Resonant Quantum Research Articles

Certifying Multimode Light-Matter Interaction in Lossy Resonators.

Quantum models based on few-mode master equations have been a central tool in the study of resonator quantum electrodynamics, extending the seminal single-mode Jaynes-Cummings model to include loss and multiple modes. Despite their broad application range, previous approaches within this framework have either relied on a Markov approximation or a fitting procedure. By combining ideas from pseudomode and quasinormal mode theory, we develop a certification criterion for multi-mode effects in lossy resonators. It is based on a witness observable, and neither requires a fitting procedure nor a Markov approximation. Using the resulting criterion, we demonstrate that such multi-mode effects are important for understanding previous experiments in x-ray cavity QED with Mössbauer nuclei and that they allow one to tune the nuclear ensemble properties.

Enhancing CO2 capture of an aminoethylethanolamine‐based non‐aqueous absorbent by using tertiary amine as a proton‐transfer mediator: From performance to mechanism

Non-aqueous absorbents (NAAs) have attracted increasing attention for CO2 capture because of their great energy-saving potential. Primary diamines which can provide high CO2 absorption loading are promising candidates for formulating NAAs but suffer disadvantages in regenerability. In this study, a promising strategy that using tertiary amines (TAs) as proton-transfer mediators was proposed to enhance the regenerability of an aminoethylethanolamine (AEEA, diamine)/dimethyl sulfoxide (DMSO) (A/D) NAA. Surprisingly, some employed TAs such as N,N-diethylaminoethanol (DEEA), N,N,N',N'',N''-pentamethyldiethylenetriamine (PMDETA), 3-dimethylamino-1-propanol (3DMA1P), and N,N-dimethylethanolamine (DMEA) enhanced not only the regenerability of the A/D NAA but also the CO2 absorption performance. Specifically, the CO2 absorption loading and cyclic loading were increased by about 12.7% and 15.5%–22.7%, respectively. The TA-enhanced CO2 capture mechanism was comprehensively explored via nuclear magnetic resonance technique and quantum chemical calculations. During CO2 absorption, the TA acted as an ultimate proton acceptor for AEEA-zwitterion and enabled more AEEA to form carbamate species (AEEACOO−) to store CO2, thus enhancing CO2 absorption. For CO2 desorption, the TA first provided protons directly to AEEACOO− as a proton donor; moreover, it functioned as a proton carrier and facilitated the low-energy step-wise proton transfer from protonated AEEA to AEEACOO−. Consequently, the presence of TA made it easier for AEEACOO− to obtain protons to decompose, resulting in enhanced CO2 desorption. In a word, introducing the TA as a proton-transfer mediator into the A/D NAA enhanced both the CO2 absorption performance and the regenerability, which was an efficient way to “kill two birds with one stone”.

Generation and Characterization of a Tetraradical Embedded in a Curved Cyclic Paraphenylene Unit.

Unique spin-spin (magnetic) interactions, ring-size effects on ground-state spin multiplicity, and in-plane aromaticity has been found in localized 1,3-diradicals embedded in curved benzene structures such as cycloparaphenylene (CPP). In this study, we characterized the magnetic interactions in a tetraradical consisting of two localized 1,3-diradical units connected by p-quaterphenyl within a curved CPP skeleton by electron paramagnetic resonance (EPR) spectroscopy and quantum chemical calculations. Persistent triplet species with zero-field splitting parameters similar to those of a triplet 1,3-diphenylcyclopentane-1,3-diyl diradical were observed by continuous wave (CW) or pulsed X-band EPR measurements. The quintet state derived from the ferromagnetic interaction between the two triplet diradical moieties was not detected at 20 K under glassy matrix conditions. At the B3LYP/6-31G(d) level of theory, the singlet state was lower in energy than the triplet and quintet states. These findings will aid in the development of open-shell species for material science application.

Magnetic quantum and spin-wave behavior of three-layer graphene-like materials

This study examines the spin-wave and magnetic quantum behavior of three-layer graphene-like based on the Heisenberg model. The system is diagonally solved for Hamiltonian quantities using the linear spin wave theory and postponed Green's functions. The effects of exchange coupling, anisotropy, and spin quantum number on the resonance frequency and quantum fluctuation are discussed, providing a basis for regulating resonance frequency and quantum fluctuation.

