Spectroscopy reveals what a system is made of and how its parts interact. Multidimensional spectroscopy correlates signals along several time or frequency axes to expose couplings and coherences that single spectra hide, while spectroscopic imaging adds spatial information. This retrospective Collection brings together influential research recently published across the Physical Review portfolio, from single atoms to quantum materials and extreme matter. All the papers in the collection have undergone our standard peer-review process.

Our editors have curated this Collection in collaboration with the Division of Chemical Physics of the American Physical Society. We invite readers to attend the associated Focus Session “Spectroscopic Imaging and Multidimensional Spectroscopy” at the APS Global Physics Summit 2027 in Atlanta.

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Multidimensional Spectroscopy Across Scales

Multidimensional spectroscopy correlates signals along several time or frequency axes, separating effects that single spectra blur. These papers show how the approach reveals collective behavior and nonlinear dynamics across scales, from atoms to quantum materials, and how quantum resources and quantum computing are beginning to extend it.

Collective resonances of two atoms revealed by zero-quantum two-dimensional coherent spectroscopy
Lexter R. Savio, Ashmita Shah, and Hebin Li
Phys. Rev. A 114, 022825 (2026)

Revealing collective nonradiative coherence with anomalous sidebands in zero-quantum two-dimensional coherent spectroscopy of alkali-metal atoms
YiFeng Geng, Can Ma, Zhong Zuo, SongPo Xu, LinQiang Hua, ShaoGang Yu, and XiaoJun Liu
Phys. Rev. A 114, 022824 (2026)

Two-Dimensional Electronic Spectroscopy with Intense Entangled-Photon Beams
Deependra Jadoun, Upendra Harbola, Vladimir Y. Chernyak, and Shaul Mukamel
Phys. Rev. Lett. 135, 223803 (2025)

Observation of cupratelike nonlinear terahertz responses in superconducting infinite-layer nickelates via two-dimensional coherent spectroscopy
Bing Cheng, Di Cheng, Kyuho Lee, Martin Mootz, Chuankun Huang, Liang Luo, Zhuoyu Chen, Yonghun Lee, Bai Yang Wang, Ilias E. Perakis, Zhi-Xun Shen, Harold Y. Hwang, and Jigang Wang
Phys. Rev. B 111, 014519 (2025)

Anomalous electronic energy relaxation and soft phonons in the Dirac semimetal Cd3As2
Rishi Bhandia, David Barbalas, Run Xiao, Juan R. Chamorro, Tanya Berry, Tyrel M. McQueen, Nitin Samarth, and N. P. Armitage
Phys. Rev. B 110, 075131 (2024)

Accelerating two-dimensional electronic spectroscopy simulations with a probe qubit protocol
José D. Guimarães, James Lim, Mikhail I. Vasilevskiy, Susana F. Huelga, and Martin B. Plenio
Phys. Rev. Research 7, 023130 (2025)

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Four-Wave Mixing as the Common Engine

Four-wave mixing, in which three input fields drive a system to emit a fourth, underlies many nonlinear and multidimensional spectroscopies, making it their common engine. These papers follow it across energy scales, from peV in spin dynamics, to meV in molecular vibrations, to eV in electron correlation, about a dozen orders of magnitude in all.

Four-Wave Mixing at peV Energy Scales
C. Simon, D. M. Silevitch, and T. F. Rosenbaum
Phys. Rev. Lett. 134, 086705 (2025)

Spectral-focusing coherent anti-Stokes Raman scattering driven by bright correlated twin beams
Yujiro Eto, Mutsuo Nuriya, and Hideaki Kano
Phys. Rev. Applied 23, 064015 (2025)

Extracting doubly excited state lifetimes in helium directly in the time domain with attosecond noncollinear four-wave-mixing spectroscopy
Patrick Rupprecht, Nicolette G. Puskar, Daniel M. Neumark, and Stephen R. Leone
Phys. Rev. Research 6, 043100 (2024)

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Spectroscopy Becomes Imaging

Spectral information gains spatial structure. These papers show how spectroscopic contrast becomes images and maps of dynamics, composition, and quantum states, in settings from soft matter and extreme conditions to quantum materials and energy devices, and through new imaging modalities.

Displacement field visualization of particle beds after slow impacts using diffusing wave spectroscopy
Tetyana Bila, Gerhard Wurm, and Jonathan E. Kollmer
Phys. Rev. E 112, 015414 (2025)

Measurement of turbulent velocity and bounds for thermal diffusivity in laser shock compressed foams by x-ray photon correlation spectroscopy
Charles Heaton, Hao Yin, Dimitri Khaghani, Hae Ja Lee, Hannah Poole, Eric Blackman, Nina Boiadjieva, Xiaoqian M. Chen, Celine Crépisson, Gilbert W. Collins, Adrien Descamps, Arianna E. Gleason, Christian Gutt, Alexander N. Petsch, Lisa Randolph, Silke Nelson, Peregrine McGehee, Rajan Plumley, Christopher Spindloe, Thomas Stevens, Charlotte Stuart, Joshua J. Turner, Hussein Aluie, Jessica K. Shang, and Gianluca Gregori
Phys. Rev. E 112, 045218 (2025)

Impact of the Annealing Temperature on the Local Se Distribution and Optical Properties in CdSexTe1−x Solar Cells by Multimodal X-ray Microscopy
Jackson L. Barp, Jr., Gero Falkenberg, Giovanni Fevola, Svenja Patjens, Niklas Pyrlik, Sven Hampel, Eric Colegrove, Andrea Mathew, Jan Garrevoet, Gerald Falkenberg, Christian Strelow, Tobias Kipp, Christian G. Schroer, and Michael E. Stuckelberger
PRX Energy 5, 033011 (2026)

Imaging Quantum Interference in a Monolayer Kitaev Quantum Spin Liquid Candidate
Y. Kohsaka, S. Akutagawa, S. Omachi, Y. Iwamichi, T. Ono, I. Tanaka, S. Tateishi, H. Murayama, S. Suetsugu, K. Hashimoto, T. Shibauchi, M. O. Takahashi, S. Nikolaev, T. Mizushima, S. Fujimoto, T. Terashima, T. Asaba, Y. Kasahara, and Y. Matsuda
Phys. Rev. X 14, 041026 (2024)

Mid-Infrared Energy Deposition Spectroscopy
Jiaze Yin, Christian Pfluegl, Chu C. Teng, Rylie Bolarinho, Guo Chen, Xinrui Gong, Dashan Dong, Daryoosh Vakhshoori, and Ji-Xin Cheng
Phys. Rev. Lett. 134, 093804 (2025)

Local, mm-scale H1 magnetic resonance imaging using atomic vapors
Sven Bodenstedt, Morgan W. Mitchell, and Michael C. D. Tayler
Phys. Rev. Applied 26, 014095 (2026)

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