The interaction between super-intense coherent x-ray light and nuclei is studied theoretically. One of the main difficulties with driving nuclear transitions arises from the very narrow nuclear excited state widths which limit the coupling between laser and nuclei. In the context of direct laser-nucleus interaction, we consider the nuclear width broadening that occurs when in solid targets, the excitation caused by a single photon is shared by a large number of nuclei, forming a collective excited state. Our results show that for certain isotopes, cooperative effects may lead to an enhancement of the nuclear excited state population by almost two orders of magnitude. Additionally, an update of previous estimates for nuclear excited state population and signal photons taking into account the experimental advances of the x-ray coherent light sources is given. The presented values are an improvement by orders of magnitude and are encouraging for the future prospects of nuclear quantum optics.
Coherent control of nuclear pumping in a three level system driven by x-ray light is investigated. In single nuclei, the pumping performance is determined by the branching ratio of the excited state populated by the x-ray pulse. Our results are based on the observation that in ensembles of nuclei, cooperative excitation and decay leads to a greatly modified nuclear dynamics, which we characterize by a time-dependent cooperative branching ratio. We discuss prospects of steering the x-ray pumping by coherently controlling the cooperative decay. First, we study an ideal case with purely superradi…
Parity-Time ($\mathcal{PT}$) symmetry has become an important concept in the design of synthetic optical materials, with exotic functionalities such as unidirectional transport and non-reciprocal reflection. At exceptional points, this symmetry is spontaneously broken, and solutions transition from those with conserved intensity to exponential growth or decay. Here we analyze a quantum-photonic surface formed by a single layer of atoms in an array with light mediating strong cooperative many-body interactions. We show how delocalized collective excitation eigenmodes can exhibit an effective $\…
For donor nuclear spins in silicon, we show how to deterministically prepare various symmetric and asymmetric Dicke states which span a complete basis of the many-body Hilbert space. The state preparation is realized by cooperative pumping of nuclear spins by coupled donor electrons, and the required controls are in situ to the prototype Kane proposal for quantum computation. This scheme only requires a sub-gigahertz donor exchange coupling which can be readily achieved without atomically precise donor placement, hence it offers a practical way to prepare multipartite entanglement of spins in …
As an extension of two-level quantum bits (qubits), multilevel systems, so-called qudits, where d represents the Hilbert space dimension, have been predicted to reduce the number of iterations in quantum computation algorithms. This has been tested in the well-known [TbPc2]0 SMM, which allowed the implementation of the Grover algorithm in a single molecular unit. In the quest for molecular systems possessing an increased number of accessible nuclear spin states, we explore herein a dimeric Tb2-SMM via single crystal μ-SQUID measurements at sub-Kelvin temperatures. We observe ferromagnetic inte…
The possibility to control the coherent decay of resonant excitations in nuclear forward scattering is investigated. By changing abruptly the direction of the nuclear hyperfine magnetic field, the coherent scattering of photons can be manipulated and even completely suppressed via quantum interference effects between the nuclear transition currents. The efficiency of the coherent decay suppression and the dependence of the scattered light polarization on the specific switching parameters is analyzed in detail. Using a sophisticated magnetic switching sequence involving four rotations of the hy…
Nuclear spins of noble-gas atoms are exceptionally isolated from the environment and can maintain their quantum properties for hours at room temperature. Here we develop a mechanism for entangling two such distant macroscopic ensembles by using coherent light input. The interaction between the light and the noble-gas spins in each ensemble is mediated by spin-exchange collisions with alkali-metal spins, which are only virtually excited. The relevant conditions for experimental realizations with ^{3}\text{He} or ^{129}\text{Xe} are outlined.