Quantum targeted energy transfer through machine learning tools.

In quantum targeted energy transfer, bosons are transferred from a certain crystal site to an alternative one, utilizing a nonlinear resonance configuration similar to the classical targeted energy transfer. We use a computational method based on machine learning algorithms in order to investigate selectivity as well as efficiency of the quantum transfer in the context of a dimer and a trimer system. We find that our method identifies resonant quantum transfer paths that allow boson transfer in unison. The method is readily extensible to larger lattice systems involving nonlinear resonances.

Applying the Action Principle of Classical Mechanics to the Thermodynamics of the Troposphere

Advances in applied mechanics have facilitated a better understanding of the recycling of heat and work in the troposphere. This goal is important to meet practical needs for better management of climate science. Achieving this objective may require the application of quantum principles in action mechanics, recently employed to analyze the reversible thermodynamics of Carnot’s heat engine cycle. The testable proposals suggested here seek to solve several problems including (i) the phenomena of decreasing temperature and molecular entropy but increasing Gibbs energy with altitude in the troposphere; (ii) a reversible system storing thermal energy to drive vortical wind flow in anticyclones while frictionally warming the Earth’s surface by heat release from turbulence; (iii) vortical generation of electrical power from translational momentum in airflow in wind farms; and (iv) vortical energy in the destructive power of tropical cyclones. The scalar property of molecular action (@t ≡ ∫mvds, J-sec) is used to show how equilibrium temperatures are achieved from statistical equality of mechanical torques (mv2 or mr2ω2); these are exerted by Gibbs field quanta for each kind of gas phase molecule as rates of translational action (d@t/dt ≡ ∫mr2ωdϕ/dt ≡ mv2). These torques result from the impulsive density of resonant quantum or Gibbs fields with molecules, configuring the trajectories of gas molecules while balancing molecular pressure against the density of field energy (J/m3). Gibbs energy fields contain no resonant quanta at zero Kelvin, with this chemical potential diminishing in magnitude as the translational action of vapor molecules and quantum field energy content increases with temperature. These cases distinguish symmetrically between causal fields of impulsive quanta (Σhν) that energize the action of matter and the resultant kinetic torques of molecular mechanics (mv2). The quanta of these different fields display mean wavelengths from 10−4 m to 1012 m, with radial mechanical advantages many orders of magnitude greater than the corresponding translational actions, though with mean quantum frequencies (v) similar to those of radial Brownian movement for independent particles (ω). Widespread neglect of the Gibbs field energy component of natural systems may be preventing advances in tropospheric mechanics. A better understanding of these vortical Gibbs energy fields as thermodynamically reversible reservoirs for heat can help optimize work processes on Earth, delaying the achievement of maximum entropy production from short-wave solar radiation being converted to outgoing long-wave radiation to space. This understanding may improve strategies for management of global changes in climate.

Quantum dynamical effects of vibrational strong coupling in chemical reactivity

Recent experiments suggest that ground state chemical reactivity can be modified when placing molecular systems inside infrared cavities where molecular vibrations are strongly coupled to electromagnetic radiation. This phenomenon lacks a firm theoretical explanation. Here, we employ an exact quantum dynamics approach to investigate a model of cavity-modified chemical reactions in the condensed phase. The model contains the coupling of the reaction coordinate to a generic solvent, cavity coupling to either the reaction coordinate or a non-reactive mode, and the coupling of the cavity to lossy modes. Thus, many of the most important features needed for realistic modeling of the cavity modification of chemical reactions are included. We find that when a molecule is coupled to an optical cavity it is essential to treat the problem quantum mechanically to obtain a quantitative account of alterations to reactivity. We find sizable and sharp changes in the rate constant that are associated with quantum mechanical state splittings and resonances. The features that emerge from our simulations are closer to those observed in experiments than are previous calculations, even for realistically small values of coupling and cavity loss. This work highlights the importance of a fully quantum treatment of vibrational polariton chemistry.

