Quantum Dynamics Research Articles

Accurate Quantum Dynamics Calculations for the Cl + CH4/CHD3/CD4 Reaction Rates.

Full-dimensional quantum dynamics simulations of the reaction of Cl with methane and its isotopomers are reported. Thermal rate constants are computed for the Cl + CH4 → HCl + CH3, Cl + CHD3 → HCl + CD3, and Cl + CD4 → DCl + CD3 reactions. Temperatures between 200 and 500 K are considered. In this temperature range, excellent agreement with the experiment is obtained. A detailed analysis of the kinetic isotope effect reveals the crucial importance of the CH3/CD3 umbrella motion. Comparison with approximate ring-polymer molecular dynamics simulations shows significant differences depending on the isotope studied.

Fidelity susceptibility probes of dynamical quantum criticality

Fidelity susceptibility is a quantum information-based approach that has been an effective tool for detecting and characterizing quantum phase transitions in an equilibrium setting. Motivated by the usefulness of the static counterpart, we propose that it can serve as a versatile tool to identify dynamical quantum phase transitions. Further, we develop linear-scale simulation methods for dynamical fidelity susceptibility calculations, which are based on the Chebyshev polynomial-expansion approach. We study the Aubry–André model as a benchmark for the validation of the computational technique. Numerical simulations show nonanalytic behaviors of the fidelity susceptibility in the time domain, signaling the existence of dynamical quantum phase transitions triggered by the incommensurate potential modulation of quantum quench systems. In addition, we find an excellent scaling collapse of the data onto a single curve in the limiting quench processes, which leads to a single-parameter scaling in the fidelity susceptibility. The feasibility of experimental measurement of the fidelity susceptibility opens up a new avenue toward an understanding of the nonequilibrium transport of quantum systems.

Enhancement of vibrationally assisted energy transfer by proximity to exceptional points, probed by fluorescence-detected vibrational spectroscopy

Emulation of energy transfer processes in natural systems on quantum platforms can further our understanding of complex dynamics in nature. One notable example is the demonstration of vibrationally assisted energy transfer (VAET) on a trapped-ion quantum emulator, which offers insights for the energetics of light harvesting. In this work, we expand the study of VAET simulation with trapped ions to a non-Hermitian quantum system comprising a PT-symmetric chromophore dimer weakly coupled to a vibrational mode. We first characterize exceptional points (EPs) and non-Hermitian features of the excitation energy transfer processes in the absence of the vibration, finding a degenerate pair of second-order EPs. Exploring the non-Hermitian dynamics of the whole system including vibrations, we find that energy transfer accompanied by absorption of phonons from a vibrational mode can be significantly enhanced near such a degenerate EP. Our calculations reveal a unique spectral feature accompanying the coalescing of eigenstates and eigenenergies that provides a unique approach to probe the degenerate EP by fluorescence-detected vibrational spectroscopy. Enhancement of the VAET process near the EP is found to be due to maximal favorability of phonon absorption at the degenerate EP, enabling multiple simultaneous excitations. Our work on improving VAET processes in non-Hermitian quantum systems paves the way for leveraging non-Hermiticity in quantum dynamics related to excitation energy transfer. Published by the American Physical Society 2024

The dynamical bulk boundary correspondence and dynamical quantum phase transitions in the Benalcazar-Bernevig-Hughes model.

In this article we demonstrate that dynamical quantum phase transitions occur for an exemplary higher order topological insulator, the Benalcazar-Bernevig-Hughes model, following quenches across a topological phase boundary. A dynamical bulk boundary correspondence is also seen both in the eigenvalues of the Loschmidt overlap matrix and the boundary return rate. The latter is found from a finite size scaling analysis for which the relative simplicity of the model is crucial. Contrary to the usual two dimensional case the dynamical quantum phase transitions in this model show up as cusps in the return rate, as for a one dimensional model, rather than as cusps in its derivative as would be typical for a two dimensional model. We explain the origin of this behaviour.&#xD.

