Atomic, molecular & optical (AMO) sensing

Spin-orbit torque (SOT) provides an efficient route for manipulating magnetization in spintronic devices, and its accurate quantification is essential. Here, we investigate Co/Gd-based synthetic ferrimagnets using complementary magnetotransport and magneto-optical techniques. We use a Sagnac magneto-optical interferometry method to directly quantify current-induced magnetization tilting and extract the damping-like SOT effective field. The Sagnac measurements show good agreement with harmonic Hall analysis across different Co/Gd and Gd/Pt/Co heterostructures, providing a quantitative determination of the damping-like SOT effective field that does not rely on electrical transport signatures. By varying the Gd thickness and multilayer stacking order, we demonstrate that the damping-like torque is strongly influenced by spin transport and angular momentum conversion at rare-earth and heavy-metal interfaces. The observation of a finite torque in Gd/Pt/Co/Pt structures, where conventional Pt spin Hall contributions are expected to compensate, highlights the active role of the Gd layer in SOT generation. Furthermore, interface engineering enables perpendicular magnetic anisotropy in Gd/Pt/Co/Al heterostructures with a 2-nm-thick Co layer, allowing current-induced SOT switching at current densities of 8-10 MA/cm². These results establish rare-earth-based synthetic ferrimagnets as a versatile platform for engineering spin-orbit phenomena and optimizing low-power spintronic devices.

High Resolution Image Download MS PowerPoint Slide Ytterbium doped cesium lead halide materials exhibit a property known as quantum cutting which allows for greater than 100% photoluminescent quantum yields (PLQYs). The local atomic structure of the defects responsible for these properties and the effectiveness of the doping for producing the desired PLQYs is not readily discerned using techniques requiring long-range order. In this work we prepared 2.5, 5, 10, and 20% Yb 3+ doped CsPbCl 3 powders using mechanosynthesis under distinct stoichiometric ratio conditions and characterized the defect incorporation and its effects on local atomic disorder using solid-state nuclear magnetic resonance (SSNMR) spectroscopy. We then correlate our observations to the observed PLQYs for each of the prepared samples. All samples prepared were found to be in an orthorhombic phase and no lattice shrinking was observed upon increased Yb 3+ doping. An increase in doping concentrations was accompanied by a decrease in 133 Cs NMR spin–lattice relaxation times T 1 consistent with a paramagnetic relaxation enhancement effect induced by Yb 3+ incorporation into the perovskite lattice. Through a comparison of synthesis methods, PLQY and NMR T 1 parameters we found that incorporated defects favorable for PLQY in mechanosynthesized samples are more likely to form in the presence of excess lead and excess chloride ions. The maximum PLQY values obtained for each set of samples correlated with T 1 parameters in the range of 13 to 35 s. In addition, we found that the observed PLQY in 5% doped samples was optimized after 1 to 2 h of interval grinding in stainless steel jars. Further grinding beyond 2 h led to a reduction in particle size below 1 μm as well as a reduction in PLQY and spin relaxation times.

Spin squeezed states provide a seminal example of how the structure of quantum mechanical correlations can be controlled to produce metrologically useful entanglement. Such squeezed states have been demonstrated in a wide variety of artificial quantum systems ranging from atoms in optical cavities to trapped ion crystals. By contrast, despite their numerous advantages as practical sensors, spin ensembles in solid-state materials have yet to be controlled with sufficient precision to generate targeted entanglement such as spin squeezing. In this work, we present the first experimental demonstration of spin squeezing in a solid-state spin system. Our experiments are performed on a strongly-interacting ensemble of nitrogen-vacancy (NV) color centers in diamond at room temperature, and squeezing (-0.5 ± 0.1 dB) is generated by the native magnetic dipole-dipole interaction between NVs. In order to generate and detect squeezing in a solid-state spin system, we overcome a number of key challenges of broad experimental and theoretical interest. First, we develop a novel approach, using interaction-enabled noise spectroscopy, to characterize the quantum projection noise in our system without directly resolving the spin probability distribution. Second, noting that the random positioning of spin defects severely limits the generation of spin squeezing, we implement a pair of strategies aimed at isolating the dynamics of a relatively ordered sub-ensemble of NV centers. Our results open the door to entanglement-enhanced metrology using macroscopic ensembles of optically active spins in solids.

