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Elucidating the role of specific vibrational modes in spin lattice relaxation is a key step to designing room temperature qubits. We executed an experimental and theoretical study on a series of Cu 2+ qubits to increase their operating temperature.
Phonon spin-lattice relaxation times for uranium and neodymium ions in calcium fluoride
Lanthanide-based single-molecule magnets (SMMs) are promising building blocks for quantum memory and spintronic devices. Designing lanthanide-based SMMs with long spin relaxation time requires a detailed understanding of their electronic structure, including the crucial role of the spin-orbit coupling (SOC). While traditional calculations of SOC using the perturbation theory applied to a solution of the non-relativistic Schrödinger equation are valid for light atoms, this approach is questionable for systems containing heavy elements such as lanthanides. We investigate the accuracy of the perturbation estimates of SOC by variationally solving the Dirac equation for the [DyO] + molecule, a prototype of a lanthanide-based SMM. We show that the energy splittings between the M J states involved in spin relaxation depend on the interplay between strong SOC and dynamic electron correlations. Here, we demonstrate that this interplay affects the resonances between the spin and vibrational transitions, and, therefore, the spin relaxation time.
Combining the synthetic tunability of molecular compounds with the optical selection rules of transition metal dichalcogenides (TMDCs) that derive from spin-valley coupling could provide interesting opportunities for the readout of quantum information. However, little is known about the electronic and spin interactions at such interfaces and the influence on spin-valley relaxation. Here, in this work, vanadyl phthalocyanine (VOPc) molecular layers are thermally evaporated on WSe 2 to explore the effect of molecular layer thickness on excited-state spin-valley polarization. The thinnest molecular layer supports an interfacial state which destroys the spin-valley polarization almost instantaneously, whereas a thicker molecular layer results in longer-lived spin-valley polarization than the WSe 2 monolayer alone. The mechanism appears to involve a tightly bound species at the molecule/TMDC interface that strengthens exchange interactions and is largely avoided in thicker VOPc layers that isolate electrons from WSe 2 holes.
Direct one phonon spin-lattice relaxation times for positive trivalent Nd and U ions in calcium difluoride at tetragonal symmetry sites
Paramagnetic molecules with a metal ion as an electron spin center are promising building blocks for molecular qubits and high-density memory arrays. However, fast spin relaxation and decoherence in these molecules lead to a rapid loss of magnetization and quantum information. Nonadiabatic coupling (NAC), closely related to spin-vibrational coupling, is the main source of spin relaxation and decoherence in paramagnetic molecules at higher temperatures. Predicting these couplings using numerical differentiation requires a large number of computationally intensive ab initio or crystal field electronic structure calculations. To reduce computational cost and improve accuracy, we derive and implement analytical NAC and state-specific energy gradient for the ab initio parametrized crystal field Hamiltonian describing single-ion molecular magnets. Our implementation requires only a single crystal field calculation. In addition, the accurate NACs and state-specific energy gradients can be used to model spin relaxation using sophisticated nonadiabatic molecular dynamics, which avoids the harmonic approximation for molecular vibrations. To test our implementation, we calculate the NAC values for three lanthanide complexes. Finally, the predicted values support the relaxation mechanisms reported in previous studies.
The fractionalization of magnetic dipoles into monopoles is revealed through a crossover in the relaxation dynamics of spin ice.
AbstractIn addition to its fundamental interest, the long-distance spin transport is essential for spintronic devices. However, the spin relaxation caused by scattering of the particles carrying the spin limits spin transport. We explored spatially indirect excitons (IXs) in van der Waals heterostructures composed of atomically thin layers of transition-metal dichalcogenides as spin carries. We observed the long-distance spin transport: the spin polarized excitons travel over the entire sample, ~10 micron away from the excitation spot, with no spin density decay. This transport is characterized by the 1/e decay distances reaching ~100 micron. The 1/e decay distances are extracted from fits over the ~10 micron sample size. The emergence of long-distance spin transport is observed at the densities and temperatures where the IX transport decay distances and, in turn, scattering times are strongly enhanced. The suppression of IX scattering suppresses the spin relaxation and enables the long-distance spin transport.
We revisit the sensitivity of Single Molecule Magnet (SMM) crystals as detectors for low-mass dark matter. In previous work, we established the concept of the ``magnetic bubble chamber'', where energy deposited by dark matter triggers a magnetic avalanche in a metastable crystal. The original sensitivity estimates relied on a conservative criterion requiring the spin relaxation time to be strictly shorter than the thermal diffusion time. Here, we demonstrate that this criterion effectively ignores the stochastic nature of spin relaxation. We derive a refined analytic estimate which accounts for the fraction of spins that relax even when diffusion is fast. We show that the Zeeman energy released by this fraction contributes to local heating, significantly lowering the energy threshold for avalanche formation. We present simulation results confirming this effect and report on experimental verification of the assumed low-temperature thermal properties of two representative SMM crystals, Mn$_{12}$-acetate and Mn$_{32}$. Together, these efforts extend this pathfinder program toward the realization of SMM-based detectors with controlled material properties and enhanced dark matter sensitivity.
