Showing 1–50 of 83 results for author: Hsieh, D

High-speed antiferromagnetic domain walls driven by coherent spin waves

Authors: Kyle L. Seyler, Hantao Zhang, Daniel Van Beveren, Costel R. Rotundu, Young S. Lee, Ran Cheng, David Hsieh

Abstract: 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 poten… ▽ More 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. △ Less

Submitted 10 November, 2025; originally announced November 2025.

Comments: 10 pages main text, 4 figures, 8 pages supplementary information

Journal ref: Nature Communications 16, 9836 (2025)

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

Authors: Xinwei Li, Iliya Esin, Youngjoon Han, Yincheng Liu, Hengdi Zhao, Honglie Ning, Cora Barrett, Jun-Yi Shan, Kyle Seyler, Gang Cao, Gil Refael, David Hsieh

Abstract: 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 ultraf… ▽ More 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. △ Less

Submitted 22 July, 2025; originally announced July 2025.

Comments: 9 pages main text, 4 figures, 21 pages supplementary information

Journal ref: Nature Physics 21, 451-457 (2025)

Subgap pumping of antiferromagnetic Mott insulators: photoexcitation mechanisms and applications

Authors: Radu Andrei, Mingyao Guo, Mustafa Ali, Hoon Kim, Richard D. Averitt, David Hsieh, Eugene Demler

Abstract: 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 Kel… ▽ More 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. △ Less

Submitted 21 May, 2025; originally announced May 2025.

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

Authors: Omar Mehio, Xinwei Li, Honglie Ning, Zala Lenarčič, Yuchen Han, Michael Buchhold, Zach Porter, Nicholas J. Laurita, Stephen D. Wilson, David Hsieh

Abstract: 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 th… ▽ More 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. △ Less

Submitted 8 May, 2025; originally announced May 2025.

Comments: 23 pages main text, 4 figures, 4 extended figures, 19 pages supplementary information

Journal ref: Nature Physics 19, 1876-1882 (2023)

Observation of excitons bound by antiferromagnetic correlations

Authors: Omar Mehio, Yuchen Han, Xinwei Li, Honglie Ning, Zach Porter, Stephen D. Wilson, David Hsieh

Abstract: 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 ant… ▽ More 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. △ Less

Submitted 8 May, 2025; originally announced May 2025.

Comments: 14 pages main text, 4 figures, 16 pages supplementary information

Journal ref: Phys. Rev. Research 7, 013114 (2025)

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

Authors: Je-Geun Park, Kaixuan Zhang, Hyeonsik Cheong, Jae Hoon Kim, Carina Belvin, David Hsieh, Honglie Ning, Nuh Gedik

Abstract: 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 re… ▽ More 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. △ Less

Submitted 5 May, 2025; originally announced May 2025.

Comments: 83 pages, 33 figures, Submitted to Review of Modern Physics

Twist-Programmable Superconductivity in Spin-Orbit Coupled Bilayer Graphene

Authors: Yiran Zhang, Gal Shavit, Huiyang Ma, Youngjoon Han, Kenji Watanabe, Takashi Taniguchi, David Hsieh, Cyprian Lewandowski, Felix von Oppen, Yuval Oreg, Stevan Nadj-Perge

Abstract: 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 moiré superlattices in which electrons directly experience a twist-angle-dependent periodic potential. Instead, it can also be employed to induce programmable sy… ▽ More 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 moiré 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. △ Less

Submitted 19 August, 2024; originally announced August 2024.

Comments: main text with four figures, extended data and supplementary information

Dynamic magnetic phase transition induced by parametric magnon pumping

Authors: Jun-Yi Shan, Jonathan B. Curtis, Mingyao Guo, Chang Jae Roh, C. R. Rotundu, Young S. Lee, Prineha Narang, Tae Won Noh, Eugene Demler, D. Hsieh

