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Ultrafast Phenomena and Nanophotonics

Two-dimensional electronic spectroscopy of many-body correlations in quantum materials

Christoph Lienau

Published Mar 19, 2025• 0 citations
Publisher
DOI
10.1117/12.3040842

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Abstract 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.
Multidimensional spectroscopy is becoming an increasingly popular tool and there is an ongoing effort to access electronic transitions and many-body dynamics in correlated materials. We apply the protocol recently proposed by Wang [Phys. Rev. A 107, 013305 (2023)] to extract two-dimensional polaron spectra in a Fermi superfluid with an impurity. The bath is described by a BCS ansatz and it assumed that the impurity can scatter at most one quasiparticle pair. The spectral response contains a symmetric contribution, which carries the same information as Ramsey spectra, and an asymmetric one. While a priori it may seem promising to probe the quasiparticle gap from the asymmetric contribution, we show explicitly that this is not the case and, in the absence of incoherent processes, multidimensional spectroscopy does not bring much additional information. Our calculation is suitable for ultracold gases, but we discuss implications for exciton polarons in two-dimensional materials.
An up-to-date selection of applications of correlation spectroscopy, in particular as far as the mapping of properties of correlated many-body systems is concerned. The book starts with a qualitative analysis of the outcome of the two-particle correlation spectroscopy of localized and delocalized electronic systems as they occur in atoms and solids. The second chapter addresses how spin-dependent interactions can be imaged by means of correlation spectroscopy, both in spin-polarized and extended systems. A further chapter discusses possible pathways for the production of interacting two-particle continuum states. After presenting some established ways of quantifying electronic correlations and pointing out the relationship to correlation spectroscopy, the author addresses in a separate chapter the electron-electron interaction in extended systems, and illustrates the ideas by some applications to fullerenes and metal clusters. The last two chapters are devoted to the investigation of the potential of two-particle spectroscopy in studying ordered surfaces and disordered samples. Throughout the book the material is analyzed using rather qualitative arguments, and the results of more sophisticated theories serve the purpose of endorsing the suggested physical scenarios. The foundations of some of these theories have been presented in a corresponding volume entitled "Concepts of Highly Excited Electronic Systems" (3-527-40335-3).