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At least 127 records · Page 7

Rotational coherence dominates early-time dynamics and produces long-time revivals in the S 2 state of azulene

Here, the ultrafast dynamics of azulene have been debated for decades, with reported picosecond decay constants variously attributed to intramolecular vibrational redistribution (IVR), internal conversion, or rotational dephasing. Using polarization- and femtosecond time-resolved resonance-enhanced multiphoton ionization spectroscopy with a nanosecond delay window, we disentangle this long-standing inconsistency and show that the early 2–5 ps decay component arises entirely from the rotational dephasing of an excited-state wavepacket. Identical time constants extracted from the decay of the parallel signal and the rise of the perpendicular signal across multiple vibronic origins provide an unambiguous rotational anisotropy signature, eliminating the need for IVR-based interpretations. Extending the measurement window to 1.3 ns reveals well-structured J-type and C-type rotational coherence revivals in S 2 azulene on top of the well-documented fluorescence decay, demonstrating that both the short- and long-time dynamics contain information about the coherent rotational dynamics. These results show that azulene, and by extension polycyclic aromatic hydrocarbons, can sustain structured rotational coherence deep into the nanosecond regime, positioning PAHs as model systems for quantum-coherent wavepacket dynamics and providing a framework for probing coherence, decoherence, and rotational control in electronically rich molecular systems.

Zhan, Jie [University of Georgia, Athens, GA (Unit↗

Out-of-time-order correlators bridge classical transport and quantum dynamics

The out-of-time-order correlator (OTOC) has emerged as a central tool for quantifying decoherence across wide-ranging physical platforms. Here, we demonstrate its direct measurement in a classical ensemble using nuclear magnetic resonance with a modulated gradient spin echo sequence and extend the method into a multidimensional correlation to track exchange phenomena. Position is encoded through magnetic field gradients and momentum through the velocity autocorrelation function, enabling experimental access to OTOCs for proton motion confined within the self-similar lattice of the metal–organic framework MOF-808. Here, water confined to specified geometries within the MOF pores gives rise to spatially distinct diffusive eigenmodes with characteristic relative entropies. We demonstrate that periodic radio frequency driving combined with gradient modulation yields entropy evolution through the selection of distinct diffusion modes. Frequency-resolved diffusion spectra connect these entropy dynamics to classical heat exchange laws, revealing how operational features of quantum systems are mirrored in confined, macroscopic spin ensembles.

Fricke, Sophia N. [University of California, Berke↗

Long-lived polaritonic coherence and polaron decoupling effects in 2D electronic spectra

Molecular polaritons, formed by coupling molecular excitons with cavity photons, offer a promising platform for exploring quantum phenomena. A key challenge is understanding how these hybrid states maintain coherence in the presence of environmental vibrations. Here, we show theoretically that collective coupling of many molecular excitons in a cavity can protect polariton coherence from phonon-induced decoherence. Under realistic conditions, the coherence time can extend up to 200 fs at room temperature, compared with 15 fs for typical molecular systems. Simulations of two-dimensional electronic spectra reveal prolonged oscillations between upper and lower polariton states, and reduced vibrational coupling as indicated by changes in the nodal line slope of the lower polariton peak. These findings provide guidance for experimental efforts to realize long-lived polaritons, such as coupling CdSe nanoplatelets to optical cavities.

2D electronic spectroscopy↗

Quantum simulation of boson-related Hamiltonians: techniques, effective Hamiltonian construction, and error analysis

Elementary quantum mechanics proposes that a closed physical system consistently evolves in a reversible manner. However, control and readout necessitate the coupling of the quantum system to the external environment, subjecting it to relaxation and decoherence. Consequently, system-environment interactions are indispensable for simulating physically significant theories. A broad spectrum of physical systems in condensed-matter and high-energy physics, vibrational spectroscopy, and circuit and cavity QED necessitates the incorporation of bosonic degrees of freedom, such as phonons, photons, and gluons, into optimized fermion algorithms for near-future quantum simulations. In particular, when a quantum system is surrounded by an external environment, its basic physics can usually be simplified to a spin or fermionic system interacting with bosonic modes. Nevertheless, troublesome factors such as the magnitude of the bosonic degrees of freedom typically complicate the direct quantum simulation of these interacting models, necessitating the consideration of a comprehensive plan. This strategy should specifically include a suitable fermion/boson-to-qubit mapping scheme to encode sufficiently large yet manageable bosonic modes, and a method for truncating and/or downfolding the Hamiltonian to the defined subspace for performing an approximate but highly accurate simulation, guided by rigorous error analysis. In this pedagogical tutorial review, we aim to provide such an exhaustive strategy, focusing on encoding and simulating certain bosonic-related model Hamiltonians, inclusive of their static properties and time evolutions. Specifically, we emphasize two aspects: (1) the discussion of recently developed quantum algorithms for these interacting models and the construction of effective Hamiltonians, and (2) a detailed analysis regarding a tightened error bound for truncating the bosonic modes for a class of fermion-boson interacting Hamiltonians.

