Electrical switching of the edge current chirality in quantum anomalous Hall insulators.

A quantum anomalous Hall (QAH) insulator is a topological phase in which the interior is insulating but electrical current flows along the edges of the sample in either a clockwise or counterclockwise direction, as dictated by the spontaneous magnetization orientation. Such a chiral edge current eliminates any backscattering, giving rise to quantized Hall resistance and zero longitudinal resistance. Here we fabricate mesoscopic QAH sandwich Hall bar devices and succeed in switching the edge current chirality through thermally assisted spin-orbit torque (SOT). The well-quantized QAH states before and after SOT switching with opposite edge current chiralities are demonstrated through four- and three-terminal measurements. We show that the SOT responsible for magnetization switching can be generated by both surface and bulk carriers. Our results further our understanding of the interplay between magnetism and topological states and usher in an easy and instantaneous method to manipulate the QAH state.

Engineering Plateau Phase Transition in Quantum Anomalous Hall Multilayers.

The plateau phase transition in quantum anomalous Hall (QAH) insulators corresponds to a quantum state wherein a single magnetic domain gives way to multiple domains and then reconverges back to a single magnetic domain. The layer structure of the sample provides an external knob for adjusting the Chern number C of the QAH insulators. Here, we employ molecular beam epitaxy to grow magnetic topological insulator multilayers and realize the magnetic field-driven plateau phase transition between two QAH states with odd Chern number change ΔC. We find that critical exponents extracted for the plateau phase transitions with ΔC = 1 and ΔC = 3 in QAH insulators are nearly identical. We construct a four-layer Chalker-Coddington network model to understand the consistent critical exponents for the plateau phase transitions with ΔC = 1 and ΔC = 3. This work will motivate further investigations into the critical behaviors of plateau phase transitions with different ΔC in QAH insulators.

Coexistence of Superconductivity and Antiferromagnetism in Topological Magnet MnBi2Te4 Films.

The interface of two materials can harbor unexpected emergent phenomena. One example is interface-induced superconductivity. In this work, we employ molecular beam epitaxy to grow a series of heterostructures formed by stacking together two nonsuperconducting antiferromagnetic materials, an intrinsic antiferromagnetic topological insulator MnBi2Te4 and an antiferromagnetic iron chalcogenide FeTe. Our electrical transport measurements reveal interface-induced superconductivity in these heterostructures. By performing scanning tunneling microscopy and spectroscopy measurements, we observe a proximity-induced superconducting gap on the top surface of the MnBi2Te4 layer, confirming the coexistence of superconductivity and antiferromagnetism in the MnBi2Te4 layer. Our findings will advance the fundamental inquiries into the topological superconducting phase in hybrid devices and provide a promising platform for the exploration of chiral Majorana physics in MnBi2Te4-based heterostructures.

Proximity-induced superconductivity in epitaxial topological insulator/graphene/gallium heterostructures.

The introduction of superconductivity to the Dirac surface states of a topological insulator leads to a topological superconductor, which may support topological quantum computing through Majorana zero modes1,2. The development of a scalable material platform is key to the realization of topological quantum computing3,4. Here we report on the growth and properties of high-quality (Bi,Sb)2Te3/graphene/gallium heterostructures. Our synthetic approach enables atomically sharp layers at both hetero-interfaces, which in turn promotes proximity-induced superconductivity that originates in the gallium film. A lithography-free, van der Waals tunnel junction is developed to perform transport tunnelling spectroscopy. We find a robust, proximity-induced superconducting gap formed in the Dirac surface states in 5-10 quintuple-layer (Bi,Sb)2Te3/graphene/gallium heterostructures. The presence of a single Abrikosov vortex, where the Majorana zero modes are expected to reside, manifests in discrete conductance changes. The present material platform opens up opportunities for understanding and harnessing the application potential of topological superconductivity.

Evolution of Dopant-Concentration-Induced Magnetic Exchange Interaction in Topological Insulator Thin Films.

