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Entangled Photon Spectroscopy

Conspectus The enhanced interest in quantum-related phenomena has provided new opportunities for chemists to push the limits of detection and analysis of chemical processes. As some have called this the second quantum revolution, a time has come to apply the rules learned from previous research in quantum phenomena toward new methods and technologies important to chemists. While there has been great interest recently in quantum information science (QIS), the quest to understand how nonclassical states of light interact with matter has been ongoing for more than two decades. Our entry into this field started around this time with the use of materials to produce nonclassical states of light. Here, the process of multiphoton absorption led to photon-number squeezed states of light, where the photon statistics are sub-Poissonian. In addition to the great interest in generating squeezed states of light, there was also interest in the formation of entangled states of light. While much of the effort is still in foundational physics, there are numerous new avenues as to how quantum entanglement can be applied to spectroscopy, imaging, and sensing. These opportunities could have a large impact on the chemical community for a broad spectrum of applications. Here, we discuss the use of entangled (or quantum) light for spectroscopy as well as applications in microscopy and interferometry. The potential benefits of the use of quantum light are discussed in detail. From the first experiments in porphyrin dendrimer systems by Dr. Dong-Ik Lee in our group to the measurements of the entangled two photon absorption cross sections of biological systems such as flavoproteins, the usefulness of entangled light for spectroscopy has been illustrated. These early measurements led the way to more advanced measurements of the unique characteristics of both entangled light and the entangled photon absorption cross-section, which provides new control knobs for manipulating excited states in molecules. The first reports of fluorescence-induced entangled processes were in organic chromophores where the entangled photon cross-section was measured. These results would later have widespread impact in applications such as entangled two-photon microscopy. From our design, construction and implementation of a quantum entangled photon excited microscope, important imaging capabilities were achieved at an unprecedented low excitation intensity of 10 7 photons/s, which is 6 orders of magnitude lower than the excitation level for the classical two-photon image. New reports have also illustrated an advantage of nonclassical light in Raman imaging as well. From a standpoint of more precise measurements, the use of entangled photons in quantum interferometry may offer new opportunities for chemistry research. Experiments that combine molecular spectroscopy and quantum interferometry, by utilizing the correlations of entangled photons in a Hong–Ou–Mandel (HOM) interferometer, have been carried out. The initial experiment showed that the HOM signal is sensitive to the presence of a resonant organic sample placed in one arm of the interferometer. In addition, parameters such as the dephasing time have been obtained with the opportunity for even more advanced phenomenology in the future.

36 MATERIALS SCIENCE↗

A Wavelength-Multiplexing Toolkit for Quantum Networks

Unleashing the power of quantum technologies at scale will depend heavily on the realization of quantum networks that can connect many hybrid quantum devices and platforms, exploiting each of their respective advantages. Entangled-photon sources and the subsequent manipulations required to link multiple nodes are critical to optimize the connectivity of optical quantum networks.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

The unitary dependence theory for characterizing quantum circuits and states

Abstract Most existing quantum algorithms are discovered accidentally or adapted from classical algorithms, and there is the need for a systematic theory to understand and design quantum circuits. Here we develop a unitary dependence theory to characterize the behaviors of quantum circuits and states in terms of how quantum gates manipulate qubits and determine their measurement probabilities. Compared to the conventional entanglement description of quantum circuits and states, the unitary dependence picture offers more practical information on the measurement and manipulation of qubits, easier generalization to many-qubit systems, and better robustness upon partitioning of the system. The unitary dependence theory can be applied to systematically understand existing quantum circuits and design new quantum algorithms.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Efficient Entanglement of Spin Qubits Mediated by a Hot Mechanical Oscillator

Localized electronic and nuclear spin qubits in the solid state constitute a promising platform for storage and manipulation of quantum information, even at room temperature. However, the development of scalable systems requires the ability to entangle distant spins, which remains a challenge today. We propose and analyze an efficient, heralded scheme that employs a parity measurement in a decoherence free subspace to enable fast and robust entanglement generation between distant spin qubits mediated by a hot mechanical oscillator. We find that high-fidelity entanglement at cryogenic and even ambient temperatures is feasible with realistic parameters and show that the entangled pair can be subsequently leveraged for deterministic controlled-NOT operations between nuclear spins. Our results open the door for novel quantum processing architectures for a wide variety of solid-state spin qubits.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Collection of fluorescence from an ion using trap-integrated photonics