Generation of single-photon entanglement is discussed in nuclear forward scattering. Using successive switchings of the direction of the nuclear hyperfine magnetic field, the coherent scattering of photons on nuclei is controlled such that two signal pulses are generated out of one initial pump pulse. The two time-resolved correlated signal pulses have different polarizations and energy in the keV regime. Spatial separation of the entangled field modes and extraction of the signal from the background can be achieved with the help of state-of-the-art x-ray polarizers and piezoelectric fast stee…
Coherent population trapping (CPT) provides a highly sensitive means for probing the energy level structure of an atomic system. For a nitrogen vacancy center in diamond, the CPT offers an alternative to the standard optically-detected magnetic resonance method for measuring the hyperfine structure of the electronic ground states. We show that the nuclear spin dependent CPT measures directly the hyperfine splitting of these states due to the 14N nuclear spin. The CPT spectral response obtained in the presence of a strong microwave field, resonant or nearly resonant with a ground state spin tra…
Coherent storage and phase modulation of x-ray single-photon wave packets in resonant scattering of light off nuclei is investigated theoretically. We show that by switching off and on again the magnetic field in the nuclear sample, phase-sensitive storage of photons in the keV regime can be achieved. Corresponding $π$ phase modulation of the stored photon can be accomplished if the retrieving magnetic field is rotated by $180^{\circ}$. The development of such x-ray single-photon control techniques is a first step towards forwarding quantum optics and quantum information to shorter wavelengths…
Nuclear spins interact weakly with their environment. In particular, they are generally insensitive to mechanical vibrations. Here, we successfully demonstrate the coherent coupling of mechanics to a single nuclear spin. This coupling is mediated by a silicon vacancy (SiV) centre in diamond, taking advantage of its large strain susceptibility and hyperfine interaction with nuclear spins. Importantly, we demonstrate that the nuclear spin retains its excellent coherence properties even in the presence of this coupling. This provides a way to leverage nuclear spins as quantum memories for mechani…
Coherent population transfer between nuclear states using x-ray laser pulses is studied. The laser pulses drive two nuclear transitions between three nuclear states in a setup reminding of stimulated Raman adiabatic passage used for atomic coherent population transfer. To compensate for the lack of $γ$-ray laser sources, we envisage accelerated nuclei interacting with two copropagating or crossed x-ray laser pulses. The parameter regime for nuclear coherent population transfer using fully coherent light generated by future X-Ray Free-Electron Laser facilities and moderate or strong acceleratio…
Photon-mediated interactions between atomic systems can arise via coupling to a common electromagnetic mode or by quantum interference. Here, we probe the role of coherence in cooperative emission arising from two distant but indistinguishable solid-state emitters because of path erasure. The primary signature of cooperative emission, the emergence of "bunching" at zero delay in an intensity correlation experiment, is used to characterise the indistinguishability of the emitters, their dephasing, and the degree of correlation in the joint system that can be coherently controlled. In a stark de…
We introduce an optical tweezer platform for assembling and individually manipulating a two-dimensional register of nuclear spin qubits. Each nuclear spin qubit is encoded in the ground $^{1}S_{0}$ manifold of $^{87}$Sr and is individually manipulated by site-selective addressing beams. We observe that spin relaxation is negligible after 5 seconds, indicating that $T_1\gg5$ s. Furthermore, utilizing simultaneous manipulation of subsets of qubits, we demonstrate significant phase coherence over the entire register, estimating $T_2^\star = \left(21\pm7\right)$ s and measuring $T_2^\text{echo}=\l…
We demonstrate coherent control of two nuclear spins mediated by the magnetic resonance of a hyperfine-coupled electron spin. This control is used to create a double nuclear coherence in one of the two electron spin manifolds, starting from an initial thermal state, in direct analogy to the creation of an entangled (Bell) state from an initially pure unentangled state. We identify challenges and potential solutions to obtaining experimental gate fidelities useful for quantum information processing in this type of system.
We demonstrate that the [Yb(trensal)] molecule is a prototypical coupled electronic qubit-nuclear qudit system. The combination of noise-resilient nuclear degrees of freedom and large reduction of nutation time induced by electron-nuclear mixing enables coherent manipulation of this qudit by radio-frequency pulses. Moreover, the multi-level structure of the qudit is exploited to encode and operate a qubit with embedded basic quantum error correction.
