arXiv subjects

David Hsieh

Publications and source records attributed to David Hsieh.

17 recordsLinked to original sources

arXiv2025

High-speed antiferromagnetic domain walls driven by coherent spin waves

The ability to rapidly manipulate domain walls (DWs) in magnetic materials is key to developing novel high-speed spintronic memory and computing devices. Antiferromagnetic (AFM) materials present a particularly promising platform due to their robustness against stray fields and their potential for exceptional DW velocities. Among various proposed driving mechanisms, coherent spin waves could potentially propel AFM DWs to the magnon group velocity while minimizing dissipation from Joule heating. However, experimental realization has remained elusive due to the dual challenges of generating coherent AFM spin waves near isolated mobile AFM DWs and simultaneously measuring high-speed DW dynamics. Here we experimentally realize an approach where ultrafast laser pulses generate coherent spin waves that drive AFM DWs and develop a technique to directly map the spatiotemporal DW dynamics. Using the room-temperature AFM insulator Sr$_2$Cu$_3$O$_4$Cl$_2$, we observe AFM DW motion with record-high velocities up to ~50 km/s. Remarkably, the direction of DW propagation is controllable through both the pump laser helicity and the sign of the DW winding number. This bidirectional control can be theoretically explained, and numerically reproduced, by the DW dynamics induced by coherent spin waves of the in-plane magnon mode - a phenomenon unique to magnets with an easy-plane anisotropy. Our work uncovers a novel DW propulsion mechanism that is generalizable to a wide range of AFM materials, unlocking new opportunities for ultrafast coherent AFM spintronics.

cond-mat.mes-hall↗

arXiv2025

Time-hidden magnetic order in a multi-orbital Mott insulator

Photo-excited quantum materials can be driven into thermally inaccessible metastable states that exhibit structural, charge, spin, topological and superconducting orders. Metastable states typically emerge on timescales set by the intrinsic electronic and phononic energy scales, ranging from femtoseconds to picoseconds, and can persist for weeks. Therefore, studies have primarily focused on ultrafast or quasi-static limits, leaving the intermediate time window less explored. Here we reveal a metastable state with broken glide-plane symmetry in photo-doped Ca$_2$RuO$_4$ using time-resolved optical second-harmonic generation and birefringence measurements. We find that the metastable state appears long after intralayer antiferromagnetic order has melted and photo-carriers have recombined. Its properties are distinct from all known states in the equilibrium phase diagram and are consistent with intralayer ferromagnetic order. Furthermore, model Hamiltonian calculations reveal that a non-thermal trajectory to this state can be accessed via photo-doping. Our results expand the search space for out-of-equilibrium electronic matter to metastable states emerging at intermediate timescales.

cond-mat.str-el↗

arXiv2025

Subgap pumping of antiferromagnetic Mott insulators: photoexcitation mechanisms and applications

We study the behavior of the 2D repulsive Hubbard model on a square lattice at half filling, under strong driving with ac electric fields, by employing a time-dependent Gaussian variational approach. Within the same theoretical framework, we analytically obtain the conventional Keldysh crossover between multiphoton and tunneling photoexcitation mechanisms, as well as two new regimes beyond the Keldysh paradigm. We discuss how dynamical renormalization of the Mott-Hubbard gap feeds back into the photoexcitation process, modulating the carrier generation rate in real time. The momentum distribution of quasiparticle excitations immediately after the drive is calculated, and shown to contain valuable information about the generation mechanism. Finally, we discuss experimental probing of the pump-induced nonequilibrium electronic state.