Energy hierarchies governing quarkonium dynamics in heavy ion collisions

In this paper, we critically examine hierarchies between the energy scales that determine quarkonium dynamics in the quark gluon plasma. A particularly important role is played by the ratio of the binding energy of species (Eb) and the medium scales; temperature (T) and Debye mass (mD). It is well known that if these ratios are much larger than 1 then the dominant process governing quarkonium evolution is dissociation by thermal gluons (gluodissociation). On the other hand, if the ratio Eb/T is much smaller than one then quarkonium dynamics is dominated by screening and Landau damping of the exchanged gluons. Here we show that over most of the evolution, the scale hierarchies do not fall in either limit and one needs to use the full structure of the gluonic spectral function to follow the dynamics of the QQ¯ pair. This has a significant bearing when we follow the quantum dynamics of quarkonia in the medium. The inverse medium relaxation time is also ≈T and if Eb is comparable (or larger) in magnitude to T, the quantum evolution of QQ¯ is nonlocal in time within the Brownian approximation. Published by the American Physical Society 2024

Non-adiabatic direct quantum dynamics using force fields: Toward solvation.

Quantum dynamics simulations are becoming a powerful tool for understanding photo-excited molecules. Their poor scaling, however, means that it is hard to study molecules with more than a few atoms accurately, and a major challenge at the moment is the inclusion of the molecular environment. Here, we present a proof of principle for a way to break the two bottlenecks preventing large but accurate simulations. First, the problem of providing the potential energy surfaces for a general system is addressed by parameterizing a standard force field to reproduce the potential surfaces of the molecule's excited-states, including the all-important vibronic coupling. While not shown here, this would trivially enable the use of an explicit solvent. Second, to help the scaling of the nuclear dynamics propagation, a hierarchy of approximations is introduced to the variational multi-configurational Gaussian method that retains the variational quantum wavepacket description of the key quantum degrees of freedom and uses classical trajectories for the remaining in a quantum mechanics/molecular mechanics like approach. The method is referred to as force field quantum dynamics (FF-QD), and a two-state ππ*/nπ* model of uracil, excited to its lowest bright ππ* state, is used as a test case.

Bond-selective effect for the dissociative chemisorption of HOD on the Ni(100) surface revealed at the full-dimensional quantum dynamical level.

We present a comprehensive investigation into the dissociative chemisorption of HOD on a rigid Ni(100) surface using an approximate full-dimensional (9D) quantum dynamics approach, which was based on the time-dependent wave-packet calculations on a full-dimensional potential energy surface obtained through neural network fitting to density functional theory energy points. The approximate-9D probabilities were computed by averaging the seven-dimensional (7D) site-specific dissociation probabilities across six impact sites with appropriate relative weights. Our results uncover a distinctive bond-selective effect, demonstrating that the vibrational excitation of a specific bond substantially enhances the cleavage of that excited bond. The product branching ratios are substantially influenced by which bond undergoes excitation, exhibiting a clear preference for the product formed through the cleavage of the excited bond over the alternative product.

Prediction through quantum dynamics simulations: Photo-excited cyclobutanone.

Quantum dynamics simulations are becoming a standard tool for simulating photo-excited molecular systems involving a manifold of coupled states, known as non-adiabatic dynamics. While these simulations have had many successes in explaining experiments and giving details of non-adiabatic transitions, the question remains as to their predictive power. In this work, we present a set of quantum dynamics simulations on cyclobutanone using both grid-based multi-configuration time-dependent Hartree and direct dynamics variational multi-configuration Gaussian methods. The former used a parameterized vibronic coupling model Hamiltonian, and the latter generated the potential energy surfaces on the fly. The results give a picture of the non-adiabatic behavior of this molecule and were used to calculate the signal from a gas-phase ultrafast electron diffraction (GUED) experiment. Corresponding experimental results will be obtained and presented at a later stage for comparison to test the predictive power of the methods. The results show that over the first 500fs after photo-excitation to the S2 state, cyclobutanone relaxes quickly to the S1 state, but only a small population relaxes further to the S0 state. No significant transfer of population to the triplet manifold is found. It is predicted that the GUED experiments over this time scale will see signals related mostly to the C-O stretch motion and elongation of the molecular ring along the C-C-O axis.

