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arXiv:2301.11460

Evidencing the squeezed dark nuclear spin state in lead halide perovskites

Erik Kirstein, Dmitry S. Smirnov, Evgeny A. Zhukov, Dmitri R. Yakovlev, N. E. Kopteva, Dmitry N. Dirin, Oleh R. Hordiichuk, Maksym V. Kovalenko, M. Bayer

Published Jan 26, 2023• 0 citations
arXivHTMLPDF

Abstract

Coherent many-body states are highly promising for robust and scalable quantum information processing. While far-reaching theoretical predictions have been made for various implementations, direct experimental evidence of their appealing properties can be challenging. Here, we demonstrate coherent optical manipulation of the nuclear spin ensemble in the lead halide perovskite semiconductor FAPbBr$_3$ (FA=formamidinium), targeting a long-postulated collective dark state that is insensitive to optical pumping. Via optical orientation of localized hole spins we drive the nuclear many-body system into an entangled state, requiring a weak magnetic field of only a few Millitesla strength at cryogenic temperatures. During its fast build-up, the nuclear polarization along the optical axis remains small, while the transverse nuclear spin fluctuations are strongly reduced, corresponding to spin squeezing as evidenced by a strong violation of the generalized nuclear squeezing-inequality with $ξ_s < 0.3$. The dark state evidenced in this process corresponds to an approximately 750-body entanglement between the nuclei. Dark nuclear spin states can be exploited to store quantum information benefiting from their long-lived many-body coherence and to perform quantum measurements with a precision beyond the standard limit.

