Circular dichroism in non-chiral metal halide perovskites
Non-chiral orthorhombic perovskite nanostructures can exhibit chiro-optic effects under off-normal illumination due to the Rashba effect.
Sercel, Peter C.↗
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Electronic Band Structures of a Germanium Halide Perovskite Semiconductor
CsGeX 3 , a class of halide perovskites, is an emergent semiconductor with ferroelectricity and potential optoelectronic properties that can be harnessed for device applications. However, measurements of the electronic structure for this class of material are still lacking. Here, in this work, we report, for the first time, the experimental band structures of CsGeI 3 , a ferroelectric halide perovskite semiconductor, through angle-resolved photoemission spectroscopy (ARPES). The crystals were cleaved along both the (110) and (111) surfaces, facilitating the observation of clear valence band dispersions in several high-symmetry momentum directions. The observed valence band is characterized by a small hole effective mass of ∼0.1m 0 at the valence band maximum, without notable spectral signatures associated with the Rashba effect. Our experimental measurements are supported by electronic structure calculations in the DFT + G0W0 framework, enabling assessment of the band orbital characteristics, dispersion, and spin-splitting. This work unveils the intrinsic electronic and transport properties of CsGeX 3 , thereby advancing the optimization of the optoelectronic properties of this class of materials.
angle-resolved photoemission spectroscopy↗
Rashba exciton in a 2D perovskite quantum dot
The Rashba effect has been proposed to give rise to a bright exciton ground state in halide perovskite nanocrystals (NCs), resulting in very fast radiative recombination at room temperature and extremely fast radiative recombination at low temperature. In this paper we find the dispersion of the “Rashba exciton”, i.e., the exciton whose bulk dispersion reflects large spin–orbit Rashba terms in the conduction and valence bands and thus has minima at non-zero quasi-momenta. Placing Rashba excitonsin quasi-2D cylindrical quantum dots, we calculate size-dependent levels of confined excitons and their oscillator transition strengths. Here, we consider the implications of this model for two-dimensional hybrid organic–inorganic perovskites, discuss generalizations of this model to 3D NCs, and establish criteria under which a bright ground exciton state could be realized.
36 MATERIALS SCIENCE↗
NASA Tech Briefs, October 2004
Topics include: Relative-Motion Sensors and Actuators for Two Optical Tables; Improved Position Sensor for Feedback Control of Levitation; Compact Tactile Sensors for Robot Fingers; Improved Ion-Channel Biosensors; Suspended-Patch Antenna With Inverted, EM-Coupled Feed; System Would Predictively Preempt Traffic Lights for Emergency Vehicles; Optical Position Encoders for High or Low Temperatures; Inter-Valence-Subband/Conduction-Band-Transport IR Detectors; Additional Drive Circuitry for Piezoelectric Screw Motors; Software for Use with Optoelectronic Measuring Tool; Coordinating Shared Activities; Software Reduces Radio-Interference Effects in Radar Data; Using Iron to Treat Chlorohydrocarbon-Contaminated Soil; Thermally Insulating, Kinematic Tensioned-Fiber Suspension; Back Actuators for Segmented Mirrors and Other Applications; Mechanism for Self-Reacted Friction Stir Welding; Lightweight Exoskeletons with Controllable Actuators; Miniature Robotic Submarine for Exploring Harsh Environments; Electron-Spin Filters Based on the Rashba Effect; Diffusion-Cooled Tantalum Hot-Electron Bolometer Mixers; Tunable Optical True-Time Delay Devices Would Exploit EIT; Fast Query-Optimized Kernel-Machine Classification; Indentured Parts List Maintenance and Part Assembly Capture Tool - IMPACT; An Architecture for Controlling Multiple Robots; Progress in Fabrication of Rocket Combustion Chambers by VPS; CHEM-Based Self-Deploying Spacecraft Radar Antennas; Scalable Multiprocessor for High-Speed Computing in Space; and Simple Systems for Detecting Spacecraft Meteoroid Punctures.
