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arXiv:2411.19070 · Photonics

Spin–Phonon Relaxation Dynamics from a Conical Intersection of Trapped Rydberg Ions

Manish Chaudhary, Rejish Nath, Weibin Li

Published Dec 2, 2024• 1 citation
arXivHTMLPDF

Abstract

Non-adiabatic processes near conical intersections are rooted in the stronger coupling between electronic and nuclear degrees of freedom. Using a system of two trapped Rydberg ions, their high polarizability and strong dipolar interactions allow to form a conical intersection, where dynamics takes place on a microsecond time scale. Rydberg lifetimes are typically from a few to tens of microseconds, which could affect the conical dynamics. We study the effect of the finite lifetime of the Rydberg state on the vibronic dynamics around the conical intersection via analyzing the master equation. Through mean field and numerical calculations, damping dynamics are found in both the phonon populations and electronic states depending on the initial states. It is found that oscillatory vibronic dynamics can be seen clearly within the Rydberg lifetime, permitting to observe the conical effect in the trapped Rydberg ion system.

DOI
10.3390/photonics11121135

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Non-adiabatic processes near conical intersections are rooted in the stronger coupling between electronic and nuclear degrees of freedom. Using a system of two trapped Rydberg ions, their high polarizability and strong dipolar interactions allow to form a conical intersection, where dynamics takes place on a microsecond time scale. Rydberg lifetimes are typically from a few to tens of microseconds, which could affect the conical dynamics. We study the effect of the finite lifetime of the Rydberg state on the vibronic dynamics around the conical intersection via analyzing the master equation. Through mean field and numerical calculations, damping dynamics are found in both the phonon populations and electronic states depending on the initial states. It is found that oscillatory vibronic dynamics can be seen clearly within the Rydberg lifetime, permitting to observe the conical effect in the trapped Rydberg ion system.
Conical intersections between electronic potential energy surfaces are paradigmatic for the study of nonadiabatic processes in the excited states of large molecules. However, since the corresponding dynamics occurs on a femtosecond timescale, their investigation remains challenging and requires ultrafast spectroscopy techniques. We demonstrate that trapped Rydberg ions are a platform to engineer conical intersections and to simulate their ensuing dynamics on larger length scales and timescales of the order of nanometers and microseconds, respectively; all this in a highly controllable system. Here, the shape of the potential energy surfaces and the position of the conical intersection can be tuned thanks to the interplay between the high polarizability and the strong dipolar exchange interactions of Rydberg ions. We study how the presence of a conical intersection affects both the nuclear and electronic dynamics demonstrating, in particular, how it results in the inhibition of the nuclear motion. These effects can be monitored in real time via a direct spectroscopic measurement of the electronic populations in a state-of-the-art experimental setup.
We study spin-phonon coupled dynamics in the vicinity of a sloped conical intersection created by laser coupling the electronic (spin) and vibrational degrees of freedom of a pair of trapped Rydberg ions. We show that the shape of the potential energy surfaces can be engineered and controlled by exploiting the sideband transitions of the crystal vibration and dipole-dipole interactions between Rydberg ions in the Lamb-Dicke regime. Using the sideband transition, we realize a sloped conical intersection whose cone axis is only tilted along one spatial axis. When the phonon wavepacket is located in the potential minimum of the lower potential surface, the spin and phonon dynamics are largely frozen owing to the geometric phase effect. When starting from the upper potential surface, the electronic and phonon states tunnel to the lower potential surface, leading to a partial revival of the initial state. In contrast, the dynamics drastically change when the initial wavepackets are away from the conical intersection. The initial state is revived, and is almost entirely irrelevant to whether it is from the lower or upper potential surface. Complete Rabi oscillations of the adiabatic states are found when the wavepacket is initialized on the upper potential surface. The dynamics occur on the microsecond and nanometer scales, implying that Rydberg ions provide a platform for simulating nonadiabatic processes in the vicinity of a sloped conical intersection.
We demonstrate coherent control of motional dynamics in trapped Rydberg ions engineered to exhibit a conical intersection between adiabatic potential-energy surfaces. Using quantum optimal control, an optimally shaped electric field drives the motional wave packet between prescribed spatial configurations on microsecond timescales. Localized nonadiabatic coupling breaks the symmetry of the dynamics and produces a directed trajectory: after only a few early passages through the conical intersection region, the packet proceeds toward the target with high fidelity. In contrast, in the Born-Oppenheimer limit, where such coupling is absent, the optimized control yields symmetric, multicycle oscillations rather than a comparably directed displacement. While both approaches reach the target at the chosen final time, the underlying trajectories are qualitatively different. This work demonstrates that engineered conical intersections can serve as a potential control resource for directional motional dynamics, complementing pulse-shaping methods in trapped-ion systems. This directional motion of the ions, enabled by the conical intersection, may provide a route toward improved control of motional states in trapped-ion quantum information processing.
Conical intersections are common in molecular physics and photochemistry, and are often invoked to explain observed reaction products. A conical intersection can occur when an excited electronic potential energy surface intersects with the ground electronic potential energy surface in the coordinate space of the nuclear positions. Theory predicts that the conical intersection will result in a geometric phase for a wavepacket on the ground potential energy surface. Although conical intersections have been observed experimentally, the geometric phase has not been observed in a molecular system. Here we use a trapped atomic ion system to perform a quantum simulation of a conical intersection. The internal state of a trapped atomic ion serves as the electronic state and the motion of the atomic nuclei are encoded into the normal modes of motion of the ions. The simulated electronic potential is constructed by applying state-dependent forces to the ion with a near-resonant laser. We experimentally observe the geometric phase on the ground-state surface using adiabatic state preparation followed by motional state measurement. Our experiment shows the advantage of combining spin and motion degrees of freedom in a quantum simulator.
Quantum simulation of interacting many-body spin systems is routinely performed with cold trapped ions, and systems with hundreds of spins have been studied in one and two dimensions. In the most common realizations of these platforms, spin degrees of freedom are encoded in low-lying electronic levels, and interactions among the spins are mediated through crystal vibrations. Here we propose a new approach which enables the quantum simulation of two-dimensional spin systems with interaction strengths that are increased by orders of magnitude. This, together with the unprecedented longevity of trapped ions, opens an avenue for the exploration of phenomena that take place on long timescales, e.g., slow and collective relaxation in frustrated and kinetically constrained systems. Our platform makes use of the strong dipolar interactions among electronic Rydberg states and planar confinement provided by a Penning trap. We investigate how the strong electric and magnetic fields that form this trap affect the properties of the Rydberg states and show that spin-spin interaction strengths on the order of MHz are achievable under experimentally realistic conditions. As a brief illustration of the capabilities of this quantum simulator, we study the entanglement in a frustrated spin system realized by three ions.
We find that energy surfaces of more than two atoms or molecules interacting via transition dipole-dipole potentials generically possess conical intersections (CIs). Typically only few atoms participate strongly in such an intersection. For the fundamental case, a circular trimer, we show how the CI affects adiabatic excitation transport via electronic decoherence or geometric phase interference. These phenomena may be experimentally accessible if the trimer is realized by light alkali atoms in a ring trap, whose interactions are induced by off-resonant dressing with Rydberg states. Such a setup promises a direct probe of the full many-body density dynamics near a CI.