Dipole-coupled subwavelength quantum emitter arrays respond cooperatively to external light fields as they may host collective delocalized excitations (a form of excitons) with super- or subradiant character. Deeply subwavelength separations typically occur in molecular ensembles, where in addition to photon-electron interactions, electron-vibron couplings and vibrational relaxation processes play an important role. We provide analytical and numerical results on the modification of super- and subradiance in molecular rings of dipoles including excitations of the vibrational degrees of freedom.…
Collective Nuclear Polaritons with Coherent and Tunable Excitation Dynamics
Zhejiang Normal University（浙江师范大学）；Zhejiang Institute of Photoelectronics（浙江省光电子研究所）；Abrikosov Center for Theoretical Physics, Moscow Center for Advanced Studies（莫斯科高级研究中心阿布里科索夫理论物理中心）；School of Science, Westlake University（西湖大学理学院）
The measurement of single quanta in a collection of coherently interacting objects is transformative in the investigations of emergent quantum phenomena. An isolated nuclear-spin ensemble is a remarkable platform owing to its coherence, but detecting its single spin excitations has remained elusive. Here, we use an electron spin qubit in a semiconductor quantum dot to sense a single nuclear-spin excitation (a nuclear magnon) with 1.9-ppm precision via the 200-kHz hyperfine shift on the 28-GHz qubit frequency. We demonstrate this single-magnon precision across multiple modes identified by nucle…
We use nominally forbidden electron-nuclear spin transitions in nitrogen-vacancy (NV) centers in diamond to demonstrate coherent manipulation of a nuclear spin ensemble using microwave fields at room temperature. We show that employing an off-axis magnetic field with a modest amplitude($\approx$ 0.01 T) at an angle with respect to the NV natural quantization axes is enough to tilt the direction of the electronic spins, and enable efficient spin exchange with the nitrogen nuclei of the NV center. We could then demonstrate fast Rabi oscillations on electron-nuclear spin exchanging transitions, c…
Detecting and controlling nuclear spin nano-ensembles is crucial for the further development of nuclear magnetic resonance (NMR) spectroscopy and for the emerging solid state quantum technology. Here we present the fabrication of a $\approx$ 1 nanometre thick diamond layer consisting of $^{13}$C nuclear spins doped with Nitrogen-Vacancy centres (NV) embedded in a spin-free $^{12}$C crystal matrix. A single NV in the vicinity of the layer is used for polarization of the $^{13}$C spins and the readout of their magnetization. We demonstrate a method for coherent control of few tens of nuclear spi…
Nuclear spins of noble gases feature extremely long coherence times but are inaccessible to optical photons. Here we realize a coherent interface between light and noble-gas spins that is mediated by alkali atoms. We demonstrate the optical excitation of the noble-gas spins and observe the coherent back-action on the light in the form of high-contrast two-photon spectra. We report on a record two-photon linewidth of 5$\pm$0.7 mHz (millihertz) above room-temperature, corresponding to a one-minute coherence time. This experiment provides a demonstration of coherent bi-directional coupling betwee…
As a unique feature, the $^{229}$Th nucleus has an isomeric transition in the vacuum ultraviolet that can be accessed by optical lasers. The interference effects occurring in the interaction between coherent optical light and an ensemble of $^{229}$Th nuclei are investigated theoretically. We consider the scenario of nuclei doped in vacuum ultraviolet-vacuum ultraviolet transparent crystals and take into account the effect of different doping sites and therefore different lattice fields that broaden the nuclear transition width. This effect is shown to come in interplay with interference effec…
Electron spin qubits in molecular systems offer high reproducibility and the ability to self assemble into larger architectures. However, interactions between neighbouring qubits are 'always-on' and although the electron spin coherence times can be several hundred microseconds, these are still much shorter than typical times for nuclear spins. Here we implement an electron-nuclear hybrid scheme which uses coherent transfer between electron and nuclear spin degrees of freedom in order to both controllably turn on/off dipolar interactions between neighbouring spins and benefit from the long nucl…
We have demonstrated electron-electron and electron-nuclear spin manipulations of Gd3+ ion in CaWO4 crystal. The results suggest that the studied system is perspective for multiqubit implementation in quantum computing.
Individually addressed Er$^{3+}$ ions in solid-state hosts are promising resources for quantum repeaters, because of their direct emission in the telecom band and compatibility with silicon photonic devices. While the Er$^{3+}$ electron spin provides a spin-photon interface, ancilla nuclear spins could enable multi-qubit registers with longer storage times. In this work, we demonstrate coherent coupling between the electron spin of a single Er$^{3+}$ ion and a single $I=1/2$ nuclear spin in the solid-state host crystal, which is a fortuitously located proton ($^1$H). We control the nuclear spi…
Hyperfine interactions with a nuclear spin environment fundamentally limit the coherence properties of confined electron spins in the solid-state. Here, we show that a quantum interference effect in optical absorption from two electronic spin states of a solid-state emitter can be used to prepare the surrounding environment of nuclear spins in well-defined states, thereby suppressing electronic spin dephasing. The evolution of the coupled electron-nuclei system into a coherent population trapping state by optical excitation induced nuclear spin diffusion can be described in terms of Levy fligh…
Coherent control of quantum dynamics is key to a multitude of fundamental studies and applications alike. In the visible or longer-wavelength domains, near-resonant light fields have become the primary tool to control electron dynamics. Recently, coherent control in the extreme-ultraviolet range was demonstrated, with timing stability of the applied light fields in the few-attosecond range. At hard x-ray energies, Mössbauer nuclei feature narrow nuclear resonances, and spectroscopy of these resonances is a widespread tool to study magnetic, structural and dynamical properties of matter. It has…
A practical source of high fidelity entangled photons is desirable for quantum information applications and exploring quantum physics. Semiconductor quantum dots have recently been shown to conveniently emit entangled light when driven electrically, however the fidelity was not optimal. Here we show that the fidelity is not limited by decoherence, but by coherent interaction with nuclei. Furthermore we predict that on 100μs timescales, strongly enhanced fidelities could be achieved. This insight could allow tailoring of quantum logic to operate using quantum dots in the fault tolerant regime.
