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Shuolong Yang

Publications and source records attributed to Shuolong Yang.

At least 19 recordsLinked to original sources

Signatures of a light-induced exciton condensate exhibiting BEC-BCS crossover

Exciton condensates provide a platform to study quasiparticle pairing, Bose-Einstein condensation-Bardeen-Cooper-Schrieffer (BEC-BCS) crossover, and excitonic topological phenomena. Achieving a nonequilibrium exciton condensate allows the ultimate tunability of these emergent phenomena. Yet, evidence of a light-induced, nonequilibrium exciton condensate and its BEC-BCS crossover remains elusive. Here, we use time- and angle-resolved photoemission spectroscopy to demonstrate signatures of a non-equilibrium exciton condensate and its BEC-BCS crossover in monolayer MnBi2Te4. Following optical excitation, a distinctive hole-like dispersion representing excitons emerges and persists for >20 ps. Strikingly, energy-domain sharpening in the valence band occurs 2 ps after time zero and exhibits a sharp onset at a threshold pump fluence of 0.84 mJ/cm2. The delayed and strongly nonlinear response is difficult to reconcile with transient field effects or conventional carrier-induced band shifts but is consistent with a model of exciton condensation governed by a Berezinskii-Kosterlitz-Thouless transition. The estimated threshold exciton density agrees quantitatively with the Nelson-Kosterlitz critical density. At higher fluences, the exciton feature develops a camel-back-shaped dispersion, consistent with the BEC-BCS crossover in the condensate framework. Our work establishes ultrathin MnBi2Te4 as a model system for studying nonequilibrium exciton condensates with a connection to superconductivity and exciton-driven topological phases.

cond-mat.mes-hall

Millimeter-Scale, Atomically Controlled 2D Topological Insulators Revealed by Multimodal Spectroscopy

Quantum spin Hall insulators, or synonymously known as 2D topological insulators, are crucial 2D systems hosting topologically protected edge states. The working temperature of this topological quantum phase is dictated by the inverted bandgap. However, the previously identified large-gap 2D topological insulators are either extremely chemically unstable, or cannot be made with atomistic precision over macroscopic scales. Here, we establish two-quintuple-layer Bi2Te3 and MnBi2Te4/Bi2Te3 heterostructures as atomically controlled, millimeter-scale 2D topological insulators, enabled by precision layer-by-layer growth that yields a carpet-like morphology extending coherently over macroscopic distances. This carpet-like growth mode renders the films amenable to mechanical exfoliation and subsequent wet or dry transfer. Multimodal spectroscopies and microscopies reveal the integer-layer tuned electronic structure of (Bi2Te3)n with excellent agreement to theory. Photon-energy-dependent photoemission and time-resolved photoemission identify band inversion and band dynamics, respectively, while scanning tunneling spectroscopy resolves topological edge states, characteristic of the 2D topological insulator phase. Thickness- and photon-energy-dependent photoemission further validates MnBi2Te4/Bi2Te3 as a robust 2D topological insulator. The large inverted gaps of ~100 meV in (Bi2Te3)2 and ~150 meV in MnBi2Te4/Bi2Te3 suggest operation near ambient temperature. These results define a scalable materials platform for next-generation, low-loss quantum and energy-efficient devices.

cond-mat.mtrl-sci

Interaction-driven flat band and charge order in Fe5GeTe2

Flat electronic bands enable fascinating emergent phenomena such as superconductivity and charge orders. A prevailing approach to realizing flat bands is to engineer lattice geometric constraints in twisted or kagome-like materials. An alternative approach is to utilize purely electronic-interaction-driven flat bands, yet a fundamental challenge is that extreme flatness requires ultrastrong interaction strength, which often leads to incoherent states. Here we demonstrate the concurrent formation of an interaction-driven flat band at the Fermi level and a $\sqrt{3}\times\sqrt{3}\,R30^\circ$ charge order in a van der Waals magnet Fe5GeTe2 using high-resolution angle-resolved photoemission spectroscopy. This charge order is manifested by band folding within 30 meV below the Fermi level, with its nesting driven by flat bands. The presence of this flat band throughout the Brillouin zone and the logarithmic temperature dependence of its spectral weight suggest a Kondo-like, coherent Fermi liquid emerging from strong correlations. Our work establishes a paradigm where an interaction-driven flat band promotes large-scale electronic ordering.

