 19 publications

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“…The other 'incoherent' contribution arises from the interaction with one of the two beams and scales quadratically in the pump intensity. Figure 7 depicts equation (36), where ω p is set on resonance with state f , versus the pump intensity |α| 2 .…”

Section: The Intensity Crossovermentioning

confidence: 99%

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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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Section: The Intensity Crossovermentioning

confidence: 99%

“…The time-and frequency-gated two-photon counting signal of beams a and b is given by a convolution of the 'bare signal' S B with the spectrograms W D of the two detectors [36,37],…”

Section: Time-and Frequency-gated Two-photon Countingmentioning

confidence: 99%

Photon statistics of intense entangled photon pulses

Schlawin

Mukamel

2013

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

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“…This is done to account for vacuum fluctuations caused by other field modes. However, we have recently shown [33] how the multipoint correlation function of the field is calculated in the joint field plus matter space given by the sum over Liouville space pathways. This microscopic method can account for all the effects of multiple vacuum modes by theses paths without adding a Langevin noise source.…”

Section: Discussionmentioning

confidence: 99%

“…[19], these commutator terms are not negligible and they are not properly incorporated in the filtering theory. Using the present superoperator approach formulated in the joint field plus matter space analysis we have earlier demonstrated that commutator terms are necessary for computing the relevant components of the nonlinear susceptibility in the parametric down conversion generation [33]. Furthermore, this approach allows to express all the correct features of the multipoint field correlation func-…”

Section: Simulationsmentioning

confidence: 97%

“…1. In particular we apply the formalism of [18] to calculate Nth order photon correlation measurements generated by a fluctuating oscillator model that represents a generic molecular system with energy and electron transport. The connection with real molecules makes time-andfrequency gated photon counting a practical spectroscopic tool for studying material systems by analyzing correlated optical signals.…”

Section: Introductionmentioning

confidence: 99%

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Time-and-frequency-gated photon coincidence counting; a novel multidimensional spectroscopy tool

Dorfman

Mukamel

2016

Phys. Scr.

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Coherent multidimensional optical spectroscopy techniques are broadly applied across the electromagnetic spectrum ranging from NMR to the UV. These reveal properties of matter through correlation plots of signal fields generated in response to sequences of short pulses with variable delays. Here we discuss a new class of multidimensional techniques obtained by time-and-frequency resolved photon coincidence counting measurements of N photons which constitutes a 2N dimensional spectrum. A compact description of these signals is developed based on time ordered superoperators rather than the normally ordered ordinary operators used in Glauber's photon counting formalism.The independent control of the time and frequency gate parameters reveals details of matter dynamics not available otherwise. Application to an anharmonic oscillator model with fluctuating energy and anharmonicity demonstrates the power of these signals.

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Quantum Susceptibilities in Time‐Domain Sampling of Electric Field Fluctuations

Kizmann

Moskalenko

Leitenstorfer

et al. 2022

Laser & Photonics Reviews

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Electro‐optic sampling has emerged as a new quantum technique enabling measurements of electric field fluctuations on subcycle time scales. In a second‐order nonlinear material, the fluctuations of a terahertz field are imprinted onto the polarization properties of an ultrashort probe pulse in the near infrared. The statistics of this time‐domain signal are calculated, incorporating the quantum nature of the involved electric fields right from the beginning. A microscopic quantum theory of the electro‐optic process is developed adopting an ensemble of noninteracting three‐level systems as a model for the nonlinear material. It is found that the response of the nonlinear medium can be separated into a conventional part, which is exploited also in sampling of coherent amplitudes, and quantum contributions, which are independent of the state of the terahertz input. Interactions between the three‐level systems which are mediated by terahertz vacuum fluctuations are causing this quantum response. Conditions under which the classical response serves as a good approximation of the electro‐optic process are also determined and how the statistics of the sampled terahertz field can be reconstructed from the electro‐optic signal is demonstrated. In a complementary regime, electro‐optic sampling can serve as a spectroscopic tool to study the pure quantum susceptibilities of matter.

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Nonlinear spectroscopy with time- and frequency-gated photon counting: A superoperator diagrammatic approach

Cited by 29 publications

References 19 publications

Photon statistics of intense entangled photon pulses

Photon statistics of intense entangled photon pulses

Time-and-frequency-gated photon coincidence counting; a novel multidimensional spectroscopy tool

Quantum Susceptibilities in Time‐Domain Sampling of Electric Field Fluctuations

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