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Attosecond physics provides unique insights into light-matter interaction on ultrafast time scales. Its core phenomenon, High Harmonic Generation (HHG), is often described by a classical recollision model, the simple-man or three-step model, where the atomic potential is disregarded. Many features are already well explained using this model; however, the simplicity of the model does not allow the possibility of classical chaotic motion. We show that beyond this model, classical chaotic motion does exist albeit on timescales that are generally longer than the first recollision time. Chaos is analyzed using tools from the theory of dynamical systems, such as Lyapunov exponents and stroboscopic maps. The calculations are done for a one-dimensional Coulomb potential subjected to a linearly polarized electric field.

In 1834-1835, Hamilton published two papers that revolutionized classical mechanics. In these papers, he introduced the Hamilton-Jacobi equation, Hamilton's equations of motion and the principle of least action. These three formulations of classical mechanics became the forerunners of quantum mechanics, but none of these is what Hamilton was looking for: he was looking for what he called the principal function, $S(q',q'',T)$, from which the entire trajectory history can be obtained just by differentiation. Here we show that all of Hamilton's formulations can be derived just by assuming that the principal function is additive, $S(q',q'',T)=S(q',Q,t_1)+S(Q,q'',t_2)$ with $t_1+t_2=T$. This simple additivity axiom can be considered the fundamental principle of classical mechanics and shows that analytical mechanics is essentially just a footnote to the problem of finding the shortest path between two points. The simplicity of the formulation could provide new perspectives on some of the major themes in classical mechanics including symplectic geometry, periodic orbit theory and Morse theory, as well as giving new perspectives on quantum mechanics. Moreover, it could potentially provide a unified description of different areas of physics, leading to insight for example, into the transition from deterministic dynamics to statistical mechanics., Comment: arXiv admin note: text overlap with arXiv:2109.09094

Reducing decoherence is an essential step toward realizing general-purpose quantum computers beyond the present noisy intermediate-scale quantum (NISQ) computers. To this end, dynamical decoupling (DD) approaches in which external fields are applied to qubits are often adopted. We numerically study DD using a two-level model system (qubit) under the influence of Markovian decoherence by using quantum optimal control theory with slightly modified settings, in which the physical objective is to maximally create and maintain a specified superposition state in a specified control period. An optimal pulse is numerically designed while systematically varying the values of dephasing, population decay, pulse fluence, and control period as well as using two kinds of objective functionals. Although the decrease in purity due to the decoherence gives rise to the upper limit of the target expectation value, i.e., the saturated value, the optimally shaped pulse effectively deals with the decoherence by gradually creating the target superposition state to realize the saturated value as much as possible., Comment: 20 pages, 12 figures, and 34 references

A dual formalism for Lagrange multipliers is developed. The formalism is used to minimize an action function $S(q_2,q_1,T)$ without any dynamical input other than that $S$ is convex. All the key equations of analytical mechanics -- the Hamilton-Jacobi equation, the generating functions for canonical transformations, Hamilton's equations of motion and $S$ as the time integral of the Lagrangian -- emerge as simple consequences. It appears that to a large extent, analytical mechanics is simply a footnote to the most basic problem in the calculus of variations: that the shortest distance between two points is a straight line.

Double ionization (DI) is a fundamental process that despite its apparent simplicity provides rich opportunities for probing and controlling the electronic motion. Even for the simplest multielectron atom, helium, new DI mechanisms are still being found. To first order in the field strength, a strong external field doubly ionizes the electrons in helium such that they are ejected into the same direction (front-to-back motion). The ejection into opposite directions (back-to-back motion) cannot be described to first order, making it a challenging target for control. Here, we address this challenge and optimize the field with the objective of back-to-back double ionization using a (1 + 1)-dimensional model. The optimization is performed using four different control procedures: (1) short-time control, (2) derivative-free optimization of basis expansions of the field, (3) the Krotov method, and (4) control of the classical equations of motion. All four procedures lead to fields with dominant back-to-back motion. All the fields obtained exploit essentially the same two-step mechanism leading to back-to-back motion: first, the electrons are displaced by the field into the same direction. Second, after the field turns off, the nuclear attraction and the electron-electron repulsion combine to generate the final motion into opposite directions for each electron. By performing quasi-classical calculations, we confirm that this mechanism is essentially classical.