Spontaneously emitted photons are entangled with the electronic and nuclear degrees of freedom of the emitting atom, so interference and measurement of these photons can entangle separate matter-based quantum systems as a resource for quantum information processing. Since confinement in a single-mode facilitates the photon interference needed for generating entanglement, the dipole emission patterns relevant in spontaneous emission present a mode-matching challenge. Current demonstrations rely on bulk photon-collection and manipulation optics that suffer from large component size and system-to-system variability—factors that impede scaling to the large numbers of entangled pairs needed for quantum information processing. To address these limitations, we demonstrate a collection method that enables passive phase stability, straightforward photonic manipulation, and intrinsic reproducibility. Specifically, we engineer a waveguide-integrated grating to couple photons emitted from a trapped ion into a single optical mode within a microfabricated ion-trap chip. Using the integrated collection optic, we characterize the collection efficiency, image the ion, and detect the ion’s quantum state. The integrated optic covers 2.18% of the solid angle and collects 1.97 ± 0.3% of the spontaneously emitted light incident on the grating for a total collection efficiency of 0.043% into a single-mode waveguide. This proof-of-principle demonstration lays the foundation for leveraging the inherent stability and reproducibility of integrated photonics to create, manipulate, and measure multipartite quantum states in arrays of quantum emitters.

Optical physics↗

Manipulating single excess electrons in monolayer transition metal dihalide

Polarons are entities of excess electrons dressed with local response of lattices, whose atomic-scale characterization is essential for understanding the many body physics arising from the electron-lattice entanglement, yet difficult to achieve. Here, using scanning tunneling microscopy and spectroscopy (STM/STS), we show the visualization and manipulation of single polarons in monolayer CoCl 2 , that are grown on HOPG substrate via molecular beam epitaxy. Two types of polarons are identified, both inducing upward local band bending, but exhibiting distinct appearances, lattice occupations and polaronic states. First principles calculations unveil origin of polarons that are stabilized by cooperative electron-electron and electron-phonon interactions. Both types of polarons can be created, moved, erased, and moreover interconverted individually by the STM tip, as driven by tip electric field and inelastic electron tunneling effect. This finding identifies the rich category of polarons in CoCl 2 and their feasibility of precise control unprecedently, which can be generalized to other transition metal halides.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Holographic measurement and bulk teleportation

Holography has taught us that spacetime is emergent and its properties depend on the entanglement structure of the dual theory. In this paper, we describe how changes in the entanglement due to a local projective measurement (LPM) on a subregion A of the boundary theory modify the bulk dual spacetime. We find that LPMs destroy portions of the bulk geometry, yielding post-measurement bulk spacetimes dual to the complementary unmeasured region A c that are cut off by end-of-the-world branes. Using a bulk calculation in AdS 3 and tensor network models of holography (in particular, the HaPPY code and random tensor networks), we show that the portions of the bulk geometry that are preserved after the measurement depend on the size of A and the state we project onto. The post-measurement bulk dual to A c includes regions that were originally part of the entanglement wedge of A prior to measurement. This suggests that LPMs performed on a boundary subregion A teleport part of the bulk information originally encoded in A into the complementary region A c . In semiclassical holography an arbitrary amount of bulk information can be teleported in this way, while in tensor network models the teleported information is upper-bounded by the amount of entanglement shared between A and A c due to finite-N effects. When A is the union of two disjoint subregions, the measurement triggers an entangled/disentangled phase transition between the remaining two unmeasured subregions, corresponding to a connected/disconnected phase transition in the bulk description. Our results shed new light on the effects of measurement on the entanglement structure of holographic theories and give insight on how bulk information can be manipulated from the boundary theory. They could also represent a first step towards a holographic description of measurement-induced phase transitions.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Measuring and Simulating T1 and T2 for Qubits

Quantum computers perform computations exploiting quantum mechanics to a possible advantage, allowing us to prepare and manipulate states that do not have a classical equivalent. In particular, phenomena like superposition and entanglement may enable quantum computers to outperform their classical counterparts in certain applications. Implementing these useful quantum algorithms is contingent upon building accurate quantum hardware that is not affected by noise. Environmental noise decreases coherence time of qubits, meaning that qubits do not stay in a desired state long enough to carry out a complex computation. To that end, harnessing the full power of quantum computers necessitate characterization of noise sources and how they impact a given quantum system. Often times, T1and T2 are used to quantify noise. In this project, we provide an approach as to how T1 and T2 values are calculated and simulated for quantum systems. In addition, we compare simulated values of T1 and T2 with those of real quantum computer’s measurements. IBMQ Experience, an open source software allowing users to simulate and use real quantum hardware, is used. QuTip, a Python-based toolbox offering quantum simulation tools for open quantum systems, is also used.