cond-mat.str-el↗

arXiv2025

A Hubbard exciton fluid in a photo-doped antiferromagnetic Mott insulator

The undoped antiferromagnetic Mott insulator naturally has one charge carrier per lattice site. When it is doped with additional carriers, they are unstable to spin fluctuation-mediated Cooper pairing as well as other unconventional types of charge, spin, and orbital current ordering. Photo-excitation can produce charge carriers in the form of empty (holons) and doubly occupied (doublons) sites that may also exhibit charge instabilities. There is evidence that antiferromagnetic correlations enhance attractive interactions between holons and doublons, which can then form bound pairs known as Hubbard excitons, and that these might self-organize into an insulating Hubbard exciton fluid. However, this out-of-equilibrium phenomenon has not been detected experimentally. Here, we report the transient formation of a Hubbard exciton fluid in the antiferromagnetic Mott insulator Sr$_{2}$IrO$_{4}$ using ultrafast terahertz conductivity. Following photo-excitation, we observe rapid spectral weight transfer from a Drude metallic response to an insulating response. The latter is characterized by a finite energy peak originating from intra-excitonic transitions, whose assignment is corroborated by our numerical simulations of an extended Hubbard model. The lifetime of the peak is short, approximately one picosecond, and scales exponentially with Mott gap size, implying extremely strong coupling to magnon modes.

cond-mat.str-el↗

arXiv2025

Observation of excitons bound by antiferromagnetic correlations

Two-dimensional Mott insulators host antiferromagnetic (AFM) correlations that are predicted to enhance the attractive interaction between empty (holons) and doubly occupied (doublons) sites, creating a novel pathway for exciton formation. However, experimental confirmation of this spin-mediated binding mechanism remains elusive. Leveraging the distinct magnetic critical properties of the Mott antiferromagnets Sr$_2$IrO$_4$ and Sr$_3$Ir$_2$O$_7$, we show using time-resolved THz spectroscopy that excitons only exist at temperatures below where short-range AFM correlation develops. The excitons remain stable up to photodoping densities approaching the predicted excitonic Mott insulator-to-metal transition, revealing a unique robustness against screening. Our results establish the viability of spin-bound excitons and introduce opportunities for excitonic control through magnetic degrees of freedom.

cond-mat.str-el↗

arXiv2025

2D van der Waals magnets: from fundamental physics to applications

Magnetism has played a central role in the long and rich history of modern condensed matter physics, with many foundational insights originating from theoretical studies of two-dimensional (2D) spin systems. The discovery of 2D van der Waals (vdW) magnets has revolutionized this area by providing real, atomically thin magnetic systems for experimental investigation. Since the first experimental reports of antiferromagnetic vdW insulators in 2016 - followed by studies on ferromagnetic vdW systems in 2017 - the field has witnessed rapid and expansive growth, with more than two dozen vdW magnetic materials now identified, including both ferro- and antiferromagnets. In this review, we present a comprehensive overview of the major scientific and technological developments in this rapidly evolving field. These include experimental realizations of various 2D spin Hamiltonians as well as unexpected phenomena such as magnetic excitons, Floquet-engineered states, and light-induced metastable magnetic phases. In parallel, 2D vdW magnets have shown significant promise in spintronics and related applications, offering a new platform for engineering quantum functionalities. We organize this review by tracing the historical development of the field, synthesizing key milestones, and highlighting its broader impact across condensed matter physics and materials science. We conclude with an Outlook section that outlines several promising directions for future research, aiming to chart a path forward in this vibrant and still rapidly growing area.

cond-mat.mtrl-sci↗

arXiv2024

Twist-Programmable Superconductivity in Spin-Orbit Coupled Bilayer Graphene

The relative twist angle between layers of near-lattice-matched van der Waals materials is critical for the emergent correlated phenomena associated with moire flat bands. However, the concept of angle rotation control is not exclusive to moir\'e superlattices in which electrons directly experience a twist-angle-dependent periodic potential. Instead, it can also be employed to induce programmable symmetry-breaking perturbations with the goal of stabilizing desired correlated states. Here, we experimentally demonstrate `moireless' twist-tuning of superconductivity together with other correlated orders in Bernal bilayer graphene proximitized by tungsten diselenide. The alignment between the two materials systematically controls the strength of the induced Ising spin-orbit coupling (SOC), profoundly altering the phase diagram. As Ising SOC is increased, superconductivity onsets at a higher displacement field and features a higher critical temperature, reaching up to 0.5K. Within the main superconducting dome and in the strong Ising SOC limit, we find an unusual phase transition characterized by a nematic redistribution of holes among trigonally warped Fermi pockets and enhanced resilience to in-plane magnetic fields. The behavior of the superconducting phase is well captured by our theoretical model, which emphasizes the role of interband interactions between Fermi pockets arising due to interaction-enhanced symmetry breaking. Moreover, we identify two additional superconducting regions, one of which descends from an inter-valley coherent normal state and exhibits a Pauli-limit violation ratio exceeding 40, among the highest for all known superconductors. Our results provide new insights into ultra-clean graphene-based superconductors and underscore the potential of utilizing moireless-twist engineering across a range of van der Waals heterostructures.

