Quantum Transitions Research Articles

Quantum phases and transitions in spin chains with non-invertible symmetries

Generalized symmetries often appear in the form of emergent symmetries in low energy effective descriptions of quantum many-body systems. Non-invertible symmetries are a particularly exotic class of generalized symmetries, in that they are implemented by transformations that do not form a group. Such symmetries appear in large families of gapless states of quantum matter and constrain their low-energy dynamics. To provide a UV-complete description of such symmetries, it is useful to construct lattice models that respect these symmetries exactly. In this paper, we discuss two families of one-dimensional lattice Hamiltonians with finite on-site Hilbert spaces: one with (invertible) S_3S3 symmetry and the other with non-invertible \mathsf{Rep}(S_3)𝖱𝖾𝗉(S3) symmetry. Our models are largely analytically tractable and demonstrate all possible spontaneous symmetry breaking patterns of these symmetries. Moreover, we use numerical techniques to study the nature of continuous phase transitions between the different symmetry-breaking gapped phases associated with both symmetries. Both models have self-dual lines, where the models are enriched by so-called intrinsically non-invertible symmetries generated by Kramers-Wannier-like duality transformations. We provide explicit lattice operators that generate these non-invertible self-duality symmetries. We show that the enhanced symmetry at the self-dual lines is described by a 2+1d symmetry-topological-order (SymTO) of type JK_4\boxtimes \overline{JK}_4JK4⊠JK¯4. The condensable algebras of the SymTO determine the allowed gapped and gapless states of the self-dual S_3S3-symmetric and \mathsf{Rep}(S_3)𝖱𝖾𝗉(S3)-symmetric models.

Nonlinear Excitation of Color Centers in a LiF Crystal by Femtosecond Laser Radiation

Experiments were carried out in which the luminescence of color centers in lithium fluoride crystals was excited by two different femtosecond lasers with significantly different energies, durations and pulse repetition rates. It was established that in all experiments the main center, the luminescence of which was excited nonlinearly, was the F3+ color center. Unusual experimental data were obtained; a laser with low pulse energy (4 nJ) excited triplet luminescence of these centers (570 nm) but did not excite singlet luminescence (540 nm). Another laser with a higher pulse energy (0.3 mJ), on the other hand, excited singlet luminescence and did not excite triplet luminescence. A proposed diagram of energy levels and quantum transitions is presented, explaining the possible mechanisms of nonlinear excitation of luminescence in these experiments.

Single and double quantum transitions in spin-mixed states under photo-excitation

Electronic spins associated with the Nitrogen-Vacancy (NV) center in diamond offer an opportunity to study spin-related phenomena with extremely high sensitivity owing to their high degree of optical polarization. Here, we study both single- and double-quantum transitions (SQT and DQT) in NV centers between spin-mixed states, which arise from magnetic fields that are non-collinear to the NV axis. We demonstrate the amplification of the ESR signal from both these types of transition under laser illumination. We obtain hyperfine-resolved X-band ESR signal as a function of both excitation laser power and misalignment of static magnetic field with the NV axis. This, combined with our analysis using a seven-level model that incorporates thermal polarization and double quantum relaxation, allows us to comprehensively analyze the polarization of NV spins under off-axis fields. Such detailed understanding of spin-mixed states in NV centers under photo-excitation can help greatly in realizing NV-diamond platform’s potential in sensing correlated magnets and biological samples, as well as other emerging applications, such as masing and nuclear hyperpolarization.

Controlled single-electron transfer enables time-resolved excited-state spectroscopy of individual molecules.

An increasing number of scanning-probe-based spectroscopic techniques provides access to diverse electronic properties of single molecules. Typically, these experiments can only study a subset of all electronic transitions, which obscures the unambiguous assignment of measured quantities to specific quantum transitions. Here we develop a single-molecule spectroscopy that enables the access to many quantum transitions of different types, including radiative, non-radiative and redox, that is, charge-related, transitions. Our method relies on controlled alternating single-charge attachment and detachment. For read-out, the spin states are mapped to charge states, which we can detect by atomic force microscopy. We can determine the relative energies of ground and excited states of an individual molecule and can prepare the molecule in defined excited states. After a proof-of-principle demonstration of the technique on pentacene, we apply it to PTCDA, the scanning-probe luminescence of which has been interpreted controversially. The method may be used to guide, understand and engineer tip-induced chemical reactions as well as phosphorescence and fluorescence of individual molecules.

