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arXiv:2603.16512

Dark state role in time-reversal symmetry breaking

Dario Fasone, Rita Veilande, Luigi Giannelli, Giuseppe A. Falci, Teodora Kirova, Sandro Wimberger, Thomas Zanon-Willette, Ennio Arimondo

quant-phcond-mat.otherSubmitted Mar 17, 2026• Announced Mar 18, 2026• 0 citations
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Abstract

We investigate the role of the global driving phase $Φ$ in the dynamics of driven few-level quantum systems, a central setting in coherent control of atomic, molecular, and solid-state platforms. In particular, we focus on systems with closed-loop couplings, where external driving fields induce interference effects that strongly influence population transfer and symmetry properties of time-evolution. While full time-reversal symmetry requires $Φ=0,π$, leading to a real Hamiltonian, we focus on a less restrictive transformation, the phase inversion (or complex conjugation of the Hamiltonian), under which population dynamics can remain symmetric even though coherences generally do not. We show that the presence of a dark (spectator) state is a sufficient condition for this population phase symmetry (P$Φ$S), as it constrains the dynamics to reduced subspaces characterized by SU(2) or open-loop SU(3) evolution. We analyze this mechanism in three- and four-level systems and derive general conditions for P$Φ$S that extend to generic $n$-level configurations, with $n$ even. These findings provide practical guidelines for achieving robust control in quantum systems, with potential applications in quantum information processing and quantum computing.

Comments
13 pages, 7 figures

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We investigate the role of the global driving phase ΦΦΦ in the dynamics of driven few-level quantum systems, a central setting in coherent control of atomic, molecular, and solid-state platforms. In particular, we focus on systems with closed-loop couplings, where external driving fields induce interference effects that strongly influence population transfer and symmetry properties of time-evolution. While full time-reversal symmetry requires Φ=0,πΦ=0,πΦ=0,π, leading to a real Hamiltonian, we focus on a less restrictive transformation, the phase inversion (or complex conjugation of the Hamiltonian), under which population dynamics can remain symmetric even though coherences generally do not. We show that the presence of a dark (spectator) state is a sufficient condition for this population phase symmetry (PΦΦΦS), as it constrains the dynamics to reduced subspaces characterized by SU(2) or open-loop SU(3) evolution. We analyze this mechanism in three- and four-level systems and derive general conditions for PΦΦΦS that extend to generic nnn-level configurations, with nnn even. These findings provide practical guidelines for achieving robust control in quantum systems, with potential applications in quantum information processing and quantum computing.
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.
A coherent mechanism of robust population inversion in atomic and molecular systems by a chirped field is presented. It is demonstrated that a field of sufficiently high chirp rate imposes a certain relative phase between a ground and excited state wavefunction of a two-level system. The value of the relative phase angle is thus restricted to be negative and close to 0 or −pi-\\pi−pi for positive and negative chirp, respectively. This explains the unidirectionality of the population transfer from the ground to the excited state. In a molecular system composed of a ground and excited potential energy surface the symmetry between the action of a pulse with a large positive and negative chirp is broken. The same framwork of the coherent mechanism can explain the symmetry breaking and the population inversion due to a positive chirped field.
We apply reverse engineering to design laser pulse shapes for controlling the time evolution of strong-field transitions under environmental effects. Our effective two-state representation of the full quantum system involves dynamic Stark shifts and multiphoton Rabi frequency. Furthermore, the environment is modeled with dephasing and dissipative terms. Solving the master equation of the two-level density matrix inversely for the field, we obtain quasianalytic laser pulse shapes that simultaneously drive the populations and relative phase according to user-defined quantum pathways. The validity of the proposed scheme is demonstrated with the example of the $3s\ensuremath{\rightarrow}\ensuremath{\rightarrow}4s$ two-photon transition of atomic sodium by solving the master equation of the multilevel system that incorporates effects beyond the adiabatic elimination and the rotating wave approximation. Due to the open character of the system, the proposed control is not always possible. We explore these situations and point out the conditions for creating steady states with large coherence.
The dark-state effect, caused by destructive interference, not only is an important fundamental research topic in atomic physics and quantum optics, but also has wide potential application in quantum physics and quantum information science. Using the arrowhead-matrix method, here we study the dark-state effect in a coupled cavity-Rydberg-atom system, in which NNN Rydberg atoms with the dipole-dipole interactions are coupled to a single-mode cavity field. We obtain the numbers and form of the dark states in certain excitation-number subspaces for the two-, three-, and four-atom cases, as well as in the single-excitation subspace for a general NNN-atom case. We also suggest to characterize the dark states by inspecting the populations of some specific quantum states, which can be detected in experiments. Furthermore, we analyze the dark-state effect in a realistic case, where both the atomic dipole-dipole interaction strengths and the atom-cavity-field coupling strengths depend on the position of the atoms. Our findings pave the way for studying dark-state physics and applications in the cavity-Rydberg-atom platform.
A coherent mechanism of robust population inversion in atomic and molecular systems by a chirped field is presented. It is demonstrated that a field of sufficiently high chirp rate imposes a certain relative phase between a ground and excited state wavefunction of a two-level system. The value of the relative phase angle is thus restricted to be negative and close to 0 or - pi for positive and negative chirp, respectively. This explains the unidirectionality of the population transfer from the ground to the excited state.In a molecular system composed of a ground and excited potential energy surface the symmetry between the action of a pulse with a large positive and negative chirp is broken. The same framwork of the coherent mechanism can explain the symmetry breaking and the population inversion due to a positive chirped field.
High fidelity and robustness in population inversion is very desirable for many quantum control applications. We expand composite pulse schemes developed for two-level dynamics and present an analytic solution for the coherent evolution of an N-level quantum system with SU(2) symmetry, for achieving high fidelity and robust population inversion. Our approach offers a platform for accurate steering of the population transfer in physical multi-level systems, which is crucial for fidelity in quantum computation and achieving fundamental excitations in nuclear magnetic resonances and atomic physics. We also introduce and discuss the geometrical trajectories of these dynamics on the Majorana sphere as an interpretation, allowing us to gain physical insight on the dynamics of many-body or high-dimensional quantum systems.