cond-mat.supr-con↗

arXiv2022

Keldysh space control of charge dynamics in a strongly driven Mott insulator

The fate of a Mott insulator under strong low frequency optical driving conditions is a fundamental problem in quantum many-body dynamics. Using ultrafast broadband optical spectroscopy, we measured the transient electronic structure and charge dynamics of an off-resonantly pumped Mott insulator Ca$_2$RuO$_4$. We observe coherent bandwidth renormalization and nonlinear doublon-holon pair production occurring in rapid succession within a sub-100 femtosecond pump pulse duration. By sweeping the electric field amplitude, we demonstrate continuous bandwidth tuning and a Keldysh cross-over from a multi-photon absorption to quantum tunneling dominated pair production regime. Our results provide a procedure to control coherent and nonlinear heating processes in Mott insulators, facilitating the discovery of novel out-of-equilibrium phenomena in strongly correlated systems.

cond-mat.str-el↗

arXiv2020

Controlling ligand-mediated exchange interactions in periodically driven magnetic materials

A periodic drive could alter the effective exchange interactions in magnetic materials. Here, we explore how exchange pathways affect the effective interactions of periodically driven magnetic materials. Aiming to apply Floquet engineering methods to two-dimensional magnetic materials, we consider realistic models and discuss the effect of a periodic drive on ligand-mediated exchange interactions. We show that depending on bond angles and the number of ligand ions involved in the exchange process, drive-induced changes can be very different from those calculated from direct-hopping models considered earlier. We study these effects and find that the presence of ligand ions must be taken into account, especially for TMTCs where ligand ion mediated next-neighbor interactions play a crucial role in determining the magnetic ground state of the system.

cond-mat.str-el↗

arXiv2019

Orbital Floquet Engineering of Exchange Interactions in Magnetic Materials

We present a new scheme to control the spin exchange interactions between two magnetic ions by manipulating the orbital degrees of freedom using a periodic drive. We discuss two different protocols for orbital Floquet engineering. In one case, we modify the properties of the ligand orbitals which mediate magnetic interactions between two transition metal ions. While in the other case, we mix the d orbitals on each magnetic ion. In contrast to previous works on Floquet engineering of magnetic properties, the present scheme makes use of the AC Stark shift of the states involved in the exchange process.

cond-mat.str-el↗

arXiv2017

Doping driven structural distortion in the bilayer iridate (Sr$_{1-x}$La$_x$)$_3$Ir$_2$O$_7$

Neutron single crystal diffraction and rotational anisotropy optical second harmonic generation data are presented resolving the nature of the structural distortion realized in electron-doped (Sr$_{1-x}$La$_x$)$_3$Ir$_2$O$_7$ with $x=0.035$ and $x=0.071$. Once electrons are introduced into the bilayer spin-orbit assisted Mott insulator Sr$_3$Ir$_2$O$_7$, previous studies have identified the appearance of a low temperature structural distortion and have suggested the presence of a competing electronic instability in the phase diagram of this material. Our measurements resolve a lowering of the structural symmetry from monoclinic $C2/c$ to monoclinic $P2_1/c$ and the creation of two unique Ir sites within the chemical unit cell as the lattice distorts below a critical temperature $T_S$. Details regarding the modifications to oxygen octahedral rotations and tilting through the transition are discussed as well as the evolution of the low temperature distorted lattice as a function of carrier substitution.