Abstract: Uncovering pathways to optically drive magnetic order-disorder transitions on ultrashort timescales can lead to the realization of novel out-of-equilibrium quantum phenomena. A long-sought pathway is to directly excite a highly non-thermal energy-momentum distribution of magnons, bypassing both charge and lattice degrees of freedom. However, this remains elusive owing to the weak coupling and larg… ▽ More Uncovering pathways to optically drive magnetic order-disorder transitions on ultrashort timescales can lead to the realization of novel out-of-equilibrium quantum phenomena. A long-sought pathway is to directly excite a highly non-thermal energy-momentum distribution of magnons, bypassing both charge and lattice degrees of freedom. However, this remains elusive owing to the weak coupling and large momentum mismatch between photons and magnons. Here we demonstrate strong parametric excitation of magnons across the entire Brillouin zone of the antiferromagnetic insulator Sr$_2$Cu$_3$O$_4$Cl$_2$ by periodically modulating the superexchange interaction with the electric field of light. The excitation efficiency is greatly enhanced by tuning to the van Hove singularity in the magnon spectrum, sufficient to transiently collapse the antiferromagnetic state using a pulsed laser field of 10$^9$ V/m. The order parameter recovery timescale increases by over 1000 times as a function of excitation density, reflecting a crossover from high- to low-energy magnon dominated decay dynamics. This electric-field induced parametric magnon pumping mechanism is applicable to a broad range of magnetic insulators and opens up the possibility of dynamically engineering magnon distributions by design. △ Less

Submitted 17 April, 2024; v1 submitted 14 February, 2024; originally announced February 2024.

Comments: The submitter did not obtain approval from all authors to post this paper. Jun-Yi Shan does not approve of posting this paper

A coherent phonon-induced hidden quadrupolar ordered state in Ca$_2$RuO$_4$

Authors: H. Ning, O. Mehio, X. Li, M. Buchhold, M. Driesse, H. Zhao, G. Cao, D. Hsieh

Abstract: Ultrafast laser excitation provides a means to transiently realize long-range ordered electronic states of matter that are hidden in thermal equilibrium. Recently, this approach has unveiled a variety of thermally inaccessible ordered states in strongly correlated materials, including charge density wave, ferroelectric, magnetic, and intertwined charge-orbital ordered states. However, more exotic… ▽ More Ultrafast laser excitation provides a means to transiently realize long-range ordered electronic states of matter that are hidden in thermal equilibrium. Recently, this approach has unveiled a variety of thermally inaccessible ordered states in strongly correlated materials, including charge density wave, ferroelectric, magnetic, and intertwined charge-orbital ordered states. However, more exotic hidden states exhibiting higher multipolar ordering remain elusive owing to the challenge of directly manipulating and detecting them with light. Here we demonstrate a method to induce a dynamical transition from a thermally allowed to a thermally forbidden spin-orbit entangled quadrupolar ordered state in Ca$_2$RuO$_4$ by coherently exciting a phonon that is strongly coupled to the order parameter. Combining probe photon energy-resolved coherent phonon spectroscopy measurements with model Hamiltonian calculations, we show that the dynamical transition is manifested through anomalies in the temperature, pump excitation fluence, and probe photon energy dependence of the strongly coupled phonon. With this procedure, we introduce a general pathway to uncover hidden multipolar ordered states and to control their re-orientation on ultrashort timescales. △ Less

Submitted 14 December, 2023; originally announced December 2023.

Comments: 8 pages, 4 figures

Journal ref: Nature Communications 14, 8258 (2023)

Nonlinear and nonreciprocal transport effects in untwinned thin films of ferromagnetic Weyl metal SrRuO$_3$

Authors: Uddipta Kar, Elisha Cho-Hao Lu, Akhilesh Kr. Singh, P. V. Sreenivasa Reddy, Youngjoon Han, Xinwei Li, Cheng-Tung Cheng, Song Yang, Chun-Yen Lin, I-Chun Cheng, Chia-Hung Hsu, D. Hsieh, Wei-Cheng Lee, Guang-Yu Guo, Wei-Li Lee