Inorganic/organic sublattice roles in band edge photodynamics of isoelectronically substituted hybrid semiconductors

Zero-dimensional organic–inorganic hybrid metal halides are unique semiconductors with fruitful physical properties. Usually, only the inorganic polyhedrons dominate the band edge electronic and photophysical properties of such hybrid semiconductors, whereas the organic components mainly act as structure-stabilizing units. Herein, we study the electronic structures and photodynamics of isoelectronically Br-substituted (I) zero-dimensional organic–inorganic copper halide semiconductors (C9H14N)3Cu3(BrxI1−x)6. They are composed of both inorganic [Cu3(BrxI1−x)6]3− units and organic C9H14N+ skeletons. It is surprising to find that unlike usual organic–inorganic metal halides, although the heavily isoelectronic substitution of halogen atoms in the (C9H14N)3Cu3I6 crystal leads to significant shrinkage of the lattice, it does not remarkably alter the bandgap and luminescence peak owing to the site-projected density of states as revealed by the density functional theory calculation. The inorganic units dominate the valence band edge quantum states, whereas the organic skeletons dominate the conduction-band edge states. However, the isoelectronic substitution significantly lowers the symmetry of the crystal, and as a result, the quantum transition probability at the band edge increases first and decreases then with increasing concentration of substituting bromine atoms. The (C9H14N)3Cu3(BrxI1−x)6 crystals exhibit dual-band luminescence with large Stokes shift and near-unity quantum yield. It arises from the excitons trapped by two kinds of centers. The critical participation of the organic skeletons in the electronic structures and band edge photodynamics refresh our knowledge of their roles in the hybrid semiconductors.

Impact and Implications of Quantum Computing on Blockchain-based Electronic Health Record Systems

Aims This study will investigate the integration of quantum computing and blockchain technology of EHR systems, evaluating the potential and major vulnerabilities of the developed blockchain platforms. In addition, through this evaluation, in this paper, transaction capabilities, energy consumption, and quantum susceptibilities of Ethereum, Bitcoin, and Ripple are being evaluated. Further, research gaps on quantum implications and transition strategies to quantum-resistant systems for achieving secure, efficient, and patient-centric Healthcare 4.0 are identified. Background The embedding of quantum computing and blockchain technology within EHR systems represents the next wave of scientific development within the healthcare sector. However, at the same time, emerging quantum capabilities have raised serious vulnerabilities for major blockchain platforms. If Ethereum and Bitcoin display quantum threats regarding their high transaction capacities, then Ripple, with its high rate of transactions, truly presents a high stake in terms of quantum threats. Further, the energy consumption discrepancies pose some environmental impacts and point to the need for research on energy-efficient quantum-resistant systems. Objective This research investigates the potential and vulnerabilities of major blockchain platforms with electronic health record systems in a new quantum computing environment. In that context, this work evaluates transaction capacities, quantum threats, and energy use for platforms like Ethereum, Bitcoin, and Ripple. Additionally, it seeks to identify research gaps and propose transition strategies toward a quantum-resistant system in support of the development of a secure and efficient Healthcare 4.0. Methods This work focused on assessing the potential and vulnerabilities of blockchain platforms under quantum computing threats in EHR systems. We analyzed transaction processing rates, quantum susceptibilities, and energy consumption metrics for the Ethereum, Bitcoin, and Ripple platforms. A complete literature review is presented with respect to realistic quantum implications and practical transition strategies toward quantum-resistant systems oriented to support the development of secure and efficient Healthcare 4.0. Results The evaluations revealed that Ethereum processed 30 transactions per second and Bitcoin processed 7, with each having low quantum vulnerability. Ripple, at 1500 transactions per second, also had significant quantum vulnerabilities. In addition to energy use, Bitcoin consumes 707 kWh per single transaction compared with Ripple's 0.0078 kWh. Other gaps in research existed in real-world quantum consequences and considerations for transitioning to quantum-resistant systems, all of which are vital for making Healthcare 4.0 secure and efficient. Conclusion This has underscored the transformative potential as well as the weaknesses involved in integrating quantum computing and blockchain technologies into EHR. However, Ethereum, Bitcoin, and Ripple vary in their transaction rates; all three face a similar quantum threat while having large differences in energy consumption. These are problems that would call for more research into quantum-resistant systems and strategic implementation. Actualization of a secure, efficient, and patient-centered Healthcare 4.0 will call for proactive research collaboration and strategic efforts towards ensuring technological and environmental sustainability.