cond-mat.str-el

Spectroscopic evidence of intra-unit-cell charge redistribution in charge-neutral magnetic topological insulator Sb-doped MnBi6Te10

The magnetic topological insulator MnBi$_{6}$Te$_{10}$ has emerged as a promising candidate for realizing the quantum anomalous Hall effect (QAHE), owing to its ability to retain ferromagnetism through precise control of anti-site defects. The next important task for realizing the QAHE is to tune the chemical potential into the energy gap formed by the broken time-reversal symmetry. Here we reveal an intra-unit-cell charge redistribution even when the overall doping suggests a near-charge-neutral condition. By performing time- and angle-resolved photoemission spectroscopy (trARPES) on the optimally 18% Sb-doped MnBi$_{6}$Te$_{10}$, we observe transient surface photovoltage (SPV) effects on both the MnBi$_{2}$Te$_{4}$ and single-Bi$_{2}$Te$_{3}$ terminations. Furthermore, we observe a time-dependent splitting of the band structure indicating multiple SPV shifts with different magnitudes. This observation suggests that adjacent plateaus with nominally the same terminating layer exhibit a strong intra-unit-cell charge redistribution, resulting in spontaneous electrical polarization. This is consistent with static micro-ARPES measurements revealing significant doping deviations from the charge-neutral configuration. Our findings underscore the challenges of engineering the family of Mn-Bi-Te materials to realize QAHE purely through chemical doping. Achieving the desired topological quantum phase requires both a uniform carrier doping and a ferromagnetic ground state. Furthermore, the light-induced polarization within each unit cell of ferromagnetic Mn(Bi$_{0.82}$Sb$_{0.18}$)$_{6}$Te$_{10}$ may open new possibilities for optoelectronic and spintronics.

cond-mat.mes-hall

A Topological Superconductor Tuned by Electronic Correlations

A topological superconductor, characterized by either a chiral order parameter or a chiral topological surface state in proximity to bulk superconductivity, is foundational to topological quantum computing. As in other topological phases of matter, electronic correlations can tune topological superconductivity via modifications of the low-energy Fermiology. Such tuning has not been realized so far. Here we uncover a unique topological superconducting phase in competition with electronic correlations in 10-unit-cell thick FeTe$_{x}$Se$_{1-x}$ films grown on SrTiO$_{3}$ substrates. When the Te content $x$ exceeds $0.7$, we observe a rapid increase of the effective mass for the Fe $d_{xy}$ band, with the emergence of a superconducting topological surface state confirmed by high-resolution angle-resolved photoemission spectroscopy; however, near the FeTe limit, the system enters an incoherent regime where the topological surface state becomes unidentifiable and superconductivity is suppressed. Theory suggests that the electron-electron interactions in the odd-parity $xy^-$ band with a strong $d_{xy}$ character lead to an orbital-selective correlated phase. Our work establishes FeTe$_{x}$Se$_{1-x}$ thin films as a unique platform where electronic correlations sensitively modulate topological superconductivity, suggesting opportunities to use tunable electron-electron interactions to engineer new topological phases in a broad class of materials.

cond-mat.supr-con

Theoretical Insights into Layered Metamaterials with Enhanced Thermal and Mechanical Properties

The inherent trade-off between ultra-low thermal conductivity and high mechanical rigidity in natural materials limits their utility in advanced applications. Inspired by the unique architecture of layered honeycomb structures, this study introduces a new class of metamaterials designed to overcome these constraints. By systematically exploring unit cell configurations and stacking arrangements, we demonstrate that a zigzag internal geometry, analogous to rhombohedral graphene stacking, optimizes thermal insulation while maintaining relatively high mechanical rigidity. Our finite element simulations predict that these layered structures can achieve a thermal conductivity of 12.5 mW/(m.K) using zirconia as the constructing material, theoretically outperforming state-of-the-art ceramic aerogels while maintaining robust mechanical stability. This novel approach paves the way for designing next-generation super-insulating materials with customizable mechanical properties, enabling innovative applications in extreme environments, lightweight aerospace structures, and advanced thermal management systems.

physics.app-ph

A Machine Learning Approach Capturing Hidden Parameters in Autonomous Thin-Film Deposition