Abstract: The identification of distinct charge transport features, deriving from nontrivial bulk band and surface states, has been a challenging subject in the field of topological systems. In topological Dirac and Weyl semimetals, nontrivial conical bands with Fermi-arc surface states give rise to negative longitudinal magnetoresistance due to chiral anomaly effect and unusual thickness dependent quantum… ▽ More The identification of distinct charge transport features, deriving from nontrivial bulk band and surface states, has been a challenging subject in the field of topological systems. In topological Dirac and Weyl semimetals, nontrivial conical bands with Fermi-arc surface states give rise to negative longitudinal magnetoresistance due to chiral anomaly effect and unusual thickness dependent quantum oscillation from Weyl-orbit effect, which were demonstrated recently in experiments. In this work, we report the experimental observations of large nonlinear and nonreciprocal transport effects for both longitudinal and transverse channels in an untwinned Weyl metal of SrRuO$_3$ thin film grown on a SrTiO$_{3}$ substrate. From rigorous measurements with bias current applied along various directions with respect to the crystalline principal axes, the magnitude of nonlinear Hall signals from the transverse channel exhibits a simple sin$α$ dependence at low temperatures, where $α$ is the angle between bias current direction and orthorhombic [001]$_{\rm o}$, reaching a maximum when current is along orthorhombic [1-10]$_{\rm o}$. On the contrary, the magnitude of nonlinear and nonreciprocal signals in the longitudinal channel attains a maximum for bias current along [001]$_{\rm o}$, and it vanishes for bias current along [1-10]$_{\rm o}$. The observed $α$-dependent nonlinear and nonreciprocal signals in longitudinal and transverse channels reveal a magnetic Weyl phase with an effective Berry curvature dipole along [1-10]$_{\rm o}$ from surface states, accompanied by 1D chiral edge modes along [001]$_{\rm o}$. △ Less

Submitted 18 March, 2024; v1 submitted 10 July, 2023; originally announced July 2023.

Comments: 27 pages, 6 figures

Journal ref: Phys. Rev. X 14, 011022 (2024)

A light-induced Weyl semiconductor-to-metal transition mediated by Peierls instability

Authors: H. Ning, O. Mehio, C. Lian, X. Li, E. Zoghlin, P. Zhou, B. Cheng, S. D. Wilson, B. M. Wong, D. Hsieh

Abstract: Elemental tellurium is a strongly spin-orbit coupled Peierls-distorted semiconductor whose band structure features topologically protected Weyl nodes. Using time-dependent density functional theory calculations, we show that impulsive optical excitation can be used to transiently control the amplitude of the Peierls distortion, realizing a mechanism to switch tellurium between three states: Weyl s… ▽ More Elemental tellurium is a strongly spin-orbit coupled Peierls-distorted semiconductor whose band structure features topologically protected Weyl nodes. Using time-dependent density functional theory calculations, we show that impulsive optical excitation can be used to transiently control the amplitude of the Peierls distortion, realizing a mechanism to switch tellurium between three states: Weyl semiconductor, Weyl metal and non-Weyl metal. Further, we present experimental evidence of this inverse-Peierls distortion using time-resolved optical second harmonic generation measurements. These results provide a pathway to multifunctional ultrafast Weyl devices and introduce Peierls systems as viable hosts of light-induced topological transitions. △ Less

Submitted 2 November, 2022; originally announced November 2022.

Comments: 7 pages main text, 4 figures, 11 pages supplementary information

Journal ref: Phys. Rev. B 106, 205118 (2022)

Direct visualization and control of antiferromagnetic domains and spin reorientation in a parent cuprate

Authors: K. L. Seyler, A. Ron, D. Van Beveren, C. R. Rotundu, Y. S. Lee, D. Hsieh

Abstract: We report magnetic optical second-harmonic generation (SHG) polarimetry and imaging on Sr$_2$Cu$_3$O$_4$Cl$_2$, which allows direct visualization of the mesoscopic antiferromagnetic (AFM) structure of a parent cuprate. Temperature- and magnetic-field-dependent SHG reveals large domains with 90$^{\circ}$ relative orientations that are stabilized by a combination of uniaxial magnetic anisotropy and… ▽ More We report magnetic optical second-harmonic generation (SHG) polarimetry and imaging on Sr$_2$Cu$_3$O$_4$Cl$_2$, which allows direct visualization of the mesoscopic antiferromagnetic (AFM) structure of a parent cuprate. Temperature- and magnetic-field-dependent SHG reveals large domains with 90$^{\circ}$ relative orientations that are stabilized by a combination of uniaxial magnetic anisotropy and the Earth's magnetic field. Below a temperature $T_R$ $\sim$ 97 K, we observe an unusual 90$^{\circ}$ spin reorientation transition, possibly driven by competing magnetic anisotropies of the two copper sublattices, which swaps the AFM domain states while preserving the domain structure. This allows deterministic switching of the AFM states by thermal or laser heating. Near $T_R$, the domain walls become exceptionally responsive to an applied magnetic field, with the Earth's field sufficient to completely expel them from the crystal. Our findings unlock opportunities to study the mesoscopic AFM behavior of parent cuprates and explore their potential for AFM technologies. △ Less

Submitted 9 October, 2022; originally announced October 2022.