Youssef, Rahaf↗

Photon-recoil and laser-focusing limits to Rydberg gate fidelity

Limits to Rydberg gate fidelity that arise from the entanglement of internal states of neutral atoms with the motional degrees of freedom due to the momentum kick from photon absorption and re-emission is quantified. This occurs when the atom is in a superposition of internal states but only one of these states is manipulated by visible or UV photons. The Schrödinger equation that describes this situation is presented and two cases are explored. In the first case, the entanglement arises because the spatial wave function shifts due to the separation in time between excitation and stimulated emission. For neutral atoms in a harmonic trap, the decoherence can be expressed within a sudden approximation when the duration of the laser pulses are shorter than the harmonic oscillator period. In this limit, the decoherence is given by simple analytic formulas that account for the momentum of the photon, the temperature of the atoms, the harmonic oscillator frequency, and atomic mass. In the second case, there is a reduction in gate fidelity because the photons causing absorption and stimulated emission are in focused beam modes. This leads to a dependence of the optically induced changes in the internal states on the center of mass atomic position. In the limit where the time between pulses is short, the decoherence can be expressed as a simple analytic formula involving the laser waist, temperature of the atoms, the trap frequency, and the atomic mass. These limits on gate fidelity are studied for the standard π-2π-π Rydberg gate and a protocol based on a single adiabatic pulse with a Gaussian envelope.

74 ATOMIC AND MOLECULAR PHYSICS↗

Fast generation of spin squeezing via resonant spin-boson coupling

Abstract We propose protocols for the creation of useful entangled states in a system of spins collectively coupled to a bosonic mode, directly applicable to trapped-ion and cavity QED setups. The protocols use coherent manipulations of the resonant spin-boson interactions naturally arising in these systems to prepare spin squeezed states exponentially fast in time. The resonance condition harnesses the full spin-boson coupling and thus avoids the slower timescales when operating in the off-resonance regime. We demonstrate the robustness of the protocols by analyzing the effects of natural sources of decoherence in these systems and show their advantage compared to more standard slower approaches where entanglement is generated with off-resonant spin-boson interactions.

Physics↗

Unraveling spin entanglement using quantum gates with scanning tunneling microscopy-driven electron spin resonance

Quantum entanglement is a fundamental resource for quantum information processing, and its controlled generation and detection remain key challenges in scalable quantum architectures. Here, we numerically demonstrate the deterministic generation of entangled spin states in a solid-state platform by implementing quantum gates via electron spin resonance combined with scanning tunneling microscopy (ESR-STM). Using two titanium atoms on a MgO/Ag(100) substrate as a model, we construct a two-qubit system whose dynamics are coherently manipulated through tailored microwave pulse sequences. We generate Bell states by implementing a Hadamard gate followed by a controlled-NOT gate, and evaluate its fidelity and concurrence using the quantum-master equation-based code TimeESR. Our results demonstrate that ESR-STM can create entangled states with significant fidelity. This study paves the way for the realization of atom-based quantum circuits and highlights ESR-STM as a powerful tool for probing and engineering entangled states on surfaces.

Switzer, Eric D. [Donostia International Physics C↗

Rapid Generation of a Macroscopic Schrödinger Cat State of Atoms with Parity-Independent Orientation

We show that using the process of one-axis-twist squeezing in an echo configuration, it is possible to control the orientation of the macroscopic magnetic moment of a large number of atoms by manipulating the quantum state of a single atom that is physically isolated from the ensemble. With this control technique, it is also possible to entangle an ensemble with a single atom deterministically, which mimics the thought experiment known as the Schrödinger cat. In addition, this technique would make it possible to generate a mesoscopic Schrödinger cat state for a large number of atoms far more rapidly that the conventional process for generating such a state, with an orientation that is independent of the parity of the number of atoms. Apart from the echo configuration, we have also investigated the behavior of one-axis-twist squeezing for some special values of the squeezing parameter. We find that the squeezing propagator can be expressed as the sum of n rotation operators if the product of n and the squeezing parameter equals pi, where n is a non-zero integer. A direct consequence of this property of one-axis-twist squeezing is that there is a hidden order in a squeezed state generated under this condition even if its Husimi quasi-probability distribution looks irregular.

Li, Jinyang↗

Characterization and Engineering of Entangled Spatial modes in Four-wave Mixing

We show the presence of a large number of pairwise-entangled spatial modes generated in four-wave mixing by calculating the spatial Schmidt spectrum from the experimentally reconstructed two-photon amplitude. By manipulating the input pump momentum, we demonstrate a modification of the spatial Schmidt modes.

