Multidimensional four-wave mixing signals detected by quantum squeezed light

Dorfman, Konstantin E.; Liu, Shengshuai; Lou, Yanbo; Wei, Tianxiang; Jing, Jietai; Schlawin, Frank; Mukamel, Shaul

doi:10.1073/pnas.2105601118

Cited by 14 publications

(7 citation statements)

References 34 publications

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“…Hence, such a state is optimal for the ETPA cross section. Conversely, the entangled state shows the smallest variation at ϕ = π/2 (not shown), where it coincides with the product state (25).…”

Section: Orientational Averagementioning

confidence: 93%

“…Their strong quantum correlations could circumvent certain classical Fourier uncertainties and thus enhance the sensing capabilities of optical measurements [8][9][10][11][12][13][14][15][16]. The detection of quantum correlations could also provide new spectroscopic information [17][18][19][20][21][22][23][24][25], and the use of quantum light in interferometric setups promises additional control knobs to analyze spectroscopic information [26][27][28][29] as well as access to out-of-time correlations [30]. The main driving force behind this development of entangled photon spectroscopy, however, is the linear scaling of nonlinear optical signals such as the two-photon absorption (TPA) rate with the incident photon flux [31][32][33][34], which could enable measurements on photosensitive samples at reduced photon numbers.…”

Section: Introductionmentioning

confidence: 99%

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Polarization-Entangled Two-Photon Absorption in Inhomogeneously Broadened Ensembles

Schlawin

2022

Front. Phys.

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Entangled photons are promising candidates for a variety of novel spectroscopic applications. In this paper, we simulate two-photon absorption (TPA) of entangled photons in a molecular ensemble with inhomogeneous broadening. We compare our results with a homogeneously broadened case and comment on the consequences for the possible quantum enhancement of TPA cross sections. We find that, while there are differences in the TPA cross section, this difference always remains small and of the order unity. We further consider the impact of the polarization degrees of freedom and carry out the orientational average of a model system Hamiltonian. We find that certain molecular geometries can give rise to a substantial polarization dependence of the entangled TPA rate. This effect can increase the TPA cross section by up to a factor of five.

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Section: Orientational Averagementioning

confidence: 93%

Section: Introductionmentioning

confidence: 99%

Polarization-Entangled Two-Photon Absorption in Inhomogeneously Broadened Ensembles

Schlawin

2022

Front. Phys.

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“…The EOM methods do not impose any restrictions on the system Hamiltonian, which can be any (possibly time-dependent) operator. With slight modifications, the EOM methods can, therefore, be applied for the simulation of signals of multidimensional IR, , mixed IR/vis, TRPES, ,− attosecond, X-ray, , cavity-QED, and quantum light , spectroscopies.…”

Section: Summary and Perspectives Of Spectroscopic Equation-of-motion...mentioning

confidence: 99%

Equation-of-Motion Methods for the Calculation of Femtosecond Time-Resolved 4-Wave-Mixing and N-Wave-Mixing Signals

2022

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Femtosecond nonlinear spectroscopy is the main tool for the time-resolved detection of photophysical and photochemical processes. Since most systems of chemical interest are rather complex, theoretical support is indispensable for the extraction of the intrinsic system dynamics from the detected spectroscopic responses. There exist two alternative theoretical formalisms for the calculation of spectroscopic signals, the nonlinear response-function (NRF) approach and the spectroscopic equation-of-motion (EOM) approach. In the NRF formalism, the system–field interaction is assumed to be sufficiently weak and is treated in lowest-order perturbation theory for each laser pulse interacting with the sample. The conceptual alternative to the NRF method is the extraction of the spectroscopic signals from the solutions of quantum mechanical, semiclassical, or quasiclassical EOMs which govern the time evolution of the material system interacting with the radiation field of the laser pulses. The NRF formalism and its applications to a broad range of material systems and spectroscopic signals have been comprehensively reviewed in the literature. This article provides a detailed review of the suite of EOM methods, including applications to 4-wave-mixing and N-wave-mixing signals detected with weak or strong fields. Under certain circumstances, the spectroscopic EOM methods may be more efficient than the NRF method for the computation of various nonlinear spectroscopic signals.

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“…In a report in PNAS, Dorfman et al (9) have generalized this to the context of nonlinear optical spectroscopy of materials, where they achieved superior precision and accuracy in comparison with the classical analogs. Most material systems are composed of manifolds of excited states, whose dynamics following photoexcitation determine their photophysical properties.…”

mentioning

confidence: 99%

“…The paper by Dorfman et al (9) represents another important milestone along the road to the full exploitation of the quantum advantage in nonlinear optical spectroscopy. In this field, theory is well ahead of experiments, and a lot of schemes still remain to be demonstrated and applied to a variety of fields ranging from biology to solid-state physics.…”

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confidence: 99%