Comments: 7 pages main text, 4 figures, 13 pages supplementary information

Journal ref: Phys. Rev. B 106, L140403 (2022)

High-pressure control of optical nonlinearity in the polar Weyl semimetal TaAs

Authors: Chen Li, Xiang Li, T. Deshpande, Xinwei Li, N. Nair, J. G. Analytis, D. M. Silevitch, T. F. Rosenbaum, D. Hsieh

Abstract: The transition metal monopnictide family of Weyl semimetals recently has been shown to exhibit anomalously strong second-order optical nonlinearity, which is theoretically attributed to a highly asymmetric polarization distribution induced by their polar structure. We experimentally test this hypothesis by measuring optical second harmonic generation (SHG) from TaAs across a pressure-tuned polar-t… ▽ More The transition metal monopnictide family of Weyl semimetals recently has been shown to exhibit anomalously strong second-order optical nonlinearity, which is theoretically attributed to a highly asymmetric polarization distribution induced by their polar structure. We experimentally test this hypothesis by measuring optical second harmonic generation (SHG) from TaAs across a pressure-tuned polar-to-nonpolar structural phase transition. Despite the high-pressure structure remaining noncentrosymmetric, the SHG yield is reduced by more than 60 % by 20 GPa as compared to the ambient pressure value. By examining the pressure dependence of distinct groups of SHG susceptibility tensor elements, we find that the yield is primarily controlled by a single element that governs the response along the polar axis. Our results confirm a connection between the polar axis and the giant optical nonlinearity of Weyl semimetals and demonstrate pressure as a means to tune this effect $in$ $situ$. △ Less

Submitted 20 July, 2022; originally announced July 2022.

Comments: 5 pages main text, 4 figures, 2 pages supplementary information

Journal ref: Phys. Rev. B 106, 014101 (2022)

Giant modulation of optical nonlinearity by Floquet engineering

Authors: Jun-Yi Shan, M. Ye, Sungmin Lee, Je-Geun Park, L. Balents, D. Hsieh

Abstract: Strong periodic driving with light offers the potential to coherently manipulate the properties of quantum materials on ultrafast timescales. Recently, strategies have emerged to drastically alter electronic and magnetic properties by optically inducing non-trivial band topologies, emergent spin interactions and even superconductivity. However, the prospects and methods of coherently engineering o… ▽ More Strong periodic driving with light offers the potential to coherently manipulate the properties of quantum materials on ultrafast timescales. Recently, strategies have emerged to drastically alter electronic and magnetic properties by optically inducing non-trivial band topologies, emergent spin interactions and even superconductivity. However, the prospects and methods of coherently engineering optical properties on demand are far less understood. Here we demonstrate coherent control and giant modulation of optical nonlinearity in a van der Waals layered magnetic insulator, manganese phosphorus trisulfide (MnPS$_3$). By driving far off-resonance from the lowest on-site manganese $d$-$d$ transition, we observe a coherent on-off switching of its optical second harmonic generation efficiency on the timescale of 100 femtoseconds with no measurable dissipation. At driving electric fields of the order of 10$^9$ volts per metre, the on-off ratio exceeds 10, which is limited only by the sample damage threshold. Floquet theory calculations based on a single-ion model of MnPS$_3$ are able to reproduce the measured driving field amplitude and polarization dependence of the effect. Our approach can be applied to a broad range of insulating materials and could lead to dynamically designed nonlinear optical elements. △ Less

Submitted 16 June, 2022; originally announced June 2022.

Comments: 5 pages main text, 4 figures, 22 pages supplementary information

Journal ref: Nature 600, 235-239 (2021)

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

Authors: Xinwei Li, Honglie Ning, Omar Mehio, Hengdi Zhao, Min-Cheol Lee, Kyungwan Kim, Fumihiko Nakamura, Yoshiteru Maeno, Gang Cao, David Hsieh

Abstract: 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 productio… ▽ More 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. △ Less

Submitted 10 May, 2022; originally announced May 2022.