We present a new trajectory formulation of high harmonic generation that treats classically allowed and classically forbidden processes within a single dynamical framework. Complex trajectories orbit the nucleus, producing the stationary Coulomb ground state. When the field is turned on, these complex trajectories continue their motion in the field-dressed Coulomb potential and therefore tunnel ionization, unbound evolution and recollision are described within a single, seamless framework. The new formulation can bring mechanistic understanding to a broad range of strong field physics effects., Comment: 6 pages, 6 figures

Stokes phenomenon refers to the fact that the asymptotic expansion of complex functions can differ in different regions of the complex plane, and that beyond the so-called Stokes lines has an unphysical divergence. An important special case is when the Stokes lines emanate from phase space caustics of a complex trajectory manifold. In this case, symmetry determines that to second order there is a double coverage of the space, one portion of which is unphysical. Building on the seminal but laconic findings of Adachi, we show that the deviation from second order can be used to rigorously determine the Stokes lines and therefore the region of the space that should be removed. The method has applications to wavepacket reconstruction from complex valued classical trajectories. With a rigorous method in hand for removing unphysical divergences, we demonstrate excellent wavepacket reconstruction for the Morse, Quartic, Coulomb and Eckart systems., Comment: 5 pages, 3 figures

We present two strategies for combining dynamical pruning with the multiconfiguration time-dependent Hartree method (DP-MCTDH), where dynamical pruning means on-the-fly selection of relevant basis functions. The first strategy prunes the primitive basis that represents the single-particle functions (SPFs). This is useful for smaller systems that require many primitive basis functions per degree of freedom, as we will illustrate for NO$_2$. Furthermore, this allows for higher-dimensional mode combination and partially lifts the sum-of-product-form requirement onto the structure of the Hamiltonian, as we illustrate for nonadiabatic 24-dimensional pyrazine. The second strategy prunes the set of configurations of SPF at each time step. We show that this strategy yields significant speed-ups with factors between 5 and 50 in computing time, making it competitive with the multilayer MCTDH method.

Complex-valued semiclassical methods hold out the promise of treating classically allowed and classically forbidden processes on the same footing. In addition, they provide a natural way to describe optical excitation with complex fields within the trajectory framework. Despite their promise, these methods have until now been limited to short time propagation, due to the numerical difficulties introduced by the complexification. Using a new Final Value Representation of the Coherent State Propagator (FINCO), combined with an analysis of the complex classical phase space, we achieve accurate wavepacket propagation all the way to the revival time of a strongly anharmonic system., Comment: 10 pages, 4 figures

We present an efficient implementation of dynamically pruned quantum dynamics, both in coordinate space and in phase space. We combine the ideas behind the biorthogonal von Neumann basis (PvB) with the orthogonalized momentum-symmetrized Gaussians (Weylets) to create a new basis, projected Weylets, that takes the best from both methods. We benchmark pruned dynamics using phase-space-localized PvB, projected Weylets, and coordinate-space-localized DVR bases, with real-world examples in up to six dimensions. We show that coordinate-space localization is most important for efficient pruning and that pruned dynamics is much faster compared to unpruned, exact dynamics. Phase-space localization is useful for more demanding dynamics where many basis functions are required. There, projected Weylets offer a more compact representation than pruned DVR bases., Comment: in press

The Comment of Brown and Carrington Jr. (BC) has two main points: 1) that the contraction idea of Shimshovitz and Tannor (ST) can be used for any DVR basis, not necessarily periodic, and 2) that the biorthogonal basis introduced by ST is unnecessary. We fully agree with the first point and in fact have several works that were in press at the time of the Comment that illustrate this. On the second point we show that BC implicitly use the biorthogonal basis of ST.