bosonic Hamiltonian↗

Digital quantum simulation of cavity quantum electrodynamics: insights from superconducting and trapped ion quantum testbeds

We explore the potential for hybrid development of quantum hardware where currently available quantum computers simulate open cavity quantum electrodynamical (CQED) systems for applications in optical quantum communication, simulation and computing. Our simulations make use of a recent quantum algorithm that maps the dynamics of a singly excited open Tavis–Cummings model containing N atoms coupled to a lossy cavity. We report the results of executing this algorithm on two noisy intermediate-scale quantum computers: a superconducting processor and a trapped ion processor, to simulate the population dynamics of an open CQED system featuring N = 3 atoms. By applying technology-specific transpilation and error mitigation techniques, we minimize the impact of gate errors, noise, and decoherence in each hardware platform, obtaining results which agree closely with the exact solution of the system. These results can be used as a recipe for efficient and platform-specific quantum simulation of cavity–emitter systems on contemporary and future quantum computers.

cavity QED↗

Quasiparticle spectroscopy in tantalum films with different Ta/sapphire interfaces

One of the crucial aspects of current research in quantum information science is the identification and control of loss mechanisms in superconducting (SC) circuits. Although microwave measurements directly quantify device performance, additional techniques that probe quasiparticle excitations in SC films are needed to understand the microscopic mechanisms underlying dissipation and decoherence. Here, we present results from quasiparticle spectroscopy of Ta/sapphire films by measuring the Meissner-state magnetic susceptibility using a precision frequency-domain resonator specifically designed for thin films. We find direct evidence for additional low-energy excitations in samples with lower internal quality factors. These excitations are consistent with deep subgap states due to two-level systems, Yu–Shiba–Rusinov states near the gap edge, and perhaps other pair-breaking mechanisms. The developed non-destructive frequency-domain quasiparticle spectroscopy is a valuable addition to the quantum materials toolbox.

metal/substrate interlayer↗

Single Electron Self-coherence and Its Wave/Particle Duality in the Electron Microscope

Intensities in high-resolution phase-contrast images from electron microscopes build up discretely in time by detecting single electrons. A wave description of pulse-like coherent-inelastic interaction of an electron with matter implies a time-dependent coexistence of coherent partial waves. Their superposition forms a wave package by phase decoherence of 0.5 - 1 radian with Heisenbergs energy uncertainty ΔE H = $\hbar$/2 Δt -1 matching the energy loss ΔE of a coherent-inelastic interaction and sets the interaction time Δt. In these circumstances, the product of Planck's constant and the speed of light hc is given by the product of the expression for temporal coherence λ 2 /Δλ and the energy loss ΔE. Experimentally, the self-coherence length was measured by detecting the energy-dependent localization of scattered, plane matter waves in surface proximity exploiting the Goos–Hänchen shift. Chromatic-aberration Cc-corrected electron microscopy on boron nitride (BN) proves that the coherent crystal illumination and phase contrast are lost if the self-coherence length shrinks below the size of the crystal unit cell at ΔE > 200 eV. Finally, in perspective, the interaction time of any matter wave compares with the lifetime of a virtual particle of any elemental interaction, suggesting the present concept of coherent-inelastic interactions of matter waves might be generalizable.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Higher-Form Anomalies on Lattices

We show that generic gapped quantum many-body states which respect an anomalous finite higher-form symmetry have an exponentially small overlap with any short-range entangled (SRE) state. Hence, anomalies of higher-form symmetries enforce $intrinsic$ long-range entanglement, which is in contrast with anomalies of ordinary (0-form) symmetries which are compatible with symmetric SRE states (specifically, symmetric cat states). As an application, we show that the anomalies of strong higher-form symmetries provide a diagnostic for mixed-state topological order in $d \geq 2$ spatial dimensions. We also identify a new (3+1)D intrinsic mixed-state topological order that does not obey remote-detectability by local decoherence of the (3+1)D Toric Code with fermionic loop excitations. This breakdown of remote detectability, as encoded in anomalies of strong higher-form symmetries, provides a partial characterization of intrinsically mixed-state topological order.

