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

doi:10.1038/s41377-025-01789-y

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Ultrafast pump-probe phase-randomized tomography

Original Articles

- Ultrafast pump-probe phase-randomized tomography
- Ultrafast pump-probe phase-randomized tomography
- LSA 2025年14卷第4期页码：1135-1142
- Affiliations：
  
  1.Dipartimento di Fisica, Università degli Studi di Trieste, Trieste, Italy
  2.Sincrotrone Trieste S.C.p.A., Basovizza, Italy
  3.Department of Physics, Harvard University, Cambridge, MA, USA
  4.Department of Physics, University of Erlangen-Nürnberg, Erlangen, Germany
  5.Istituto Nazionale di Fisica Nucleare, Sezione di Trieste, Trieste, Italy
- Author bio：
  
  Daniele Fausti (daniele.fausti@fau.de)
- Funds：
- DOI：10.1038/s41377-025-01789-y
  中图分类号：
- 收稿日期：2024-08-18，
  
  修回日期：2025-01-24，
  
  录用日期：2025-02-13，
  
  网络出版日期：2025-03-06，
  
  纸质出版日期：2025-04-30
- Accepted：
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Ultrafast pump-probe phase-randomized tomography[J]. LSA, 2025,14(4):1135-1142.

Glerean, F. et al. Ultrafast pump-probe phase-randomized tomography. Light: Science & Applications, 14, 1135-1142 (2025).
Ultrafast pump-probe phase-randomized tomography[J]. LSA, 2025,14(4):1135-1142. DOI： 10.1038/s41377-025-01789-y.

Glerean, F. et al. Ultrafast pump-probe phase-randomized tomography. Light: Science & Applications, 14, 1135-1142 (2025). DOI： 10.1038/s41377-025-01789-y.

摘要

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.

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references

Keimer, B. & Moore, J. E. The physics of quantum materials. Nat. Phys. 13 , 1045–1055 (2017)..

Basov, D. N., Averitt, R. D. & Hsieh, D. Towards properties on demand in quantum materials. Nat. Mater. 16 , 1077–1088 (2017)..

Fausti, D. et al. Light-induced superconductivity in a stripe-ordered cuprate. Science 331 , 189–191 (2011)..

Hu, W. et al. Optically enhanced coherent transport in YBa 2 Cu 3 O 6.5 by ultrafast redistribution of interlayer coupling. Nat. Mater. 13 , 705–711 (2014)..

Mitrano, M. et al. Possible light-induced superconductivity in K 3 C 60 at high temperature. Nature 530 , 461–464 (2016)..

Giusti, F. et al. Signatures of enhanced superconducting phase coherence in optimally doped Bi 2 Sr 2 Y 0.08 Ca 0.92 Cu 2 O 8+δ driven by midinfrared pulse excitations. Phys. Rev. Lett. 122 , 067002 (2019)..

Nova, T. F. et al. Metastable ferroelectricity in optically strained SrTiO 3 . Science 364 , 1075–1079 (2019)..

Li, X. et al. Terahertz field–induced ferroelectricity in quantum paraelectric SrTiO 3 . Science 364 , 1079–1082 (2019)..

Marciniak, A. et al. Vibrational coherent control of localized d – d electronic excitation. Nat. Phys. 17 , 368–373 (2021)..

Mukamel, S. et al. Roadmap on quantum light spectroscopy. J. Phys. B 53 , 072002 (2020)..

Lewenstein, M. et al. Generation of optical Schrödinger cat states in intense laser–matter interactions. Nat. Phys. 17 , 1104–1108 (2021)..

Pizzi, A. et al. Light emission from strongly driven many-body systems. Nat. Phys. 19 , 551–561 (2023)..

Gorlach, A. et al. High-harmonic generation driven by quantum light. Nat. Phys. 19 , 1689–1696 (2023)..

Even Tzur, M. et al. Photon-statistics force in ultrafast electron dynamics. Nat. Photonics 17 , 501–509 (2023)..

Heimerl, J. et al. Multiphoton electron emission with non-classical light. Nat. Phys. 20 , 945–950 (2024)..

Kira, M. et al. Quantum spectroscopy with Schrödinger-cat states. Nat. Phys. 7 , 799–804 (2011)..

Riek, C. et al. Direct sampling of electric-field vacuum fluctuations. Science 350 , 420–423 (2015)..

Riek, C. et al. Subcycle quantum electrodynamics. Nature 541 , 376–379 (2017)..

Benea-Chelmus, I. C. et al. Electric field correlation measurements on the electromagnetic vacuum state. Nature 568 , 202–206 (2019)..

Cosacchi, M. et al. Transiently changing shape of the photon number distribution in a quantum-dot-cavity system driven by chirped laser pulses. Phys. Rev. B 101 , 205304 (2020)..

Esposito, M. et al. Photon number statistics uncover the fluctuations in non-equilibrium lattice dynamics. Nat. Commun. 6 , 10249 (2015)..

Randi, F. et al. Probing the fluctuations of optical properties in time-resolved spectroscopy. Phys. Rev. Lett. 119 , 187403 (2017)..

Grosse, N. B. et al. Pump-probe quantum state tomography in a semiconductor optical amplifier. Opt. Express 22 , 32520–32525 (2014)..

Cheng, R. S. et al. A 100-pixel photon-number-resolving detector unveiling photon statistics. Nat. Photonics 17 , 112–119 (2023)..

