Internal Quantum States Research Articles

Near-complete chiral selection in rotational quantum states

Controlling the internal quantum states of chiral molecules for a selected enantiomer has a wide range of fundamental applications from collision and reaction studies, quantum information to precision spectroscopy. Achieving full enantiomer-specific state transfer is a key requirement for such applications. Using tailored microwave fields, a chosen rotational state can be enriched for a selected enantiomer, even starting from a racemic mixture. This enables rapid switching between samples of different enantiomers in a given state, holding great promise, for instance, for measuring parity violation in chiral molecules. Although perfect state-specific enantiomeric enrichment is theoretically feasible, achieving the required experimental conditions seemed unrealistic. Here, we realize near-ideal conditions, overcoming both the limitations of thermal population and spatial degeneracy in rotational states. We achieve over 92% enantiomer-specific state transfer efficiency using enantiopure samples. This indicates that 96% state-specific enantiomeric purity can be obtained from a racemic mixture, in an approach that is universally applicable to all chiral molecules of C1 symmetry. Our work integrates the control over internal quantum states with molecular chirality, thus expanding the field of state-selective molecular beams studies to include chiral research.

A new kinetic model on hydrolysis of sulfur mustard non-dissolved and dissolved in aqueous solution

This paper aims to establish a hydrolysis extent equation and rate dependence of initial and boundary conditions for sulfur mustard (HD) non-dissolved and dissolved in water by the following work. Firstly, non-homogeneous hydrolysis extent was found to be accurately described by a product of logistic with exponential convex growth function because of slow collision-complex formation between activated H2O and HD molecule to non-linearly couple with transition state decay, while the homogeneous has grown up only in an exponential convex function because of fast collision-complex formation to make its initial extent ratio extremely quickly close to unity. Secondly, initial non-temperature effects from (ethanol, acid, base) additives, HD concentration and droplet size, and rotation speed on hydrolysis rate could be summarized into a Boltzmann function of rate constant with initial molar free energy because of a thermal equilibrium distribution of internal quantum state at a given energy for bi-molecular structures before and after complexing. The results from 5 mL solution under vortex was nearly similar to the stirring 100 mL solution and would helpfully clarify the detoxification kinetics to establish a standard method for evaluating reactivity of aqueous decontaminants against chemical warfare agents at necessarily specified conditions.

An optical tweezer array of ultracold polyatomic molecules.

Polyatomic molecules have rich structural features that make them uniquely suited to applications in quantum information science1-3, quantum simulation4-6, ultracold chemistry7 and searches for physics beyond the standard model8-10. However, a key challenge is fully controlling both the internal quantum state and the motional degrees of freedom of the molecules. Here we demonstrate the creation of an optical tweezer array of individual polyatomic molecules, CaOH, with quantum control of their internal quantum state. The complex quantum structure of CaOH results in a non-trivial dependence of the molecules' behaviour on the tweezer light wavelength. We control this interaction and directly and non-destructively image individual molecules in the tweezer array with a fidelity greater than 90%. The molecules are manipulated at the single internal quantum state level, thus demonstrating coherent state control in a tweezer array. The platform demonstrated here will enable a variety of experiments using individual polyatomic molecules with arbitrary spatial arrangement.

Bundle theoretic descriptions of massless single-particle state spaces; how do we perceive a moving quantum particle

Recently, a bundle theoretic description of massive single-particle state spaces, which is better suited for Relativistic Quantum Information Theory than the ordinary Hilbert space description, has been suggested. However, the mathematical framework presented in that work does not apply to massless particles. It is because, unlike massive particles, massless particles cannot assume the zero momentum state and hence the mass shell associated with massless particles has non-trivial cohomology. To overcome this difficulty, this paper suggests a new framework that can be applied to massless particles. Applications to the cases of massless particles with spin-1 and 2, namely photon and graviton, will reveal that the field equations, the gauge conditions, and the gauge freedoms of Electromagnetism and General Relativity naturally arise as manifestations of an inertial observer’s perception of the internal quantum states of a photon and a graviton, respectively. Finally, we show that gauge freedom is exhibited by all massless particles, except those with spin-0 and 1/2.