Adaptive projected variational quantum dynamics

Adaptive projected variational quantum dynamics

Quantum dynamics of O(3P) + HBr → OH + Br reaction: integral cross sections and rate constants and their initial state dependence.

The integral cross sections (ICSs) and rate constants (RCs) for the title reaction are calculated by means of accurate quantum wave packet method employing the recent ab initio potential energy surface developed by Peterson and co-workers. Hundreds of partial wave contributions (up to J=150) are calculated explicitly taking Coriolis coupling into account. The ICSs are found to increase monotonically with energy and their energy dependences are smooth except in the energy range below the potential energy barrier, where several resonance peaks are observed. The temperature dependences of the RCs obey in general the Arrhenius law. These behaviors manifest the dominance of abstract mechanism. Initial rotational state (ji) excitations are found to greatly enhance the reactivity starting from ji=4, while exhibiting a complicated dependence for ji<4. From Boltzmann average of the initial state specified RCs (for ji=0-15) we obtained thermal RCs which are in reasonable agreement with available experimental results.

Length control of a McKibben pneumatic actuator using a dynamic quantizer

McKibben pneumatic actuators (MPAs) are soft actuators that exert tension by applying compressed air to expand a rubber tube. Although electro-pneumatic regulators can control air pressure, most are large and expensive. This study utilizes a dynamic quantizer to control the MPA with a small solenoid valve that can only open and close the valve instead of an electro-pneumatic regulator. A dynamic quantizer is one of the quantizers that converts continuous signals to discrete signals. Our previous study confirmed that tension control of MPA under isometric conditions could be realized using a dynamic quantizer. However, it is often necessary to control the length of the MPA as well as the tension of the MPA. This study implements a dynamic quantizer to control the length of the MPA with a small solenoid valve. Numerical simulations and experimental tests verify the effectiveness of the proposed method. The results of the numerical simulations and experimental tests confirmed that the length of the MPA can be controlled using the dynamic quantizer.

Transition role of entangled data in quantum machine learning

Entanglement serves as the resource to empower quantum computing. Recent progress has highlighted its positive impact on learning quantum dynamics, wherein the integration of entanglement into quantum operations or measurements of quantum machine learning (QML) models leads to substantial reductions in training data size, surpassing a specified prediction error threshold. However, an analytical understanding of how the entanglement degree in data affects model performance remains elusive. In this study, we address this knowledge gap by establishing a quantum no-free-lunch (NFL) theorem for learning quantum dynamics using entangled data. Contrary to previous findings, we prove that the impact of entangled data on prediction error exhibits a dual effect, depending on the number of permitted measurements. With a sufficient number of measurements, increasing the entanglement of training data consistently reduces the prediction error or decreases the required size of the training data to achieve the same prediction error. Conversely, when few measurements are allowed, employing highly entangled data could lead to an increased prediction error. The achieved results provide critical guidance for designing advanced QML protocols, especially for those tailored for execution on early-stage quantum computers with limited access to quantum resources.

Ultrafast state-selective tunneling in two-dimensional semiconductors with a phase- and amplitude-controlled THz-scanning tunneling microscope

THz-pulse driven scanning tunneling microscopy (THz-STM) enables access to the ultrafast quantum dynamics of low-dimensional material systems at simultaneous ultrafast temporal and atomic spatial resolution. State-selective tunneling requires precise amplitude and phase control of the THz pulses combined with quantitative near-field waveform characterization. Here, we employ our state-of-the-art THz-STM with multi-MHz repetition rates, efficient THz generation, and precisely tunable THz waveforms to investigate a single sulfur vacancy in monolayer MoS2. We demonstrate that 2D transition metal dichalcogenides (TMDs) are an ideal platform for near-field waveform sampling by THz cross-correlation. Furthermore, we determine the THz voltage via QEV scans, which measure the THz rectified charge Q as a function of THz field amplitude E and dc bias Vdc. Mapping the complex energy landscape of localized states with a resolution down to 0.01 electrons per pulse facilitates state-selective tunneling to the HOMO and LUMO orbitals of a charged sulfur vacancy.

