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arXiv:2512.22912

Controlling Nonadiabatic Transitions Through Engineered Ultrafast Laser Fields at Conical Intersections

Xuanchao Zhang, Yang-Cheng Ye, Panpan Zhang, Xiangmei Duan, R. J. Dwayne Miller, Fulu Zheng, Ajay Jha, Hong-Guang Duan

quant-phphysics.opticsSubmitted Dec 28, 2025• Announced Dec 30, 2025• Revised Jan 1, 2026 (v2)
v1 · Dec 28, 2025v2 · Jan 1, 2026
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Abstract

In this paper, we investigate coherent control of nonadiabatic dynamics at a conical intersection (CI) using engineered ultrafast laser pulses. Within a model vibronic system, we tailor pulse chirp and temporal profile and compute the resulting wave-packet population and coherence dynamics using projections along the reaction coordinate. This approach allows us to resolve the detailed evolution of wave-packets as they traverse the degeneracy region with strong nonadiabatic coupling. By systematically varying pulse parameters, we demonstrate that both chirp and pulse duration modulate vibrational coherence and alter branching between competing pathways, leading to controlled changes in quantum yield. Our results elucidate the dynamical mechanisms underlying pulse-shaped control near conical intersections and establish a general framework for manipulating ultrafast nonadiabatic processes.

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Coherent control of bond making: the performance of rationally phase-shaped femtosecond laser pulses*

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In this paper, we investigate coherent control of nonadiabatic dynamics at a conical intersection (CI) using engineered ultrafast laser pulses. Within a model vibronic system, we tailor pulse chirp and temporal profile and compute the resulting wave-packet population and coherence dynamics using projections along the reaction coordinate. This approach allows us to resolve the detailed evolution of wave-packets as they traverse the degeneracy region with strong nonadiabatic coupling. By systematically varying pulse parameters, we demonstrate that both chirp and pulse duration modulate vibrational coherence and alter branching between competing pathways, leading to controlled changes in quantum yield. Our results elucidate the dynamical mechanisms underlying pulse-shaped control near conical intersections and establish a general framework for manipulating ultrafast nonadiabatic processes.
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.
High Resolution Image Download MS PowerPoint Slide Conical intersections are crossing points or lines between two or more adiabatic electronic potential energy surfaces in the multidimensional coordinate space of colliding atoms and molecules. Conical intersections and corresponding nonadiabatic coupling can greatly affect molecular dynamics and chemical properties. In this paper, we predict significant or measurable nonadiabatic effects in an ultracold atom–ion charge-exchange reaction in the presence of laser-induced conical intersections (LICIs). We investigate the fundamental physics of these LICIs on molecular reactivity under unique conditions: those of relatively low laser intensity of 10 8 W/cm 2 and ultracold temperatures below 1 mK. We predict irregular interference effects in the charge-exchange rate coefficients between K and Ca + as functions of the laser frequency. These irregularities occur in our system due to the presence of two LICIs. To further elucidate the role of the LICIs on the reaction dynamics, we compare these rate coefficients with those computed for a system where the CIs have been “removed”. In the laser frequency window, where conical interactions are present, the difference in rate coefficients can be as large as 1 × 10 –9 cm 3 /s.
Analog quantum simulators, which efficiently represent model systems, have the potential to provide new insight toward naturally occurring phenomena beyond the capabilities of classical computers.Incorporating dissipation as a resource unlocks a wider range of out-of-equilibrium processes such as chemical reactions.Here, we operate a hybrid qubit-oscillator circuit quantum electrodynamics simulator and model nonadiabatic molecular dynamics through a conical intersection.We identify dephasing of the electronic qubit as the mechanism that drives wave-packet branching when the corresponding oscillator undergoes large amplitude motion.Furthermore, we directly observe enhanced branching when the wave-packet passes through the conical intersection.Thus, the forces that influence a chemical reaction can be viewed from the perspective of measurement backaction in quantum mechanics-there is an effective measurement-induced dephasing rate that depends on the position of the wave packet relative to the conical intersection.Our results set the groundwork for more complex simulations of chemical dynamics using quantum simulators, offering deeper insight into the role of dissipation in determining macroscopic quantities of interest such as the quantum yield of a chemical reaction.
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.
Abstract The first step in the coherent control of a photoinduced binary reaction is bond making or photoassociation. We have recently demonstrated coherent control of bond making in multi-photon femtosecond photoassociation of hot magnesium atoms, using linearly chirped pulses (Levin et al 2015 Phys. Rev. Lett. 114 233003 ). The detected yield of photoassociated magnesium dimers was enhanced by positively chirped pulses which is explained theoretically by a combination of purification and chirp-dependent Raman transitions. The yield could be further enhanced by pulse optimization resulting in pulses with an effective linear chirp and a sub-pulse structure, where the latter allows for exploiting vibrational coherences. Here, we systematically explore the efficiency of phase-shaped pulses for the coherent control of bond making, employing a parametrization of the spectral phases in the form of cosine functions. We find up to an order of magnitude enhancement of the yield compared to the unshaped transform-limited pulse. The highly performing pulses all display an overall temporally increasing instantaneous frequency and are composed of several overlapping sub-pulses. The time delay between the first two sub-pulses fits very well the vibrational frequency of the generated intermediate wavepacket. These findings are in agreement with chirp-dependent Raman transitions and exploitation of vibrational dynamics as underlying control mechanisms.