Non‐Reciprocal Cavity Polariton with Atoms Strongly Coupled to Optical Cavity

AbstractBreaking the time‐reversal symmetry of light is of great importance for fundamental physics and has attracted increasing interest in the study of non‐reciprocal photonic devices. Here, a chiral cavity quantum electrodynamics system with multiple atoms strongly coupled to a Fabry–Pérot cavity is experimentally demonstrated. By polarizing the internal quantum state of the atoms, the time‐reversal symmetry of the atom‐cavity interaction is broken. The strongly coupled atom‐cavity system can be described by non‐reciprocal quasiparticles, that is, the cavity polariton. When it works in the linear regime, the inherent nonreciprocity makes the system work as a single‐photon‐level optical isolator. Benefiting from the collective enhancement of multiple atoms, an isolation ratio exceeding 30 dB on the single‐quanta level (≈ 0.1 photon on average) is achieved. The validity of the non‐reciprocal device under zero magnetic field and the reconfigurability of the isolation direction are also experimentally demonstrated. Moreover, when the cavity polariton works in the nonlinear regime, the quantum interference between polaritons with weak anharmonicity induces non‐reciprocal nonclassical statistics of cavity transmission from coherent probe light.

Bundle theoretic descriptions of massive single-particle state spaces; with a view toward relativistic quantum information theory

Relativistic Quantum Information Theory (RQI) is a flourishing research area of physics, yet, there has been no systematic mathematical treatment of the field. In this paper, we suggest bundle theoretic descriptions of massive single-particle state spaces, which are basic building blocks of RQI. In the language of bundle theory, one can construct a vector bundle over the set of all possible motion states of a massive particle, in whose fibers the moving particle’s internal quantum state as perceived by a fixed inertial observer is encoded. A link between the usual Hilbert space description is provided by a generalized induced representation construction on the L 2-section space of the bundle. The aim of this paper is two-fold. One is to communicate the basic ideas of RQI to mathematicians and the other is to suggest an improved formalism for single-particle state spaces that encompasses all known massive particles including those which have never been dealt with in the RQI literature. Some of the theoretical implications of the formalism will be explored at the end of the paper.

Materials challenges for trapped-ion quantum computers

Trapped-ion quantum information processors store information in atomic ions maintained in position in free space by electric fields. Quantum logic is enacted through manipulation of the ions’ internal and shared motional quantum states using optical and microwave signals. Although trapped ions show great promise for quantum-enhanced computation, sensing and communication, materials research is needed to design traps that allow for improved performance by means of integration of system components, including optics and electronics for ion-qubit control, while minimizing the near-ubiquitous electric-field noise produced by trap-electrode surfaces. In this Review, we consider the materials requirements for such integrated systems, with a focus on problems that hinder current progress towards practical quantum computation. We give suggestions for how materials scientists and trapped-ion technologists can work together to develop materials-based integration and noise-mitigation strategies to enable the next generation of trapped-ion quantum computers. Trapped-ion qubits have great potential for quantum computation, but materials improvements are needed. This Review surveys materials opportunities to improve the performance of trapped-ion qubits, from understanding the surface science that leads to electric-field noise to developing methods for building ion traps with integrated optics and electronics.

Photo-excitation of long-lived transient intermediates in ultracold reactions

Controlling the pathways and outcomes of reactions is a broadly pursued goal in chemistry. In gas phase reactions, this is typically achieved by manipulating the properties of the reactants, including their translational energy, orientation, and internal quantum state. In contrast, here we influence the pathway of a reaction via its intermediate complex, which is generally too short-lived to be affected by external processes. In particular, the ultracold preparation of potassium-rubidium (KRb) reactants leads to a long-lived intermediate complex (K$_2$Rb$_2^*$), which allows us to steer the reaction away from its nominal ground-state pathway onto a newly identified excited-state pathway using a laser source at 1064 nm, a wavelength commonly used to confine ultracold molecules. Furthermore, by monitoring the change in the complex population after the sudden removal of the excitation light, we directly measure the lifetime of the complex to be $360 \pm 30$ ns, in agreement with our calculations based on the Rice-Ramsperger-Kassel-Marcus (RRKM) statistical theory. Our results shed light on the origin of the two-body loss widely observed in ultracold molecule experiments. Additionally, the long complex lifetime, coupled with the observed photo-excitation pathway, opens up the possibility to spectroscopically probe the structure of the complex with high resolution, thus elucidating the reaction dynamics.