Source record↗
Rashba splitting in organic–inorganic lead–halide perovskites revealed through two-photon absorption spectroscopy
Abstract The Rashba splitting in hybrid organic–inorganic lead–halide perovskites (HOIP) is particularly promising and yet controversial, due to questions surrounding the presence or absence of inversion symmetry. Here we utilize two-photon absorption spectroscopy to study inversion symmetry breaking in different phases of these materials. This is an all-optical technique to observe and quantify the Rashba effect as it probes the bulk of the materials. In particular, we measure two-photon excitation spectra of the photoluminescence in 2D, 3D, and anionic mixed HOIP crystals, and show that an additional band above, but close to the optical gap is the signature of new two-photon transition channels that originate from the Rashba splitting. The inversion symmetry breaking is believed to arise from ionic impurities that induce local electric fields. The observation of the Rashba splitting in the bulk of HOIP has significant implications for the understanding of their spintronic and optoelectronic device properties.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Large Magnetic Gap in a Designer Ferromagnet–Topological Insulator–Ferromagnet Heterostructure
Abstract Combining magnetism and nontrivial band topology gives rise to quantum anomalous Hall (QAH) insulators and exotic quantum phases such as the QAH effect where current flows without dissipation along quantized edge states. Inducing magnetic order in topological insulators via proximity to a magnetic material offers a promising pathway toward achieving the QAH effect at a high temperature for lossless transport applications. One promising architecture involves a sandwich structure comprising two single‐septuple layers (1SL) of MnBi 2 Te 4 (a 2D ferromagnetic insulator) with ultrathin few quintuple layer (QL) Bi 2 Te 3 in the middle, and it is predicted to yield a robust QAH insulator phase with a large bandgap greater than 50 meV. Here, the growth of a 1SL MnBi 2 Te 4 /4QL Bi 2 Te 3 /1SL MnBi 2 Te 4 heterostructure via molecular beam epitaxy is demonstrated and the electronic structure probed using angle‐resolved photoelectron spectroscopy. Strong hexagonally warped massive Dirac fermions and a bandgap of 75 ± 15 meV are observed. The magnetic origin of the gap is confirmed by the observation of the exchange‐Rashba effect, as well as the vanishing bandgap above the Curie temperature, in agreement with density functional theory calculations. These findings provide insights into magnetic proximity effects in topological insulators and reveal a promising platform for realizing the QAH effect at elevated temperatures.
36 MATERIALS SCIENCE↗
Reaching the Excitonic Limit in 2D Janus Monolayers by In Situ Deterministic Growth
Abstract Named after the two‐faced Roman god of transitions, transition metal dichalcogenide (TMD) Janus monolayers have two different chalcogen surfaces, inherently breaking the out‐of‐plane mirror symmetry. The broken mirror symmetry and the resulting potential gradient lead to the emergence of quantum properties such as the Rashba effect and the formation of dipolar excitons. Experimental access to these quantum properties, however, hinges on the ability to produce high‐quality 2D Janus monolayers. Here, these results introduce a holistic 2D Janus synthesis technique that allows real‐time monitoring of the growth process. This prototype chamber integrates in situ spectroscopy, offering fundamental insights into the structural evolution and growth kinetics, that allow the evaluation and optimization of the quality of Janus monolayers. The versatility of this method is demonstrated by synthesizing and monitoring the conversion of SWSe, SNbSe, and SMoSe Janus monolayers. Deterministic conversion and real‐time data collection further aid in conversion of exfoliated TMDs to Janus monolayers and unparalleled exciton linewidth values are reached, compared to the current best standard. The results offer an insight into the process kinetics and aid in the development of new Janus monolayers with high optical quality, which is much needed to access their exotic properties.
2D materials↗
Observation of large Rashba spin–orbit coupling at room temperature in compositionally engineered perovskite single crystals and application in high performance photodetectors
Indirect absorption extended below the direct transition edge and increase in carrier lifetime derived from Rashba spin–orbit coupling may advance the optoelectronic applications of metal halide perovskites. Spin-orbit coupling in halide perovskites is due to the presence of heavy elements in their structure. However, when these materials lack an inversion symmetry, for example by the application of strain, spin–orbit coupling becomes odd in the electron’s momentum giving rise to a splitting in the electronic energy bands. Here we report on the observation of a large Rashba splitting of 117 meV at room temperature, as predicted by relativistic first-principles calculations, in halide perovskite single crystals through a facile compositional engineering approach. Partial substitution of organic cations by rubidium in single crystals induces significant indirect absorption and dual peak photoluminescence as a result of a large Rashba splitting. We measured circularly polarized photoluminescence and magneto-photoluminescence in perovskite films printed by single crystals as well as magneto-electroluminescence and magneto-photocurrent in spin-LEDs based on perovskite single crystals. They indicated significant spin-momentum locking due to the large Rashba effect. A hybrid perovskite single crystal photodetector achieved record figures of merit, including detectivity of more than 1.3 × 10 18 Jones which represents a three orders of magnitude improvement compared to the to date record. Furthermore, these findings show that facile compositional engineering of perovskite single crystals holds great promise for further advancing the optoelectronic properties of existing materials.