Quantum sensing is broadly defined as the use of quantum materials, quantum coherence, and/or quantum entanglement to measure physical quantities and/or to enhance the sensitivity of classical analytical measurements. Certain materials exhibit interesting quantum properties that have the potential to be utilized in quantum sensing applications. One such quantum property is electronic spin, which is utilized in this work. Here, we built a custom apparatus capable of conducting both optically detected magnetic resonance (ODMR) and spin relaxometry. The quantum material investigated was an ensemble of nitrogen vacancies (NV) in nanodiamonds. We have characterized the system and measured ODMR spectra for different strengths of the applied DC magnetic field and clearly observed the expected splitting of the resonances due to Zeeman splitting. We also have measured the spin relaxation times for two different powers of the applied AC magnetic field. The lower power dataset exhibited expected exponential temporal dependence of the relaxation of a modified spin state, whereas the higher power dataset exhibited stretched exponential dependence of the evolution of the modified spin state, indicating the presence of high-power phenomena that emerge that retard the relaxation of the spin state.
Quantum sensing is broadly defined as the use of quantum materials, quantum coherence, and/or quantum entanglement to measure physical quantities and/or to enhance the sensitivity of classical analytical measurements. Certain materials exhibit interesting quantum properties that have the potential to be utilized in quantum sensing applications. One such quantum property is electronic spin, which is utilized in this work. Here, we built a custom apparatus capable of conducting both optically detected magnetic resonance (ODMR) and spin relaxometry. The quantum material investigated was an ensemble of nitrogen vacancies (NV) in nanodiamonds. We have characterized the system and measured ODMR spectra for different strengths of the applied DC magnetic field and clearly observed the expected splitting of the resonances due to Zeeman splitting. We also have measured the spin relaxation times for two different powers of the applied AC magnetic field. The lower power dataset exhibited expected exponential temporal dependence of the relaxation of a modified spin state, whereas the higher power dataset exhibited stretched exponential dependence of the modified spin state, indicating the presence of high-power phenomena that emerge that retard the relaxation of the spin state.
Iridates with the 5$d^4$ electronic configuration have attracted recent interest due to reports of magnetically ordered ground states despite longstanding expectations that their strong spin-orbit coupling would generate a $\textit{J}$ = 0 electronic ground state for each Ir 5+ ion. The major focus of prior research has been on the double perovskite iridates Ba 2 YIrO 6 and Sr 2 YIrO 6 , where the nature of the ground states (i.e., ordered vs nonmagnetic) is still controversial. Here, in this work, we present neutron powder diffraction, high-energy-resolution fluorescence-detected x-ray absorption spectroscopy (HERFD-XAS), resonant inelastic x-ray scattering (RIXS), magnetic susceptibility, and muon spin relaxation data on the related double perovskite iridates Ba 2 LuIrO 6 , Sr 2 LuIrO 6 , Ba 2 ScIrO 6 , and Sr 2 ScIrO 6 that enable us to gain a general understanding of the electronic and magnetic properties for this family of materials. Our HERFD-XAS and RIXS measurements establish $\textit{J}$ = 0 electronic ground states for the Ir 5+ ions in all cases, with similar values for Hund's coupling $J_H$ and the spin-orbit coupling constant $λ_{\text{SOC}}$. Our bulk susceptibility and muon spin relaxation data find no evidence for long-range magnetic order or spin freezing, but they do exhibit weak magnetic signals that are consistent with extrinsic local moments. Our results indicate that the large $λ_{\text{SOC}}$ is the key driving force behind the electronic and magnetic ground states realized in the $5d^4$ double perovskite iridates, which agrees well with conventional wisdom.
Here a spin glass system with emergent planar ordered spin clusters is investigated. The mixed B-site pyrochlore Gd 2 ScNbO 7 has been synthesized and characterized through a variety of techniques, including x-ray diffraction, magnetic susceptibility, muon spin relaxation, heat capacity and neutron scattering. Despite a Curie–Weiss temperature of -3.93(3) K, indicating net antiferromagnetic interactions, no signs of long ranged magnetic ordering are found down to T = 0.3 K. Instead, a disordered magnetic state emerges with a small correlation length of 2.1(1) Å of single tetrahedra. A Reverse Monte Carlo analysis of the polarized neutron scattering data reveals short-range antiferromagnetic order with emergent XY spin ordering similar to the parent pyrochlore compounds. Muon spin relaxation, and AC susceptibility measurements confirm that the magnetization condenses into a glass, with 10 % of the potential entropy missing in the specific heat. This magnetic ground state is similar to what is observed in Gd 2 Sn 2 O 7 just above the ordering temperature, without the eventual long-range ordering at low temperature.