To date, the quantum anomalous Hall effect has been realized in chromium (Cr)- and/or vanadium(V)-doped topological insulator (Bi,Sb)2Te3 thin films. In this work, we use molecular beam epitaxy to synthesize both V- and Cr-doped Bi2Te3 thin films with controlled dopant concentration. By performing magneto-transport measurements, we find that both systems show an unusual yet similar ferromagnetic response with respect to magnetic dopant concentration; specifically the Curie temperature does not increase monotonically but shows a local maximum at a critical dopant concentration. We attribute this unusual ferromagnetic response observed in Cr/V-doped Bi2Te3 thin films to the dopant-concentration-induced magnetic exchange interaction, which displays evolution from van Vleck-type ferromagnetism in a nontrivial magnetic topological insulator to Ruderman-Kittel-Kasuya-Yosida (RKKY)-type ferromagnetism in a trivial diluted magnetic semiconductor. Our work provides insights into the ferromagnetic properties of magnetically doped topological insulator thin films and facilitates the pursuit of high-temperature quantum anomalous Hall effect.

Environmental Doping-Induced Degradation of the Quantum Anomalous Hall Insulators.

The quantum anomalous Hall (QAH) insulator carries dissipation-free chiral edge current and thus provides a unique opportunity to develop energy-efficient transformative information technology. Despite promising advances, the QAH insulator has thus far eluded any practical applications. In addition to its low working temperature, the QAH state in magnetically doped topological insulators usually deteriorates with time in ambient conditions. In this work, we store three QAH devices with similar initial properties in different environments. The QAH device without a protection layer in air shows clear degradation and becomes hole-doped. The QAH device kept in an argon glovebox without a protection layer shows no measurable degradation after 560 h, and the device protected by a 3 nm AlOx protection layer in air shows minimal degradation with stable QAH properties. Our work shows a route to preserve the dissipation-free chiral edge state in QAH devices for potential applications in quantum information technology.

Confinement-Induced Chiral Edge Channel Interaction in Quantum Anomalous Hall Insulators.

In quantum anomalous Hall (QAH) insulators, the interior is insulating but electrons can travel with zero resistance along one-dimensional (1D) conducting paths known as chiral edge channels (CECs). These CECs have been predicted to be confined to the 1D edges and exponentially decay in the two-dimensional (2D) bulk. In this Letter, we present the results of a systematic study of QAH devices fashioned in a Hall bar geometry of different widths under gate voltages. At the charge neutral point, the QAH effect persists in a Hall bar device with a width of only ∼72 nm, implying the intrinsic decaying length of CECs is less than ∼36 nm. In the electron-doped regime, we find that the Hall resistance deviates quickly from the quantized value when the sample width is less than 1 µm. Our theoretical calculations suggest that the wave function of CEC first decays exponentially and then shows a long tail due to disorder-induced bulk states. Therefore, the deviation from the quantized Hall resistance in narrow QAH samples originates from the interaction between two opposite CECs mediated by disorder-induced bulk states in QAH insulators, consistent with our experimental observations.

Stable Negative Optical Torque in Optically Bound Nanoparticle Dimers.

Negative optical torque is a counterintuitive optomechanical phenomenon that can emerge in light-assembled nanoparticle (NP) clusters (i.e., optical matter) under circular polarization. However, in experiments, stable negative torque was limited to optical matter with 3 or more NPs. Here, we show that by increasing the particle size, the sign of optical torque can be reversed in optical matter dimers, where stable negative torque arises in dimers of 300 nm diameter Au or 490 nm diameter polystyrene NPs. Our computational analysis reveals that the multipolar resonances in large NPs can enhance the forward scattering along the spin angular momentum (SAM) direction of light, creating a recoil negative torque due to momentum conservation. The observation of stable negative torque in dimers pushes the limit to the smallest optical matter, demonstrating the universal existence of negative torque in such a system. The underlying principle also provides new strategies for making light-driven nanomotors.

Zero Magnetic Field Plateau Phase Transition in Higher Chern Number Quantum Anomalous Hall Insulators.