36 MATERIALS SCIENCE↗
Driving ultrafast spin and energy modulation in quantum well states via photo-induced electric fields
Abstract The future of modern optoelectronics and spintronic devices relies on our ability to control the spin and charge degrees of freedom at ultrafast timescales. Rashba spin-split quantum well states, 2D states that develop at the surface of strong spin-orbit coupling materials, are ideal given the tunability of their energy and spin states. So far, however, most studies have only demonstrated such control in a static way. In this study, we demonstrate control of the spin and energy degrees of freedom of surface quantum well states on Bi 2 Se 3 at picosecond timescales. By means of a focused laser pulse, we modulate the band-bending, producing picosecond time-varying electric fields at the material’s surface, thereby reversibly modulating the quantum well spectrum and Rashba effect. Moreover, we uncover a dynamic quasi-Fermi level, dependent on the Lifshitz transition of the second quantum well band bottom. These results open a pathway for light-driven spintronic devices with ultrafast switching of electronic phases, and offer the interesting prospect to extend this ultrafast photo-gating technique to a broader host of 2D materials.
36 MATERIALS SCIENCE↗
Understanding lead halide perovskites
It has been ten years since research on lead halide perovskites (LHPs) took off spectacularly and expanded into one of the most active fields today in chemistry, physics, materials science, and engineering. There is no doubt that the rapid growth of this field has been fueled by the exceptional performance of this class of materials in solar cells, light emitting devices, and other electronic, optoelectronic, and photonic devices. Such application oriented advance has been accompanied by major development in mechanistic understanding. Growing mechanistic studies on LHPs have revealed structure–property relationships including, among others, structural instability, unique defect chemistry, dynamic disorder and anharmonicity of phonons, local symmetry breaking, efficient screening of charge carriers in large polaron formation, and the Rashba effect due to spin–orbital coupling and the presence of local electric fields. This special issue collects the cutting edge of our understanding of why LHPs work and what lessons LHPs have taught us about structure and dynamics, in general.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Weak magnetic field-dependent photoluminescence properties of lead bromide perovskites
The strong spin–orbit coupling (SOC) in lead halide perovskites, when inversion symmetry is lifted, has provided opportunities for investigating the Rashba effect in these systems. Moreover, the strong orbital moment, which, in turn, impacts the spin-pair in singlet and triplet electronic states, plays a significant role in enhancing the optoelectronic properties in the presence of external magnetic fields in lead halide perovskites. Here, we investigate the effect of weak magnetic fields (<1 T) on the photoluminescence (PL) properties of CsPbBr 3 nanocrystals with and without Ruddlesden–Popper (RP) faults and single crystals of CH 3 NH 3 PbBr 3 . Along with an enhancement in the PL intensity as a function of an external magnetic field, which is observed in both lead bromide perovskites, the PL emission red-shifts in CsPbBr 3 nanocrystals. Density-functional theory calculations of the electronic band-edge in CsPbBr 3 show almost no change in the energy gap as a function of the external magnetic field. The experimental results, thus, suggest the role of mixing of the triplet and singlet excitonic states under weak magnetic fields. This is further deduced from an enhancement in PL lifetimes as a function of the field in CsPbBr 3 . In CH 3 NH 3 PbBr 3 , an increase in PL intensity is observed under weak magnetic fields; however, no changes in the peak energy or PL lifetimes are observed. The internal magnetic fields due to SOC are characterized for all three samples and found to be the highest for CsPbBr 3 nanocrystals with RP faults.