Quantized filtering for switched memristive neural networks against deception attacks

This paper deals with the quantized mixed H∞/L2−L∞ filtering issue for switched memristive neural networks in the presence of deception attacks, in which the switching of parameters is not only subject to neural states, but also to the persistent dwell-time switching rule in the continuous-time case. First, a switched dynamic quantizer is utilized to quantize the measurement output before being transmitted to the filter. Second, deception attacks governed by a Bernoulli distribution are considered during the quantized output transmission. Then, in virtue of the Lyapunov stability theory together with stochastic analysis theory, a sufficient condition is given to ensure the global uniform asymptotic stability in the mean-square sense for the filtering error system with a mixed H∞/L2−L∞ performance. Furthermore, a co-design scheme for the desired mode-dependent filter gain and dynamic parameter is provided. Ultimately, the effectiveness of the proposed method is verified by a numerical example.

Gaussians for Electronic and Rovibrational Quantum Dynamics.

The assumptions underpinning the adiabatic Born-Oppenheimer (BO) approximation are broken for molecules interacting with attosecond laser pulses, which generate complicated coupled electronic-nuclear wave packets that generally will have components of electronic and dissociation continua as well as bound-state contributions. The conceptually most straightforward way to overcome this challenge is to treat the electronic and nuclear degrees of freedom on equal quantum-mechanical footing by not invoking the BO approximation at all. Explicitly correlated Gaussian (ECG) basis functions have proved successful for non-BO calculations of stationary molecular states and energies, reproducing rovibrational absorption spectra with very high accuracy. In this Article, we present a proof-of-principle study of the ability of fully flexible ECGs (FFECGs) to capture the intricate electronic and rovibrational dynamics generated by short, high-intensity laser pulses. By fitting linear combinations of FFECGs to accurate wave function histories obtained on a large real-space grid for a regularized 2D model of the hydrogen atom and for the 2D Morse potential, we demonstrate that FFECGs provide a very compact description of laser-driven electronic and rovibrational dynamics.

Dynamical quantum state tomography with time-dependent channels

Abstract In this paper, we establish a dynamical quantum state tomography framework. Under this framework, it is feasible to obtain complete knowledge of any unknown state of a $d$-level system via only one operator of a special type of positive operator-valued measure (POVM) in dimension $d$. We define a new channel, referred to as the time-dependent average channel. Utilizing this channel, we show that we can acquire a collection of projective operators that is informationally complete (IC) and thus obtain the corresponding informationally complete POVMs (IC-POVMs). Zauner conjectured that for any dimension $d$ there exists a fiducial vector, such that all remaining $d^{2}-1$ elements of the desired symmetric informationally complete POVM (SIC-POVM) can be obtained by acting on said vector with unitary matrices representing elements of the Weyl-Heisenberg group. We show that under certain condition, it is possible to obtain infinite families of projective operators that are IC, and obtain infinite families of corresponding IC-POVMs; otherwise, Zauner's conjecture is incorrect. We also show how to simulate a SIC-POVM on any unknown quantum state by using the time-dependent average channel.&amp;#xD;

Designing Variational Ansatz for Quantum‐Enabled Simulation of Non‐Unitary Dynamical Evolution ‐ An Excursion into Dicke Supperradiance

AbstractAdaptive Variational Quantum Dynamics (AVQD) algorithms offer a promising approach to providing quantum‐enabled solutions for systems treated within the purview of open quantum dynamical evolution. In this study, the unrestricted‐vectorization variant of AVQD is employed to simulate and benchmark various non‐unitarily evolving systems. Exemplification of how construction of an expressible ansatz unitary and the associated operator pool can be implemented to analyze examples such as the Fenna–Matthews–Olson complex (FMO) and even the permutational invariant Dicke model of quantum optics. Furthermore, an efficient decomposition scheme is shown for the ansatz used, which can extend its applications to a wide range of other open quantum system scenarios in near future. In all cases the results obtained are in excellent agreement with exact numerical computations that bolsters the effectiveness of this technique. The successful demonstrations pave the way for utilizing this adaptive variational technique to study complex systems in chemistry and physics, like light‐harvesting devices, thermal, and opto‐mechanical switches, to name a few.