The integration of machine learning and robotics into thin film deposition is transforming material discovery and optimization. However, challenges remain in achieving a fully autonomous cycle of deposition, characterization, and decision-making. Additionally, the inherent sensitivity of thin film growth to hidden parameters such as substrate conditions and chamber conditions can compromise the performance of machine learning models. In this work, we demonstrate a fully autonomous physical vapor deposition system that combines in-situ optical spectroscopy, a high-throughput robotic sample handling system, and Gaussian Process Regression models. By employing a calibration layer to account for hidden parameter variations and an active learning algorithm to optimize the exploration of the parameter space, the system fabricates silver thin films with optical reflected power ratios within 2.5% of the target in an average of 2.3 attempts. This approach significantly reduces the time and labor required for thin film deposition, showcasing the potential of machine learning-driven automation in accelerating material development.

cond-mat.mtrl-sci

Distinguishing Surface and Bulk Electromagnetism via Their Dynamics in an Intrinsic Magnetic Topological Insulator

The indirect exchange interaction between local magnetic moments via surface electrons has been long predicted to bolster the surface ferromagnetism in magnetic topological insulators (MTIs), which facilitates the quantum anomalous Hall effect. This unconventional effect is critical to determining the operating temperatures of future topotronic devices. However, the experimental confirmation of this mechanism remains elusive, especially in intrinsic MTIs. Here we combine time-resolved photoemission spectroscopy with time-resolved magneto-optical Kerr effect measurements to elucidate the unique electromagnetism at the surface of an intrinsic MTI MnBi2Te4. Theoretical modeling based on 2D Ruderman-Kittel-Kasuya-Yosida interactions captures the initial quenching of a surface-rooted exchange gap within a factor of two but over-estimates the bulk demagnetization by one order of magnitude. This mechanism directly explains the sizable gap in the quasi-2D electronic state and the nonzero residual magnetization in even-layer MnBi2Te4. Furthermore, it leads to efficient light-induced demagnetization comparable to state-of-the-art magnetophotonic crystals, promising an effective manipulation of magnetism and topological orders for future topotronics.

cond-mat.str-el

When Superconductivity Crosses Over: From BCS to BEC

New developments in superconductivity, particularly through unexpected and often astonishing forms of superconducting materials, continue to excite the community and stimulate theory. It is now becoming clear that there are two distinct platforms for superconductivity: natural and synthetic materials. The study of these artificial materials has greatly expanded in the last decade or so, with the discoveries of new forms of superfluidity in artificial heterostructures and the exploitation of proximitization. Natural superconductors continue to surprise through the Fe-based pnictides and chalcogenides, and nickelates as well as others. It is the goal of this review to present this two-pronged investigation into superconductors, with a focus on those that we have come to understand belong somewhere between the Bardeen-Cooper-Schrieffer (BCS) and Bose-Einstein condensation (BEC) regimes. We characterize in detail the nature of this "crossover" superconductivity, which is to be distinguished from crossover superfluidity in atomic Fermi gases. In the process, we address the multiple ways of promoting a system out of the BCS and into the BCS-BEC crossover regime within the context of concrete experimental realizations. These involve natural materials, such as organic conductors, as well as artificial, mostly two-dimensional materials, such as magic-angle twisted bilayer and trilayer graphene, or gate-controlled devices, as well as one-layer and interfacial superconducting films. This work should be viewed as a celebration of BCS theory by showing that even though this theory was initially implemented with the special case of weak correlations in mind, it can in a very natural way be extended to treat the case of these more exotic strongly correlated superconductors.

cond-mat.supr-con

Preservation of Topological Surface States in Millimeter-Scale Transferred Membranes

Ultrathin topological insulator membranes are building blocks of exotic quantum matter. However, traditional epitaxy of these materials does not facilitate stacking in arbitrary orders, while mechanical exfoliation from bulk crystals is also challenging due to the non-negligible interlayer coupling therein. Here we liberate millimeter-scale films of topological insulator Bi$_2$Se$_3$, grown by molecular beam epitaxy, down to 3 quintuple layers. We characterize the preservation of the topological surface states and quantum well states in transferred Bi$_{2}$Se$_{3}$ films using angle-resolved photoemission spectroscopy. Leveraging the photon-energy-dependent surface sensitivity, the photoemission spectra taken with $6$ eV and $21.2$ eV photons reveal a transfer-induced migration of the topological surface states from the top to the inner layers. By establishing clear electronic structures of the transferred films and unveiling the wavefunction relocation of the topological surface states, our work paves the physics foundation crucial for the future fabrication of artificially stacked topological materials with single-layer precision.

