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Physical Review A

Design of tailored microwave pulses to create rotational coherent states for an asymmetric-top molecule

Juan Ortigoso

Published Jun 1, 1998• 17 citations
Publisher

Abstract

Tailored microwave pulses, to guide asymmetric-top molecules from selected rotational states belonging to the vibronic ground state to generalized angular-momentum coherent states, are designed by using optimal control theory. Characteristics that the molecules have to fulfill in order to achieve the goal with feasible pulses are discussed. Properties of the pulses are discussed as well. The further dephasing among the components of the wave packet which, for the simplest coherent state, is a form of dynamical tunneling, can be locked by exploiting the changes that energy levels and eigenfunctions undergo in the presence of an external static electric field with appropriate intensity. For the special case with $M=0$, periodic fields are more flexible in avoiding dephasing. This is shown by examining properties of quasienergies and dressed states resulting from the diagonalization of a truncated Floquet matrix.

DOI
10.1103/physreva.57.4592

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Tailored microwave pulses, to guide asymmetric-top molecules from selected rotational states belonging to the vibronic ground state to generalized angular-momentum coherent states, are designed by using optimal control theory. Characteristics that the molecules have to fulfill in order to achieve the goal with feasible pulses are discussed. Properties of the pulses are discussed as well. The further dephasing among the components of the wave packet which, for the simplest coherent state, is a form of dynamical tunneling, can be locked by exploiting the changes that energy levels and eigenfunctions undergo in the presence of an external static electric field with appropriate intensity. For the special case with M=0M=0M=0, periodic fields are more flexible in avoiding dephasing. This is shown by examining properties of quasienergies and dressed states resulting from the diagonalization of a truncated Floquet matrix.
Molecules in selected rotational states can remain well aligned for extended periods of time in the presence of an appropriate periodic train of nonresonant laser pulses. Here, we show that these states can be prepared by slowly switching the electromagnetic field amplitude during a sequence of laser pulses. For low-temperature ensembles, a high degree of alignment can be achieved by designing pulse trains that take into account the distribution of avoided crossings between quasienergy curves. Additionally, we present calculations that illustrate several effects causing misalignment. A discussion of subtleties concerning systems with unbounded rotational spectra is also included.
An intuitive scheme for controlling the rotational quantum state of a Rydberg molecule is demonstrated experimentally. We determine the accumulated phase difference between the various components of a molecular electron wave packet, and then employ a sequence of phase-locked optical pulses to selectively enhance or depopulate specific rotational states. The angular momentum composition of the resulting wave packet, and the efficiency of the control scheme, is determined by calculating the multipulse response of the time-dependent Rydberg populations.
We have numerically examined optimization of the experimentally achievable shapes of mid-infrared femtosecond laser pulses to construct elementary quantum gates using molecular rovibrational states of a single molecule. Instead of optimizing the electric field by optimal control theory, the method generally used in theoretical studies of coherent control, the transmittance and the phase shift of conventional pulse shapers were optimized in the frequency domain by a genetic algorithm. The target molecular system we examined was the rotation-vibration states of CO in the $X({^{1}\ensuremath{\Sigma}}^{+})$ ground electronic state. Although the existence of the rotational degrees of freedom makes the quantum gate operation complicated, high fidelity of over 0.95 was achieved for one-rovibrational-qubit systems, which indicates that a molecular quantum computer may be feasible for at least one-qubit calculations on a diatomic molecule. On the other hand, two-qubit calculations are more difficult to achieve in a single CO molecule using rotational and vibrational degrees of freedom as different qubits. The importance of the control of the rotational in addition to the vibrational wave packet in order to realize a molecular quantum computer is discussed.
This paper considers vibronic population inversion in the presence of molecular rotation. The objective is to invert the population of a vibronic level with populated rotational levels to a specific vibrational level in the excited electronic state regardless of the detailed population distribution in the final rotational levels. The control of the multilevel population inversion is achieved by design of a pump pulse through optimal control theory. The total energy fluence and the pulse peak intensity are imposed as physical constraints in the design cost functional. A model diatomic molecule is used as an example to investigate molecular rotational effects on the vibronic population inversion and the control properties at different target times. The numerical results indicate that the shape-optimized pulses can achieve nearly complete population inversion and largely overcome the difficulty that a rectangular pulse faces due to energy mismatches and multiple dipole transition moments.
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.