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arXiv:2409.10816 · ACS Nano

Time Crystals from Single-Molecule Magnet Arrays

Subhajit Sarkar, Yonatan Dubi

Published Oct 3, 2024• 4 citations
arXivHTMLPDF

Abstract

Time crystals, a unique nonequilibrium quantum phenomenon with promising applications in current quantum technologies, mark a significant advance in quantum mechanics. Although traditionally studied in atom-cavity and optical lattice systems, pursuing alternative nanoscale platforms for time crystals is crucial. Here we theoretically predict discrete time crystals in a periodically driven molecular magnet array, modeled by a spin-S Heisenberg Hamiltonian with significant quadratic anisotropy, taken with realistic and experimentally relevant physical parameters. Surprisingly, we find that the time crystal response frequency correlates with the energy levels of the individual magnets and is essentially independent of the exchange coupling. The latter is unexpectedly manifested through a pulse-like oscillation in the magnetization envelope, signaling a many-body response. These results show that molecular magnets can be a rich platform for studying time-crystalline behavior and possibly other out-of-equilibrium quantum many-body dynamics.

DOI
10.1021/acsnano.4c05817

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Time crystals, a unique nonequilibrium quantum phenomenon with promising applications in current quantum technologies, mark a significant advance in quantum mechanics. Although traditionally studied in atom-cavity and optical lattice systems, pursuing alternative nanoscale platforms for time crystals is crucial. Here we theoretically predict discrete time crystals in a periodically driven molecular magnet array, modeled by a spin-S Heisenberg Hamiltonian with significant quadratic anisotropy, taken with realistic and experimentally relevant physical parameters. Surprisingly, we find that the time crystal response frequency correlates with the energy levels of the individual magnets and is essentially independent of the exchange coupling. The latter is unexpectedly manifested through a pulse-like oscillation in the magnetization envelope, signaling a many-body response. These results show that molecular magnets can be a rich platform for studying time-crystalline behavior and possibly other out-of-equilibrium quantum many-body dynamics.
Molecular magnets are ideal systems to probe the realm that borders quantum and classical physics, as well as to study decoherence phenomena in nanoscale systems. The control of the quantum behavior of these materials and their structural characteristics requires synthesis of new complexes with desirable properties which will allow probing of the fundamental aspects of nanoscale physics and quantum information processing. Of particular interest among the magnetic molecular materials are single-molecule magnets (SMMs) and antiferromagnetic (AFM) molecular wheels in which the spin state of the molecule is known to behave quantum mechanically at low temperatures. In previous experiments the dynamics of the magnetic moment of the molecules is governed by incoherent quantum tunneling. Short decoherence times are mainly due to interactions between molecular magnets within the crystal and interactions of the electronic spin with the nuclear spin of neighboring ions within the molecule. This decoherence problem has imposed a limit to the understanding of the molecular spin dynamics and the sources of decoherence in condensed matter systems. Particularly, intermolecular dipolar interactions within the crystal, which shorten the coherence times in concentrated samples, have stymied progress in this direction. Several recent works have reported a direct measurement of the decoherence time in molecular magnets. This has been done by eliminating the dephasing created by dipolar interactions between neighboring molecules. This has been achieved by a) a dilution of the molecules in a liquid solution to decrease the dipolar interaction by separating the molecules, and b) by polarizing the spin bath by applying a high magnetic field at low temperatures. Unfortunately, both approaches restrict the experimental studies of quantum dynamics. For example, the dilution of molecular magnets in liquid solution causes a dispersion of the molecular spin orientation and anisotropy axes, while the large fields required to polarize the spin bath overcome the anisotropy of the molecular spin. In this thesis I have explored two methods to overcome dipolar interactions in molecular magnets: a) studying the dynamics of molecular magnets in single crystals where the separation between magnetic molecules is obtained by chemical doping or where the high crystalline quality allows observations intrinsic to the quantum mechanical nature of the tunneling of the spin, and b) studying the electronic transport through an individual magnetic molecule which has been carefully placed in a single-electron transistor device. I have used EPR microstrip resonators to measure Fe17Ga molecular wheels within single crystals of Fe18 AFM wheels, as well as demonstrating, for the first time in a Single Molecule Magnet, the complete suppression of a Quantum Tunneling of the Magnetization transition forbidden by molecular symmetry.