cond-mat.str-el↗

arXiv2016

Structural investigation of the bilayer iridate Sr3Ir2O7

A complete structural solution of the bilayer iridate compound Sr3Ir2O7 presently remains outstanding. Previously reported structures for this compound vary and all fail to explain weak structural violations observed in neutron scattering measurements as well as the presence of a net ferromagnetic moment in the basal plane. In this paper, we present single crystal neutron diffraction and rotational anisotropy second harmonic generation measurements unveiling a lower, monoclinic symmetry inherent to Sr3Ir2O7 . Combined with density functional theory, our measurements identify the correct structural space group as No. 15 (C2/c) and provide clarity regarding the local symmetry of Ir 4+ cations within this spin-orbit Mott material.

cond-mat.str-el↗

arXiv2014

Experimental Discovery of Topological Surface States - A New Type of 2D Electron Systems (Review Article)

Topological Surface States (TSS) represent new types of two dimensional electron systems with novel and unprecedented properties distinct from any quantum Hall-like or spin-Hall effects. Their Z$_2$ topological order can be realized at room temperatures without magnetic fields and they can be turned into magnets, exotic superconductors or Kondo insulators leading to worldwide interest and activity in the topic. We review the basic concepts defining such topological matter and the experimental discovery via the key experimental probe that revealed the Z$_2$ topological order in the bulk of these spin-orbit interaction dominated insulators for the first time. This review focuses on the key results that demonstrated the fundamental Z$_2$ topological properties such as spin-momentum locking, non-trivial Berry's phases, mirror Chern number, absence of backscattering, bulk-boundary correspondence (topology), protection by time-reversal and other discrete (mirror) symmetries and their remarkable persistence up to the room temperature elaborating on results first briefly discussed in an early review by M.Z. Hasan and C.L. Kane [Rev. of Mod. Phys., 82, 3045 (2010)]. Additionally, key results on broken symmetry phases such as quantum magnetism and superconductivity induced in topological materials are briefly discussed. Topological insulators beyond the Z$_2$ classification such as Topological Crystalline Insulators (TCI) are discussed based on their spin properties (mirror Chern invariants). The experimental methodologies detailed here have been used in most of the subsequent studies of Z$_2$ topological physics in almost all bulk topological insulator materials to this date.

cond-mat.mes-hall↗

arXiv2011

A topological insulator surface under strong Coulomb, magnetic and disorder perturbations

Three dimensional topological insulators embody a newly discovered state of matter characterized by conducting spin-momentum locked surface states that span the bulk band gap as demonstrated via spin-resolved ARPES measurements . This highly unusual surface environment provides a rich ground for the discovery of novel physical phenomena. Here we present the first controlled study of the topological insulator surfaces under strong Coulomb, magnetic and disorder perturbations. We have used interaction of iron, with a large Coulomb state and significant magnetic moment as a probe to \textit{systematically test the robustness} of the topological surface states of the model topological insulator Bi$_2$Se$_3$. We observe that strong perturbation leads to the creation of odd multiples of Dirac fermions and that magnetic interactions break time reversal symmetry in the presence of band hybridization. We also present a theoretical model to account for the altered surface of Bi$_2$Se$_3$. Taken collectively, these results are a critical guide in manipulating topological surfaces for probing fundamental physics or developing device applications.

cond-mat.mes-hall↗

arXiv2011

Nonequilibrium Quasiparticle Relaxation Dynamics in Single Crystals of Hole and Electron doped BaFe$_2$As$_2$