cond-mat.mtrl-sci

Layer-by-layer disentanglement of Bloch states via frequency-domain photoemission

Layer-by-layer material engineering has enabled exotic quantum phenomena such as interfacial superconductivity and the quantum anomalous Hall effect. Meanwhile, deciphering electronic states layer-by-layer remains a fundamental scientific challenge. This is exemplified by the difficulty in understanding the layer origins of topological electronic states in magnetic topological insulators, which is key to understanding and controlling topological quantum phases. Here, we report a layer-encoded frequency-domain ARPES experiment on a magnetic topological insulator (MnBi2Te4)(Bi2Te3) to characterize the layer origins of electronic states. Infrared laser excitations launch coherent lattice vibrations with the layer index encoded by the vibration frequency; photoemission spectroscopy tracks the electron dynamics, where the layer information is decoded in the frequency domain. This layer-frequency correspondence reveals a surprising wavefunction relocation of the topological surface state from the top magnetic layer into the buried second layer, reconciling the controversy over the vanishing broken-symmetry energy gap in (MnBi2Te4)(Bi2Te3) and its related compounds. The layer-frequency correspondence can be harnessed to disentangle electronic states layer-by-layer in a broad class of van der Waals superlattices.

cond-mat.mes-hall

Delicate Ferromagnetism in MnBi$_6$Te$_{10}$

Tailoring magnetic orders in topological insulators is critical to the realization of topological quantum phenomena. An outstanding challenge is to find a material where atomic defects lead to tunable magnetic orders while maintaining a nontrivial topology. Here, by combining magnetization measurements, angle-resolved photoemission spectroscopy, and transmission electron microscopy, we reveal disorder-enabled, tunable magnetic ground states in MnBi$_6$Te$_{10}$. In the ferromagnetic phase, an energy gap of 15 meV is resolved at the Dirac point on the MnBi$_2$Te$_4$ termination. In contrast, antiferromagnetic MnBi$_6$Te$_{10}$ exhibits gapless topological surface states on all terminations. Transmission electron microscopy and magnetization measurements reveal substantial Mn vacancies and Mn migration in ferromagnetic MnBi$_6$Te$_{10}$. We provide a conceptual framework where a cooperative interplay of these defects drives a delicate change of overall magnetic ground state energies, and leads to tunable magnetic topological orders. Our work provides a clear pathway for nanoscale defect-engineering towards the realization of topological quantum phases.

cond-mat.mtrl-sci

An Integrated Quantum Material Testbed with Multi-Resolution Photoemission Spectroscopy

We present the development of a multi-resolution photoemission spectroscopy (MRPES) setup which probes quantum materials in energy, momentum, space, and time. This versatile setup integrates three light sources in one photoemission setup, and can conveniently switch between traditional angle-resolved photoemission spectroscopy (ARPES), time-resolved ARPES (trARPES), and micron-scale spatially resolved ARPES ($μ$ARPES). It provides a first-time all-in-one solution to achieve an energy resolution $< 4$ meV, a time resolution $< 35$ fs, and a spatial resolution $\sim 10$ $μ$m in photoemission spectroscopy. Remarkably, we obtain the shortest time resolution among the trARPES setups using solid-state nonlinear crystals for frequency upconversion. Furthermore, this MRPES setup is integrated with a shadow-mask assisted molecular beam epitaxy system, which transforms the traditional photoemission spectroscopy into a quantum device characterization instrument. We demonstrate the functionalities of this novel quantum material testbed using FeSe/SrTiO$_3$ thin films and MnBi$_4$Te$_7$ magnetic topological insulators.

physics.ins-det

Origins of electronic bands in antiferromagnetic topological insulator MnBi$_2$Te$_4$