We introduce a novel protocol, which enables Heisenberg-limited quantum-enhanced sensing using the dynamics of any interacting many-body Hamiltonian. Our approach - dubbed butterfly metrology - utilizes a single application of forward and reverse time evolution to produce a coherent superposition of a "scrambled" and "unscrambled" quantum state. In this way, we create metrologically-useful long-range entanglement from generic local quantum interactions. The sensitivity of butterfly metrology is given by a sum of local out-of-time-order correlators (OTOCs) - the prototypical diagnostic of quantum information scrambling. Our approach broadens the landscape of platforms capable of performing quantum-enhanced metrology; as an example, we provide detailed blueprints and numerical studies demonstrating a route to scalable quantum-enhanced sensing in ensembles of solid-state spin defects.

Can superconductivity arise from strong repulsive interactions between electrons in a lattice model with topological bands? Here, the authors answer this question in the affirmative via DMRG numerical simulations of an interacting spinful bilayer Hofstadter model featuring low-lying bands of opposite Chern number. Furthermore, by developing a new technique to probe the pairing symmetry in number-conserving DMRG, the authors demonstrate that superconductivity is $p$-wave, tantalizingly reminiscent of nodal pairing recently observed in twisted bilayer graphene, which shares many structural similarities with their model. This work thus showcases the possibility of an all-electronic pairing mechanism in the strong coupling limit in two dimensions, which can be tested directly with cold fermions in an optical lattice.

Spin squeezing is a form of entanglement that reshapes the quantum projection noise to improve measurement precision. Here, we provide numerical and analytic evidence for the following conjecture: any Hamiltonian exhibiting finite-temperature easy-plane ferromagnetism can be used to generate scalable spin squeezing, thereby enabling quantum-enhanced sensing. Our conjecture is guided by a connection between the quantum Fisher information of pure states and the spontaneous breaking of a continuous symmetry. We demonstrate that spin squeezing exhibits a phase diagram with a sharp transition between scalable squeezing and non-squeezing. This transition coincides with the equilibrium phase boundary for XY order at a finite temperature. In the scalable squeezing phase, we predict a sensitivity scaling that lies between the standard quantum limit and the scaling achieved in all-to-all coupled one-axis twisting models. A corollary of our conjecture is that short-ranged versions of two-axis twisting cannot yield scalable metrological gain. Our results provide insights into the landscape of Hamiltonians that can be used to generate metrologically useful quantum states. Generating highly squeezed states for quantum sensing requires precise entanglement properties, which makes it a hard task. Now a conjecture identifies a realistic regime of magnetic order at finite temperatures that enables scalable spin squeezing.

Characterizing strongly correlated matter is an increasingly central challenge in quantum science, where structure is often obscured by massive entanglement. It is becoming clear that in the quantum regime, state preparation and characterization should not be treated separately-entangling the two processes provides a quantum advantage in information extraction. Here, we present an approach that we term "manybody Ramsey interferometry" that combines adiabatic state preparation and Ramsey spectroscopy: Leveraging our recently developed one-to-one mapping between computational-basis states and manybody eigenstates, we prepare a superposition of manybody eigenstates controlled by the state of an ancilla qubit, allow the superposition to evolve relative phase, and then reverse the preparation protocol to disentangle the ancilla while localizing phase information back into it. Ancilla tomography then extracts information about the manybody eigenstates, the associated excitation spectrum, and thermodynamic observables. This work illustrates the potential for using quantum computers to efficiently probe quantum matter.

Interactions govern the flow of information and the formation of correlations between constituents of many-body quantum systems, dictating phases of matter found in nature and forms of entanglement generated in the laboratory. Typical interactions decay with distance and thus produce a network of connectivity governed by geometry—such as the crystalline structure of a material or the trapping sites of atoms in a quantum simulator1,2. However, many envisioned applications in quantum simulation and computation require more complex coupling graphs including non-local interactions, which feature in models of information scrambling in black holes3–6 and mappings of hard optimization problems onto frustrated classical magnets7–11. Here we describe the realization of programmable non-local interactions in an array of atomic ensembles within an optical cavity, in which photons carry information between atomic spins12–19. By programming the distance dependence of the interactions, we access effective geometries for which the dimensionality, topology and metric are entirely distinct from the physical geometry of the array. As examples, we engineer an antiferromagnetic triangular ladder, a Möbius strip with sign-changing interactions and a treelike geometry inspired by concepts of quantum gravity5,20–22. The tree graph constitutes a toy model of holographic duality21,22, in which the quantum system lies on the boundary of a higher-dimensional geometry that emerges from measured correlations23. Our work provides broader prospects for simulating frustrated magnets and topological phases24, investigating quantum optimization paradigms10,11,25,26 and engineering entangled resource states for sensing and computation27,28. The reported network of connectivity between atomic ensembles is entirely programmable and independent of its geometrical arrangement, because of the interaction with an optical cavity.

