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arXiv:2604.11984

High-harmonic generation in systems with chiral Bloch states: application to rhombohedral graphene

Jessica O. de Almeida, Wilton J. M. Kort-Kamp, Mathias S. Scheurer

cond-mat.mes-hallphysics.opticsquant-phSubmitted Apr 13, 2026• Announced Apr 15, 2026
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Abstract

Nonlinear light-matter interaction and, in particular, high-harmonic generation (HHG) are fundamentally interesting and frequently discussed as versatile probes of quantum materials with potential for optical information processing applications. Meanwhile, there has also been significant progress in graphene-based multilayer systems to engineer interesting band structures and boost correlation effects. Motivated by the successful demonstration of HHG in graphene, we here study this effect in rhombohedral stacks of $n$ layers of graphene, a recent very prominent representative of correlated multilayer graphene systems. We show how the chiral Bloch states of the valleys of this system crucially affect the HHG. The "winding" of the Bloch states scales linearly with $n$, just like the dominant harmonic order. The location of the strongest quantum geometry in momentum space on a ring of finite radius is shown to be imprinted on the time-dependent momentum distribution at the beginning of the strong laser pulse. We further demonstrate that the presence of an interaction-induced splitting of the two valleys leads to a complex interplay of the opposite chiralities of the two valleys, directly visible in the $n$ dependence of the circular dichroism. We also analyze the impact of doping and identify a quantity that tracks the net chirality of the occupied states. Our findings show that rhombohedral graphene constitutes a promising platform for exploring rich nonlinear optical phenomena.

Comments
17 pages, 10 figures

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High harmonic generation (HHG) has emerged as a powerful probe of ultrafast electron dynamics in solids. However, in strongly correlated materials, where electronic excitations arise from many-body interactions rather than single-particle band dispersion, the field remains in its infancy. Here, we report HHG up to the 23rd^{rd}rd order in the prototypical Mott insulator La2_22​CuO4_44​. We observe a robust 4 eV cutoff that is independent of driving field strength, revealing an intrinsic energy scale defined by the Hubbard bands. Using time-resolved high harmonic spectroscopy, we disentangle the distinct contributions of carrier creation, intraband acceleration, and interband recombination to the nonequilibrium radiation spectrum. We demonstrate that photo-doping triggers a fundamental reorganization of the many-body manifolds above a critical excitation density, a process that renormalizes the band curvature and suppresses nonlinear intraband currents, thereby directly imprinting the signature of many-body band reconstruction onto the harmonic emission. These results establish HHG as a sensitive probe of subtle correlation-driven electronic reconstructions and highlight that many-body interactions enable extreme nonlinear optical responses that are highly tunable in nonequilibrium states.