36 MATERIALS SCIENCE↗
Out-of-plane carrier spin in transition-metal dichalcogenides under electric current
Significance Although out-of-plane current-induced spin polarization (CISP) is important for perpendicular-magnetization reorientation, and it has been realized by the crystalline symmetry breaking, its material examples are relatively fewer compared with in-plane CISP in Rashba systems. With the help of intrinsic spin–orbit coupling, an intriguing out-of-plane CISP is designed in transition-metal dichalcogenides by the symmetry breaking in the spin space, which provides opportunities for out-of-plane magnetization rotation and electric control of valley splitting. Moreover, the spin polarization is associated with valley-dependent responses to electric current and adds a dimension, valley degree of freedom, to the study of CISP. The symmetry argument and non-Rashba effective model also helps to illuminate these physics and broaden the scope of the CISP.
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
Strong influence of nonmagnetic ligands on the momentum-dependent spin splitting in antiferromagnets
Here, recent studies show the nonrelativistic antiferromagnetic ordering could generate momentum-dependent spin splitting analogous to the Rashba effect but free from the requirement of relativistic spin-orbit coupling. Whereas the classification of such compounds can be illustrated by different spin-splitting prototypes (SSTs) from symmetry analysis and density-functional-theory calculations, the huge variation in chemical bonding and structures of these diverse compounds possibly clouds the issue of how much of the variation in spin splitting can be traced back to the symmetry-defined characteristics, rather to the underlining chemical and structural diversity. The alternative model Hamiltonian approaches do not confront the issues of chemical and structural complexity but often consider only the magnetic sublattice, dealing with the all-important effects of the nonmagnetic ligands via renormalizing the interactions between the magnetic sites. To this end, we constructed a DFT model Hamiltonian that allows us to study SSTs at constant chemistry while retaining the realistic atomic-scale structure including ligands. This is accomplished by using a single, universal magnetic skeletal lattice (Ni 2+ ions in rocksalt NiO) and designing small displacements of the nonmagnetic (oxygen) sublattice which produce, by design, the different SST magnetic symmetries. We show that (i) even similar crystal structures having very similar band structures can lead to contrasting behavior of spin splitting vs momentum, and (ii) even subtle deformations of the nonmagnetic ligand sublattice could cause a giant spin splitting in AFM-induced SST. This is a paradigm shift relative to the convention of modeling magnets without considering the nonmagnetic ligand that mediates indirect magnetic interaction (e.g., superexchange).
36 MATERIALS SCIENCE↗
Large Dzyaloshinskii-Moriya interaction induced by chemisorbed oxygen on a ferromagnet surface
The Dzyaloshinskii-Moriya interaction (DMI) is an antisymmetric exchange interaction that stabilizes chiral spin textures. It is induced by inversion symmetry breaking in noncentrosymmetric lattices or at interfaces. Recently, interfacial DMI has been found in magnetic layers adjacent to transition metals due to the spin-orbit coupling and at interfaces with graphene due to the Rashba effect. We report direct observation of strong DMI induced by chemisorption of oxygen on a ferromagnetic layer at room temperature. The sign of this DMI and its unexpectedly large magnitude—despite the low atomic number of oxygen—are derived by examining the oxygen coverage–dependent evolution of magnetic chirality. We find that DMI at the oxygen/ferromagnet interface is comparable to those at ferromagnet/transition metal interfaces; it has enabled direct tailoring of skyrmion’s winding number at room temperature via oxygen chemisorption. This result extends the understanding of the DMI, opening up opportunities for the chemisorption-related design of spin-orbitronic devices.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Materials for Ultra‐Coherent, Mobile, Electron‐Spin Qubits
This research project has had the goal of gaining a better understanding of the physics of electrons bound to the surface of superfluid helium from both experimental and theoretical perspectives. It has particularly been aimed at two areas which had not been well studied: the relaxation and decoherence of the spin of the electrons on the helium surface and how the properties of underlying metallic layers affect the behavior of the electrons when the helium covering the metal is thin. This work is motivated in part by interest in using the spin of these electrons as a quantum bit, or qubit. Low levels of decoherence are advantageous for qubits, and moving the electrons, as one might do in a quantum processor, will be easiest if thin helium films can be employed. It had been suggested that spin decoherence should be very weak for electrons bound to superfluid He, but before this work there