DOI
10.48550/arxiv.2301.11460

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Coherent many-body states are highly promising for robust and scalable quantum information processing. While far-reaching theoretical predictions have been made for various implementations, direct experimental evidence of their appealing properties can be challenging. Here, we demonstrate coherent optical manipulation of the nuclear spin ensemble in the lead halide perovskite semiconductor FAPbBr3_33​ (FA=formamidinium), targeting a long-postulated collective dark state that is insensitive to optical pumping. Via optical orientation of localized hole spins we drive the nuclear many-body system into an entangled state, requiring a weak magnetic field of only a few Millitesla strength at cryogenic temperatures. During its fast build-up, the nuclear polarization along the optical axis remains small, while the transverse nuclear spin fluctuations are strongly reduced, corresponding to spin squeezing as evidenced by a strong violation of the generalized nuclear squeezing-inequality with ξs<0.3ξ_s < 0.3ξs​<0.3. The dark state evidenced in this process corresponds to an approximately 750-body entanglement between the nuclei. Dark nuclear spin states can be exploited to store quantum information benefiting from their long-lived many-body coherence and to perform quantum measurements with a precision beyond the standard limit.
Abstract Coherent many-body states are highly promising for robust quantum information processing. While far-reaching theoretical predictions have been made for various implementations, direct experimental evidence of their appealing properties can be challenging. Here, we demonstrate optical manipulation of the nuclear spin ensemble in the lead halide perovskite semiconductor FAPbBr3 (FA = formamidinium), targeting a long-postulated collective dark state that is insensitive to optical pumping after its build-up. Via optical orientation of localized hole spins we drive the nuclear many-body system into this entangled state, requiring a weak magnetic field of only a few milli-Tesla strength at cryogenic temperatures. During its fast establishment, the nuclear polarization along the optical axis remains small, while the transverse nuclear spin fluctuations are strongly reduced, corresponding to spin squeezing as evidenced by a strong violation of the generalized nuclear squeezing-inequality with ξs < 0.5. The dark state corresponds to an ~35-body entanglement between the nuclei. Dark nuclear spin states can be exploited to store quantum information benefiting from their long-lived many-body coherence and to perform quantum measurements with a precision beyond the standard limit.
Spin degrees of freedom have been extensively explored in the context of quantum information processing. Many proposals of quantum computation architectures use spins as carriers of quantum of information. A central problem is to efficiently generate quantum entanglement between spin qubits which proves to be a crucial resource for quantum information tasks. On the other hand, uncontrollable spin degrees of freedom in the environment of spin qubits are the major causes of errors at low temperature, for example, the lattice nuclear spins hyperfine coupled to single electron spin qubit localized in semiconductor nano-structures. An outstanding problem for scalable quantum computation is to suppress the collective fluctuations from such spin baths so that the coherence time of the spin qubit can be improved. With these two motivations, the problems of suppressing collective spin fluctuations and generating entanglement in various spin ensembles are addressed in this thesis.\n\n\n\nIn the first half of the thesis, two approaches are introduced for suppressing the collective fluctuations in the nuclear spin bath so that the quantum coherence time of electron spin qubit in semiconductor quantum dots can be improved. The first approach works for a coupled double dot system. A theory for the interaction with the nuclear spins is developed when the two-electron singlet state is in resonance with one of the triplet state in moderate external magnetic field. At this resonance condition, the nuclear-electron flip-flop process caused by the hyperfine interaction can lead to a feedback mechanism, which can be used to suppress the nuclear hyperfine field. The second approach works for a single dot system. It is shown that strong pumping of the nuclear spins in dynamic nuclear polarization processes can saturate the nuclear spin bath towards the collective “dark states”. In such dark states, the transverse nuclear field fluctuation can be substantially suppressed compared to the value at thermal equilibrium. Two physical schemes are proposed to realize the nuclear dark states for suppression of the nuclear field fluctuations.\n\n\n\nIn the second half of the thesis, schemes are presented for generating large scale quantum entanglement in two types of spin qubit systems. For atomic spin qubits in optical lattices, schemes are proposed on how to prepare pure spin coherent state (SCS) with low collective spin by incoherent pumping with collective spin raising and lowering operations. Such SCS realize networks of mutually entangled spins which can be idea resources for the quantum telecloning algorithm. For donor nuclear spin qubits in silicon architecture, proposals are shown on how to deterministic prepare Dicke states which constitute an important class of multipartite entangled states. Our scheme is capable of preparing both symmetric and asymmetric Dicke states which form a complete basis set of the spin Hilbert space. The required controls are in situ to the prototype Kane’s quantum computer. The preparation is robust because each desired Dicke state is the steady state under designed pumping process. The schemes presented here also make possible the construction of decoherence free subspaces where quantum information is protected from collective noises.
Isolation from environment leads to the days-long lifetime of noble-gas nuclear spins, but also brings great challenges to the preparation, manipulation, and measurement of nuclear-spin quantum states. Here we find that nuclear spin squeezing, with ultra-long lifetime and huge atomic number, can be efficiently obtained and manipulated based on the coherent spin-exchange interaction between alkali-metal and noble-gas ensembles. Thanks to the considerable advantage of our proposal in preparing the spin squeezing of the macroscopic atomic ensemble with a huge atomic number, even the nuclear spin-squeezed state containing 10^20 atoms or more is obtainable with preexisting techniques. Further, the days-long storage and measurement of nuclear spin squeezing can be performed by the coherent manipulation of a magnetic field. This proposal can be implemented in hot atomic ensembles, whose ease of access and high adaptability to various environments will significantly facilitate the research and application of nuclear-spin nonclassical states in precision measurement, quantum information, and fundamental physics.
Long spin coherence times of carriers are essential for implementing quantum technologies using semiconductor devices for which, however, a possible obstacle is spin relaxation. For the spin dynamics, decisive features are the band structure, crystal symmetry, and quantum confinement. Perovskite semiconductors recently have come into focus of studies of their spin states, notivated by efficient optical access and potentially long-living coherence. Here, we report an electron spin coherence time T2T_2T2​ of the order of 1 ms, measured for a bulk FA0.95_{0.95}0.95​Cs0.05_{0.05}0.05​PbI3_33​ lead halide perovskite crystal. Using periodic laser pulses, we synchronize the electron spin Larmor precession about an external magnetic field in an inhomogeneous ensemble, the effect known as spin mode locking. It appears as a decay of the optically created ensemble spin polarization within the dephasing time T2∗T_2^*T2∗​ of up to 20 ns and its revival during the spin coherence time T2T_2T2​ reaching the millisecond range. This exceptionally long spin coherence time in a bulk crystal is complemented by millisecond-long longitudinal spin relaxation times T1T_1T1​ for electrons and holes, measured by optically-detected magnetic resonance. These long-lasting spin dynamics highlight perovskites as promising platform for the quantum devices with all-optical control.
Coherent excitation of an ensemble of quantum objects offers the opportunity to realise robust entanglement generation and information storage in a quantum memory [1]. Thus far, interfacing with such a collective excitation deterministically has remained elusive owing to the difficulty of controlling a probe spin in the midst of a complex many-body system. In the strained atomic lattice of a semiconductor quantum dot, nuclear quadrupole effects generate an electron-nuclear interaction that can be engineered by driving the electron spin (Fig. 1a). By implementing an all-optical approach to access the individual quantised electronic-nuclear spin transitions, we have experimentally demonstrated coherent optical rotations of a single collective nuclear spin excitation corresponding to a spin wave called a nuclear magnon [2] (Fig. 1b).
Helium-3 nuclear spins form an exceptionally stable quantum system with extremely long coherence time, offering exciting opportunities for quantum technologies. In particular, nuclear spin-squeezed states promise enhanced precision for sensing tasks and tests of new physics. A central challenge for all these applications is the realization of a controllable light-nuclear spin interface. Here we experimentally demonstrate such an interface by exploiting metastability-exchange collisions in a low-pressure helium-3 gas cell at room temperature. A radio-frequency discharge produces a small population of metastable atoms that both enables efficient optical pumping and mediates an effective Faraday interaction between the collective nuclear spin and an optical probe. We quantitatively characterize the strength of this interaction as a function of the nuclear polarization, applied magnetic field, and probe-beam parameters. Moreover, we show that using a multi-pass cell enhances this interaction by effectively increasing the optical depth. Extrapolating to a tenfold increase of the probe power used in the present experiment, we project a measurement-induced squeezing rate of 0.52 s−1^{-1}−1. Our results provide a practical pathway for optical access to helium-3 nuclear spins and open prospects for generating long-lived, macroscopic nuclear spin-squeezed states for quantum metrology.