skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Electric fields and substrates dramatically accelerate spin relaxation in graphene
Electrons in graphene are theoretically expected to retain spin states much longer than most materials, making graphene a promising platform for spintronics and quantum information technologies. Here, we use first-principles density-matrix (FPDM) dynamics simulations to show that interaction with electric fields and substrates strongly enhances spin relaxation through scattering with phonons. Consequently, the relaxation time at room temperature reduces from microseconds in free-standing graphene to nanoseconds in graphene on the hexagonal boron nitride (hBN) substrate, which is the order of magnitude typically measured in experiments. Further, inversion symmetry breaking by hBN introduces a stronger asymmetry in electron and hole spin lifetimes than predicted by the conventional D'yakonov-Perel' (DP) model for spin relaxation. Deviations from the conventional DP model are stronger for in-plane spin relaxation, resulting in out-of-plane to in-plane lifetime ratios much greater than 1/2 with a maximum close to the Dirac point. These FPDM results, independent of symmetry-specific assumptions or material-dependent parameters, also validate recent modifications of the DP model to explain such deviations. Overall, our results indicate that spin-phonon relaxation in the presence of substrates may be more important in graphene than typically assumed, requiring consideration for graphene-based spin technologies at room temperature.  more » « less
Award ID(s):
1956015
PAR ID:
10347316
Author(s) / Creator(s):
; ; ;
Date Published:
Journal Name:
Physical review
Volume:
105
ISSN:
2469-9985
Page Range / eLocation ID:
115122
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Continuum mechanics break down in bending stiffness calculations of mono- and few-layered two-dimensional (2D) van der Waals crystal sheets, because their layered atomistic structures are uniquely characterized by strong in-plane bonding coupled with weak interlayer interactions. Here, we elucidate how the bending rigidities of pristine mono- and few-layered molybdenum disulfide (MoS 2 ), graphene, and hexagonal boron nitride (hBN) are governed by their structural geometry and intra- and inter-layer bonding interactions. Atomic force microscopy experiments on the self-folded conformations of these 2D materials on flat substrates show that the bending rigidity of MoS 2 significantly exceeds those of graphene or hBN of comparable layers, despite its much lower tensile modulus. Even on a per-thickness basis, MoS 2 is found to possess similar bending stiffness to hBN and is much stiffer than graphene. Density functional theory calculations suggest that this high bending rigidity of MoS 2 is due to its large interlayer thickness and strong interlayer shear, which prevail over its weak in-plane bonding. 
    more » « less
  2. Using hexagonal boron nitride (hBN) as a substrate for graphene has shown faster carrier cooling which makes it ideal for high‐power graphene‐based devices. However, the effect of using boron‐isotope‐enriched hBN has not been explored. Herein, femtosecond pump‐probe spectroscopy is utilized to measure and compare the time dynamics of photo‐excited carriers in graphene‐hBN heterostructures for hBN with the natural distribution of boron isotopes (20%10B and 80%11B) and hBN enriched to 100%10B and11B. The carriers cool down faster for systems with isotopically pure hBN substrates by a factor of ≈1.7 times. This difference in relaxation times arises from the interfacial coupling between carriers in graphene and the hBN phonon modes. The results show that the boron isotopic purity of the hBN substrate can help to reduce the hot phonon bottleneck that limits the cooling in graphene devices. 
    more » « less
  3. null (Ed.)
    The recently discovered spin defects in hexagonal boron nitride (hBN), a layered van der Waals material, have great potential in quantum sensing. However, the photoluminescence and the contrast of the optically detected magnetic resonance (ODMR) of hBN spin defects are relatively low so far, which limits their sensitivity. Here we report a record-high ODMR contrast of 46% at room temperature and simultaneous enhancement of the photoluminescence of hBN spin defects by up to 17-fold by the surface plasmon of a gold film microwave waveguide. Our results are obtained with shallow boron vacancy spin defects in hBN nanosheets created by low-energy He+ ion implantation and a gold film microwave waveguide fabricated by photolithography. We also explore the effects of microwave and laser powers on the ODMR and improve the sensitivity of hBN spin defects for magnetic field detection. Our results support the promising potential of hBN spin defects for nanoscale quantum sensing. 
    more » « less
  4. Abstract Optically active spin defects in solids1,2are leading candidates for quantum sensing3,4and quantum networking5,6. Recently, single spin defects were discovered in hexagonal boron nitride (hBN)7–11, a layered van der Waals (vdW) material. Owing to its two-dimensional structure, hBN allows spin defects to be positioned closer to target samples than in three-dimensional crystals, making it ideal for atomic-scale quantum sensing12, including nuclear magnetic resonance (NMR) of single molecules. However, the chemical structures of these defects7–11remain unknown and detecting a single nuclear spin with a hBN spin defect has been elusive. Here we report the creation of single spin defects in hBN using13C ion implantation and the identification of three distinct defect types based on hyperfine interactions. We observed bothS = 1/2 andS = 1 spin states within a single hBN spin defect. We demonstrated atomic-scale NMR and coherent control of individual nuclear spins in a vdW material, with a π-gate fidelity up to 99.75% at room temperature. By comparing experimental results with density functional theory (DFT) calculations, we propose chemical structures for these spin defects. Our work advances the understanding of single spin defects in hBN and provides a pathway to enhance quantum sensing using hBN spin defects with nuclear spins as quantum memories. 
    more » « less
  5. Hexagonal boron nitride (hBN) has been grown on sapphire substrates by ultrahigh-temperature molecular beam epitaxy (MBE). A wide range of substrate temperatures and boron fluxes have been explored, revealing that high crystalline quality hBN layers are grown at high substrate temperatures, >1600℃ , and low boron fluxes, ∼1 × 10%& Torr beam equivalent pressure. In situ reflection high-energy electron diffraction revealed the growth of hBN layers with 60° rotational symmetry and the [112+ 0] axis of hBN parallel to the [11+ 00] axis of the sapphire substrate. Unlike the rough, polycrystalline films previously reported, atomic force microscopy and transmission electron microscopy characterization of these films demonstrate smooth, layered, few-nanometer hBN films on a nitridated sapphire substrate. This demonstration of high-quality hBN growth by MBE is a step toward its integration into existing epitaxial growth platforms, applications, and technologies. 
    more » « less