Feng, Yitao [Peking University, Beijing (China)] (↗

Electronic structures and pseudogap nature of the strongly correlated Kondo semimetals and insulators CeNiSn and CeRhX(X=As, Sb)

Employing temperature (T)-dependent angle-resolved photoemission spectroscopy (ARPES) near the Ce 4d absorption edge, we have investigated the electronic structures of the strongly correlated Kondo insulators (KIs) and/or Kondo semimetals of CeNiSn and CeRhX (X=As, Sb), which also belong to potential topological KIs (TKIs). Good agreement is found between the Fermi surfaces (FSs) measured at the Ce 4d→4f on resonance and those calculated and unfolded into the Ce-only Brillouin zone, supporting the crucial Ce 4f contribution to the Fermi-edge states in them. While the FSs of CeRhSb and CeNiSn are similar to each other, they are quite different from those of CeRhAs, which is understood to originate from the semimetallic Kondo ground states of CeNiSn and CeRhSb in contrast to the insulating Kondo ground state of CeRhAs. T-dependent ARPES demonstrates the existence of the Kondo resonance above the Fermi level (EF) and its T-driven decoherence in CeNiSn and CeRhSb, and the existence of the Ce 4f Kondo-like peak well below EF with a pseudogap in CeRhAs. With increasing T, the tail of the Kondo resonance in CeNiSn and CeRhSb loses its coherence, whereas the Ce 4f Kondo-like peak in CeRhAs persists up to T≥200 K. The Kondo temperatures (TKs) are estimated via the analysis of T-dependent ARPES, yielding TK≈80 K (CeNiSn), TK≈180 K (CeRhSb), and TK≫200 K (CeRhAs). High-resolution, low-T ARPES confirms the Kondo resonance just above EF in CeNiSn and CeRhSb Kondo semimetals and the KI ground state of CeRhAs with a pseudogap of Δ≈30 meV, demonstrating the importance of the coherent Kondo states in determining their potential topological properties. The differences in the T-dependent ARPES of CeNiSn and CeRhSb suggest the weaker f-c hybridization in CeNiSn than in CeRhSb (c: conduction electron), which is likely due to the more localized Ni 3d orbitals than the delocalized Rh 4d orbitals. The differences between the T-dependent ARPES of CeNiSn/CeRhSb Kondo semimetals and those of CeRhAs Kondo insulator are likely due to the smaller volume of CeRhAs than those of CeNiSn/CeRhSb.

Kang, J-S↗

Tracing Long-Lived Atomic Coherences Generated via Molecular Conical Intersections

Accessing coherences is key to fully understand and control ultrafast dynamics of complex quantum systems like molecules. Most photochemical processes are mediated by conical intersections, which generate coherences between electronic states in molecules. We show with accurate calculations performed on gas-phase methyl iodide that electronic coherences of spin-orbit-split states persist in atomic iodine after dissociation. Our simulation predicts a maximum magnitude of vibronic coherence in the molecular regime of 0.75% of the initially photoexcited state population. Upon dissociation, one-third of this coherence magnitude is transferred to a long-lived atomic coherence where vibrational decoherence can no longer occur. To trace these dynamics, we propose a tabletop experimental approach—heterodyned attosecond four-wave-mixing spectroscopy. This technique can temporally resolve small electronic coherence magnitudes and reconstruct the full complex coherence function via phase cycling. Hence, heterodyned attosecond four-wave-mixing spectroscopy leads the way to a complete understanding and optimal control of spin-orbit-coupled electronic states in photochemistry.

Chemical Physics↗

Entanglement-fidelity limits of photonically networked atomic qubits from recoil and timing

The remote entanglement of two atomic quantum memories through photonic interactions is accompanied by atomic momentum recoil. When the interactions occur at different times, such as from the random emission over the lifetime of the atomic excited state, the difference in recoil timing can expose “which-path” information and ultimately lead to decoherence. Time-bin encoded photonic qubits can be particularly sensitive to asynchronous recoil timing. In this paper we study the limits of entanglement fidelity in atomic systems due to recoil and other timing imbalances and show how these effects can be suppressed or even eliminated through proper experimental design.

