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arXiv:2411.08855 · Light Science & Applications

Ultrafast pump-probe phase-randomized tomography

Filippo Glerean, Enrico Maria Rigoni, Giacomo Jarc, Shahla Yasmin Mathengattil, Angela Montanaro, Francesca Giusti, Matteo Mitrano, Fabio Benatti, Daniele Fausti

Published Mar 6, 2025• 4 citations
arXivHTMLPDF

Abstract

Measuring fluctuations in matter's low-energy excitations is the key to unveiling the nature of the non-equilibrium response of materials. A promising outlook in this respect is offered by spectroscopic methods that address matter fluctuations by exploiting the statistical nature of light-matter interactions with weak few-photon probes. Here we report the first implementation of ultrafast phase randomized tomography, combining pump-probe experiments with quantum optical state tomography, to measure the ultrafast non-equilibrium dynamics in complex materials. Our approach utilizes a time-resolved multimode heterodyne detection scheme with phase-randomized coherent ultrashort laser pulses, overcoming the limitations of phase-stable configurations and enabling a robust reconstruction of the statistical distribution of phase-averaged optical observables. This methodology is validated by measuring the coherent phonon response in α-quartz. By tracking the dynamics of the shot-noise limited photon number distribution of few-photon probes with ultrafast resolution, our results set an upper limit to the non-classical features of phononic state in α-quartz and provide a pathway to access non-equilibrium quantum fluctuations in more complex quantum materials.

DOI
10.1038/s41377-025-01789-y

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Measuring fluctuations in matter's low-energy excitations is the key to unveiling the nature of the non-equilibrium response of materials. A promising outlook in this respect is offered by spectroscopic methods that address matter fluctuations by exploiting the statistical nature of light-matter interactions with weak few-photon probes. Here we report the first implementation of ultrafast phase randomized tomography, combining pump-probe experiments with quantum optical state tomography, to measure the ultrafast non-equilibrium dynamics in complex materials. Our approach utilizes a time-resolved multimode heterodyne detection scheme with phase-randomized coherent ultrashort laser pulses, overcoming the limitations of phase-stable configurations and enabling a robust reconstruction of the statistical distribution of phase-averaged optical observables. This methodology is validated by measuring the coherent phonon response in α-quartz. By tracking the dynamics of the shot-noise limited photon number distribution of few-photon probes with ultrafast resolution, our results set an upper limit to the non-classical features of phononic state in α-quartz and provide a pathway to access non-equilibrium quantum fluctuations in more complex quantum materials.
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We introduce an algorithm for reconstructing high-dimensional multimode Gaussian quantum states, which are completely characterized by the covariance matrix of the quadratures of fully distinguishable pulses. The reconstruction is achieved by orthogonalizing the overlapping time windows of the correlation measurement in post-processing. We compare a homodyne-based implementation to electro-optic sampling and develop an optimization scheme for the latter, to mitigate the shot noise in the non-perturbative regime of strong nonlinear interactions. Furthermore, we derive the full-counting statistics of the field-correlation measurement and theoretically demonstrate the reconstruction of pulsed Fock states. This opens an avenue to the full tomography of highly multimode non-Gaussian states. In the third and last step, we derive a formalism to simplify the description of the up-conversion required in electro-optic sampling. 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The rich structure of pulsed quantum states of light can be a powerful resource, but also challenging to operate with, in theory as well as in experiment. The characterization methods and theoretical tools developed in this thesis, tailored to pulsed quantum light and the nonlinear interaction thereof, can pave the way to the application of this resource to fundamental research as well as quantum technologies.
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The variance of the time dependent atomic positions and momenta is directly mapped into the quantum uctuations of the photon number of the scattered probing light. A fully quantum de-scription of the non-linear interactions between photonic and phononic fields unveils evidences of squeezing of thermal phonons. In here a pump-probe spectroscopy was proposed to observe phonon squeezing in solids. Numerical simulation showed pump-probe response due to coherent phonon and squeezed phonon in alpha-quartz.