Numerous conceptually important quantum algorithms rely on a blackbox device known as an oracle, which is typically difficult to construct without knowing the answer to the problem that the algorithm is intended to solve.A notable example is Grover's search algorithm.Here we propose a Grover search for solutions to a class of NP-complete decision problems known as subset sum problems, including the special case of number partitioning.Each problem instance is encoded in the couplings of a set of qubits to a central spin or boson, which enables a realization of the oracle without knowledge of the solution.The algorithm provides a quantum speedup across a known phase transition in the computational complexity of the partition problem, and we identify signatures of the phase transition in the simulated performance.Whereas the naive implementation of our algorithm requires a spectral resolution that scales exponentially with system size for NP-complete problems, we also present a recursive algorithm that enables scalability.We propose and analyze implementation schemes with cold atoms, including Rydberg-atom and cavity-QED platforms.

Using an ensemble of atoms in an optical cavity, we engineer a family of nonlocal Heisenberg Hamiltonians with continuously tunable anisotropy of the spin-spin couplings. We thus gain access to a rich phase diagram, including a paramagnetic-to-ferromagnetic Ising phase transition that manifests as a diverging magnetic susceptibility at the critical point. The susceptibility displays a symmetry between Ising interactions and XY (spin-exchange) interactions of the opposite sign, which is indicative of the spatially extended atomic system behaving as a single collective spin. Images of the magnetization dynamics show that spin-exchange interactions protect the coherence of the collective spin, even against inhomogeneous fields that completely dephase the noninteracting and Ising systems. Our results underscore prospects for harnessing spin-exchange interactions to enhance the robustness of spin squeezing protocols.

Quantum electrodynamics is rapidly finding a set of new applications in thresholdless lasing, photochemistry, and quantum entanglement due to the development of sophisticated patterning techniques to couple nanoscale photonic emitters with photonic and plasmonic cavities. Colloidal and epitaxial semiconductor nanocrystals or quantum dots (QDs) are promising candidates for emitters within these architectures but are dramatically less explored in this role than are molecular emitters. This perspective reviews the basic physics of emitter-cavity coupling in the weak-to-strong coupling regimes, describes common architectures for these systems, and lists possible applications (in particular, photochemistry), with a focus on the advantages and issues associated with using QDs as the emitters.

We propose an experimentally realizable quantum spin model that exhibits fast scrambling, based on nonlocal interactions that couple sites whose separation is a power of 2. By controlling the relative strengths of deterministic, nonrandom couplings, we can continuously tune from the linear geometry of a nearest-neighbor spin chain to an ultrametric geometry in which the effective distance between spins is governed by their positions on a tree graph. The transition in geometry can be observed in quench dynamics, and is furthermore manifest in calculations of the entanglement entropy. Between the linear and treelike regimes, we find a peak in entanglement and exponentially fast spreading of quantum information across the system. Our proposed implementation, harnessing photon-mediated interactions among cold atoms in an optical cavity, offers a test case for experimentally observing the emergent geometry of a quantum many-body system.

We report direct observations of photon-mediated spin-exchange interactions in an atomic ensemble. Interactions extending over a distance of 500 μm are generated within a cloud of cold rubidium atoms coupled to a single mode of light in an optical resonator. We characterize the system via quench dynamics and imaging of the local magnetization, verifying the coherence of the interactions and demonstrating optical control of their strength and sign. Furthermore, by initializing the spin-1 system in the m_{f}=0 Zeeman state, we observe correlated pair creation in the m_{f}=±1 states, a process analogous to spontaneous parametric down-conversion and to spin mixing in Bose-Einstein condensates. Our work opens new opportunities in quantum simulation with long-range interactions and in entanglement-enhanced metrology.

Recent advances in ultrafast measurement in cold atoms, as well as pump-probe spectroscopy of K_{3}C_{60} films, have opened the possibility of rapidly quenching systems of interacting fermions to, and across, a finite temperature superfluid transition. However, determining that a transient state has approached a second-order critical point is difficult, as standard equilibrium techniques are inapplicable. We show that the approach to the superfluid critical point in a transient state may be detected via time-resolved transport measurements, such as the optical conductivity. We leverage the fact that quenching to the vicinity of the critical point produces a highly time dependent density of superfluid fluctuations, which affect the conductivity in two ways. First, by inelastic scattering between the fermions and the fluctuations, and second by direct conduction through the fluctuations, with the latter providing a lower resistance current carrying channel. The competition between these two effects leads to nonmonotonic behavior in the time-resolved optical conductivity, providing a signature of the critical transient state.