Optically induced quantum transitions in direct probed mesoscopic NbSe2 for prototypical bolometers

Superconducting transition-edge sensors (TES) have emerged as fascinating devices to detect broadband electromagnetic radiation with low thermal noise. The advent of metallic transition metal dichalcogenides, such as NbSe2, has also created an impetus to understand their low-temperature properties, including superconductivity. Interestingly, NbSe2-based sensor within the TES framework remains unexplored. In this work, direct-probed superconducting NbSe2 absorbers led to a proof-of-concept demonstration for the transduction of incoming light to heat, where a thermodynamic superconducting phase transition in NbSe2 was evident to switch it to the normal state, when biased below its superconducting transition temperature. A wavelength-dependent response of its optical absorption properties was observed, based on the incident optical excitation source used. Furthermore, extensive optical characterization studies were conducted using Raman spectroscopy, where the in-plane and out-of-plane thermal conductivity was empirically determined. Our results open possibilities for the use of NbSe2 in superconducting radiation detectors, including in a TES framework.

Measurement-induced phase transitions in quantum raise-and-peel models

Measurement-induced phase transitions in quantum raise-and-peel models

(Keynote) Unified Quantum Theory of Electrochemical Kinetics Based on Coupled Ion-Electron Transfer

A general theory of coupled ion–electron transfer (CIET) is presented, which unifies quantum kinetics of electron transfer (ET) with classical kinetics of bond-breaking ion transfer (IT) in a general framework of non-equilibrium thermodynamics [1]. In the limit of large reorganization energy, the theory predicts Marcus kinetics of “electron-coupled ion transfer” (ECIT). In the limit of large ion-transfer energies, the theory predicts generalized Butler–Volmer kinetics of “ion-coupled electron transfer” (ICET), where the charge transfer coefficient and exchange current are connected to microscopic properties of the electrode/electrolyte interface. In the ICET regime, the reductive and oxidative branches of Tafel’s law are predicted to hold over a wide but finite range of overpotentials, bounded by the ion-transfer energies for oxidation and reduction, respectively. The probability distribution of transferring electron energies in CIET smoothly interpolates between a shifted Gaussian distribution for ECIT (as in the Gerischer–Marcus theory of ET) to an asymmetric, fat-tailed Meixner distribution centered at the Fermi level for ICET. The latter may help interpret asymmetric line shapes in x-ray photo-electron spectroscopy (XPS) and Auger electron spectroscopy (AES) for oxidized metal surfaces in terms of shake-up relaxation of the ionized atom and its image polaron by ICET. In the limit of large overpotentials, the theory predicts a transition to inverted Marcus ECIT, leading to a universal reaction-limited current for metal electrodes, dominated by barrierless quantum transitions. Uniformly valid, closed-form asymptotic approximations are derived that smoothly transition between the limiting rate expressions for ICET and ECIT for metal electrodes, using simple but accurate mathematical functions. The theory is applied to lithium intercalation in lithium iron phosphate (LFP) and found to provide a consistent description of the observed current dependence on overpotential, temperature and concentration, learned from x-ray images [2]. CIET theory thus provides a critical bridge between quantum electrochemistry and electrochemical engineering.[1] M. Z. Bazant, Unified quantum theory of electrochemical kinetics by coupled ion-electron transfer, Faraday Discussions 246, 60-124 (2023).[2] H. Zhao, H. D. Deng, A. E. Cohen, J. Lim, Y. Li, D. Fraggedakis, B. Jiang, B. D. Storey, W. C. Chueh, R. D. Braatz, and M. Z. Bazant, Learning heterogeneous reaction kinetics from X-ray movies pixel-by-pixel, Nature 621, 289-294 (2023). Figure 1

In Situ High-Pressure Correlated Transportation of Heavy Rare-Earth Perovskite Nickelates as Batch Synthesized within Eutectic Molten Salts at MPa-pO2.

The multiple magneto-/electrical quantum transitions discovered with d-band correlated metastable perovskite oxides, such as rare-earth nickelate (ReNiO3), enable applications in artificial intelligence and multifunctional sensors. Nevertheless, to date such investigation merely focuses on ReNiO3 with light or middle rare-earth composition, while the analogous explorations toward heavy rare-earth (ReHNiO3, ReH after Gd) are impeded by their ineffective material synthesis relying on GPa pressure. Herein, for the first time we synthesized the powder of ReHNiO3 in grams/batch with ∼1000 times lower pressure and ∼300 °C lower temperature in comparison to the previous ∼101 milligram/batch results, assisted by their eutectic precipitation and heterogeneous growth within alkali-metal halide molten salt at MPa oxygen pressures. Further in situ characterizations under high pressures within a diamond anvil cell reveal a distinguishing pressure predominated bad metal transport within the nonequilibrium state of ReHNiO3 showing high-pressure sensitivity up to 10 GPa, and the temperature dependences in electrical transportations are effectively frozen.

Orders of Magnitude Improved Cyclotron-Mode Cooling for Nondestructive Spin Quantum Transition Spectroscopy with Single Trapped Antiprotons.

