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Communications Physics

All-optical control of pendular qubit states with nonresonant two-color laser pulses

Je Hoi Mun, Shinichirou Minemoto, Dong Eon Kim, Hirofumi Sakai

Published Sep 14, 2022• 4 citations
Publisher

Abstract

Abstract Practical methodologies for quantum qubit controls are established by two prerequisites, i.e., preparation of a well-defined initial quantum state and coherent control of that quantum state. Here we propose a new type of quantum control method, realized by irradiating nonresonant nanosecond two-color ($\omega$ and 2$\omega$) laser pulses to molecules in the pendular (field-dressed) ground state. The two-color field nonadiabatically splits the initial pendular ground state $\vert\tilde{0},\tilde{0}\rangle$ to a superposition state of $\vert\tilde{0},\tilde{0}\rangle$ and $\vert\tilde{1},\tilde{0}\rangle$, whose relative probability amplitudes can be controlled by the peak intensity of one wavelength component ($\omega$) while the peak intensity of the other component (2$\omega$) is fixed. The splitting of the quantum paths is evidenced by observing degrees of orientation of ground-state-selected OCS molecules by the velocity map imaging technique. This quantum control method is highly advantageous in that any type of polar molecules can be controlled regardless of the molecular parameters, such as rotational energy, permanent dipole moment, polarizability, hyperpolarizability, and hyperfine energy structures.