A time crystal is a state of periodically driven matter that breaks discrete time-translation symmetry.Time crystals have been demonstrated experimentally in various programmable quantum simulators, and they exemplify how nonequilibrium, driven quantum systems can exhibit intriguing and robust properties absent in systems at equilibrium.These robust driven states need to be stabilized by some mechanism, with the preeminent candidates being many-body localization and prethermalization.This introduces additional constraints that make it challenging to experimentally observe time crystallinity in naturally occurring systems.Recent theoretical work has developed the notion of prethermalization without temperature, expanding the class of time-crystal systems to explain time-crystalline observations at (or near) infinite temperature.In this work, we conclusively observe the emergence of a prethermal Uð1Þ time-crystalline state at quasi-infinite temperature in a solid-state NMR quantum emulator by verifying the requisites of prethermalization without temperature.In addition to observing the signature period-doubling behavior, we show the existence of a long-lived prethermal regime whose lifetime is significantly enhanced by strengthening an emergent Uð1Þ conservation law.Not only do we measure this enhancement through the global magnetization, but we also exploit on-site disorder to measure local observables, ruling out the possibility of many-body localization and confirming the emergence of long-range correlations.
Time crystals in periodically driven systems have initially been studied assuming either the ability to quench the Hamiltonian between different many-body regimes, the presence of disorder or long-range interactions. Here we propose the simplest scheme to observe discrete time crystal dynamics in a one-dimensional driven quantum system of the Ising type with short-range interactions and no disorder. The system is subject only to a periodic kick by a global magnetic field, and no extra Hamiltonian quenching is performed. We analyze the emerging time crystal stabilizing mechanisms via extensive numerics as well as using an analytic approach based on an off-resonant transition model. Due to the simplicity of the driven Ising model, our proposal can be implemented with current experimental platforms including trapped ions, Rydberg atoms, and superconducting circuits.
Abstract Discrete time-crystals are periodically driven quantum many-body systems with broken discrete time translational symmetry, a non-equilibrium steady state representing self-organization of motion of quantum particles. Observations of discrete time-crystalline order are currently limited to magneto-optical experiments and it was never observed in a transport experiment performed on systems connected to external electrodes. Here we demonstrate that both discrete time-crystal and quasi-crystal survive a very general class of environments corresponding to single-particle gain and loss through system-electrode coupling over experimentally relevant timescales. Using dynamical symmetries, we analytically identify the conditions for observing time-crystalline behavior in a periodically driven open Fermi-Hubbard chain attached to electrodes. We show that the spin-polarized transport current directly manifests the existence of a time-crystalline behavior. Our findings are verifiable in present-day experiments with quantum-dot arrays and Fermionic ultra-cold atoms in optical lattices.
Floquet (periodically driven) systems can give rise to unique nonequilibrium phases of matter without equilibrium analogs. The most prominent example is the realization of discrete time crystals. An intriguing question emerges: What other novel phases can manifest when the constraint of time periodicity is relaxed? In this study, we explore quantum systems subjected to a quasiperiodic drive. Leveraging a strongly interacting spin ensemble in diamond, we identify the emergence of long-lived discrete time quasicrystals. Unlike conventional time crystals, time quasicrystals exhibit robust subharmonic responses at multiple incommensurate frequencies. Furthermore, we show that the multifrequency nature of the quasiperiodic drive allows for the formation of diverse patterns associated with different discrete time quasicrystalline phases. Our findings demonstrate the existence of nonequilibrium phases in quasi-Floquet settings, significantly broadening the catalog of novel phenomena in driven many-body quantum systems.
Discrete time crystals are related to nonequilibrium dynamics of periodically driven quantum many-body systems where the discrete time-translation symmetry of the Hamiltonian is spontaneously broken into another discrete symmetry. Recently, the concept of phase transitions has been extended to nonequilibrium dynamics of time-independent systems induced by a quantum quench, i.e., a sudden change of some parameter of the Hamiltonian. There, the return probability of a system to the ground state reveals singularities in time which are dubbed dynamical quantum phase transitions. We show that the quantum quench in a discrete time crystal leads to dynamical quantum phase transitions where the return probability of a periodically driven system to a Floquet eigenstate before the quench reveals singularities in time. It indicates that dynamical quantum phase transitions are not restricted to time-independent systems and can be also observed in systems that are periodically driven. We discuss how the phenomenon can be observed in ultracold atomic gases.