We demonstrate efficient subthermal cooling of the modified cyclotron mode of a single trapped antiproton and reach particle temperatures T_{+}=E_{+}/k_{B} below 200mK in preparation times shorter than 500s. This corresponds to the fastest resistive single-particle cyclotron cooling to subthermal temperatures ever demonstrated. By cooling trapped particles to such low energies, we demonstrate the detection of antiproton spin transitions with an error rate <0.000 023, more than 3 orders of magnitude better than in previous best experiments. This method has enormous impact on multi-Penning-trap experiments that measure magnetic moments with single nuclear spins for tests of matter and antimatter symmetry, high-precision mass spectrometry, and measurements of electron g factors bound to highly charged ions that test quantum electrodynamics and establish standards for magnetometry.

Synthesis, structure, spectral and luminescence studies of novel guanidinium aryl(oxy)(sulfanyl)(sulfonyl)acetates

A series of promising luminescent materials, nonlinear optical crystals, and physiologically active compounds – aryl(oxy)(sulfanyl)(sulfonyl)acetates of guanidine (A) of unknown type was synthesized. Various functional groups present in (A) were identified using FTIR spectroscopy. 1H and 13C NMR spectral studies further confirm the molecular structure (A). Crystals of guanidinium 4-chlorophenyl(sulfanyl)acetate (1) and guanidinium 4-chlorophenyl(sulfonyl)acetate (2) were successfully grown. They belong to the same lowest symmetry category, but to different crystal systems: monoclinic (1) and orthorhombic (2).It has been established that intrinsic optical absorption begins at a wavelength of ∼ 290 nm for crystalline compound (1) and ∼ 335 nm for crystal (2). The intrinsic luminescence spectrum of crystal (1) includes two bands with maxima at 300 and 515 nm. In the intrinsic luminescence spectrum of crystal (2), only one band is observed with a maximum at 350 nm. Such luminescence in both crystals is excited in the intrinsic absorption bands, as well as by X-ray radiation. In addition, in the near ultraviolet and throughout the visible region, where optical absorption is not detected (it is very weak), low-inertia (less than 10 ns) rather intense luminescence of uncontrolled impurity-defect centers is excited.The spectral bands of optical absorption, photo- and X-ray luminescence discovered in experiments were systematized using a diagram of energy levels and quantum transitions in crystals and defect centers of the compounds under study.

Coherent control from quantum commitment probabilities.

We introduce a general definition of a quantum committor in order to clarify reaction mechanisms and facilitate control in processes where coherent effects are important. With a quantum committor, we generalize the notion of a transition state to quantum superpositions and quantify the effect of interference on the progress of the reaction. The formalism is applicable to any linear quantum master equation supporting metastability for which absorbing boundary conditions designating the reactant and product states can be applied. We use this formalism to determine the dependence of the quantum transition state on coherences in a polaritonic system and optimize the initialization state of a conical intersection model to control reactive outcomes, achieving yields of the desired state approaching 100%. In addition to providing a practical tool, the quantum committor provides a conceptual framework for understanding reactions in cases when classical intuitions fail.

Size‐Dependent Optical Properties and Exciton Self‐Trapping Emission in Carbon Quantum Dots

AbstractCarbon quantum dots (CQDs), synthesized through controlled microplasma treatment of orange juice, exhibit unique luminescent characteristics. The impact of synthesis time on particle size was investigated. Deconvoluted emission spectra displayed broad bands, peaking at an excitation wavelength of 350 nm for CQD sizes of 2.06, 2.4, and 3.09 nm, indicating multiple fluorescence peaks. This suggests a mixture of CQDs with different excitation energies on their surfaces. Luminescence kinetics unveiled three exponential decay components with time constants of 2.73, 4.61, and 3.27 ns, indicating multiple luminescent centers. Emission behavior affected by excitation wavelengths ranging from 350 to 490 nm suggests that quantum transition probabilities are influenced by impurities or defects. These findings emphasize the size‐dependent optical properties and exciton self‐trapping (EST) emission of CQDs. The calculation of the Huang‐Rhys factor S values underscores the profound influence of carrier‐phonon coupling and the Huang‐Rhys factor on the emergence of ESTs within CQDs. Understanding these interactions is crucial for fully utilizing the capabilities of CQDs in applications spanning optoelectronics, sensors, bioimaging, and various technological fields.