Despite the rapid progress in understanding the first intrinsic magnetic topological insulator MnBi$_2$Te$_4$, its electronic structure remains a topic under debates. Here we perform a thorough spectroscopic investigation into the electronic structure of MnBi$_2$Te$_4$ via laser-based angle-resolved photoemission spectroscopy. Through quantitative analysis, we estimate an upper bound of 3 meV for the gap size of the topological surface state. Furthermore, our circular dichroism measurements reveal band chiralities for both the topological surface state and quasi-2D bands, which can be well reproduced in a band hybridization model. A numerical simulation of energy-momentum dispersions based on a four-band model with an additional step potential near the surface provides a promising explanation for the origin of the quasi-2D bands. Our study represents a solid step forward in reconciling the existing controversies in the electronic structure of MnBi$_2$Te$_4$, and provides an important framework to understand the electronic structures of other relevant topological materials MnBi$_{2n}$Te$_{3n+1}$.

cond-mat.mtrl-sci

Interfacial Electron-Phonon Coupling Constants Extracted from Intrinsic Replica Bands in Monolayer FeSe/SrTiO$_3$

The observation of replica bands by angle-resolved photoemission spectroscopy has ignited interest in the study of electron-phonon coupling at low carrier densities, particularly in monolayer FeSe/SrTiO$_3$, where the appearance of replica bands has motivated theoretical work suggesting that the interfacial coupling of electrons in the FeSe layer to optical phonons in the SrTiO$_3$ substrate might contribute to the enhanced superconducting pairing temperature. Alternatively, it has also been recently proposed that such replica bands might instead originate from extrinsic final state losses associated with the photoemission process. Here, we perform a quantitative examination of replica bands in monolayer FeSe/SrTiO$_3$, where we are able to conclusively demonstrate that the replica bands are indeed signatures of intrinsic electron-boson coupling, and not associated with final state effects. A detailed analysis of the energy splittings between the higher-order replicas, as well as other self-energy effects, allow us to determine that the interfacial electron-phonon coupling in the system corresponds to a value of $λ= 0.19 \pm 0.02$.

cond-mat.mtrl-sci

Incoherent Cooper pairing and pseudogap behavior in single-layer FeSe/SrTiO$_3$

In many unconventional superconductors, the presence of a pseudogap - a suppression in the electronic density of states extending above the critical temperature - has been a long-standing mystery. Here, we employ combined \textit{in situ} electrical transport and angle-resolved photoemission spectroscopy (ARPES) measurements to reveal an unprecedentedly large pseudogap regime in single-layer FeSe/SrTiO$_3$, an interfacial superconductor where incoherent Cooper pairs are initially formed above $T_Δ$ $\approx$ 60 K, but where a zero resistance state is only achieved below $T_{0}$ $<$ 30 K. We show that this behavior is accompanied by distinct transport signatures of two-dimensional phase fluctuating superconductivity, suggesting a mixed vortex state hosting incoherent Cooper pairs which persist well above the maximum clean limit $T_{c}$ of $\approx$ 40 K. Our work establishes the critical role of reduced dimensionality in driving the complex interplay between Cooper pairing and phase coherence in two-dimensional high-$T_c$ superconductors, providing a paradigm for understanding and engineering higher-$T_{c}$ interfacial superconductors.

cond-mat.supr-con

The Future of the Correlated Electron Problem

A central problem in modern condensed matter physics is the understanding of materials with strong electron correlations. Despite extensive work, the essential physics of many of these systems is not understood and there is very little ability to make predictions in this class of materials. In this manuscript we share our personal views on the major open problems in the field of correlated electron systems. We discuss some possible routes to make progress in this rich and fascinating field. This manuscript is the result of the vigorous discussions and deliberations that took place at Johns Hopkins University during a three-day workshop January 27, 28, and 29, 2020 that brought together six senior scientists and 46 more junior scientists. Our hope, is that the topics we have presented will provide inspiration for others working in this field and motivation for the idea that significant progress can be made on very hard problems if we focus our collective energies.

cond-mat.str-el

Band resolved imaging of photocurrent in a topological insulator

We study the microscopic origins of photocurrent generation in the topological insulator Bi$_2$Se$_3$ via time- and angle-resolved photoemission spectroscopy. We image the unoccupied band structure as it evolves following a circularly polarized optical excitation and observe an asymmetric electron population in momentum space, which is the spectroscopic signature of a photocurrent. By analyzing the rise times of the population we identify which occupied and unoccupied electronic states are coupled by the optical excitation. We conclude that photocurrents can only be excited via resonant optical transitions coupling to spin-orbital textured states. Our work provides a microscopic understanding of how to control photocurrents in systems with spin-orbit coupling and broken inversion symmetry.

cond-mat.mtrl-sci