Speed-adjustable atomic beam of metastable helium for precision measurement

A bright beam of metastable helium atoms is useful in various studies. Laser spectroscopy of helium in an atomic beam can provide a determination of the fine-structure constant and the nuclear charge radius, towards a test of quantum electrodynamics (QED). In these measurements, it is necessary to control not only the internal quantum state but also the translation motion of the helium atom. Here we present a setup producing an intense and speed-adjustable continuous beam of helium atoms. By using a combination of laser cooling, focusing, and deflection, helium atoms are prepared at the single quantum state of ${2}^{\phantom{\rule{0.16em}{0ex}}3}{S}_{1}$ ($m=0$), with a very narrow distribution of the longitudinal speed ($\ensuremath{\delta}{v}_{z}l\ifmmode\pm\else\textpm\fi{}4.5$ m/s). At the same time, we obtain a flux of $1.8\ifmmode\times\else\texttimes\fi{}{10}^{13}$ (atoms/s)/sr with a fractional fluctuation below 0.02%. The atomic-beam quality was investigated by laser spectroscopy, indicating a considerable improvement over those used in previous helium precision-spectroscopy measurements.

Controlling the dynamical scale factor in a trapped atom Sagnac interferometer

Sagnac interferometers with massive particles promise unique advantages in achieving high precision measurements of rotation rates over their optical counterparts. Recent proposals and experiments are exploring non-ballistic Sagnac interferometers where trapped atoms are transported along a closed path. This is achieved by using superpositions of internal quantum states and their control with state-dependent potentials. We address emergent questions regarding the dynamical behavior of Bose-Einstein condensates in such an interferometer and its impact on rotation sensitivity. We investigate complex dependencies on atomic interactions as well as trap geometries, rotation rates, and speed of operation. We find that temporal transport profiles obtained from a simple optimization strategy for non-interacting particles remain surprisingly robust also in the presence of interactions over a large range of realistic parameters. High sensitivities can be achieved for short interrogation times far from the adiabatic regime. This highlights a route to building fast and robust guided ring Sagnac interferometers with fully trapped atoms.

Quantum-state-specific reaction rate measurements for the photo-induced reaction Ca+ + O2 → CaO+ + O

ABSTRACTAtoms and molecules often react at different rates depending on their internal quantum states. Thus, controlling which internal states are populated can be used to manipulate the reactivity and can lead to a more detailed understanding of reaction mechanisms. We demonstrate this control of reactions by studying the electronically excited state reaction . This reaction is exothermic only if Ca is in one of its excited electronic states. Using laser-cooling and electrodynamic trapping, we cool and trap Ca at millikelvin temperatures for several minutes. We can then change the fraction of time they spend in each of the two excited states by adjusting the detunings of the cooling lasers. This allows us to disentangle the reactions that begin with Ca in the 2P-state from the ones where Ca is in the 2D-state. Using time-of-flight mass spectrometry, we determine independent reaction rate constants for Ca in both electronically excited states.

Atom interferometers with weak-measurement path detectors and their quantum mechanical analysis**Project supported by the National Key Research and Development Program of China (Grant No. 2018YFA 0306200), the National Natural Science Foundation of China (Grant No. 11434017), and the Guangdong Innovative and Entrepreneurial Research Team Program, China (Grant No. 2016ZT06C594).