Comments: 6 pages main text, 4 figures, 16 pages supplementary information

Journal ref: Phys. Rev. Lett. 128, 187402 (2022)

Decoupling of static and dynamic criticality in a driven Mott insulator

Authors: A. de la Torre, K. L. Seyler, M. Buchhold, Y. Baum, G. Zhang, N. J. Laurita, J. W. Harter, L. Zhao, I. Phinney, X. Chen, S. D. Wilson, G. Cao, R. D. Averitt, G. Refael, D. Hsieh

Abstract: Dynamically driven interacting quantum many-body systems have the potential to exhibit properties that defy the laws of equilibrium statistical mechanics. A widely studied model is the impulsively driven antiferromagnetic Mott insulator, which is predicted to realize exotic transient phenomena including dynamical phase transitions into thermally forbidden states and highly non-thermal magnon distr… ▽ More Dynamically driven interacting quantum many-body systems have the potential to exhibit properties that defy the laws of equilibrium statistical mechanics. A widely studied model is the impulsively driven antiferromagnetic Mott insulator, which is predicted to realize exotic transient phenomena including dynamical phase transitions into thermally forbidden states and highly non-thermal magnon distributions. However such far-from-equilibrium regimes, where conventional time-dependent Ginzburg-Landau descriptions fail, are experimentally challenging to prepare and to probe especially in solid state systems. Here we use a combination of time-resolved second harmonic optical polarimetry and coherent magnon spectroscopy to interrogate $n$-type photo-doping induced ultrafast magnetic order parameter dynamics in the Mott insulator Sr$_2$IrO$_4$. We uncover an unusual far-from-equilibrium critical regime in which the divergences of the magnetic correlation length and relaxation time are decoupled. This violation of conventional thermal critical behavior arises from the interplay of photo-doping and non-thermal magnon population induced demagnetization effects. Our findings, embodied in a non-equilibrium "phase diagram", provide a blueprint for engineering the out-of-equilibrium properties of quantum matter, with potential applications to terahertz spintronics technologies. △ Less

Submitted 15 December, 2021; originally announced December 2021.

Comments: 7 pages main text, 4 figures, 19 pages supplementary information

Journal ref: Commun. Phys. 5, 35 (2022)

Magnetic order, disorder, and excitations under pressure in the Mott insulator Sr$_2$IrO$_4$

Authors: Xiang Li, S. E. Cooper, A. Krishnadas, A. de la Torre, R. S. Perry, F. Baumberger, D. M. Silevitch, D. Hsieh, T. F. Rosenbaum, Yejun Feng

Abstract: Protected by the interplay of on-site Coulomb interactions and spin-orbit coupling, Sr$_2$IrO$_4$ at high pressure is a rare example of a Mott insulator with a paramagnetic ground state. Here, using optical Raman scattering, we measure both the phonon and magnon evolution in Sr$_2$IrO$_4$ under pressure, and identify three different magnetically-ordered phases, culminating in a spin-disordered sta… ▽ More Protected by the interplay of on-site Coulomb interactions and spin-orbit coupling, Sr$_2$IrO$_4$ at high pressure is a rare example of a Mott insulator with a paramagnetic ground state. Here, using optical Raman scattering, we measure both the phonon and magnon evolution in Sr$_2$IrO$_4$ under pressure, and identify three different magnetically-ordered phases, culminating in a spin-disordered state beyond 18 GPa. A strong first-order structural phase transition drives the magnetic evolution at $\sim$10 GPa with reduced structural anisotropy in the IrO$_6$ cages, leading to increasingly isotropic exchange interactions between the Heisenberg spins and a spin-flip transition to $c$-axis-aligned antiferromagnetic order. In the disordered phase of Heisenberg $J_\mathrm{eff}=1/2$ pseudospins, the spin excitations are quasi-elastic and continuous to 10 meV, potentially hosting a gapless quantum spin liquid in Sr$_2$IrO$_4$. △ Less

Submitted 22 October, 2021; originally announced October 2021.