Means to coherently control single x-ray photons in resonant scattering of light off nuclei by electric or magnetic fields are investigated theoretically. In order to derive the time response in nuclear forward scattering, we adapt the Maxwell-Bloch equations known from quantum optics to describe the resonant light pulse propagation through a nuclear medium. Two types of time-dependent perturbations of nuclear forward scattering are considered for coherent control of the resonantly scattered x-ray quanta. First, the simultaneous coherent propagation of two pulses through the nuclear sample is …
We show that [VO(TPP)] (vanadyl tetraphenylporphyrinate) is a promising system suitable to implement quantum computation algorithms based on encoding information in multi-level (qudit) units. Indeed, it embeds an electronic spin 1/2 coupled through hyperfine interaction to a nuclear spin 7/2, both characterized by remarkable coherence. We demonstrate this by an extensive broadband nuclear magnetic resonance study, which allow us to characterize the nuclear spin-Hamiltonian and to measure the spin dephasing time as a function of the magnetic field. In addition, we combine targeted measurements …
Quantum effects, prevalent in the microscopic scale, generally elusive in macroscopic systems due to dissipation and decoherence. Quantum phenomena in large systems emerge only when particles are strongly correlated as in superconductors and superfluids. Cooperative interaction of correlated atoms with electromagnetic fields leads to superradiance, the enhanced quantum radiation phenomenon, exhibiting novel physics such as quantum Dicke phase and ultranarrow linewidth for optical clocks. Recent researches to imprint atomic correlation directly demonstrated controllable collective atom-field in…
Distance measurements via the dipolar interaction are fundamental to the application of nuclear magnetic resonance (NMR) to molecular structure determination, but they only provide information on the absolute distance $r$ and polar angle $θ$ between spins. In this Letter, we present a protocol to also retrieve the azimuth angle $ϕ$. Our method relies on measuring the nuclear precession phase after application of a control pulse with a calibrated external radio-frequency coil. We experimentally demonstrate three-dimensional positioning of individual carbon-13 nuclear spins in a diamond host cry…
Interfacing between various elements of a computer - from memory to processors to long range communication - will be as critical for quantum computers as it is for classical computers today. Paramagnetic rare earth doped crystals, such as Nd$^{3+}$:Y$_2$SiO$_5$ (YSO), are excellent candidates for such a quantum interface: they are known to exhibit long optical coherence lifetimes (for communication via optical photons), possess a nuclear spin (memory) and have in addition an electron spin that can offer hybrid coupling with superconducting qubits (processing). Here we study two of these three …
We theoretically demonstrate that nuclear spins can be harnessed to coherently control two-electron spin states in a double quantum dot. Hyperfine interactions lead to an avoided crossing between the spin singlet state and the ms = +1 triplet state, T_+ . We show that a coherent superposition of singlet and triplet states can be achieved using finite-time Landau-Zener-Stückelberg interferometry. In this system the coherent rotation rate is set by the Zeeman energy, resulting in ~1 nanosecond single spin rotations. We analyze the coherence of this spin qubit by considering the coupling to the n…
Future communication and computation technologies that exploit quantum information require robust and well-isolated qubits. Electron spins in III-V semiconductor quantum dots, while promising candidates, see their dynamics limited by undesirable hysteresis and decohering effects of the nuclear spin bath. Replacing electrons with holes should suppress the hyperfine interaction and consequently eliminate strong nuclear effects. Using picosecond optical pulses, we demonstrate coherent control of a single hole qubit and examine both free-induction and spin-echo decay. In moving from electrons to h…
Coherent control of quantum systems has far-reaching implications in quantum engineering. In this context, coherent population trapping (CPT) involving dark resonances has played a prominent role, leading to a wealth of major applications including laser cooling of atoms and molecules, optical magnetometry, light storage and highly precise atomic clocks. Extending CPT methods to individual solid-state quantum systems has been only achieved in cryogenic environments for electron spin impurities and superconducting circuits. Here, we demonstrate efficient CPT of a single nuclear spin in a room t…