According to the orthodox interpretation of quantum physics, wave-particle duality (WPD) is the intrinsic property of all massive microscopic particles. All gedanken or realistic experiments based on atom interferometers (AI) have so far upheld the principle of WPD, either by the mechanism of the Heisenberg’s position-momentum uncertainty relation or by quantum entanglement. In this paper, we propose and make a systematic quantum mechanical analysis of several schemes of weak-measurement atom interferometer (WM-AI) and compare them with the historical schemes of strong-measurement atom interferometer (SM-AI), such as Einstein’s recoiling slit and Feynman’s light microscope. As the critical part of these WM-AI setups, a weak-measurement path detector (WM-PD) deliberately interacting with the atomic internal electronic quantum states is designed and used to probe the which-path information of the atom, while only inducing negligible perturbation of the atomic center-of-mass motion. Another instrument that is used to directly interact with the atomic center-of-mass while being insensitive to the internal electronic quantum states is used to monitor the atomic center-of-mass interference pattern. Two typical schemes of WM-PD are considered. The first is the micromaser-cavity path detector, which allows us to probe the spontaneously emitted microwave photon from the incoming Rydberg atom in its excited electronic state and record unanimously the which-path information of the atom. The second is the optical-lattice Bragg-grating path detector, which can split the incoming atom beam into two different directions as determined by the internal electronic state and thus encode the which-path information of the atom into the internal states of the atom. We have used standard quantum mechanics to analyze the evolution of the atomic center-of-mass and internal electronic state wave function by directly solving Schrödinger’s equation for the composite atom-electron-photon system in these WM-AIs . We have also compared our analysis with the theoretical and experimental studies that have been presented in the previous literature. The results show that the two sets of instruments can work separately, collectively, and without mutual exclusion to enable simultaneous observation of both wave and particle nature of the atoms to a much higher level than the historical SM-AIs, while avoiding degradation from Heisenberg’s uncertainty relation and quantum entanglement. We have further investigated the space–time evolution of the internal electronic quantum state, as well as the combined atom–detector system and identified the microscopic origin and role of quantum entanglement, as emphasized in numerous previous studies. Based on these physics insights and theoretical analyses, we have proposed several new WM-AI schemes that can help to elucidate the puzzling physics of the WPD of the atoms. The principle of WM-AI scheme and quantum mechanical analyses made in this work can be directly extended to examine the principle of WPD for other massive particles.

Reaction kinetics of ultracold molecule-molecule collisions

Studying chemical reactions on a state-to-state level tests and improves our fundamental understanding of chemical processes. For such investigations it is convenient to make use of ultracold atomic and molecular reactants as they can be prepared in well defined internal and external quantum states. Here, we investigate a single-channel reaction of two Li2-Feshbach molecules where one of the molecules dissociates into two atoms 2AB ⇒ AB + A + B. The process is a prototype for a class of four-body collisions where two reactants produce three product particles. We measure the collisional dissociation rate constant of this process as a function of collision energy/temperature and scattering length. We confirm an Arrhenius-law dependence on the collision energy, an a4 power-law dependence on the scattering length a and determine a universal four body reaction constant.

Quantum simulation of Abelian lattice gauge theories via state-dependent hopping

We develop a quantum simulator architecture that is suitable for the simulation of $U(1)$ Abelian gauge theories such as quantum electrodynamics. Our approach relies on the ability to control the hopping of a particle through a barrier by means of the internal quantum states of a neutral or charged impurity-particle sitting at the barrier. This scheme is experimentally feasible, as the correlated hopping does not require fine-tuning of the intra- and inter-species interactions. We investigate the applicability of the scheme in a double well potential, which is the basic building block of the simulator, both at the single-particle and the many-body mean-field level. Moreover, we evaluate its performance for different particle interactions and trapping, and, specifically for atom-ion systems, in the presence of micro-motion.

Angle-resolved molecular beam scattering of NO at the gas-liquid interface.