Journal ref: Physical Review B 114, L201111 (2021)

Implications of second harmonic generation for hidden order in Sr$_2$CuO$_2$Cl$_2$

Authors: A. de la Torre, S. Di Matteo, D. Hsieh, M. R. Norman

Abstract: Sr$_2$CuO$_2$Cl$_2$ (SCOC) is a model undoped cuprate with $I4/mmm$ crystallographic symmetry, and a simple magnetic space group $C_Amca$ with associated magnetic point group $mmm1'$. However, recent second harmonic spectroscopy in the antiferromagnetic phase has challenged this picture, suggesting instead a magnetic point group $4/mm'm'$ that co-exists with the antiferromagnetism and breaks the t… ▽ More Sr$_2$CuO$_2$Cl$_2$ (SCOC) is a model undoped cuprate with $I4/mmm$ crystallographic symmetry, and a simple magnetic space group $C_Amca$ with associated magnetic point group $mmm1'$. However, recent second harmonic spectroscopy in the antiferromagnetic phase has challenged this picture, suggesting instead a magnetic point group $4/mm'm'$ that co-exists with the antiferromagnetism and breaks the two orthogonal mirror planes containing the tetragonal $c$-axis. Here, we analyze the symmetry of SCOC in light of the second harmonic results, and discuss possible ground states that are consistent with the data. △ Less

Submitted 12 March, 2021; originally announced March 2021.

Journal ref: Phys. Rev. B 104, 035138 (2021)

Signatures of ultrafast reversal of excitonic order in Ta$_2$NiSe$_5$

Authors: H. Ning, O. Mehio, M. Buchhold, T. Kurumaji, G. Refael, J. G. Checkelsky, D. Hsieh

Abstract: In the presence of electron-phonon coupling, an excitonic insulator harbors two degenerate ground states described by an Ising-type order parameter. Starting from a microscopic Hamiltonian, we derive the equations of motion for the Ising order parameter in the phonon coupled excitonic insulator Ta$_2$NiSe$_5$ and show that it can be controllably reversed on ultrashort timescales using appropriate… ▽ More In the presence of electron-phonon coupling, an excitonic insulator harbors two degenerate ground states described by an Ising-type order parameter. Starting from a microscopic Hamiltonian, we derive the equations of motion for the Ising order parameter in the phonon coupled excitonic insulator Ta$_2$NiSe$_5$ and show that it can be controllably reversed on ultrashort timescales using appropriate laser pulse sequences. Using a combination of theory and time-resolved optical reflectivity measurements, we report evidence of such order parameter reversal in Ta$_2$NiSe$_5$ based on the anomalous behavior of its coherently excited order-parameter-coupled phonons. Our work expands the field of ultrafast order parameter control beyond spin and charge ordered materials. △ Less

Submitted 23 December, 2020; originally announced December 2020.

Comments: 6 pages main text, 4 figures, 8 pages supplementary information

Journal ref: Phys. Rev. Lett. 125, 267602 (2020)

Spin-orbit-enhanced magnetic surface second-harmonic generation in Sr$_2$IrO$_4$

Authors: K. L. Seyler, A. de la Torre, Z. Porter, E. Zoghlin, R. Polski, M. Nguyen, S. Nadj-Perge, S. D. Wilson, D. Hsieh

Abstract: An anomalous optical second-harmonic generation (SHG) signal was previously reported in Sr$_2$IrO$_4$ and attributed to a hidden odd-parity bulk magnetic state. Here we investigate the origin of this SHG signal using a combination of bulk magnetic susceptibility, magnetic-field-dependent SHG rotational anisotropy, and overlapping wide-field SHG imaging and atomic force microscopy measurements. We… ▽ More An anomalous optical second-harmonic generation (SHG) signal was previously reported in Sr$_2$IrO$_4$ and attributed to a hidden odd-parity bulk magnetic state. Here we investigate the origin of this SHG signal using a combination of bulk magnetic susceptibility, magnetic-field-dependent SHG rotational anisotropy, and overlapping wide-field SHG imaging and atomic force microscopy measurements. We find that the anomalous SHG signal exhibits a two-fold rotational symmetry as a function of in-plane magnetic field orientation that is associated with a crystallographic distortion. We also show a change in SHG signal across step edges that tracks the bulk antiferromagnetic stacking pattern. While we do not rule out the existence of hidden order in Sr$_2$IrO$_4$, our results altogether show that the anomalous SHG signal in parent Sr$_2$IrO$_4$ originates instead from a surface-magnetization-induced electric-dipole process that is enhanced by strong spin-orbit coupling. △ Less

Submitted 23 November, 2020; originally announced November 2020.