Marino Valle, Alberto↗

A perspective on the pathway to a scalable quantum internet using rare-earth ions

The ultimate realization of a global quantum internet will require advances in scalable technologies capable of generating, storing, and manipulating quantum information. The essential devices that will perform these tasks in a quantum network are quantum repeaters, which will enable the long-range distribution of entanglement between distant network nodes. Here, in this review, we provide an overview of the primary functions of a quantum repeater and discuss progress that has been made toward the development of repeaters with rare-earth ion doped materials while noting challenges that are being faced as the technologies mature. We give particular attention to erbium, which is well suited for networking applications. Finally, we provide a discussion of near-term benchmarks that can further guide rare-earth ion platforms for impact in near-term quantum networks.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Evidence for the utility of quantum computing before fault tolerance

Quantum computing promises to offer substantial speed-ups over its classical counterpart for certain problems. However, the greatest impediment to realizing its full potential is noise that is inherent to these systems. The widely accepted solution to this challenge is the implementation of fault-tolerant quantum circuits, which is out of reach for current processors. Here we report experiments on a noisy 127-qubit processor and demonstrate the measurement of accurate expectation values for circuit volumes at a scale beyond brute-force classical computation. We argue that this represents evidence for the utility of quantum computing in a pre-fault-tolerant era. These experimental results are enabled by advances in the coherence and calibration of a superconducting processor at this scale and the ability to characterize and controllably manipulate noise across such a large device. We establish the accuracy of the measured expectation values by comparing them with the output of exactly verifiable circuits. In the regime of strong entanglement, the quantum computer provides correct results for which leading classical approximations such as pure-state-based 1D (matrix product states, MPS) and 2D (isometric tensor network states, isoTNS) tensor network methods break down. These experiments demonstrate a foundational tool for the realization of near-term quantum applications.

97 MATHEMATICS AND COMPUTING↗

Quantum optical memory for entanglement distribution

Optical photons are powerful carriers of quantum information, which can be delivered in free space by satellites or in fibers on the ground over long distances. Entanglement of quantum states over long distances can empower quantum computing, quantum communications, and quantum sensing. Quantum optical memories are devices designed to store quantum information in the form of stationary excitations, such as atomic coherence, and are capable of coherently mapping these excitations to flying qubits. Quantum memories can effectively store and manipulate quantum states, making them indispensable elements in future long-distance quantum networks. Over the past two decades, quantum optical memories with high fidelities, high efficiencies, long storage times, and promising multiplexing capabilities have been developed, especially at the single-photon level. In this review, we introduce the working principles of commonly used quantum memory protocols and summarize the recent advances in quantum memory demonstrations. We also offer a vision for future quantum optical memory devices that may enable entanglement distribution over long distances.

Lei, Yisheng↗

Integrated photonic structures for photon-mediated entanglement of trapped ions

Trapped atomic ions are natural candidates for quantum information processing and have the potential to realize or improve quantum computing, sensing, and networking. These applications often require the collection of individual photons emitted from ions into guided optical modes, in some cases for the production of entanglement between separated ions. Proof-of-principle demonstrations of such photon collection from trapped ions have been performed using high-numerical-aperture lenses or cavities and single-mode fibers, but integrated photonic elements in ion-trap structures offer advantages in scalability and manufacturability over traditional optics. In this paper we analyze structures monolithically fabricated with an ion trap for collecting ion-emitted photons, coupling them into waveguides, and manipulating them via interference. We calculate geometric limitations on collection efficiency for this scheme, simulate a single-layer grating that shows performance comparable to demonstrated free-space optics, and discuss practical fabrication and fidelity considerations. Based on this analysis, we conclude that integrated photonics can support scalable systems of trapped ions that can distribute quantum information via photon-mediated entanglement.

Knollmann, Felix W.↗

Quantum Computing with Exciton Qubits in Colloidal Semiconductor Nanocrystals

The present work evaluates the feasibility of quantum computing with exciton qubits in coupled colloidal semiconductor nanocrystals (NCs). A strategy for manipulating two-qubit states of colloidal NC hetero-dimers is described. We show that a sequence of laser pulses with the same photon energy can bring excitonic states of a nanocrystal hetero-dimer into entanglement and perform arbitrary qubit rotations (quantum gates). Our simulations of a realistic two-particle assembly of CdSe/CdS core/shell NCs demonstrate that such two-qubit gate operations can be driven by optical parametric oscillators with a theoretical error of 0.1%. Furthermore, a strategy for upscaling two-qubit hetero-dimers to N-qubit exciton gates in semiconductor NC assemblies is discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