Theory of multiple quantum coherence signals in dilute thermal gases

Ames, Benedikt; Carnio, Edoardo G.; Shatokhin, Vyacheslav; Buchleitner, Andreas

doi:10.1088/1367-2630/ac4054

Cited by 5 publications

(3 citation statements)

References 51 publications

(257 reference statements)

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“…1(A). 2QC signatures have been previously observed in alkali vapors at similar densities, but at higher temperatures, and they have been attributed to interparticle interactions [15][16][17]. We thus interpret the mere existence of the observed 2QC peak as signature of interacting 7 Li atoms or atom pairs.…”

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confidence: 75%

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Two-dimensional electronic spectroscopy of an ultracold gas

Landmesser¹,

Sixt²,

Dulitz³

et al. 2022

Preprint

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Femtosecond coherent multidimensional spectroscopy is demonstrated for an ultracold gas. For this, a setup for phase modulation spectroscopy is used to probe the 3 2 S 1/2 − 2 2 P 1/2,3/2 transition in a 800 µK-cold sample of 7 Li atoms confined in a magneto-optical trap. The observation of a double quantum coherence response, a signature of interparticle interactions, paves the way for detailed investigations of few-and many-body effects in ultracold atomic and molecular gases using this technique. The experiment combines a frequency resolution of 3 GHz with a potential time resolution of 200 fs, which allows for high-resolution studies of ultracold atoms and molecules both in the frequency and in the time domain.

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supporting

confidence: 75%

“…multi-excitonic states [14]. This property has been used to gain access to interparticle interactions in thermal atomic vapors, where cooperative effects are otherwise covered by inhomogeneous broadenings [15][16][17].…”

mentioning

confidence: 99%

Two-dimensional electronic spectroscopy of an ultracold gas

Landmesser¹,

Sixt²,

Dulitz³

et al. 2022

Preprint

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“…A number of femtosecond 4WM experiments revealed that richer information on the photoinduced dynamics in atomic vapors, − polyatomic chromophores, − multichromophore aggregates, − and nanosystems − can be obtained by applying more intense laser pulses (see refs − for reviews). On the theoretical side, a variety of simulations of 4WM signals beyond the limit of weak system–field coupling have been reported. ,,,,− Single-molecule femtosecond spectroscopy of individual chromophores − and antenna complexes , also usually requires strong pulses. Nonlinear spectroscopy in nanocavities, in which material systems are strongly coupled to vacuum cavity electromagnetic modes, has become a booming research field recently. − …”

Section: Nonperturbative Calculation Of the Nonlinear Polarizationmentioning

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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Double-quantum spectroscopy of dense atomic vapors: Interplay between Doppler and self-broadenings

Falvo

2023

The Journal of Chemical Physics

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In this article, we present a simulation study of the linear and nonlinear spectroscopy of dense atomic vapors. Motivated by recent experiments, we focus on double quantum spectroscopy, which directly probes dipole–dipole interactions. By explicitly including thermal velocity, we show that temperature has an important impact on the self-broadening mechanisms of the linear and nonlinear spectra. We also provide analytical expressions for the response functions in the short time limit using the two-body approximation, which shows that double quantum spectroscopy for atomic vapors directly probes the transition amplitude of the electronic excitation between two atoms. We also propose an expression for the double quantum spectrum that includes the effect of Doppler broadening, and we discuss the effect of density on the spectrum. We show that when Doppler broadening is negligible compared to self-broadening, the double quantum spectrum scales with the atomic density, while when Doppler broadening dominates, it scales as the square of the density.

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Theory of multiple quantum coherence signals in dilute thermal gases

Cited by 5 publications

References 51 publications

Two-dimensional electronic spectroscopy of an ultracold gas

Two-dimensional electronic spectroscopy of an ultracold gas

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

Double-quantum spectroscopy of dense atomic vapors: Interplay between Doppler and self-broadenings

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