We show that a combination of a half-cycle pulse and a short nonresonant laser pulse produces a strongly enhanced postpulse orientation. Robust transients that display both efficient and long-lived orientation are obtained. The mechanism is analyzed in terms of optimal oriented target states in finite Hilbert subspaces and shows that hybrid pulses can prove useful for other control issues.
This study shows the unexpected and counter-intuitive possibility of simultaneously orienting a molecule while delocalizing its molecular axis in a plane in field-free conditions. The corresponding quantum states are characterized and different control strategies using shaped THz laser pulses are proposed to reach such states at zero and nonzero temperatures. The robustness against temperature effects of a simple control procedure combining a laser and a THz pulse is shown. Such control strategies can be applied not only to linear molecules but also to symmetric top molecules.
We present a combined analytical and numerical investigation to show how an optimal control field can be designed to generate maximum field-free orientation of molecules for three populated rotational states. Based on a model involving pure rotational ladder-climbing excitation between rotational states, a set of optimal amplitude and phase conditions are analytically derived for the applied control fields. The maximum degree of orientation can be achieved when the field satisfies amplitude and phase conditions at the two transition frequencies. Multiple optimal solutions exist and to examine …
We present a theoretical study of the shaping of the time-evolution of field-free orientation of linear molecules. We show the extend to which the degree of orientation can be steered along a desired periodic time-dependent signal. The objective of this study is not to optimize molecular orientation but to propose a general procedure to precisely control rotational dynamics through the first moment of the molecular axis distribution. Rectangular and triangular signals are taken as illustrative examples. At zero temperature, we compute the quantum states leading to such field-free dynamics. A T…
The phenomenon of quantum revivals resulting from the self-interference of wave packets has been observed in several quantum systems and utilized widely in spectroscopic applications. Here, we present a combined analytical and numerical study on the generation of orientational quantum revivals (OQRs) exclusively using a single-cycle THz pulse. As a proof of principle, we examine the scheme in the linear polar molecule HCN with experimentally accessible pulse parameters and obtain strong field-free OQR without requiring the condition of the sudden-impact limit. To visualize the involved quantum…
Control of molecular rotations by laser fields is an active area of research focusing on the alignment/orientation of otherwise isotropic molecular samples. Oriented molecules are useful in many applications, such as molecular orbital tomography, femtosecond imaging of molecular structure, dynamics and chemical reaction control. In this work, we present a novel, previously unreported phenomenon appearing in thermal ensembles of non-linear polar molecules excited by a single THz pulse. We find that the induced orientation lasts long after the excitation pulse is over. In the case of symmetric-t…
Making the best of mixed-field orientation of polar molecules: A recipe for achieving adiabatic dynamics in an electrostatic field combined with laser pulses
We present a comprehensive study of enantioselective orientation of chiral molecules excited by a pair of delayed cross-polarized femtosecond laser pulses. We show that by optimizing the pulses' parameters, a significant (~ 10%) degree of enantioselective orientation can be achieved at zero and at five kelvin rotational temperatures. This study suggests a set of reasonable experimental conditions for inducing and measuring strong enantioselective orientation. The strong enantioselective orientation and the wide availability of the femtosecond laser systems required for the proposed experiments…
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…
Coupled pairs of spin-1/2 nuclei support one singlet state and three triplet states. In many circumstances the nuclear singlet order, defined as the difference between the singlet population and the mean of the triplet populations, is a long-lived state which persists for a relatively long time in solution. Various methods have been proposed for generating singlet order, starting from nuclear magnetization. This requires the stimulation of singlet-to-triplet transitions by modulated radiofrequency fields. We show that a recently described pulse sequence, known as PulsePol (Schwartz $\textit{et…