Quantum communication↗

Electronic Origin of Delicate Antiferromagnetism in Fe 𝑥 ⁢NbS 2

Among the family of intercalated transition-metal dichalcogenides (TMDs), Fe 𝑥 ⁢NbS 2 is found to possess unique current-induced resistive switching behaviors, tunable antiferromagnetic states, and a commensurate charge order, all of which are tied to a critical Fe doping of 𝑥 𝑐 = 1/3. However, the electronic origin of such extreme stoichiometry sensitivities remains unclear. Combining angle-resolved photoemission spectroscopy (ARPES) with density functional theory (DFT) calculations, we identify and characterize a dramatic eV-scale electronic restructuring that occurs across the 𝑥𝑐. Moment-carrying Fe 3⁢𝑑 𝑧 2 electrons manifest as narrow bands within 200 meV of the Fermi level, distinct from other transition metal intercalated TMD magnets. These states strongly hybridize with itinerant electrons in the TMD layer and rapidly lose coherence above 𝑥 𝑐 due to correlation-driven effects. This sudden quasiparticle decoherence collapses the Fe-Nb hybridization, which explicitly suppresses the out-of-plane effective Fe-Fe exchange interaction, driving the transformation of the magnetic ground state from an antiferromagnetic stripe phase to a zigzag phase. Furthermore, these observations resemble the exceptional electronic and magnetic sensitivity of strongly correlated systems, and demonstrate that quantifying orbital-specific hybridization via ARPES offers an alternative pathway to evaluate effective magnetic exchange in metallic magnets, complementing inelastic neutron and resonant x-ray scattering probes.

Angle-resolved photoemission spectroscopy↗

Ultrafast x-ray imaging of coherently controlled molecular dynamics in real space and time

Coherent control aims to manipulate chemical processes on the latent length and timescales of atoms and bonds, scales that are intrinsic to molecular dynamics but not directly resolved by most experimental probes. As a result, existing coherent-control experiments, which overwhelmingly rely on spectroscopic observables, leave a crucial blind spot: the direct, real-space recovery of all atomic and molecular rearrangements in response to coherently controlled excitations. Here, we overcome this limitation by integrating a Tannor-Kosloff-Rice pump-control-probe scheme with ultrafast X-ray scattering to capture snapshots of the wavepacket motion in a benchmark molecular system. We demonstrate this by photoexciting diatomic iodine vapor with a visible pump pulse, selectively steering the wavepacket toward ground-state recombination or dissociative pathways with a time-delayed near-IR control pulse, and recording the dynamics with angstrom and femtosecond precision with an ultrashort hard X-ray probe pulse. By comparing these structural observations with numerical solutions of the time-dependent Schrödinger equation, we reveal how coherent control actively reshapes the molecular charge density distribution. Our results pave the way for leveraging structural feedback as a control handle and provide a fundamental microscopic visualization of quantum decoherence and energy redistribution at the atomic level.

Hopper, Thomas R. [SLAC National Accelerator Labor↗

Parametric amplification of spin-motion coupling in three-dimensional trapped-ion crystals

Three-dimensional (3D) crystals offer a route to scaling up trapped-ion systems for quantum sensing and quantum simulation applications; however, engineering coherent spin-motion couplings and effective spin-spin interactions in large crystals poses technical challenges associated with decoherence and prolonged timescales to generate appreciable entanglement. Here, we explore the possibility of speeding up these interactions in 3D crystals via parametric amplification. For this purpose, we derive a general Hamiltonian for the parametric amplification of spin-motion coupling that is broadly applicable to normal modes with motion transverse to or along the spatial extent of the crystal. Unlike in lower-dimensional crystals, we find that the ability to faithfully (uniformly) amplify the spin-spin interactions in 3D crystals depends on the physical implementation of the spin-motion coupling. We consider the light-shift gate, and the so-called phase-insensitive and phase-sensitive Mølmer-Sørensen (MS) gates, and we find that only the phase-sensitive MS gate can be faithfully amplified in general 3D crystals. We discuss a situation where nonuniform amplification can be advantageous. We also reconsider the effect of counter-rotating terms on parametric amplification and find that they are not as detrimental as previous studies suggest.

