Sub-cycle multidimensional spectroscopy of strongly correlated materials

Valmispild VN, Gorelov E, Eckstein M, Lichtenstein AI, Aoki H, Katsnelson MI, Ivanov MY, Smirnova O (2024)

Publication Type: Journal article

Publication year: 2024


DOI: 10.1038/s41566-023-01371-1


Strongly correlated solids are complex and fascinating quantum systems, where new electronic states continue to emerge, especially when interaction with light triggers interplay between them. In this interplay, a sub-laser-cycle electronic response is particularly attractive as a tool for the ultrafast manipulation of matter at the petahertz scale. Here we introduce a new type of nonlinear multidimensional spectroscopy, which allows us to unravel charge and energy flows in strongly correlated systems interacting with few-cycle infrared pulses and the complex interplay between different correlated states evolving on the sub-femtosecond timescale. We demonstrate that the sub-cycle spectroscopy of a single-particle electronic response is extremely sensitive to correlated many-body dynamics and provides direct access to many-body response functions. For the two-dimensional Hubbard model under the influence of ultrashort, intense electric-field transients, we resolve the sub-femtosecond pathways of charge and energy flows between localized and delocalized many-body states and the creation of a highly correlated state surviving after the end of the laser pulse. Our findings open the way towards a regime of imaging and manipulating strongly correlated materials at optical rates, beyond the multicycle approach employed in Floquet engineering, with the sub-cycle response being a key tool for accessing many-body phenomena.

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How to cite


Valmispild, V.N., Gorelov, E., Eckstein, M., Lichtenstein, A.I., Aoki, H., Katsnelson, M.I.,... Smirnova, O. (2024). Sub-cycle multidimensional spectroscopy of strongly correlated materials. Nature Photonics.


Valmispild, V. N., et al. "Sub-cycle multidimensional spectroscopy of strongly correlated materials." Nature Photonics (2024).

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