There has been great interest in recent years in quantum control landscapes. Given an objective $J$ that depends on a control field $\varepsilon$ the dynamical landscape is defined by the properties of the Hessian $\delta^2 J/\delta\varepsilon^2$ at the critical points $\delta J/\delta\varepsilon=0$. We show that contrary to recent claims in the literature the dynamical control landscape can exhibit trapping behavior due to the existence of special critical points and illustrate this finding with an example of a 3-level $\Lambda$-system. This observation can have profound implications for both theoretical and experimental quantum control studies.

We show that the second order traps in the control landscape for a three-level $\Lambda$-system found in our previous work {\it Phys. Rev. Lett.} {\bf 106}, 120402 (2011) are not local maxima: there exist directions in the space of controls in which the objective grows. The growth of the objective is slow --- at best 4th order for weak variations of the control. This implies that simple gradient methods would be problematic in the vicinity of second order traps, where more sophisticated algorithms that exploit the higher order derivative information are necessary to climb up the control landscape efficiently. The theory is supported by a numerical investigation of the landscape in the vicinity of the $\varepsilon(t)=0$ second order trap, performed using the GRAPE and BFGS algorithms.

Quantum computation places very stringent demands on gate fidelities, and experimental implementations require both the controls and the resultant dynamics to conform to hardware-specific constraints. Superconducting qubits present the additional requirement that pulses must have simple parameterizations, so they can be further calibrated in the experiment, to compensate for uncertainties in system parameters. Other quantum technologies, such as sensing, require extremely high fidelities. We present a novel, conceptually simple and easy-to-implement gradient-based optimal control technique named Gradient Optimization of Analytic conTrols (GOAT), which satisfies all the above requirements, unlike previous approaches. To demonstrate GOAT's capabilities, with emphasis on flexibility and ease of subsequent calibration, we optimize fast coherence-limited pulses for two leading superconducting qubits architectures - flux-tunable transmons and fixed-frequency transmons with tunable couplers.

We consider manipulation of the transmission coefficient for a quantum particle moving in one dimension where the shape of the potential is taken as the control. We show that the control landscape---the transmission as a functional of the potential---has no traps, i.e., any maxima correspond to full transmission.

We propose a new formalism for signal compression based on the Gabor basis set. By convolving the conventional Gabor functions with Dirichlet functions we obtain a periodic version of the Gabor basis set (pg). The pg basis is exact for functions that are band-limited with finite support, bypassing the Balian-Low theorem. The calculation of the pg coefficients is trivial and numerically stable, but the representation does not allow compression. However, by exchanging the pg basis with its biorthogonal basis and using the localized pg basis to calculate the coefficients, large compression factors are achieved. We illustrate the method on three examples: a rectangular pulse, an audio signal and a benchmark example from image processing., Comment: 7 pages, 7 figures

We propose a phase space method to propagate a quantum wavepacket driven by a strong external field. The method employs the so-called biorthogonal von Neumann basis recently introduced for the calculation of the energy eigenstates of time-independent quantum systems [A. Shimshovitz and D.J. Tannor, arXiv:1201.2299v1]. While the individual elements in this basis set are time-independent, a small subset is chosen in a time-dependent manner to adapt to the evolution of the wavepacket in phase space. We demonstrate the accuracy and efficiency of the present propagation method by calculating the electronic wavepacket in a one-dimensional soft-core atom interacting with a superposition of an intense, few-cycle, near-infrared laser pulse and an attosecond extreme-ultraviolet laser pulse., Comment: 4 pages, 4 figures. The following article has been submitted to the Journal of Chemical Physics. After it is published, it will be found at http://jcp.aip.org/

We propose a method for solving the time independent Schr\"odinger equation based on the von Neumann (vN) lattice of phase space Gaussians. By incorporating periodic boundary conditions into the vN lattice [F. Dimler et al., New J. Phys. 11, 105052 (2009)] we solve a longstanding problem of convergence of the vN method. This opens the door to tailoring quantum calculations to the underlying classical phase space structure while retaining the accuracy of the Fourier grid basis. The method has the potential to provide enormous numerical savings as the dimensionality increases. In the classical limit the method reaches the remarkable efficiency of 1 basis function per 1 eigenstate. We illustrate the method for a challenging two-dimensional potential where the FGH method breaks down., Comment: 5 figures. Includes supplementary material. arXiv admin note: substantial text overlap with arXiv:1010.2588