Optical parametric oscillators & amplifiers↗

Niobium coaxial cavities with internal quality factors exceeding 1.4 × 10 9 for circuit quantum electrodynamics

Group-V materials such as niobium and tantalum have become popular choices for extending the performance of circuit quantum electrodynamics (cQED) platforms, allowing for quantum processors and memories with reduced error rates and more modes. The complex surface chemistry of niobium, however, makes identifying the main modes of decoherence difficult at millikelvin temperatures and single-photon powers. We use niobium coaxial quarter-wave cavities to study the impact of etch chemistry, prolonged atmospheric exposure, and the significance of cavity conditions prior to and during cooldown—in particular, niobium hydride evolution—on single-photon coherence. We demonstrate cavities with quality factors Q int ≳ 1.4 × 10 9 in the single-photon regime, a 15-fold improvement over aluminum cavities of the same geometry. We rigorously quantify the sensitivity of our fabrication process to various loss mechanisms and demonstrate a two- to fourfold reduction in the two-level system loss tangent and a three- to fivefold improvement in the residual resistance over traditional buffered chemical polishing etching techniques. Finally, we demonstrate transmon integration and coherent cavity control while maintaining a cavity coherence of 11.3 ms. The accessibility of our method, which can be easily replicated in academic laboratory settings, together with the demonstration of its performance, mark an advancement in three-dimensional cQED.

Oriani, Andrew E. [Chicago U., EFI; Chicago U.] (O↗

Control of Dipolar Dynamics by Geometrical Programming

We propose and theoretically analyze methods for quantum many-body control through geometric reshaping of molecular tweezer arrays. Dynamic rearrangement during entanglement is readily available due to the extended coherence times of molecular rotational qubits. We show how motional dephasing can be suppressed and enhanced spin squeezing can be achieved in an actively rearranged short-range XY model. We also analyze in detail a specific static geometry that significantly suppresses decoherence. These general methods as applied to programmable quantum systems offer robust control modalities that are well suited to molecules.

optical tweezers↗

Lieb-Mattis States for Robust Entangled Differential Phase Sensing

We explore a two-node, entanglement-enhanced sensor network for differential phase sensing that exploits decoherence-free subspaces to suppress common-mode noise, a primary limitation of many state-of-the-art quantum sensors. We identify a class of entangled states that, while not strictly optimal, achieve the same asymptotic sensitivity scaling as optimal states and can be prepared efficiently from initially unentangled atomic ensembles. Importantly, the preparation time decreases with increasing system size, which makes the states compatible with realistic noise processes in present-day quantum sensors that operate with large particle numbers but lack full error correction. We illustrate these ideas using two cavity-mediated preparation protocols: (i) coherent, unitary entanglement generation analogous to bosonic two-mode squeezing, yielding Heisenberg scaling, and (ii) dissipative preparation through collective emission into a shared cavity mode, providing a square-root improvement beyond the standard quantum limit. Numerical simulations show that both approaches remain effective at experimentally realistic cavity cooperativities, establishing a practical path toward scalable, quantum-enhanced differential phase sensing.

Kaubruegger, Raphael [National Institute of Standa↗

Formation of niobium hydride precipitates in superconducting qubits

We report evidence for the formation of niobium hydride phase within niobium films on silicon substrates in superconducting qubits fabricated at Rigetti Computing. For this study, we combined complementary techniques—including room-temperature and cryogenic atomic force microscopy (AFM), synchrotron x-ray diffraction, and time-of-flight secondary ion mass spectroscopy (ToF-SIMS)—to directly reveal the existence of niobium hydride precipitates on the surface of superconducting qubits. Upon cryogenic cooling, we observed variation in the size and morphology of the hydrides, ranging from small (∼5 nm) irregular shapes to large (∼10–100 nm) domains within the Nb grains, which were fully converted to niobium hydrides. Since niobium hydrides are nonsuperconducting and can easily change in size and location upon different cooldowns to cryogenic temperature, our finding highlights a previously unknown source of decoherence in superconducting qubits. This contributes to quasiparticle losses, offering a potential explanation for changes in qubit performance upon cooldowns. Finally, by leveraging the RF performance of a 3D bulk Nb resonator, we quantify RF dissipation in a superconducting qubit caused by hydrogen concentration variation, and propose a practical engineering pathway to mitigate the formation of Nb hydrides for superconducting qubit applications.

Sung, Zuhawn [Fermi National Accelerator Laborator↗