This study presents first results on angle-resolved, inelastic collision dynamics of thermal and hyperthermal molecular beams of NO at gas-liquid interfaces. Specifically, a collimated incident beam of supersonically cooled NO (2Π1/2, J = 0.5) is directed toward a series of low vapor pressure liquid surfaces ([bmim][Tf2N], squalane, and PFPE) at θinc = 45(1)°, with the scattered molecules detected with quantum state resolution over a series of final angles (θs = -60°, -30°, 0°, 30°, 45°, and 60°) via spatially filtered laser induced fluorescence. At low collision energies [Einc = 2.7(9) kcal/mol], the angle-resolved quantum state distributions reveal (i) cos(θs) probabilities for the scattered NO and (ii) electronic/rotational temperatures independent of final angle (θs), in support of a simple physical picture of angle independent sticking coefficients and all incident NO thermally accommodating on the surface. However, the observed electronic/rotational temperatures for NO scattering reveal cooling below the surface temperature (Telec < Trot < TS) for all three liquids, indicating a significant dependence of the sticking coefficient on NO internal quantum state. Angle-resolved scattering at high collision energies [Einc = 20(2) kcal/mol] has also been explored, for which the NO scattering populations reveal angle-dependent dynamical branching between thermal desorption and impulsive scattering (IS) pathways that depend strongly on θs. Characterization of the data in terms of the final angle, rotational state, spin-orbit electronic state, collision energy, and liquid permit new correlations to be revealed and investigated in detail. For example, the IS rotational distributions reveal an enhanced propensity for higher J/spin-orbit excited states scattered into near specular angles and thus hotter rotational/electronic distributions measured in the forward scattering direction. Even more surprisingly, the average NO scattering angle (⟨θs⟩) exhibits a remarkably strong correlation with final angular momentum, N, which implies a linear scaling between net forward scattering propensity and torque delivered to the NO projectile by the gas-liquid interface.

Sub-Doppler laser cooling using electromagnetically induced transparency

We propose a sub-Doppler laser cooling mechanism that takes advantage of the unique spectral features and extreme dispersion generated by the phenomenon of electromagnetically induced transparency (EIT). EIT is a destructive quantum interference phenomenon experienced by atoms with multiple internal quantum states when illuminated by laser fields with appropriate frequencies. By detuning the lasers slightly from the "dark resonance", we observe that, within the transparency window, atoms can be subject to a strong viscous force, while being only slightly heated by the diffusion caused by spontaneous photon scattering. In contrast to other laser cooling schemes, such as polarization gradient cooling or EIT-sideband cooling, no external magnetic field or strong external confining potential is required. Using a semiclassical approximation, we derive analytically quantitative expressions for the steady-state temperature, which is confirmed by full quantum mechanical numerical simulations. We find that the lowest achievable temperatures approach the single-photon recoil energy. In addition to dissipative forces, the atoms are subject to a stationary conservative potential, leading to the possibility of spatial confinement. We find that under typical experimental parameters this effect is weak and stable trapping is not possible.

Quantum optical circulator controlled by a single chirally coupled atom.

Integrated nonreciprocal optical components, which have an inherent asymmetry between their forward and backward propagation direction, are key for routing signals in photonic circuits. Here, we demonstrate a fiber-integrated quantum optical circulator operated by a single atom. Its nonreciprocal behavior arises from the chiral interaction between the atom and the transversally confined light. We demonstrate that the internal quantum state of the atom controls the operation direction of the circulator and that it features a strongly nonlinear response at the single-photon level. This enables, for example, photon number-dependent routing and novel quantum simulation protocols. Furthermore, such a circulator can in principle be prepared in a coherent superposition of its operational states and may become a key element for quantum information processing in scalable integrated optical circuits.

Phonon Guided Biology. Architecture of Life and Conscious Perception Are Mediated by Toroidal Coupling of Phonon, Photon and Electron Information Fluxes at Discrete Eigenfrequencies.