Long-lived coherences, emerging under periodic pulse driving in the disordered ensembles of strongly interacting spins, offer immense advantages for future quantum technologies, but the physical origin and the key properties of this phenomenon remain poorly understood. We theoretically investigate this effect in ensembles of different dimensionality, and predict existence of the long-lived coherences in two-dimensional and infinite-dimensional (where every spin is coupled to all others) systems, which are of particular importance for quantum sensing and quantum information processing. We explo…
We theoretically consider the phenomenon of field-free long-lasting orientation of symmetric-top molecules ionized by two-color laser pulses. The anisotropic ionization produces a significant long-lasting orientation of the surviving neutral molecules. The degree of orientation increases with both the pulse intensity and, counterintuitively, with the rotational temperature. The orientation may be enhanced even further by using multiple delayed two-color pulses. The long-lasting orientation may be probed by even harmonic generation or by Coulomb-explosion-based methods. The effect may enable th…
Ultrashort laser pulses are widely used for transient field-free molecular orientation -- a phenomenon important in chemical reaction dynamics, ultrafast molecular imaging, high harmonics generation, and attosecond science. However, significant molecular orientation usually requires rotationally cold molecules, like in rarified molecular beams, because chaotic thermal motion is detrimental to the orientation process. Here we propose to use the mechanism of the echo phenomenon previously observed in hadron accelerators, free-electron lasers, and laser-excited molecules to overcome the destructi…
We present a combined analytical and numerical study for coherent terahertz control of a single molecular polariton, formed by strongly coupling two rotational states of a molecule with a single-mode cavity. Compared to the bare molecules driven by a single terahertz pulse, the presence of a cavity strongly modifies the post-pulse orientation of the polariton, making it difficult to obtain its maximal degree of orientation. To solve this challenging problem toward achieving complete quantum coherent control, we derive an analytical solution of a pulse-driven quantum Jaynes-Cummings model by ex…
Large-scale quantum networks require quantum memories featuring long-lived storage of non-classical light together with efficient, high-speed and reliable operation. The concurrent realization of these features is challenging due to inherent limitations of matter platforms and light-matter interaction protocols. Here, we propose an approach to overcome this obstacle, based on the implementation of the Autler-Townes-splitting (ATS) quantum-memory protocol on a Bose-Einstein condensate (BEC) platform. We demonstrate a proof-of-principle of this approach by storing short pulses of single-photon-l…
We have theoretically investigated the molecular orientation by a asymmetric potential created by the superposition of two-color laser fields. The time-dependent Schrodinger equation is solved numerically for different field parameters. We have shown how enhancement or suppression of the molecular orientation can be manipulated by the laser field parameters, such as time between laser pulses, the different intensity of the pulses, etc.
Long-lived state of a helium-like magnesium donor in silicon
Institute for Physics of Microstructures of the Russian Academy of Sciences（俄罗斯科学院微结构物理研究所）；Lobachevsky State University of Nizhny Novgorod（下诺夫哥罗德罗巴切夫斯基国立大学）；Ioffe Institute（约费研究所）；Institut für Kristallzüchtung (IKZ)（晶体生长研究所）
As demonstrated in our previous work [J. Chem. Phys. 149, 174109 (2018)], the kinetic energy imparted to a quantum rotor by a non-resonant electromagnetic pulse with a Gaussian temporal profile exhibits quasi-periodic drops as a function of the pulse duration. Herein, we show that this behaviour can be reproduced with a simple waveform, namely a rectangular electric pulse of variable duration, and examine, both numerically and analytically, its causes. Our analysis reveals that the drops result from the oscillating populations that make up the wavepacket created by the pulse and that they are …
We study a unitary time evolution of a symmetry-broken state in a form of a charge density wave in a finite system of interacting hard-core bosons, which can be mapped onto the XXZ Heisenberg chain. Moreover, we introduce a spatially-homogenous and time-dependent vector potential that mimics a short laser pulse. We establish the range of amplitudes of the vector potential for which the onset of charge density wave order can be controlled. We propose a protocol that reveals non-thermal long-lived states, which are characterized by a non-zero charge density wave order translated by one lattice s…
Spin bath mediated long-lived coherent oscillations of NV centers in diamond
Bennett University（贝内特大学）；IIT Madras（印度理工学院马德拉斯分校）；Technische Universität Dortmund（多特蒙德工业大学）；Center For Quantum Information, Communication And Computing, IIT Madras（印度理工学院马德拉斯分校量子信息、通信与计算中心）；London center for Nanotechnology, UCL（伦敦纳米技术研究中心，伦敦大学学院）；SIAS, Krea University（克里亚大学SIAS学院）