Localization and coherent control of 25 nuclear spins in Silicon Carbide
University of Stuttgart（斯图加特大学）；Eötvös Loránd University（罗兰大学）；MTA–ELTE Lendület “Momentum” NewQubit Research Group（匈牙利科学院-罗兰大学Lendulet“动量”NewQubit研究组）；Leibniz-Institute of Surface Engineering (IOM)（莱布尼兹表面工程研究所）；Linköping University（林雪平大学）；Max Planck Institute for solid state physics（马克斯·普朗克固体物理研究所）
Magnetic fluctuations caused by the nuclear spins of a host crystal are often the leading source of decoherence for many types of solid-state spin qubit. In group-IV materials, the spin-bearing nuclei are sufficiently rare that it is possible to identify and control individual host nuclear spins. This work presents the first experimental detection and manipulation of a single $^{29}$Si nuclear spin. The quantum non-demolition (QND) single-shot readout of the spin is demonstrated, and a Hahn echo measurement reveals a coherence time of $T_2 = 6.3(7)$ ms - in excellent agreement with bulk experi…
An experimental platform of ultralow-temperature pulsed ENDOR (electron-nuclear double resonance) spectroscopy is constructed for the bulk materials. Coherent property of the coupled electron and nuclear spins of the rare-earth (RE) dopants in a crystal (143Nd3+:Y2SiO5) is investigated from 100 mK to 6 K. At the lowest working temperatures, two-pulse-echo coherence time exceeding 2 ms and 40 ms are achieved for the electron and nuclear spins, while the electronic Zeeman and hyperfine population lifetimes are more than 15 s and 10 min. With the aid of the near-unity electron spin polarization a…
Direct dynamics methods using Gaussian wavepackets have to rely only on local properties, such as gradients and hessians at the center of the wavepacket, so as to be compatible with the usual quantum chemistry methods. Matrix elements of the potential energy surfaces between wavepackets therefore usually have to be approximated. It is shown, that if a modified form of valence bond theory is used instead of the usual MO-based theories, the matrix elements can be obtained exactly. This is so because the molecular Hamiltonian only contains the Coulomb potential, for which matrix elements between …
Working with nuclear magnetic resonance (NMR) in quadrupolar spin systems, in this paper we transfer the concept of atomic coherent state to the nuclear spin context, where it is referred to as pseudo-nuclear spin coherent state (pseudo-NSCS). Experimentally, we discuss the initialization of the pseudo-NSCSs and also their quantum control, implemented by polar and azimuthal rotations. Theoretically, we compute the geometric phases acquired by an initial pseudo-NSCS on undergoing three distinct cyclic evolutions: $ i) $ the free evolution of the NMR quadrupolar system and, by analogy with the e…
The understanding of weak measurements and interaction-free measurements has greatly expanded the conceptual and experimental toolbox to explore the quantum world. Here we demonstrate single-shot variable-strength weak measurements of the electron and the nuclear spin states of a single $^{31}$P donor in silicon. We first show how the partial collapse of the nuclear spin due to measurement can be used to coherently rotate the spin to a desired pure state. We explicitly demonstrate that phase coherence is preserved throughout multiple sequential single-shot weak measurements, and that the parti…
Coherent excitation of an ensemble of quantum objects underpins quantum many-body phenomena, and offers the opportunity to realize a quantum memory to store information from a qubit. Thus far, a deterministic and coherent interface between a single quantum system, e.g. a qubit, and such an ensemble has remained elusive. We first use an electron to cool the mesoscopic nuclear-spin ensemble of a semiconductor quantum dot to the nuclear sideband-resolved regime. We then implement an all-optical approach to access these individual quantized electronic-nuclear spin transitions. Finally, we perform …
We investigate the electron and nuclear spin coherence properties of ytterbium ($\mathrm{Yb}^{3+}$) ions with non-zero nuclear spin, within an yttrium orthosilicate (Y$_2$SiO$_5$) crystal, with a view to their potential application in quantum memories or repeaters. We find electron spin-lattice relaxation times are maximised at low magnetic field ($<100$ mT) where $g~\sim6$, reaching 5 s at 2.5 K, while coherence times are maximised when addressing ESR transitions at higher fields where $g\sim0.7$ where a Hahn echo measurement yields $T_2$ up to 73 $μ$s. Dynamical decoupling (XY16) can be used…