The plateau-to-plateau transition in quantum Hall effect under high magnetic fields is a celebrated quantum phase transition between two topological states. It can be achieved by either sweeping the magnetic field or tuning the carrier density. The recent realization of the quantum anomalous Hall (QAH) insulators with tunable Chern numbers introduces the channel degree of freedom to the dissipation-free chiral edge transport and makes the study of the quantum phase transition between two topological states under zero magnetic field possible. Here, we synthesized the magnetic topological insulator (TI)/TI pentalayer heterostructures with different Cr doping concentrations in the middle magnetic TI layers using molecular beam epitaxy. By performing transport measurements, we found a potential plateau phase transition between C=1 and C=2 QAH states under zero magnetic field. In tuning the transition, the Hall resistance monotonically decreases from h/e^{2} to h/2e^{2}, concurrently, the longitudinal resistance exhibits a maximum at the critical point. Our results show that the ratio between the Hall resistance and the longitudinal resistance is greater than 1 at the critical point, which indicates that the original chiral edge channel from the C=1 QAH state coexists with the dissipative bulk conduction channels. Subsequently, these bulk conduction channels appear to self-organize and form the second chiral edge channel in completing the plateau phase transition. Our study will motivate further investigations of this novel Chern number change-induced quantum phase transition and advance the development of the QAH chiral edge current-based electronic and spintronic devices.

Optical trapping and manipulation for single-particle spectroscopy and microscopy.

Optical tweezers can control the position and orientation of individual colloidal particles in solution. Such control is often desirable but challenging for single-particle spectroscopy and microscopy, especially at the nanoscale. Functional nanoparticles that are optically trapped and manipulated in a three-dimensional (3D) space can serve as freestanding nanoprobes, which provide unique prospects for sensing and mapping the surrounding environment of the nanoparticles and studying their interactions with biological systems. In this perspective, we will first describe the optical forces underlying the optical trapping and manipulation of microscopic particles, then review the combinations and applications of different spectroscopy and microscopy techniques with optical tweezers. Finally, we will discuss the challenges of performing spectroscopy and microscopy on single nanoparticles with optical tweezers, the possible routes to address these challenges, and the new opportunities that will arise.

Three-dimensional optical trapping and orientation of microparticles for coherent X-ray diffraction imaging.

Optical trapping has been implemented in many areas of physics and biology as a noncontact sample manipulation technique to study the structure and dynamics of nano- and mesoscale objects. It provides a unique approach for manipulating microscopic objects without inducing undesired changes in structure. Combining optical trapping with hard X-ray microscopy techniques, such as coherent diffraction imaging and crystallography, provides a nonperturbing environment where electronic and structural dynamics of an individual particle in solution can be followed in situ. It was previously shown that optical trapping allows the manipulation of micrometer-sized objects for X-ray fluorescence imaging. However, questions remain over the ability of optical trapping to position objects for X-ray diffraction measurements, which have stringent requirements for angular stability. Our work demonstrates that dynamic holographic optical tweezers are capable of manipulating single micrometer-scale anisotropic particles in a microfluidic environment with the precision and stability required for X-ray Bragg diffraction experiments-thus functioning as an "optical goniometer." The methodology can be extended to a variety of X-ray experiments and the Bragg coherent diffractive imaging of individual particles in solution, as demonstrated here, will be markedly enhanced with the advent of brighter, coherent X-ray sources.

Plasmonic SERS Biosensor Based on Multibranched Gold Nanoparticles Embedded in Polydimethylsiloxane for Quantification of Hematin in Human Erythrocytes.

This work reports a plasmonic surface-enhanced Raman scattering (SERS) biosensor that allows for quantitative analysis of hematin in erythrocytes without the need of separating it from hemoglobin (Hb). The biosensor exploits the tunable localized surface plasmon resonance (LSPR) characteristics of multibranched gold nanoparticles (M-AuNPs) and the strong plasmon coupling between an Au thin film and a flexible substrate consisting of M-AuNPs embedded in polydimethylsiloxane (PDMS) (i.e., M-AuNP-embedded PDMS substrate). In the assay, the hematin (or hematin-containing erythrocyte hemolysate) was deposited on Au film surface and covered with M-AuNP-embedded PDMS. Strong SERS signals were generated under excitation at 785 nm; the signals were sensitive to hematin concentration but not to several common coexisting biological substances. The intensities of the SERS signal (at 1623 cm-1) displayed a wide linear range using hematin concentrations in a range of at least ∼1.5 nM-1.1 µM; the limit of detection (LOD) was ∼0.03 ± 0.01 nM at a signal/noise (S/N) of 3. This assay is simple and sensitive without tedious separation procedures, thereby saving time and enhancing efficiency. This biosensor can be used to determine hematin concentration in human erythrocyte cytosols giving concentrations of ∼18.5 ± 4.5 (by averaging eight samples) and 51.5 ± 6.2 µM (by averaging three samples) for healthy and sickle erythrocytes, respectively, making it a potential application in clinical detection.

