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Low-Dimensional Materials and Devices

Strong-field-driven dynamics and high-harmonic generation in interacting 1D systems (Conference Presentation)

Sandra de Vega, Joel D. Cox, Fernando Sols, F. Javier Garcı́a de Abajo

Published Sep 9, 2019• 0 citations
Publisher
DOI
10.1117/12.2529209

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High-harmonic generation (HHG) is a prototypical strong-field process in which intense light drives matter to emit radiation at integer multiples of the driving frequency. Extending HHG into the quantum-optical regime offers new opportunities to probe and control strongly nonlinear light-matter interactions using nonclassical states of light. Yet describing this regime requires a fully quantum treatment of the correlated electron-photon dynamics, which becomes computationally challenging for broadband, strongly squeezed fields. Here we solve the quantum-electrodynamical dynamics of a two-level system driven by bright squeezed vacuum in a converged multimode Hilbert space. Both the driving field and emitted harmonics are fully quantized, with the light-matter interaction treated nonperturbatively. This enables direct access to the multimode quantum state and its higher-order correlations beyond semiclassical sampling or perturbative descriptions. We show that squeezed-vacuum driving produces harmonic emission with qualitatively distinct second- and third-order photon correlations compared with coherent excitation. Moreover, back-action from the driven emitter strongly reshapes the incident squeezed field, generating pronounced Wigner-function negativities that evolve on attosecond timescales. Our results establish a fully quantum framework for broadband strong-field dynamics with squeezed light and provide a route to predicting and interpreting quantum-HHG experiments and their extension to more complex emitters.
We experimentally observe a new type of quantum-path interference, in two-dimensions (2D-QPI), in high-harmonic generation (HHG) driven by an orthogonally-polarised highly-bichromatic field. This regime is marked by comparable intensities of the two orthogonal colours. In this highly-bichromatic regime, we demonstrate that 2D-QPI is encoded in the measured harmonic intensity modulations with respect to the relative phase of the two-colour field. The modulations of the odd-order harmonics show a monomodal behaviour, whereas the even harmonics are modulated in a bimodal structure. Our calculations using the strong-field approximation and saddle-point method disentangle contributions from multiple quantum orbits in this HHG regime, revealing that the dipole response for both odd and even harmonics inherits the dynamic symmetry of the orthogonally-polarised driving field. This new type of 2D-QPI offers a novel route to HHG spectroscopy of attosecond electron dynamics by lifting up the dimensionality of the quantum paths involved in the interference.
For decades, most research of high harmonic generation (HHG) considered matter as quantum but light as classical. Recently, HHG driven by quantum states of light such as bright squeezed vacuum was predicted to reach beyond the classical HHG cutoff. Moreover, in squeezed coherent illumination, it was shown that the underlying dynamics are significantly modified by the photon statistics effective force. Here we show that HHG driven by quantum light results in quantum high harmonics. We derive a formula for the quantum state of the high harmonics, when driven by arbitrary quantum light states, and then explore specific cases of experimental relevance. Specifically, for a moderately squeezed pump, HHG driven by squeezed coherent light results in squeezed high harmonics. Harmonic squeezing is optimized by syncing ionization times with the pump's squeezing phase. Beyond this regime, as pump squeezing is increased, the harmonics initially acquire squeezed thermal photon statistics, and then occupy an intricate quantum state which strongly depends on the semiclassical nonlinear response function of the interacting system. Our results pave the way for generation of squeezed extreme-ultraviolet ultrashort pulses, and more generally, quantum frequency conversion into previously inaccessible spectral ranges, which may enable ultrasensitive attosecond metrology. Published by the American Physical Society 2024