Probing the real time dynamics of a reacting molecule remains one of the central challenges in chemistry. In this letter we show how the time-dependent wavefunction of an excited-state reacting molecule can be completely reconstructed from resonant coherent anti-Stokes Raman spectroscopy. The method assumes knowledge of the ground-state potential but not of any excited-state potential, although we show that the latter can be computed once the time-dependent excited-state wavefunction is known. The formulation applies to polyatomics as well as diatomics and to bound as well as dissociative excited potentials. We demonstrate the method on the Li$_2$ molecule with its bound first excited-state, and on a model Li$_2$-like system with a dissociative excited state potential., Comment: The article includes 5 pages. One page of supplementary material is also included. The paper was submitted and now resubmitted to PRL

We propose a new method for solving quantum mechanical problems, which combines the flexibility of Gaussian basis set methods with the numerical accuracy of the Fourier method. The method is based on the incorporation of periodic boundary conditions into the von Neumann basis of phase space Gaussians [F. Dimler et al., New J. Phys. 11, 105052 (2009)]. In this paper we focus on the Time-independent Schr\"odinger Equation and show results for the harmonic, Morse and Coulomb potentials that demonstrate that the periodic von Neumann method or pvN is significantly more accurate than the usual vN method. Formally, we are able to show an exact equivalence between the pvN and the Fourier Grid Hamiltonian (FGH) methods. Moreover, due to the locality of the pvN functions we are able to remove Gaussian basis functions without loss of accuracy, and obtain significantly better efficiency than that of the FGH. We show that in the classical limit the method has the remarkable efficiency of 1 basis function per 1 eigenstate., Comment: 5 pages, 5 figures

Path integral derivations are presented for two recently developed complex trajectory techniques for the propagation of wave packets, Complex WKB and BOMCA. Complex WKB is derived using a standard saddle point approximation of the path integral, but taking into account the hbar dependence of both the amplitude and the phase of the intial wave function, thus giving rise to the need for complex classical trajectories. BOMCA is derived using a modification of the saddle point technique, in which the path integral is approximated by expanding around a near-classical path, chosen so that up to some predetermined order there is no need to add any correction terms to the leading order approximation. Both Complex WKB and BOMCA give the same leading order approximation; in Complex WKB higher accuracy is achieved by adding correction terms, while in BOMCA no additional terms are ever added -higher accuracy is achieved by changing the path along which the original approximation is computed. The path integral derivation of the methods explains the need to incorporate contributions from more than one trajectory, as observed in previous numerical work. On the other hand, it emerges that the methods provide efficient schemes for computing the higher order terms in the asymptotic evaluation of path integrals. The understanding we develop of BOMCA suggests that there should exist near-classical trajectories that give exact quantum dynamical results when used in the computation of the path integral keeping just the leading order term. We also apply our path integral techniques to give a compact derivation of the semiclassical approximation to the coherent state propagator., Comment: 41 pages; references and citations were corrupted in first two versions, sorry

We present a significant improvement to a time-dependent WKB (TDWKB) formulation developed by Boiron and Lombardi [JCP {\bf108}, 3431 (1998)] in which the TDWKB equations are solved along classical trajectories that propagate in the complex plane. Boiron and Lombardi showed that the method gives very good agreement with the exact quantum mechanical result as long as the wavefunction does not exhibit interference effects such as oscillations and nodes. In this paper we show that this limitation can be overcome by superposing the contributions of crossing trajectories. We also demonstrate that the approximation improves when incorporating higher order terms in the expansion. These improvements could make the TDWKB formulation a competitive alternative to current time-dependent semiclassical methods.