Impact of electronic correlation on strong laser-induced bound-state transitions

Electron correlation (EC) plays a crucial role in all multi-electron systems and dynamic processes. In this work, we focus on strong laser-induced bound-bound transitions (BBT), which are fundamental to optical absorption measurements. We use the helium atom, the simplest two-electron system, as our test case, utilizing the ab initio code package HeTDSE. We examined the bound state energy levels, transition dipole moments (TDMs), and the dynamics of strong laser-induced BBT, both with and without considering EC. Our results indicate that EC significantly impacts the energy levels of the bound states and the TDMs. These effects collectively influence the transition dynamics of the excited states. Although EC does not alter the quantum transition pathways between resonance states, it generally increases the probability of resonance transitions in most cases. Our findings provide a quantitative description of EC in laser-induced BBT.

The quantum transition of the two-dimensional Ising spin glass

Quantum annealers are commercial devices that aim to solve very hard computational problems1, typically those involving spin glasses2,3. Just as in metallurgic annealing, in which a ferrous metal is slowly cooled4, quantum annealers seek good solutions by slowly removing the transverse magnetic field at the lowest possible temperature. Removing the field diminishes the quantum fluctuations but forces the system to traverse the critical point that separates the disordered phase (at large fields) from the spin-glass phase (at small fields). A full understanding of this phase transition is still missing. A debated, crucial question regards the closing of the energy gap separating the ground state from the first excited state. All hopes of achieving an exponential speed-up, compared to classical computers, rest on the assumption that the gap will close algebraically with the number of spins5–9. However, renormalization group calculations predict instead that there is an infinite-randomness fixed point10. Here we solve this debate through extreme-scale numerical simulations, finding that both parties have grasped parts of the truth. Although the closing of the gap at the critical point is indeed super-algebraic, it remains algebraic if one restricts the symmetry of possible excitations. As this symmetry restriction is experimentally achievable (at least nominally), there is still hope for the quantum annealing paradigm11–13.

Interplay between short-range and critical long-range fluctuations in the out-of-equilibrium behavior of the particle density at quantum transitions

Interplay between short-range and critical long-range fluctuations in the out-of-equilibrium behavior of the particle density at quantum transitions

Synthesis, structure and luminescence properties of PbLaTb(WO4)4 phosphor ceramics for LEDs applications: Role of Tb rare earth

The development and applications of phosphor ceramics have been driven by their ability to convert various forms of energy into visible light with high efficiency, durability, and specific color outputs. This study reports on synthesis of a novel series of solid solutions, PbLa2-2xTb2x(WO4)4 (0 ≤ x ≤ 0.5), using the solid-phase reaction method. The crystal structure, photoluminescence, excitation spectrum, decay kinetics, diffused reflectance spectra, and morphology of the compounds are characterized. The results reveal that the energy band gap has become even lower due to an increase in the concentration of the activator, and an absorption band of the Tb3+ ion is also observed at 380, 370, 354 and 342 nm, respectively; they correspond to the following quantum transitions 7F6 → 5D3, 7F6 → 5G6, 7F6 → 5L10 and 7F6 → 5L9, respectively. Our prepared PbLaTb(WO4) phosphor ceramics have a wide range of applications, from everyday lighting to advanced display technologies and medical devices, highlights their importance in modern technology.

준 2차원 시스템에서 두 방향의 광 회전 입사에 대한 GaN의 전자 변위와 상호작용에 의한 광 양자 전이 특성

In this paper, optical quantum transition line shapes (QTLSs) and optical quantum transition line widths (QTLWs) are studied in relation to magnetic-field-dependent properties of the electron-deformation potential phonon interaction system. We considered two systems - one was subjected to the right and the other to the left circularly oscillating external fields. The main purpose of this work was to compare the QTLSs, which indicate the absorption power in the two oscillating external fields. The results indicate that the QTLSs of the right are larger than those of the left circularly oscillating external fields, whereas the opposite holds for the QTLWs. In this study, we found that the properties of QTLW and QTLS of GaN significantly increased with increasing temperature and magnetic field strength. The phonon emission transition was found to be the dominant scattering process.

Keldysh Field Theory of Dynamical Exciton Condensation Transitions in Nonequilibrium Electron-Hole Bilayers.

Recent experiments have realized steady-state electrical injection of interlayer excitons in electron-hole bilayers subject to a large bias voltage. In the ideal case in which interlayer tunneling is negligibly weak, the system is in quasiequilibrium with a reduced effective band gap. Interlayer tunneling introduces a current and drives the system out of equilibrium. In this work we derive a nonequilibrium field theory description of interlayer excitons in biased electron-hole bilayers. In the large bias limit, we find that p-wave interlayer tunneling reduces the effective band gap and increases the effective temperature for intervalley excitons. We discuss possible experimental implications for InAs/GaSb quantum wells and transition metal dichalcogenide bilayers.