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Nanophotonics

Coherent control of symmetry breaking in transverse‐field Ising chains using few‐cycle pulses

Nikolai D. Klimkin, Alexey N. Rubtsov, Misha Ivanov

Published Feb 28, 2023• 2 citations
Publisher

Abstract

Coherent control of quantum systems with phase-stable pulses offers enticing new opportunities for lightwave electronics. Here we extend this approach to many-body systems with spin degrees of freedom, demonstrating that a single few-cycle control pulse can create a sizable population asymmetry between the two degenerate polar ground states of the Ising model. This opens a route for femtosecond-scale data processing and storage, allowing one to control the final ground state of a correlated system in an all-optical way.

DOI
10.1515/nanoph-2022-0811

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Coherent control of quantum systems with phase-stable pulses offers enticing new opportunities for lightwave electronics. Here we extend this approach to many-body systems with spin degrees of freedom, demonstrating that a single few-cycle control pulse can create a sizable population asymmetry between the two degenerate polar ground states of the Ising model. This opens a route for femtosecond-scale data processing and storage, allowing one to control the final ground state of a correlated system in an all-optical way.
Weak-field coherent phase control of atomic non-resonant multiphoton excitation induced by shaped femtosecond pulses is studied theoretically in the single-cycle regime. The carrier-envelope phase (CEP) of the pulse, which in the multi-cycle regime does not play any control role, is shown here to be a new effective control parameter that its effect is highly sensitive to the spectral position of the ultrabroad spectrum. Rationally chosen position of the ultrabroadband spectrum coherently induces several groups of multiphoton transitions from the ground state to the excited state of the system: transitions involving only absorbed photons as well as Raman transitions involving both absorbed and emitted photons. The intra-group interference is controlled by the relative spectral phase of the different frequency components of the pulse, while the inter-group interference is controlled jointly by the CEP and the relative spectral phase. Specifically, non-resonant two- and three-photon excitation is studied in a simple model system within the perturbative frequency-domain framework. The developed intuition is then applied to weak-field multiphoton excitation of atomic cesium (Cs), where the simplified model is verified by non-perturbative numerical solution of the time-dependent Schrödinger equation. We expect this work to serve as a basis for a new line of femtosecond coherent control experiments.
Coherent control of the atomic two-photon absorption with shaped single-cycle pulses is examined theoretically in the weak-field regime. The control over the stabilized carrier-envelope phase (CEP) of the pulses is determined as a key parameter allowing the full utilization of the ultrabroad pulse spectrum. This bandwidth is sufficient to provide besides the sequential two-photon pathways, additional Raman-type pathways coupling between the ground and the excited states. The interference between the different pathways is efficiently controlled via the control over the CEP. Simplified two-level model is analyzed in the frequency domain where the rational pulse shaping is applied. The developed intuition is applied to atomic Cs and verified by the exact numerical solution of time-dependent Schrodinger equation.
In the regime of resonant coherent light-matter interaction, light pulses may interact with each other indirectly via a polarization wave created by the other pulse. We show that such interaction allows fast creation and erasing of high-contrast dynamic population density gratings, as well as control of their period in a few-cycle regime. Our scheme uses counter-propagating optical pulses, which do not cross each other in the medium. The mechanism is able to work with pulse durations up to the single-cycle limit. Somewhat surprisingly, ultrafast grating wave vector control requires the generation of polarization waves with the phase velocity much smaller than that of light.
We present and experimentally demonstrate for the first time the observation and femtosecond coherent control over the temporal evolution of a transient population that is excited via nonresonant two-photon absorption. Based on symmetry properties of the two-photon absorption process, the exciting femtosecond pulses are phase-shaped to photoinduce different evolutions of the transient excited population for a given final excited population. As a study case, we focus here on the attractive case of two-photon dark pulses that, although inducing zero final population (hence, the terminology of "dark pulses"), they induce a transient excited population during the pulse irradiation that can significantly deviate from zero. This nonzero transient population can be viewed as the bright side of such dark pulses. The symmetry-based coherent control is demonstrated first with dark pulses that we shape to induce transient excited population that at all times is kept below different target levels. Then, it is further demonstrated with pairs of dark pulses where one is rationally shaped to induce temporal evolution of the transient excited population that is the inverse of the evolution induced by the other. The work is conducted in the weak-field regime with the sodium atom as the model system. The approach developed here is general, conceptually simple, and very effective.
Coherent control of resonant and non-resonant two-photon absorption processes was examined using a spatio-temporal pulse-shaping technique. By utilizing a combination of temporal focusing and femtosecond pulse-shaping techniques, we spatially control multiphoton absorption processes in a completely deterministic manner. Distinctive symmetry properties emerge through two-dimensional mapping of spatio-temporal data. These symmetries break down in the transition to strong fields, revealing details of strong-field effects such as power broadenings and dynamic Stark shifts. We also present demonstrations of chirp-dependent population transfer in atomic rubidium, as well as the spatial separation of resonant and non-resonant excitation pathways in atomic caesium.