In recent years, intensive effort has gone into developing numerical tools for exact quantum mechanical calculations that are based on Bohmian mechanics. As part of this effort we have recently developed as alternative formulation of Bohmian mechanics in which the quantum action, S, is taken to be complex [JCP {125}, 231103 (2006)]. In the alternative formulation there is a significant reduction in the magnitude of the quantum force as compared with the conventional Bohmian formulation, at the price of propagating complex trajectories. In this paper we show that Bohmian mechanics with complex action is able to overcome the main computational limitation of conventional Bohmian methods -- the propagation of wavefunctions once nodes set in. In the vicinity of nodes, the quantum force in conventional Bohmian formulations exhibits rapid oscillations that pose severe difficulties for existing numerical schemes. We show that within complex Bohmian mechanics, multiple complex initial conditions can lead to the same real final position, allowing for the description of nodes as a sum of the contribution from two or more crossing trajectories. The idea is illustrated on the reflection amplitude from a one-dimensional Eckart barrier. We believe that trajectory crossing, although in contradiction to the conventional Bohmian trajectory interpretation, provides an important new tool for dealing with the nodal problem in Bohmian methods.

We present a unified derivation of Bohmian methods that serves as a common starting point for the derivative propagation method (DPM), Bohmian mechanics with complex action (BOMCA) and the zero-velocity complex action method (ZEVCA). The unified derivation begins with the ansatz $\psi=e^{\frac{iS}{\hbar}}$ where the action, $S$, is taken to be complex and the quantum force is obtained by writing a hierarchy of equations of motion for the phase partial derivatives. We demonstrate how different choices of the trajectory velocity field yield different formulations such as DPM, BOMCA and ZEVCA. The new derivation is used for two purposes. First, it serves as a common basis for comparing the role of the quantum force in the DPM and BOMCA formulations. Second, we use the new derivation to show that superposing the contributions of real, crossing trajectories yields a nodal pattern essentially identical to that of the exact quantum wavefunction. The latter result suggests a promising new approach to deal with the challenging problem of nodes in Bohmian mechanics.

In recent years there has been a resurgence of interest in Bohmian mechanics as a numerical tool because of its local dynamics, which suggest the possibility of significant computational advantages for the simulation of large quantum systems. However, closer inspection of the Bohmian formulation reveals that the nonlocality of quantum mechanics has not disappeared -- it has simply been swept under the rug into the quantum force. In this paper we present a new formulation of Bohmian mechanics in which the quantum action, S, is taken to be complex. This leads to a single equation for complex S, and ultimately complex x and p but there is a reward for this complexification -- a significantly higher degree of localization. The quantum force in the new approach vanishes for Gaussian wavepacket dynamics, and its effect on barrier tunneling processes is orders of magnitude lower than that of the classical force. We demonstrate tunneling probabilities that are in virtually perfect agreement with the exact quantum mechanics down to 10^{-7} calculated from strictly localized quantum trajectories that do not communicate with their neighbors. The new formulation may have significant implications for fundamental quantum mechanics, ranging from the interpretation of non-locality to measures of quantum complexity.

We present a local optimal control strategy to produce desired unitary transformations. Unitary transformations are central to all quantum computational algorithms. Many realizations of quantum computation use a submanifold of states, comprising the quantum register, coupled by an external driving field to a collection of additional mediating excited states. Previous attempts to apply control theory to induce unitary transformations on the quantum register, while successful, produced pulses that drive the population out of the computational register at intermediate times. Leakage of population from the register is undesirable since often the states outside the register are prone to decay and decoherence, and populating them causes a decrease in the final fidelity. In this work we devise a local optimal control method for achieving target unitary transformations on a quantum register, while avoiding intermediate leakage out of the computational submanifold. The technique exploits a phase locking of the field to the system such as to eliminate the undesirable excitation. This method is then applied to produce an SU(6) Fourier transform on the vibrational levels of the ground electronic state of the Na$_2$ molecule. The emerging mechanism uses two photon resonances to create a transformation on the quantum register while blocking one photon resonances to excited states., Comment: 5 pages

We extend a recently introduced mapping model, which explains the bunching phenomenon in an ion beam resonator for two ions [Geyer, Tannor, J. Phys. B 37 (2004) 73], to describe the dynamics of the whole ion bunch. We calculate the time delay of the ions from a model of the bunch geometry and find that the bunch takes on a spherical form at the turning points in the electrostatic mirrors. From this condition we derive how the observed bunch length depends on the experimental parameters. We give an interpretation of the criteria for the existence of the bunch, which were derived from the experimental observations by Pedersen et al [Pedersen etal, Phys. Rev. A 65 042704]., Comment: 25 pages, 6 figures; added new section 5 and clarified text; submitted to J. Phys. B