A new efficient approach for the calculation of cross-sections with application to Yukawa potential

Large-scale and systematic calculations of scattering amplitudes and cross-sections for charged particle collisions are of fundamental importance for understanding the physical properties of materials in different research fields. However, the elaborated theoretical methods for cross-sections are generally restricted to a finite range of impact energies. Here, we present an efficient approach for the calculation of the scattering amplitude and cross-sections ranging from low to high collision energies based on the variable phase method, where the Wentzel–Kramers–Brillouin and Born approximations for scattering phase shifts (SPSs) are incorporated into the numerical algorithm to alleviate the computational cost. For this purpose, quantitative criteria for the validity of these approximations are established based on the properties of the turning points of the potentials. For different scattering potentials, the corresponding planes can be established as a guideline to select the optimal combination for calculating the scattering amplitude and cross-section. The demand for quantum treatment of phase shifts is reduced by one to two orders of magnitude, which strongly benefits the computation of cross-sections for high-energy scattering. It has been found that the quantum treatment for SPSs is necessary near the quantum states involving quantum tunneling and resonance. To testify the validity of the approach, the SPSs and also transport cross-sections are calculated for Yukawa potentials, and good agreements are obtained in comparison with other available high-precision calculations. The proposed numerical approach can be straightforwardly generalized to other scattering potentials and permits one to efficiently calculate the scattering cross-sections for a large energy range.

Fractional Floquet theory

A fractional generalization of the Floquet theorem is suggested for fractional Schrödinger equations (FTSE)s with the time-dependent periodic Hamiltonians. The obtained result, called the fractional Floquet theorem (fFT), is formulated in the form of the Mittag-Leffler function, which is considered as the eigenfunction of the Caputo fractional derivative. The suggested formula makes it possible to reduce the FTSE to the standard quantum mechanics with the time-dependent Hamiltonian, where the standard Floquet theorem is valid. Two examples related to quantum resonances are considered as well to support the obtained result.

Many-body localization in the random-field Heisenberg chain with Dzyaloshinskii-Moriya interaction

We study the one-dimensional spin-1/2 Heisenberg chain with Dzyaloshinskii-Moriya interaction in a random magnetic field using exact diagonalization. In order to obtain many-body mobility edge at infinite temperature, we employ a polynomial filtered Lanczos method that can avoid the fill-in problem when implementing the commonly used shift-and-invert transformation. In stark contrast to the original Heisenberg model, although the localized phase always conforms to Poisson statistics, the ergodic phase exhibits the Gaussian unitary ensemble rather than the Gaussian orthogonal ensemble statistics due to the lack of complex conjugation symmetry. The boundary between the ergodic and localized phases is determined by carefully performing finite-size scalings for the level statistics, entanglement entropy and its standard deviation, as well as fluctuations of the total spin of the system. The two phases are also well distinguished by the full delocalization or localization in the Hilbert space wherein the participation entropies present. To indicate the localized phase in experiment, we propose a scheme for realizing the out-of-time-order correlator on a modern nuclear magnetic resonance quantum simulator.

Non-radiative charge transfer process of proton impcating B atom

Electron transfer in heavy particle collisions, involving complicated electron correlation mechanisms, greatly affects the charge state balance in plasma, and is also one of important sources for X-ray radiation. Electron transfer cross section and rate coefficient are important atomic parameters required for the development of nuclear fusion plasma in the national defense industry. We systematically investigate the electron transfer process of proton impacting boron atom in an energy range of <inline-formula><tex-math id="M4">\begin{document}${10}^{-3}-{10}^{3}\;{\rm{e}}{\rm{V}}/{\rm{u}}$\end{document}</tex-math><alternatives><graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="16-20230470_M4.jpg"/><graphic xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="16-20230470_M4.png"/></alternatives></inline-formula> based on a fully quantum non-radiative molecular orbital close-coupling method. A total of 15 channels of electron transfer, excitation, and elastic scattering are obtained by using the multi-reference configuration interaction method, and the corresponding molecular energy of each channel is in good agreement with the experimental results. The phenomenon of avoiding crossing between the adiabatic potential energy curves of molecular states is obvious, which constituents the main pathway of electron transfer. The calculation shows that the electron transfer of the 2s orbital is dominated in the process of proton impacting boron atom, while the electron transfer of the 2p orbital contributes a little. In the low energy region, there are obvious quantum resonances in the electron transfer cross section, which originate from the coupling between high energy channel and low energy channel. In addition, we calculate the electron transfer rates of proton-impact boron atom at different temperatures, which can provide important atomic parameter which support for simulating and diagnosing complex plasma environments.