Eaton, M. et al. Resolution of 100 photons and quantum generation of unbiased random numbers. Nat. Photonics 17 , 106–111 (2023)..

Glerean, F. et al. Time-resolved multimode heterodyne detection for dissecting coherent states of matter. Opt. Lett. 45 , 3498–3501 (2020)..

Allevi, A., Olivares, S. & Bondani, M. Manipulating the non-Gaussianity of phase-randomized coherent states. Opt. Express 20 , 24850–24855 (2012)..

Allevi, A. et al. Characterization of phase-averaged coherent states. J. Optical Soc. Am. B 30 , 2621–2627 (2013)..

Yuan, X. et al. Simulating single photons with realistic photon sources. Phys. Rev. A 94 , 062305 (2016)..

Valente, P. & Lezama, A. Probing single-photon state tomography using phase-randomized coherent states. J. Optical Soc. Am. B 34 , 924–929 (2017)..

Auyuanet, A. et al. Full statistics of ideal homodyne detection using real (noisy) local oscillator. J. Optical Soc. Am. B 36 , 140–145 (2019)..

Lo, H. K., Ma, X. F. & Chen, K. Decoy state quantum key distribution. Phys. Rev. Lett. 94 , 230504 (2005)..

Smith, P. R. et al. Simple source device-independent continuous-variable quantum random number generator. Phys. Rev. A 99 , 062326 (2019)..

Zhang, Y. Z., Wei, K. J. & Xu, F. H. Generalized Hong-Ou-Mandel quantum interference with phase-randomized weak coherent states. Phys. Rev. A 101 , 033823 (2020)..

Munroe, M. et al. Photon-number statistics from the phase-averaged quadrature-field distribution: theory and ultrafast measurement. Phys. Rev. A 52 , R924(R) (1995)..

Leonhardt, U. et al. Sampling of photon statistics and density matrix using homodyne detection. Opt. Commun. 127 , 144–160 (1996)..

Lvovsky, A. I. & Raymer, M. G. Continuous-variable optical quantum-state tomography. Rev. Mod. Phys. 81 , 299–332 (2009)..

Roumpos, G. & Cundiff, S. T. Photon number distributions from a diode laser. Opt. Lett. 38 , 139–141 (2013)..

Lvovsky, A. I. Iterative maximum-likelihood reconstruction in quantum homodyne tomography. J. Opt. B Quantum Semiclassical Opt. 6 , S556–S559 (2004)..

Hloušek, J. et al. Accurate detection of arbitrary photon statistics. Phys. Rev. Lett. 123 , 153604 (2019)..

Banaszek, K. Maximum-likelihood estimation of photon-number distribution from homodyne statistics. Phys. Rev. A 57 , 5013–5015 (1998)..

Glerean, F. et al. Quantum model for impulsive stimulated Raman scattering. J. Phys. B At. Mol. Optical Phys. 52 , 145502 (2019)..

Brabec, T. & Krausz, F. Intense few-cycle laser fields: frontiers of nonlinear optics. Rev. Mod. Phys. 72 , 545–591 (2000)..

Jones, D. J. et al. Carrier-envelope phase control of femtosecond mode-locked lasers and direct optical frequency synthesis. Science 288 , 635–639 (2000)..

Baltuška, A., Fuji, T. & Kobayashi, T. Controlling the carrier-envelope phase of ultrashort light pulses with optical parametric amplifiers. Phys. Rev. Lett. 88 , 133901 (2002)..

Yan, Y. X., Gamble, E. B. Jr & Nelson, K. A. Impulsive stimulated scattering: general importance in femtosecond laser pulse interactions with matter, and spectroscopic applications. J. Chem. Phys. 83 , 5391–5399 (1985)..

Merlin, R. Generating c oherent THz phonons with light pulses. Solid State Commun. 102 , 207–220 (1997)..

von Volkmann, et al. Ultrafast dynamics of coherent optical phonons in α-quartz. In: Ultrafast Phenomena XVI Springer Series in Chemical Physics , Vol. 92 (Springer, 2009).

Sparapassi, G. et al. Transient measurement of phononic states with covariance-based stochastic spectroscopy. Light Sci. Appl. 11 , 44 (2022)..

Rundquist, A. et al. Polarization-dependent detection of impulsive stimulated Raman scattering in α-quartz. J. Mod. Opt. 52 , 2501–2510 (2005)..

Johansson, J. R., Nation, P. D. & Nori, F. QuTiP 2: a python framework for the dynamics of open quantum systems. Comput. Phys. Commun. 184 , 1234–1240 (2013)..

Frérot, I. & Roscilde, T. Quantum variance: a measure of quantum coherence and quantum correlations for many-body systems. Phys. Rev. B 94 , 075121 (2016)..

Hauke, P. et al. Me asuring multipartite entanglement through dynamic susceptibilities. Nat. Phys. 12 , 778–782 (2016)..

Laurell, P. et al. Quantifying and controlling entanglement in the quantum magnet Cs 2 CoCl 4 . Phys. Rev. Lett. 127 , 037201 (2021)..

Hales, J. et al. Witnessing light-driven entanglement using time-resolved resonant inelastic X-ray scattering. Nat. Commun. 14 , 3512 (2023)..

Laubereau, A., von der Linde, D. & Kaiser, W. Direct measurement of the vibrational lifetimes of molecules in liquids. Phys. Rev. Lett. 28 , 1162–1165 (1972)..

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