Synergy of Intensity, Phase, and Polarization Enables Versatile Optical Nanomanipulation.

Micromanipulation by optical tweezers mainly relies on the trapping force derived from the intensity gradient of light. Here we show that the synergy of intensity, phase, and polarization in structured light allows versatile optical manipulation of nanostructures. When a metal nanoparticle is confined by a linearly polarized laser field, the sign of optical force depends on the particle shape and the laser intensity, phase, and polarization profiles. By tuning these parameters in optical line traps, optical trapping, transporting, and sorting of silver nanostructures have been demonstrated. These findings inspired us to control the motion of nanostructures with designed intensity, phase, and polarization of light using holographic optical tweezers with advanced beam shaping techniques. This work provides a new perspective on active colloidal nanomanipulation in fully controlled optical landscapes, which largely expands the existing optical manipulation toolbox.

Tuning Nanoparticle Electrodynamics by an Optical-Matter-Based Laser Beam Shaper.

Spatially modulated optical fields provide the perspective of tuning nanoparticle (NP) dynamics in a colloidal suspension. Here, it is shown that the lateral interferometric optical field created by a chain of optically bound Au NPs (i.e., optical matter) can tailor the electrodynamic interactions among more Au NPs. The free-standing NP chain, which is assembled and confined by an auxiliary optical line, shapes the main trapping beam and guides the self-organization of Au NPs under an optimized polarization direction. We find that the NP chain can largely enhance the anisotropic optical binding interaction of two nearby NPs but suppress the anisotropic interaction of multiple NPs, leading to isotropic self-organization. The dynamics and structural transitions of the NPs are well-reproduced in a simulation by using a coupled finite-difference time-domain (FDTD)-Langevin dynamics approach. Our work provides a new dual-beam optical trapping and in situ laser beam shaping approach to study and control interparticle electrodynamic interactions among colloidal NPs.

Creating Multifunctional Optofluidic Potential Wells for Nanoparticle Manipulation.

Optical forces have enabled various nanomanipulation in microfluidics such as optical trapping, sorting, and transporting of nanoparticles (NPs), but the manipulation is usually specific with a certain optical field. Tightly focused Gaussian beams can trap NPs but not sort them; moderately focused Gaussian beams allow sorting microparticles in a flow but not NPs; quasi-Bessel beams can sort NPs in a flow but cannot control their positions due to low trapping stiffness. All these methods rely on the axial variation of laser intensity. Here we show that multifunctional and tunable optofluidic potential wells can be created for nanomanipulation by synchronizing optical phase gradient force with fluid drag force. We demonstrate controlled trapping and transporting of 150 nm Ag NPs over 10 µm and sorting of 80 and 100 nm Au NPs using optical line traps with tunable phase gradients in experiments. Our simulations further predict that simultaneous sorting and trapping of sub-50 nm Au NPs can be achieved with a sorting resolution of 1 nm using optimized optical fields. Our method provides great freedom and flexibility for nanomanipulation in optofluidics with potential applications in nanophotonics and biomedicine.

Probing Spatiotemporal Stability of Optical Matter by Polarization Modulation.