have been no quantitative studies of spin relaxation and decoherence. It is especially important to know how moving the electrons across the helium surface would affect their spin coherence. Calculations performed as part of this project show that the Rashba effective magnetic field, the mechanism which limits the spin coherence of mobile electrons in silicon-based devices (an actively pursued qubit technology), is exceptionally weak for electrons bound to helium. This project has identified other decoherence mechanisms which are stronger, but still weak compared to analogous silicon-based structures. Calculated spin coherence times for mobile electrons approach one day, as compared to microseconds in silicon. With coherence times of this magnitude, the spin qubit errors on helium will be completely dominated by errors in the quantum gates. In related work, the possibility of using an artificial spin-orbit interaction (a gradient magnetic field) for quantum operations on the electrons spins was considered. The calculations show that a moderate gradient field, small enough to be generated by a narrow superconducting wire, will enable high-fidelity quantum operations on electrons held in lithographically-defined quantum dots by driving them with a microwave electric field. The spin and motional coherence of the electrons is sufficient to allow high-fidelity 2-qubit quantum operations between electrons in neighboring quantum dots. As an outgrowth of experiments aiming to measure electron spin coherence it was discovered that very high densities of electrons can be stably supported on thin helium films coating ultra-smooth amorphous metallic layers. The measured densities are high enough that the electron system has almost certainly transitioned from an ordered array of electrons, known as a Wigner crystal (ordered by the electrons’ mutual repulsion), to a quantum fluid known as a Fermi liquid. This transition has been a subject of intense interest for over 40 years, since the electron Wigner crystal was first observed with electrons bound to superfluid helium, but it has never been unambiguously observed. Experiments are still underway in these new structures to definitively determine whether true quantum melting of the Wigner crystal has been demonstrated. This work has also catalyzed the development of a new approach for measuring the transport of electrons across very thin helium films, as will be needed for some of the quantum computing applications. The high electron density experiments as well as experiments with electrons bound in quantum dots have led to new techniques which may enable spin coherence measurements.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Magnetic asymmetry induced anomalous spin-orbit torque in IrMn
We demonstrate an anomalous spin-orbit torque induced by the broken magnetic symmetry in the antiferromagnet IrMn. We study the magnetic structure of three phases of IrMn thin films using neutron diffraction technique. The magnetic mirror symmetry M ' is broken laterally in both L 1 0 - IrMn and L 1 2 - IrM n 3 but not γ - IrM n 3 . We observe an out-of-plane dampinglike spin-orbit torque in both L 1 0 - IrMn /permalloy and L 1 2 - IrM n 3 /permalloy bilayers but not in γ - IrM n 3 /permalloy. This is consistent with both the symmetry analysis on the effects of a broken M ' on spin-orbit torque and the theoretical predictions of the spin Hall effect and the Rashba-Edelstein effect. In addition, the measured spin-orbit torque efficiencies are 0.61 ± 0.01, 1.01 ± 0.03, and 0.80 ± 0.01 for the L 1 0 , L 1 2 , and γ phases, respectively. Our work highlights the critical roles of the magnetic asymmetry in spin-orbit torque generation.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Rashba spin-orbit coupling enhanced magnetoresistance in junctions with one ferromagnet
We explain how Rashba spin-orbit coupling (SOC) in a two-dimensional electron gas (2DEG), or in a conventional s-wave superconductor, can lead to a large magnetoresistance even with one ferromagnet. However, such enhanced magnetoresistance is not generic and can be nonmonotonic and change its sign with Rashba SOC. For an in-plane rotation of magnetization, it is typically negligibly small for a 2DEG and depends on the perfect transmission which emerges from a spin-parity-time symmetry of the scattering states, while this symmetry is generally absent from the Hamiltonian of the system. The key difference from considering the normal-state magnetoresistance is the presence of the spin-dependent Andreev reflection at superconducting interfaces. In the fabricated junctions of quasi-2D van der Waals ferromagnets with conventional s-wave superconductors (Fe 0.29 TaS 2 /NbN) we find another example of enhanced magnetoresistance where the presence of Rashba SOC reduces the effective interfacial strength and is responsible for an equal-spin Andreev reflection. The observed nonmonotonic trend in the out-of-plane magnetoresistance with the interfacial barrier is an evidence for the proximity-induced equal-spin-triplet superconductivity.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