We report on the nonequilibrium quasiparticle dynamics in BaFe$_2$As$_2$ on both the hole doped (Ba$_{1-x}$K$_x$Fe$_2$As$_2$) and electron doped (BaFe$_{2-y}$Co$_y$As$_2$) sides of the phase diagram using ultrafast pump-probe spectroscopy. Below $T_c$, measurements conducted at low photoinjected quasiparticle densities in the optimally and overdoped Ba$_{1-x}$K$_x$Fe$_2$As$_2$ samples reveal two distinct relaxation processes: a fast component whose decay rate increases linearly with excitation density and a slow component with an excitation density independent decay rate. We argue that these two processes reflect the recombination of quasiparticles in the two hole bands through intraband and interband processes. We also find that the thermal recombination rate of quasiparticles increases quadratically with temperature in these samples. The temperature and excitation density dependence of the decays indicates fully gapped hole bands and nodal or very anisotropic electron bands. At higher excitation densities and lower hole dopings, the dependence of the dynamics on quasiparticle density disappears as the data are more readily understood in terms of a model which accounts for the quasiequilibrium temperature attained by the sample. In the BaFe$_{2-y}$Co$_y$As$_2$ samples, dependence of the recombination rate on quasiparticle density at low dopings (i.e., $y=0.12$) is suppressed upon submergence of the inner hole band and quasiparticle relaxation occurs in a slow, density independent manner.

cond-mat.supr-con↗

arXiv2011

Electron dynamics in topological insulator based semiconductor-metal interfaces (topological p-n interface based on Bi2Se3 class)

Single-Dirac-cone topological insulators (TI) are the first experimentally discovered class of three dimensional topologically ordered electronic systems, and feature robust, massless spin-helical conducting surface states that appear at any interface between a topological insulator and normal matter that lacks the topological insulator ordering. This topologically defined surface environment has been theoretically identified as a promising platform for observing a wide range of new physical phenomena, and possesses ideal properties for advanced electronics such as spin-polarized conductivity and suppressed scattering. A key missing step in enabling these applications is to understand how topologically ordered electrons respond to the interfaces and surface structures that constitute a device. Here we explore this question by using the surface deposition of cathode (Cu/In/Fe) and anode materials (NO$_2$) and control of bulk doping in Bi$_2$Se$_3$ from P-type to N-type charge transport regimes to generate a range of topological insulator interface scenarios that are fundamental to device development. The interplay of conventional semiconductor junction physics and three dimensional topological electronic order is observed to generate novel junction behaviors that go beyond the doped-insulator paradigm of conventional semiconductor devices and greatly alter the known spin-orbit interface phenomenon of Rashba splitting. Our measurements for the first time reveal new classes of diode-like configurations that can create a gap in the interface electron density near a topological Dirac point and systematically modify the topological surface state Dirac velocity, allowing far reaching control of spin-textured helical Dirac electrons inside the interface and creating advantages for TI superconductors as a Majorana fermion platform over spin-orbit semiconductors.

cond-mat.mes-hall↗

arXiv2011

A new experimental approach for the exploration of topological quantum phenomena : Topological Insulators and Superconductors

The three-dimensional topological insulator (originally called "topological insulators") is the first example in nature of a topologically ordered electronic phase existing in three dimensions that cannot be reduced to multiple copies of quantum-Hall-like states. Their topological order can be realized at room temperatures without magnetic fields and they can be turned into magnets and exotic superconductors leading to world-wide interest and activity in topological insulators. One of the major challenges in going from quantum Hall-like 2D states to 3D topological insulators is to develop new experimental approaches/methods to precisely probe this novel form of topological-order since the standard tools and settings that work for IQH-state also work for QSH states. The method to probe 2D topological-order is exclusively with charge transport, which either measures quantized transverse conductance plateaus in IQH systems or longitudinal conductance in quantum spin Hall (QSH) systems. In a 3D topological insulator, the boundary itself supports a two dimensional electron gas (2DEG) and transport is not (Z$_2$) topologically quantized. In this paper, we review the birth of momentum- and spin-resolved spectroscopy as a new experimental approach and as a directly boundary sensitive method to study and prove topological-order in three-dimensions via the direct measurements of the topological invariants {$ν_o$} that are associated with the Z$_2$ topology of the spin-orbit band structure and opposite parity band inversions, which led to the experimental discovery of the first 3D topological insulators. We also discuss how spectroscopic methods are leading to the identification of spin-orbit superconductors that may work as Majorana platforms and can be used to identify topological superconductors - yet another class of new state of matter.

cond-mat.mes-hall↗