A new physical implementation for quantum computation is proposed. The vibrational modes of molecules are used to encode qubit systems. Global quantum logic gates are realized using shaped femtosecond laser pulses which are calculated applying optimal control theory. The scaling of the system is favourable, sources for decoherence can be eliminated. A complete set of one and two quantum gates is presented for a specific molecule. Detailed analysis regarding experimental realization shows that the structural resolution of today's pulse shapers is easiliy sufficient for pulse formation.
Using a photonic quantum computer for boson sampling has been demonstrated a tremendous advantage over classical supercomputers. It is highly desirable to develop boson sampling algorithms for realistic scientific problems. In this work, we propose a hybrid quantum-classical sampling (HQCS) algorithm to calculate the optical spectrum for complex molecules considering anharmonicity and Duschinsky rotation (DR) effects. The classical sum-over-state method for this problem has a computational complexity that exponentially increases with system size. In the HQCS algorithm, an intermediate harmonic…
Strong coupling between light and matter is possible with a variety of organic materials. In contrast to the simpler inorganic case, organic materials often have a complicated spectrum, with vibrationally dressed electronic transitions. Strong coupling to light competes with this vibrational dressing, and if strong enough, can suppress the entanglement between electronic and vibrational degrees of freedom. By exploiting symmetries, we can perform exact numerical diagonalization to find the polaritonic states for intermediate numbers of molecules, and use these to define and validate accurate e…
Local-field corrections to the decay rate of excited molecules in absorbing cavities: the Onsager model
采用Onsager局域场模型，计算了位于色散吸收介质球中心的受激分子（原子）的衰变率和经典辐射功率。发现分子的外部（辐射和吸收）功率损耗的局部场校正因子为$|3ε(ω)/[3ε(ω)+1]|^2$，其中$ε(ω)$为球体的介电函数。然而，发现对分子总衰变率（功率损失）的局部场校正要复杂得多，包括Scheel等人最近导出的无限腔介质中的衰变率（Rev. A 60，4094（1999）），以及对腔诱导衰变率的类似校正。所得到的结果可以转换成与模型无关的形式。这表明，一般的结果为局域场校正的衰减率和外部功率损失的分子在吸收腔有效的分子位置远离腔壁。
We develop two novel models of the H$_2^+$ molecule and its isotopes from which we assess quantum-mechanically and semi-classically whether the molecule anti-aligns with the field in the first excited electronic state. The results from both models allow us to predict anti-alignment dynamics even for the HD$^+$ isotope, which possesses a permanent dipole moment. The molecule dissociates at angles perpendicular to the field polarization in both the excited and the ground electronic state, as the population is exchanged through a conical intersection. The quantum mechanical dispersion of the init…
A barrier to realizing the potential of molecules for quantum information science applications is a lack of high-fidelity, single-molecule imaging techniques. Here, we present and theoretically analyze a general scheme for dispersive imaging of electronic ground-state molecules. Our technique relies on the intrinsic anisotropy of excited molecular rotational states to generate optical birefringence, which can be detected through polarization rotation of an off-resonant probe laser beam. Using \narb and \rbcs as examples, we construct a formalism for choosing the molecular state to be imaged an…
We characterize excited state quantum phase transitions in the two dimensional limit of the vibron model with the quantum fidelity susceptibility, comparing the obtained results with the information provided by the participation ratio. As an application, we perform fits using a four-body algebraic Hamiltonian to bending vibrational data for several molecular species and, using the optimized eigenvalues and eigenstates, we locate the eigenstate closest to the barrier to linearity and determine the linear or bent character of the different overtones.
Impulsive orientation of symmetric-top molecules excited by two-color femtosecond pulses is considered. In addition to the well-known transient orientation appearing immediately after the pulse and then reemerging periodically due to quantum revivals, we report the phenomenon of field-free long-lasting orientation. Long-lasting means that the time averaged orientation remains non-zero until destroyed by other physical effects, e.g. intermolecular collisions. The effect is caused by the combined action of the field-polarizability and field-hyperpolarizability interactions. The dependence of deg…
We study the excitation of asymmetric-top (including chiral) molecules by two-color femtosecond laser pulses. In the cases of non-chiral asymmetric-top molecules excited by an orthogonally polarized two-color pulse, we demonstrate, classically and quantum mechanically, three-dimensional orientation. For chiral molecules, we show that the orientation induced by a cross-polarized two-color pulse is enantioselective along the laser propagation direction, namely, the two enantiomers are oriented in opposite directions. On the short time scale, the classical and quantum simulations give results tha…
We combine experimental and theoretical approaches to explore excited rotational states of molecules embedded in helium nanodroplets using CS$_2$ and I$_2$ as examples. Laser-induced nonadiabatic molecular alignment is employed to measure spectral lines for rotational states extending beyond those initially populated at the 0.37 K droplet temperature. We construct a simple quantum mechanical model, based on a linear rotor coupled to a single-mode bosonic bath, to determine the rotational energy structure in its entirety. The calculated and measured spectral lines are in good agreement. We show…