We propose an approach to quantum phase estimation that can attain precision near the Heisenberg limit without requiring single-particle-resolved state detection. We show that the "one-axis twisting" interaction, well known for generating spin squeezing in atomic ensembles, can also amplify the output signal of an entanglement-enhanced interferometer to facilitate readout. Applying this interaction-based readout to oversqueezed, non-Gaussian states yields a Heisenberg scaling in phase sensitivity, which persists in the presence of detection noise as large as the quantum projection noise of an unentangled ensemble. Even in dissipative implementations-e.g., employing light-mediated interactions in an optical cavity or Rydberg dressing-the method significantly relaxes the detection resolution required for spectroscopy beyond the standard quantum limit.

We study the response of a highly excited time-dependent quantum many-body state to a sudden local perturbation, a sort of orthogonality catastrophe problem in a transient nonequilibrium environment. To this extent we consider, as a key quantity, the overlap between time-dependent wave functions, which we write in terms of a novel two-time correlator generalizing the standard Loschmidt echo. We discuss its physical meaning, general properties, and its connection with experimentally measurable quantities probed through nonequilibrium Ramsey interferometry schemes. Then we present explicit calculations for a one-dimensional interacting Fermi system brought out of equilibrium by a sudden change of the interaction, and perturbed by the switching on of a local static potential. We show that different scattering processes give rise to remarkably different behaviors at long times, quite opposite from the equilibrium situation. In particular, while the forward scattering contribution retains its power-law structure even in the presence of a large nonequilibrium perturbation, with an exponent that is strongly affected by the transient nature of the bath, the backscattering term is a source of nonlinearity which generates an exponential decay in time of the Loschmidt Echo, reminiscent of an effective thermal behavior.

Nylon nucleic acids containing oligouridine nucleotides with pendent polyamide linkers and flanked by unmodified heteronucleotide sequences were prepared by DNA templated synthesis. Templation was more efficient than the single-stranded synthesis: Coupling step yields were as high as 99.2%, with up to 7 amide linkages formed in the synthesis of a molecule containing 8 modified nucleotides. Controlled digestion by calf spleen phosphodiesterase enabled the mapping of modified nucleotides in the sequences. A combination of complete degradation of nylon nucleic acids by snake venom phosphodiesterase and dephosphorylation of the resulting nucleotide fragments by bacterial alkaline phosphatase, followed by LCMS analysis, clarified the linear structure of the oligo-amide linkages. The templated synthesis strategy afforded nylon nucleic acids in the target structure and was compatible with the presence heteronucleotides. The complete digestion procedure produced a new species of DNA analogues, nylon ribonucleosides, which display nucleosides attached via a 2'-alkylthio linkage to each diamine and dicarboxylate repeat unit of the original nylon nucleic acids. The binding affinity of a nylon ribonucleoside octamer to the complementary DNA was evaluated by thermal denaturing experiments. The octamer was found to form stable duplexes with an inverse dependence on salt concentration, in contrast to the salt-dependent DNA control.

A combination of host-guest chemistry and coordination chemistry in the design of electrochemical sensors for alkali metal and ammonium ions is described. The sensor molecules are coordination complexes between a copper ion and a functionalized tripodal ligand. Upon presentation of the ion to the sensor molecule, a shift in the redox potential of the copper ion occurs. In the course of the study, three new alkoxyphenyl-substituted derivatives of the ligand tris(2-pyridylmethyl)amine (TPA) were prepared and characterized. The synthesis of the new ligands involved the preparation of bromopyridyl-TPA derivatives followed by Suzuki coupling with substituted phenylboronic acids. Cyclic voltammetry studies of copper complexes of the ligands indicated that steric effects played a dominant role in the overall determination of the copper redox couple. Studies of the alkoxyphenyl ligands indicated that small but reproducible changes in the copper redox couple occurred upon presentation of a guest cation that would be expected to form a complex with the copper-ligand complex.

Abstract The synthesized hemispherands (VII) and (IX)‐(X) form complexes with alkali picrates or alkylammonium picrates.