Ligand-based drug design against Herpes Simplex Virus-1 capsid protein by modification of limonene through in silico approaches

The pharmacological effects of limonene, especially their derivatives, are currently at the forefront of research for drug development and discovery as well and structure-based drug design using huge chemical libraries are already widespread in the early stages of therapeutic and drug development. Here, various limonene derivatives are studied computationally for their potential utilization against the capsid protein of Herpes Simplex Virus-1. Firstly, limonene derivatives were designed by structural modification followed by conducting a molecular docking experiment against the capsid protein of Herpes Simplex Virus-1. In this research, the obtained molecular docking score exhibited better efficiency against the capsid protein of Herpes Simplex Virus-1 and hence we conducted further in silico investigation including molecular dynamic simulation, quantum calculation, and ADMET analysis. Molecular docking experiment has documented that Ligands 02 and 03 had much better binding affinities (− 7.4 kcal/mol and − 7.1 kcal/mol) to capsid protein of Herpes Simplex Virus-1 than Standard Acyclovir (− 6.5 kcal/mol). Upon further investigation, the binding affinities of primary limonene were observed to be slightly poor. But including the various functional groups also increases the affinities and capacity to prevent viral infection of the capsid protein of Herpes Simplex Virus-1. Then, the molecular dynamic simulation confirmed that the mentioned ligands might be stable during the formation of drug-protein complexes. Finally, the analysis of ADMET was essential in establishing them as safe and human-useable prospective chemicals. According to the present findings, limonene derivatives might be a promising candidate against the capsid protein of Herpes Simplex Virus-1 which ultimately inhibits Herpes Simplex Virus-induced encephalitis that causes interventions in brain inflammation. Our findings suggested further experimental screening to determine their practical value and utility.

Adaptive event‐triggered tracking control for nonlinear networked systems with dynamic quantization and deception attacks

AbstractThe problem of adaptive event‐triggered security tracking controller design is studied for interval type‐2 (IT2) Takagi‐Sugeno (T‐S) fuzzy‐approximation‐based nonlinear networked systems with deception attacks, privacy protection, and dynamic quantization in this paper. To reduce the network burden, the adaptive event‐triggered schemes (AETSs) and dynamic quantization are introduced to reduce unnecessary transmission and the number of network packets, respectively. Under the framework of network security, a novel security co‐design scheme with the tracking controller, AETSs, and the quantizers is developed, in which the privacy protection of the reference model and the deception attacks of the controller are taken into consideration simultaneously. Sufficient conditions for the results system to be mean‐square asymptotically stable with a tracking performance are established. Finally, two practical simulation examples demonstrate the effectiveness and novelty of the proposed design strategy.

Necessary condition for information transfer under simulated parity-time-symmetric evolution

Abstract Parity-time $(\mathcal{PT})$ symmetric quantum theory can broaden the scope of quantum dynamics beyond unitary evolution which may lead to numerous counter-intuitive phenomena, including single-shot discrimination of non-orthogonal states, faster evolution of state than the standard quantum speed limit, and violation of no-signaling principle. On the other hand, $\mathcal{PT}$-symmetric evolution can be realized as reduced dynamics of a subsystem in real experiments within the scope of standard QT. In this experimental setup, if one side of a composite system is evolved according to a $\mathcal{PT}$-symmetric way, a non-trivial information transfer can happen, i.e., the operation performed at one side can be gathered by the other side. By considering an arbitrary shared state between two parties situated in two distant locations and arbitrary measurements, we show that the $\mathcal{PT}$-symmetric evolution of the reduced subsystem at one side is not sufficient for this information transfer to occur. Specifically, we prove that the information transfer can only happen when the density matrix and the corresponding measurements contain complex numbers. Moreover, we connect the entanglement content of the shared state with the efficacy of information transfer. We find evidence that the task becomes more efficient with the increase of dimension. &amp;#xD;&amp;#xD;&amp;#xD;&amp;#xD;