DOI
10.1038/s42005-022-01005-y

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Abstract Practical methodologies for quantum qubit controls are established by two prerequisites, i.e., preparation of a well-defined initial quantum state and coherent control of that quantum state. Here we propose a new type of quantum control method, realized by irradiating nonresonant nanosecond two-color (ω\omegaω and 2ω\omegaω) laser pulses to molecules in the pendular (field-dressed) ground state. The two-color field nonadiabatically splits the initial pendular ground state ∣0~,0~⟩\vert\tilde{0},\tilde{0}\rangle∣0~,0~⟩ to a superposition state of ∣0~,0~⟩\vert\tilde{0},\tilde{0}\rangle∣0~,0~⟩ and ∣1~,0~⟩\vert\tilde{1},\tilde{0}\rangle∣1~,0~⟩, whose relative probability amplitudes can be controlled by the peak intensity of one wavelength component (ω\omegaω) while the peak intensity of the other component (2ω\omegaω) is fixed. The splitting of the quantum paths is evidenced by observing degrees of orientation of ground-state-selected OCS molecules by the velocity map imaging technique. This quantum control method is highly advantageous in that any type of polar molecules can be controlled regardless of the molecular parameters, such as rotational energy, permanent dipole moment, polarizability, hyperpolarizability, and hyperfine energy structures.
Quantum entanglement and coherence are both essential physical resources in quantum theory. Cold polar molecules have long coherence time and strong dipole-dipole interaction and thus have been suggested as a platform for quantum information processing. In this paper, we employ the pendular states of the polar molecules trapped in static electric fields as the qubits, and put forward several theoretical schemes to generate the entanglement and coherence for two coupled dipoles by using optimal control theory. Through the designs of appropriate laser pulses, the transitions from the ground state to the Bell state and maximally coherent state can be realized with high fidelities 0.9906 and 0.9943 in the two-dipole system, respectively. Meanwhile, we show that the degrees of entanglement and coherence between the two pendular qubits are effectively enhanced with the help of optimized control fields. Furthermore, our schemes are generalized to the preparation of the Hardy state and even to the creation of arbitrary two-qubit states. Our findings can shed some light on the implementation of quantum information tasks with the molecular pendular states.
The capability to control molecular rotation for field-free orientation, which arranges molecules in specific spatial directions without external fields, is crucial in physics, chemistry, and quantum information science. However, conventional methods typically lead to transient orientations characterized by periodic directional reversals and necessitate the generation of coherent superpositions across a broad spectrum of rotational states of ultracold molecules. In this work, we develop a theoretical framework for achieving unidirectional field-free orientation by selectively manipulating two specific rotational states of symmetric top molecules. By leveraging the interplay between coherent superpositions and the precise selection of initial states, we demonstrate that both the maximum achievable orientation and its direction can be effectively controlled. To attain the desired two-state orientation, we present a quantum control strategy that utilizes a single control pulse, significantly simplifying the complexities of conventional multistate or multipulse schemes. Numerical simulations validate the effectiveness and feasibility of this approach for methyl iodide (CH3_33​I) molecules, even when accounting for molecular centrifugal distortion.The results highlight the critical roles of initial-state selection and quantum coherence in achieving long-lasting, high unidirectional molecular orientation, opening new directions in stereochemistry, precision spectroscopy, and quantum computing.
We present an experimental and theoretical investigation of the quantum control of ground-state rotational coherence in a linear molecule. A sequence of two temporally separated laser pulses creates a rotational superposition state in CO2{\mathrm{CO}}_{2}CO2​ whose evolution is monitored through a polarization technique. We study the influence of the phase difference between the two pulses. We show that the overlapping of the two wave packets, produced by each pulse, gives rise to quantum interference that affects the orientational anisotropy of the sample. Because of the large number of coherently excited levels, the interference produces well-separated temporal structures, whose magnitude can be controlled through the relative delay of the two pulses.
Implementation of quantum gates are important for quantum computations in physical system made of polar molecules. We investigate the feasibility of implementing gates based on pendular states of the molecular system by two different quantum optical control methods. Firstly, the Multi-Target optimal control theory and the Multi-Constraint optimal control theory are described for optimizing control fields and accomplish the optimization of quantum gates. Numerical results show that the controlled NOT gate (CNOT) can be realized under the control of above methods with high fidelities (0.975 and 0.999) respectively. In addition, in order to examine the dependence of the fidelity on energy difference in the same molecular system, the SWAP gate in the molecular system is also optimized with high fidelity (0.999) by the Multi-Constraint optimal control theory with the zero-area and constant-fluence constraints.
We theoretically investigate strong-field ionization of hydrogen atoms by orthogonally polarized two-color (OTC) laser pulses consisting of a fundamental field that is resonant with the 1s - 2p transition and its second harmonic. Numerical simulations are performed by solving the two-dimensional time-dependent Schrödinger equation and recording the photoelectron momentum distribution. In this strong-field resonant ionization, the atom undergoes many Rabi cycles and the electron can be emitted within a completed Rabi-cycle leading to the splitting of the localized momentum distribution. Here, the splitting is attributed to dynamic Rabi-splitting as a result of the dynamic Stark effect. The employed OTC scheme is shown to be efficient for controlling the dynamic Rabi-splitting through the control of quantum-path interferences involved in one-photon and two-photon absorption processes. The control scheme is accomplished by varying the relative ratio intensity and optical phase between the two pulses, and its footprint is mapped in the momentum distribution. This is shown to lead to an asymmetric distribution and suppression of the ionization process. The obtained results suggest the OTC scheme as a tool for coherent control of dynamic Rabi-oscillations via the controlled quantum-path interferences, thus opening new directions towards designing quantum states via the control OTC scheme.
The lack of a direct map between control fields and desired control objectives poses a significant challenge in applying quantum control theory to quantum technologies. Here, we propose an analytical framework to precisely control a limited set of quantum states and construct desired coherent superpositions using a well-designed laser pulse sequence with optimal amplitudes, phases, and delays. This theoretical framework that corresponds to a multilevel pulse-area theorem establishes a straightforward mapping between the control parameters of the pulse sequence and the amplitudes and phases of rotational states within a specific subspace. As an example, we utilize this approach to generate 15 distinct and desired rotational superpositions of ultracold polar molecules, leading to 15 desired field-free molecular orientations. By optimizing the superposition of the lowest 16 rotational states, we demonstrate that this approach can achieve a maximum orientation value of | 〈 cos θ 〉 | max above 0.99, which is very close to the global optimal value of 1 that could be achieved in an infinite-dimensional state space. This work marks a significant advancement in achieving precise control over multilevel subsystems within molecules. It holds potential applications in molecular alignment and orientation, as well as in various interdisciplinary fields related to the precise quantum control of ultracold polar molecules, opening up considerable opportunities in molecular-based quantum techniques.