Highly Selective Absorption of Low-Concentration SO2 over CO2 in Flue Gas through Cation-Tunable Protic Ionic Liquids

A cation-tunable strategy was reported for highly selective absorption of low-concentration SO2 over CO2 in flue gas, where the cation had a significant effect on the selectivity. The absorption capacity and selectivity of low-concentration SO2 by various ionic liquids (ILs) were investigated; therein, protic IL [THEEDH][Tetz] showed the best selectivity of 80.6 (120.4) under the atmosphere of 2000 ppm of SO2 and 15% CO2. Nuclear magnetic resonance spectroscopic investigations and quantum chemical calculations indicated that the effect of the cation on the electronegativity of the anion was significant, leading to an obvious increase in selectivity. This cation-tunable IL offered a significant improvement in the selective absorption of SO2 compared to traditional ILs, indicating its potential in acid gas separation in industry.

High-Yield Production of Quantum Corrals in a Surface Reconstruction Pattern

The power of surface chemistry to create atomically precise nanoarchitectures offers intriguing opportunities to advance the field of quantum technology. Strategies for building artificial electronic lattices by individually positioning atoms or molecules result in precisely tailored structures but lack structural robustness. Here, taking the advantage of strong bonding of Br atoms on noble metal surfaces, we report the production of stable quantum corrals by dehalogenation of hexabromobenzene molecules on a preheated Au(111) surface. The byproducts, Br adatoms, are confined within a new surface reconstruction pattern and aggregate into nanopores with an average size of 3.7 ± 0.1 nm, which create atomic orbital-like quantum resonance states inside each corral due to the interference of scattered electron waves. Remarkably, the atomic orbitals can be hybridized into molecular-like orbitals with distinct bonding and antibonding states. Our study opens up an avenue to fabricate quantum structures with high yield and superior robustness.

Spatial phase effect on quantum resonance ratchet transport of cold atoms

We investigate the transport dynamics of a cold atom exposed to a sawthooth-like optical lattice potential subject to periodic δ-kicks. By means of the computed transport current, at Quantum Resonance regimes, interesting phenomenon induced by the potential spatial phase θ have been resolved. From a zero-phase High Order Quantum Resonance case, where current reversal is possible, we show by turning on the spatial phase θ that current enhancement, current rectification and zero current are achieved. Specifically, θ can be used to turn a negative current into a positive one and vice-versa, to enhance current, or to set current to zero. With the help of current landscapes displayed as function of θ and the potential P, optimal currents are generated. Such a picture clearly shows regions of optimal currents, at critical values of θ and P, where prospective experiments can be done with present-day optical lattice set-up.

Quantum tunneling in ultra-near-integrable systems.

We study the tunneling tail of eigenfunctions of the quantum map using arbitrary precision arithmetic and find that nonmonotonic decaying tails accompanied by step structures appear even when the corresponding classical system is extremely close to the integrable limit. Using the integrable basis constructed with the Baker-Campbell-Hausdorff (BCH) formula, we clarify that the observed structure emerges due to the coupling with excited states via the quantum resonance mechanism. Further calculations reveal that the step structure gives stretched exponential decay as a function of the inverse Planck constant, which is not expected to appear in normal tunneling processes.

DMPO Spin Trapping Study of the Photolysis of 2-(4-Nitrophenyl)-1H-indolyl-3-methyl Derivatives

The transient radical species generated in the photolysis of 2-(4-nitrophenyl)-1H-indoly-3-methyl (NPIM) derivatives were investigated by 5,5-dimethyl-1-pyrroline-N-oxide (DMPO) spin trapping studies. The structures of the DMPO spin adducts were determined by electron paramagnetic resonance spectroscopy, mass spectrometry, and quantum chemical calculations. These results revealed that the homolytic bond cleavage occurs in the photolysis of NPIM derivatives.