The directed movement of spin-bearing excitations in semiconductors can enable many potential schemes for spintronic applications. Understanding the mechanism of spin motion, as opposed to charge carrier or exciton motion, may require specialized techniques and sample conditions. Here we employ the noncontact and time-resolved technique of light-induced transient grating spectroscopy (LITG) to measure both carrier and spin motion in a perovskite semiconductor with varying crystallinity. The carrier motion aligns with expectations from past studies undertaken at low fluence, revealing an ambipolar diffusion coefficient on the order of 1 cm 2 /sec and diffusion length of roughly 1.5 μm for single crystals that is strongly attenuated as crystallite size decreases. The spin diffusion is measured with cross-polarized excitation beams and uncovers an intensity-dependent coefficient rising above 100 cm 2 /sec. The fast room-temperature spin relaxation limits the spin diffusion length, but the remarkable speedup of spin over carrier diffusion suggests a mechanism involving a combination of exchange-mediated and doping effects that enhance spin transport.
Fluorescent nanodiamonds (FNDs) containing negatively charged nitrogen-vacancy (NV − ) centers are vital for many emerging quantum sensing applications from magnetometry to intracellular sensing in biology. However, developing a scalable fabrication method for FNDs hosting color centers with consistent bulk-like photoluminescence (PL) and spin coherence properties remains a highly desired but unrealized goal. Here, we investigate optimized ball milling of single-crystal diamonds produced via chemical vapor deposition (CVD) and containing 2 ppm of substitutional nitrogen and 0.3 ppm of NV − to achieve this goal. The NV charge state, PL lifetime, and spin properties of bulk CVD diamond samples are directly compared to milled CVD FNDs and commercial high-pressure high-temperature (HPHT) FNDs. We find that on average, the relative contribution of the NV − charge state to the total NV PL is lower and the NV PL lifetime is longer in CVD FNDs compared to HPHT FNDs, both likely due to the lower N s 0 concentration in CVD FNDs. The CVD bulk and CVD FNDs on average show similar average T 1 spin relaxation times of 3.2 ± 0.7 ms and 4.7 ± 1.6 ms, respectively, compared to 0.17 ± 0.01 ms for commercial HPHT FNDs. Our results demonstrate that ball milling of CVD diamonds enables the large-scale fabrication of NV ensembles in FNDs with bulk-like T 1 spin relaxation properties.
Improving the performance of molecular qubits is a fundamental milestone towards unleashing the power of molecular magnetism in the second quantum revolution. Taming spin relaxation and decoherence due to vibrations is crucial to reach this milestone, but this is hindered by our lack of understanding on the nature of vibrations and their coupling to spins. Here we propose a synergistic approach to study a prototypical molecular qubit. It combines inelastic X-ray scattering to measure phonon dispersions along the main symmetry directions of the crystal and spin dynamics simulations based on DFT. We show that the canonical Debye picture of lattice dynamics breaks down and that intra-molecular vibrations with very-low energies of 1-2 meV are largely responsible for spin relaxation up to ambient temperature. We identify the origin of these modes, thus providing a rationale for improving spin coherence. The power and flexibility of our approach open new avenues for the investigation of magnetic molecules with the potential of removing roadblocks toward their use in quantum devices.
We present analytical expressions for the D'yakonov-Perel' spin relaxation rates under the combined action of bulk and structural inversion asymmetry for zincblende heterostructures when terms up to linear and third order in k are included in the Hamiltonian. We see for heterostructures that, under the right conditions, the lowest-order-in-k component of the spin relaxation tensor can be made to vanish for all spin components at the same time. We study how the inclusion of terms of higher order in k affects these results.
The delafossitelike compound NaYbO 2 hosts a triangular lattice of Yb 3+ moments and is a promising candidate for the realization of a quantum spin liquid ground state—an exotic, quantum-disordered magnetic phase featuring long-range entanglement of spins. Tuning this system away from this quantum-disordered regime toward classical order or spin freezing is a powerful approach to shed light on the nature of the parent ground state. Here we leverage the substitution of nonmagnetic Lu 3+ onto the Yb 3+ sites to study the effects of magnetic disorder in NaYbO 2 using low-temperature ac susceptibility, heat capacity, and muon spin relaxation (𝜇SR) measurements. Here, our 𝜇SR measurements reveal resilient, correlated magnetic fluctuations that persist to at least 15% dilution, precluding conventional spin freezing and magnetic inhomogeneity. Heat capacity and magnetic susceptibility resolve a rapid suppression of the field-induced “up-up-down” magnetic order upon dilution and a crossover in the power-law behavior of the low-temperature magnetic excitations associated with the zero-field quantum disordered ground state. Taken together, these results support the notion of a robust network of entangled moments in NaYbO 2 and provide experimental validation of several models of a Heisenberg triangular lattice antiferromagnet in the presence of disorder.