We study the problem of optimal control of dissipative quantum dynamics. Although under most circumstances dissipation leads to an increase in entropy (or a decrease in purity) of the system, there is an important class of problems for which dissipation with external control can decrease the entropy (or increase the purity) of the system. An important example is laser cooling. In such systems, there is an interplay of the Hamiltonian part of the dynamics, which is controllable and the dissipative part of the dynamics, which is uncontrollable. The strategy is to control the Hamiltonian portion of the evolution in such a way that the dissipation causes the purity of the system to increase rather than decrease. The goal of this paper is to find the strategy that leads to maximal purity at the final time. Under the assumption that Hamiltonian control is complete and arbitrarily fast, we provide a general framework by which to calculate optimal cooling strategies. These assumptions lead to a great simplification, in which the control problem can be reformulated in terms of the spectrum of eigenvalues of $\rho$, rather than $\rho$ itself. By combining this formulation with the Hamilton-Jacobi-Bellman theorem we are able to obtain an equation for the globaly optimal cooling strategy in terms of the spectrum of the density matrix. For the three-level $\Lambda$ system, we provide a complete analytic solution for the optimal cooling strategy. For this system it is found that the optimal strategy does not exploit system coherences and is a 'greedy' strategy, in which the purity is increased maximally at each instant., Comment: 9 pages, 3 figs

We present a two particle model to explain the mechanism that stabilizes a bunch of positively charged ions in an "ion trap resonator" [Pedersen etal, Phys. Rev. Lett. 87 (2001) 055001]. The model decomposes the motion of the two ions into two mappings for the free motion in different parts of the trap and one for a compressing momentum kick. The ions' interaction is modelled by a time delay, which then changes the balance between adjacent momentum kicks. Through these mappings we identify the microscopic process that is responsible for synchronization and give the conditions for that regime., Comment: 12 pages, 9 figures; submitted to Phys Rev A

It has been proposed that the adiabatic loading of a Bose-Einstein Condensate (BEC) into an optical lattice via the Mott-insulator transition can be used to initialize a quantum computer [D. Jaksch, {\it et al.}, Phys. Rev. Lett. {\bf 81}, 3108 (1998)]. The loading of a BEC into the lattice without causing band excitation is readily achievable; however, unless one switches on an optical lattice very slowly, the optical lattice causes a phase to accumulate across the condensate. We show analytically and numerically that a cancellation of this effect is possible by adjusting the harmonic trap force-constant of the magnetic trap appropriately, thereby facilitating quick loading of an optical lattice for quantum computing purposes. A simple analytical theory is developed for a non-stationary BEC in a harmonic trap., Comment: LaTeX 11 Pages, 6 figures

Using a set of general methods developed by Krotov [A. I. Konnov and V. A. Krotov, Automation and Remote Control, {\bf 60}, 1427 (1999)], we extend the capabilities of Optimal Control Theory to the Nonlinear Schr\"odinger Equation (NLSE). The paper begins with a general review of the Krotov approach to optimization. Although the linearized version of the method is sufficient for the linear Schr\"odinger equation, the full flexibility of the general method is required for treatment of the nonlinear Schr\"odinger equation. Formal equations for the optimization of the NLSE, as well as a concrete algorithm are presented. As an illustration, we consider a Bose-Einstein condensate initially at rest in a harmonic trap. A phase develops across the BEC when an optical lattice potential is turned on. The goal is to counter this effect and keep the phase flat by adjusting the trap strength. The problem is formulated in the language of Optimal Control Theory (OCT) and solved using the above methodology. To our knowledge, this is the first rigorous application of OCT to the Nonlinear Schr\"odinger equation, a capability that is bound to have numerous other applications., Comment: 11 pages, 4 figures, A reference added, Some typos corrected