Mapping Single Electron Spins with Magnetic Tomography

Mapping the positions of single electron spins is a highly desired capability for applications such as nanoscale magnetic resonance imaging and quantum network characterization. Here, we demonstrate a method based on rotating an external magnetic field to identify the precise location of single electron spins in the vicinity of a quantum spin sensor. We use a nitrogen-vacancy center in diamond as a quantum sensor and modulate the dipolar coupling to a proximate electron spin in the crystal by varying the magnetic field vector. The modulation of the dipolar coupling contains information on the coordinates of the spin, from which we extract its position with an uncertainty of 0.9\,\AA. We show that the method can be used to locate electron spins with nanometer precision up to 10\,nm away from the sensor. We discuss the method's applicability to mapping hyperfine coupled electron spins, and show it may be applied to locating nitroxide radicals. The magnetic tomography method can be utilized for distance measurements for studying the structure of individual molecules.

Metabolic profiling of preovulatory follicular fluid in jennies

Follicular fluid is formed from the transudation of theca and granulosa cells in the growing follicular antrum. Its main function is to provide an optimal intrafollicular microenvironment to modulate oocyte maturation. The aim of this study was to determine the metabolomic profile of preovulatory follicular fluid (PFF) in jennies. For this purpose, PFF was collected from 10 follicles of five jennies in heat. Then, PFF samples were analysed by nuclear magnetic resonance (NMR) and heteronuclear single quantum correlation (2D 1H/13C HSQC). Our study revealed the presence of at least 27 metabolites in the PFF of jennies (including common amino acids, carboxylic acids, amino acid derivatives, alcohols, saccharides, fatty acids, and lactams): 3-hydroxybutyrate, acetate, alanine, betaine, citrate, creatine, creatine phosphate, creatinine, ethanol, formate, glucose, glutamine, glycerol, glycine, hippurate, isoleucine, lactate, leucine, lysine, methanol, phenylalanine, proline, pyruvate, threonine, tyrosine, valine, and τ-methylhistidine. The metabolites found here have an important role in the oocyte development and maturation, since the PFF surrounds the follicle and provides it with the needed nutrients. Our results indicate a unique metabolic profile of the jennies PFF, as it differs from those previously observed in the PFF of the mare, a phylogenetically close species that is taken as a reference for establishing reproductive biotechnology techniques in donkeys. The metabolites found here also differ from those described in the TCM-199 medium enriched with fetal bovine serum (FBS), which is the most used medium for in vitro oocyte maturation in equids. These differences would suggest that the established conditions for in vitro maturation used so far may not be suitable for donkeys. By providing the metabolic composition of jenny PFF, this study could help understand the physiology of oocyte maturation as a first step to establish in vitro reproductive techniques in this species.

The hydrogen bond rotation of confined water affected by quantum resonance tunnelling

In this work, we report quantum tunnelling effects on the confined water chain flipping, different from the spatial size and even electronic correlation effects of the confinement environment. First-principles calculations and analyses confirm that quantum tunnelling from the water chain itself enhances the hydrogen bond rotation. Importantly, the neglected resonant tunnelling can result in tunnelling rotation of hydrogen bonds with a probability close to 1 through the provided 0.6 eV energy, while the probability of generally recognized sequential tunnelling is only 10−6. Not only that, compared to sequential tunnelling, resonant tunnelling leads to a 20 K higher flipping temperature of the water chain. Additionally, the ratio of the resonant tunnelling probability to the thermal disturbance probability at 200 K is at least ten times larger than that of sequential tunnelling, which further illustrates the enhancement of hydrogen bond rotation brought about by resonant tunnelling.

Observation of the p -wave shape resonance in atom-molecule collisions

Partial wave resonances are quasi-bound states that are formed by tunneling through the centrifugal barrier. Such states are important to collisions that deviate from the Langevin limit where direct collision path is suppressed due to quantum symmetry or a potential barrier. In such a case, quantum resonances play a major role in the dynamics at low temperatures where scattering process can be described mainly by the resonance contribution. Here we present the first observation of the lowest-lying partial wave resonance in the Penning ionization collisions between metastable neon and rovibrationally ground state HD molecules. We observe the resonance at an energy of $k_B\times$22mK taking advantage of the phase space correlation similar to atomic delta kick cooling. We show that the $p$-wave resonance position is particularly sensitive to the leading term of the van der Waals interaction. We also measure shape resonance at a higher angular momentum state, $l=6$, allowing us to disentangle and probe the short and the long parts of the intermolecular interaction.