Light-driven self-organization of plasmonic nanoparticles via optical binding interactions offers a unique route to assemble mesoscale photonic clusters and chains. However, stability becomes an issue when more nanoparticles are added into the clusters and chains, since the theoretical optical binding strength is inhomogeneous and anisotropic in optical matter systems. Here we study the spatiotemporal stability of optical matter chains self-organized by two to eight ultrauniform gold nanospheres in a linearly polarized optical line trap. Perturbations are introduced into the nanosphere chains by periodically switching the polarization to be either parallel or perpendicular to the orientation of the chains, where the spatial and temporal variation of optical binding strength has been revealed. In addition, we found that the average oscillation amplitude and stability of the particles can be tuned by the frequency of polarization modulation. These results demonstrate a new way to study and improve the stability of optical matter and provide a promising strategy in engineering optical forces at the mesoscale.

Sorting Metal Nanoparticles with Dynamic and Tunable Optical Driven Forces.

Precise sorting of colloidal nanoparticles is a challenging yet necessary task for size-specific applications of nanoparticles in nanophotonics and biochemistry. Here we present a new strategy for all-optical sorting of metal nanoparticles with dynamic and tunable optical driven forces generated by phase gradients of light. Size-dependent optical forces arising from the phase gradients of optical line traps can drive nanoparticles of different sizes with different velocities in solution, leading to their separation along the line traps. By using a sequential combination of optical lines to create differential trapping potentials, we realize precise sorting of silver and gold nanoparticles in the diameter range of 70-150 nm with a resolution down to 10 nm. Separation of the nanoparticles agrees with the analysis of optical forces acting on them and with simulations of their kinetic motions. The results provide new insights into all-optical nanoparticle manipulation and separation and reveal that there is still room to sort smaller nanoparticle with nanometer precision using dynamic phase-gradient forces.

Light-Driven Self-Healing of Nanoparticle-Based Metamolecules.

Metamolecules and crystals consisting of nanoscale building blocks offer rich models to study colloidal chemistry, materials science, and photonics. Herein we demonstrate the self-assembly of colloidal Ag nanoparticles into quasi-one-dimensional metamolecules with an intriguing self-healing ability in a linearly polarized optical field. By investigating the spatial stability of the metamolecules, we found that the origin of self-healing is the inhomogeneous interparticle electrodynamic interactions enhanced by the formation of unusual nanoparticle dimers, which minimize the free energy of the whole structure. The equilibrium configuration and self-healing behavior can be further tuned by modifying the electrical double layers surrounding the nanoparticles. Our results reveal a unique route to build self-healing colloidal structures assembled from simple metal nanoparticles. This approach could potentially lead to reconfigurable plasmonic devices for photonic and sensing applications.

Fabrication of a material assembly of silver nanoparticles using the phase gradients of optical tweezers.

Optical matter can be created using the intensity gradient and electrodynamic (e.g., optical binding) forces that nano- and microparticles experience in focused optical beams. Here we show that the force associated with phase gradient is also important. In fact, in optical line traps the phase gradient force is crucial in determining the structure and stability of optical matter arrays consisting of Ag nanoparticles (NPs). NP lattices can be repeatedly assembled and disassembled simply by changing the sign of the phase gradient. The phase gradient creates a compressive force (and thus a stress) in the optically bound Ag NP lattices, causing structural transitions (a stress response) from 1D "chains" to 2D lattices, and even to amorphous structures. The structural transitions and dynamics of driven transport are well described by electrodynamics simulations and modeling using a drift-diffusion Langevin equation.

Enhancing nanoparticle electrodynamics with gold nanoplate mirrors.

Mirrors and optical cavities can modify and enhance matter-radiation interactions. Here we report that chemically synthesized Au nanoplates can serve as micrometer-size mirrors that enhance electrodynamic interactions. Because of their plasmonic properties, the Au nanoplates enhance the brightness of scattered light from Ag nanoparticles near the nanoplate surface in dark-field microscopy. More importantly, enhanced optical trapping and optical binding of Ag nanoparticles are demonstrated in interferometric optical traps created from a single laser beam and its reflection from individual Au nanoplates. The enhancement of the interparticle force constant is ≈20-fold more than expected from the increased intensity due to standing wave interference. We show that the additional stability for optical binding arises from the restricted axial thermal motion of the nanoparticles that couples to and reduces the fluctuations in the lateral plane. This new mechanism greatly advances the photonic synthesis of ultrastable nanoparticle arrays and investigation of their properties.