Recently, a novel biological principle, revealing specific electromagnetic (EM) radiation frequencies that sustain life, was presented by us on the basis of an evaluation of 175 biological articles concerning beneficial effects of electromagnetic waves on the state of living cells. This concept was also based on a very similar range of frequencies emitted by a clay-mineral catalyst of RNA synthesis that may have been instrumental in the evolutionary initiation of first life, and therefore was tentatively designated as “Algorithm of Life”. The particular spectrum of frequency bands indicate that nature seems to employ discrete eigenfrequencies or standing waves that match precisely with an acoustic scale, with frequency ratios of 1:2, and closely approximated by 2:3, 3:4, 3:5, 4:5 and higher partials, allowing the discrete frequencies to be expressed in scalars. Our further studies clearly indicate now that this “life algorithm” pattern matches very well with the mathematical calculations of W. Ritz (1909) to compute eigenfrequencies of the sound induced geometric patterns. These have been earlier demonstrated through membrane vibration experiments of E. Chladni (1787), as well as several follow up studies from 1970-2013. Our findings, therefore, touch upon the science of acoustics, also since we show that the discrete frequencies could be modeled by music torus geometry. We postulate that the spectrum of EM frequencies detected, exhibit a quantum ordering effect on life cells on the basis of induction of geometric wave patterns. These constitute phonon/photon and electron wave energies, and quantum oscillations at far-infrared frequencies, that are communicated through toroidal constructive interference into scalar wave information. This idea is supported through our identification of potential intrinsic toroidal eigenfrequencies and minimal energy levels. The particular torus topology for information processing may also provide quantum error correction and protection against decoherence. Finally we propose a phonon guided organization of cells and integral brain function by three elementary processes: 1) A phonon mediated geometric organization of coherent arrangement of water molecules in cellular plasma, leading to instructive functional organization of cellular structures and metabolic processes and enabling the origination and sustainment of life processes. 2) Toroidal phonon/photon/electron coupling, protecting standing wave coherency of resonant cell components such as proteins and DNA. 3) A toroidal integration of electromagnetic and phononic fluxes of information into scalar standing waves, promoting quantum flux of informational excitons such as Ca2+- ions and electrons (polaron and polariton formation). Our brain, therefore, can be placed in a 4+1 geometry, supported by internal and external quantum states and makes use of geometrical defined information fluxes, that are converted to standing waves. The integration of these interrelated processes is considered to be instrumental in the creation of conscious perception and is proposed to be organized in a fractal, nested, 4-D toroidal geometry.

Cold molecules: Formation, ro-vibrational cooling and electronic conversion

The possibility of controlling all the motion as well as the internal quantum state of a sample of molecules is a long term goal in the cold molecules field. Although many different techniques have been used to produce ultra-cold molecules, in this paper, we will concentrate on the optical pumping technique successfully used to achieve rotational and vibrational cooling of Cs2molecules. We will review the different photo-association schemes for molecule formation, the detection schemes through photoionization, the ro-vibrational cooling into a single level and finally the electronic conversion. In addition, we will present a theoretical model for both ro-vibrational cooling and electronic conversion that can be used for the preparation of different experiments.

The cryogenic storage ring CSR.

An electrostatic cryogenic storage ring, CSR, for beams of anions and cations with up to 300 keV kinetic energy per unit charge has been designed, constructed, and put into operation. With a circumference of 35 m, the ion-beam vacuum chambers and all beam optics are in a cryostat and cooled by a closed-cycle liquid helium system. At temperatures as low as (5.5 ± 1) K inside the ring, storage time constants of several minutes up to almost an hour were observed for atomic and molecular, anion and cation beams at an energy of 60 keV. The ion-beam intensity, energy-dependent closed-orbit shifts (dispersion), and the focusing properties of the machine were studied by a system of capacitive pickups. The Schottky-noise spectrum of the stored ions revealed a broadening of the momentum distribution on a time scale of 1000 s. Photodetachment of stored anions was used in the beam lifetime measurements. The detachment rate by anion collisions with residual-gas molecules was found to be extremely low. A residual-gas density below 140 cm(-3) is derived, equivalent to a room-temperature pressure below 10(-14) mbar. Fast atomic, molecular, and cluster ion beams stored for long periods of time in a cryogenic environment will allow experiments on collision- and radiation-induced fragmentation processes of ions in known internal quantum states with merged and crossed photon and particle beams.