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: Searching for Circular Photo Galvanic Effect in Oxyhalide Perovskite Bi 4 NbO 8 Cl
Abstract The ability to reconfigure spin structure and spin‐photon interactions by an external electric field is a prerequisite for seamless integration of opto‐spintronics into modern electronics. In this study, the use of electric field on the tuning of circular photo galvanic effect in a quasi‐2D oxyhalide perovskite Bi4NbO8Cl is reported. The electrical transport measurements are applied to study the switching characteristics of the microsheet devices. The electric field is used to tune the nanoscale devices and an optical orientation approach is applied to understand the field‐tuned spin‐polarized band structures. It is found that the circular photogalvanic current can be erased and re‐created by poling, indicating the electric‐field‐based control over spin structure. The study enriches the basic understanding of the symmetry‐regulated optoelectronic response in ferroelectrics with spin‐orbit coupling.  more » « less
Award ID(s):
2039380 2005096 2031692 1916652
PAR ID:
10371580
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  ;  more » ;  ;  ;   « less
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Advanced Functional Materials
Volume:
32
Issue:
47
ISSN:
1616-301X
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract All‐optical control and detection of magnetic states for high‐density recording necessitate nanophotonic approaches to amplify local light intensity below the diffraction limit. Sculpting the near‐field phase and polarization can additionally strengthen magneto‐optical effects that rely on circularly polarized pulses, such as all‐optical helicity‐dependent switching, imaging, and spin‐wave excitation. Here, high‐refractive‐index dielectric nanoantennas illuminated with circularly polarized light resonantly enhance local electric field rotation by more than sixfold within [Pt/Co]Nthin films. Sub‐wavelength arrays of amorphous Si nanodisks, or metasurfaces, patterned on perpendicularly magnetized films support Mie‐type resonances that modulate reflection and transmission dissymmetry by >±2% in experiments. Spatial and spectral interference between dipolar modes, proximity effects, and gain are evaluated by varying disk aspect ratio, metasurface–metal separation, and magnetic film thickness, respectively. Simulated enhancements in magnetic circular birefringence and differential absorption are correlated with amplified local field rotation at electric dipolar modes. Greater achievable amplifications are shown via simulations with single‐crystalline Si metasurfaces exhibiting lower losses, including a 12‐fold strengthened electric field rotation within ferromagnetic layers. The metasurface design rules established here could enable nanoscale localization of all‐optical magnetic switching with lowered laser fluence thresholds, as well as enhanced magneto‐optical responses for light‐assisted reading in spintronic devices. 
    more » « less
  2. Abstract Here, the observation of spin‐polarized emission for the Au25(SC8H9)18monolayer‐protected cluster (MPC) is reported. Variable‐temperature variable‐field magnetic circular photoluminescence (VTV‐MCPL) measurements are combined with VT‐PL spectroscopy to provide state‐resolved characterization of the transient electronic structure and spin‐polarized electron‐hole recombination dynamics of Au25(SC8H9)18. Through analysis of VTV‐MCPL measurements, a low energy (1.64 eV) emission peak is assigned to intraband relaxation between core‐metal‐localized superatom‐D to ‐P orbitals. Two higher energy interband components (1.78 eV, 1.94 eV) are assigned to relaxation from superatom‐D orbitals to states localized to the inorganic semirings. For both intraband superatom‐based or interband relaxation mechanisms, the extent of spin‐polarization, quantified as the degree of circular polarization (DOCP), is determined by state‐specific electron‐vibration coupling strengths and energy separations of bright and dark electronic fine‐structure levels. At low temperatures (<60 K), metal–metal superatom‐based intraband transitions dominate the global PL emission. At higher temperatures (>60 K), interband ligand‐based emission is dominant. In the low‐temperature PL regime, increased sample temperature results in larger global PL intensity. In the high‐temperature regime, increased temperature quenches interband radiative recombination. The relative intensity for each PL mechanism is discussed in terms of state‐specific electronic‐vibrational coupling strengths and related to the total angular momentum, quantified by Landég‐factors. 
    more » « less
  3. Abstract Bismuth ferrite (BiFeO3) is a multiferroic material that exhibits both ferroelectricity and canted antiferromagnetism at room temperature, making it a unique candidate in the development of electric-field controllable magnetic devices. The magnetic moments in BiFeO3are arranged into a spin cycloid, resulting in unique magnetic properties which are tied to the ferroelectric order. Previous understanding of this coupling has relied on average, mesoscale measurements. Using nitrogen vacancy-based diamond magnetometry, we observe the magnetic spin cycloid structure of BiFeO3in real space. This structure is magnetoelectrically coupled through symmetry to the ferroelectric polarization and this relationship is maintained through electric field switching. Through a combination of in-plane and out-of-plane electrical switching, coupled with ab initio studies, we have discovered that the epitaxy from the substrate imposes a magnetoelastic anisotropy on the spin cycloid, which establishes preferred cycloid propagation directions. The energy landscape of the cycloid is shaped by both the ferroelectric degree of freedom and strain-induced anisotropy, restricting the spin spiral propagation vector to changes to specific switching events. 
    more » « less
  4. Abstract Excitons in two-dimensional (2D) semiconductors have offered an attractive platform for optoelectronic and valleytronic devices. Further realizations of correlated phases of excitons promise device concepts not possible in the single particle picture. Here we report tunable exciton “spin” orders in WSe2/WS2moiré superlattices. We find evidence of an in-plane (xy) order of exciton “spin”—here, valley pseudospin—around exciton fillingvex = 1, which strongly suppresses the out-of-plane “spin” polarization. Upon increasingvexor applying a small magnetic field of ~10 mT, it transitions into an out-of-plane ferromagnetic (FM-z) spin order that spontaneously enhances the “spin” polarization, i.e., the circular helicity of emission light is higher than the excitation. The phase diagram is qualitatively captured by a spin-1/2 Bose–Hubbard model and is distinct from the fermion case. Our study paves the way for engineering exotic phases of matter from correlated spinor bosons, opening the door to a host of unconventional quantum devices. 
    more » « less
  5. Abstract The rapid development of computing applications demands novel low‐energy consumption devices for information processing. Among various candidates, magnetoelectric heterostructures hold promise for meeting the required voltage and power goals. Here, a route to low‐voltage control of magnetism in 30 nm Fe0.5Rh0.5/100 nm 0.68PbMg1/3Nb2/3O3‐0.32PbTiO3(PMN‐PT) heterostructures is demonstrated wherein the magnetoelectric coupling is achieved via strain‐induced changes in the Fe0.5Rh0.5mediated by voltages applied to the PMN‐PT. We describe approaches to achieve high‐quality, epitaxial growth of Fe0.5Rh0.5on the PMN‐PT films and, a methodology to probe and quantify magnetoelectric coupling in small thin‐film devices via studies of the anomalous Hall effect. By comparing the spin‐flop field change induced by temperature and external voltage, the magnetoelectric coupling coefficient is estimated to reach ≈7 × 10−8 s m−1at 325 K while applying a −0.75 V bias. 
    more » « less