Comments: 6 pages main text, 4 figures, 12 pages supplementary information

Journal ref: Phys. Rev. B 102, 201113(R) (2020)

Controlling ligand-mediated exchange interactions in periodically driven magnetic materials

Authors: Swati Chaudhary, Alon Ron, David Hsieh, Gil Refael

Abstract: 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.… ▽ More 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. △ Less

Submitted 2 September, 2020; originally announced September 2020.

Anomalous mirror symmetry breaking in a model insulating cuprate Sr$_2$CuO$_2$Cl$_2$

Authors: A. de la Torre, K. L. Seyler, L. Zhao, S. Di Matteo, M. S. Scheurer, Y. Li, B. Yu, M. Greven, S. Sachdev, M. R. Norman, D. Hsieh

Abstract: Understanding the complex phase diagram of cuprate superconductors is an outstanding challenge. The most actively studied questions surround the nature of the pseudogap and strange metal states and their relationship to superconductivity. In contrast, there is general agreement that the low energy physics of the Mott insulating parent state is well captured by a two-dimensional spin $S$ = 1/2 anti… ▽ More Understanding the complex phase diagram of cuprate superconductors is an outstanding challenge. The most actively studied questions surround the nature of the pseudogap and strange metal states and their relationship to superconductivity. In contrast, there is general agreement that the low energy physics of the Mott insulating parent state is well captured by a two-dimensional spin $S$ = 1/2 antiferromagnetic (AFM) Heisenberg model. However, recent observations of a large thermal Hall conductivity in several parent cuprates appear to defy this simple model and suggest proximity to a magneto-chiral state that breaks all mirror planes perpendicular to the CuO$_2$ layers. Here we use optical second harmonic generation to directly resolve the point group symmetries of the model parent cuprate Sr$_2$CuO$_2$Cl$_2$. We report evidence of an order parameter $Φ$ that breaks all perpendicular mirror planes and is consistent with a magneto-chiral state in zero magnetic field. Although $Φ$ is clearly coupled to the AFM order parameter, we are unable to realize its time-reversed partner ($-Φ$) by thermal cycling through the AFM transition temperature ($T_{\textrm{N}}$ $\approx$ 260 K) or by sampling different spatial locations. This suggests that $Φ$ onsets above $T_{\textrm{N}}$ and may be relevant to the mechanism of pseudogap formation. △ Less

Submitted 14 August, 2020; originally announced August 2020.

Comments: 6 pages main text, 4 figures, 24 pages supplementary information

Journal ref: Nature Physics 17, 777-781 (2021)

Evidence for an extended critical fluctuation region above the polar ordering transition in LiOsO$_3$

Authors: Jun-Yi Shan, A. de la Torre, N. J. Laurita, L. Zhao, C. D. Dashwood, D. Puggioni, C. X. Wang, K. Yamaura, Y. Shi, J. M. Rondinelli, D. Hsieh

Abstract: Metallic LiOsO$_3$ undergoes a continuous ferroelectric-like structural phase transition below $T_c$ = 140 K to realize a polar metal. To understand the microscopic interactions that drive this transition, we study its critical behavior above $T_c$ via electromechanical coupling - distortions of the lattice induced by short-range dipole-dipole correlations arising from Li off-center displacements.… ▽ More Metallic LiOsO$_3$ undergoes a continuous ferroelectric-like structural phase transition below $T_c$ = 140 K to realize a polar metal. To understand the microscopic interactions that drive this transition, we study its critical behavior above $T_c$ via electromechanical coupling - distortions of the lattice induced by short-range dipole-dipole correlations arising from Li off-center displacements. By mapping the full angular distribution of second harmonic electric-quadrupole radiation from LiOsO$_3$ and performing a simplified hyper-polarizable bond model analysis, we uncover subtle symmetry-preserving lattice distortions over a broad temperature range extending from $T_c$ up to around 230 K, characterized by non-uniform changes in the short and long Li-O bond lengths. Such an extended region of critical fluctuations may explain anomalous features reported in specific heat and Raman scattering data, and suggests the presence of competing interactions that are not accounted for in existing theoretical treatments. More broadly, our results showcase how electromechanical effects serve as a probe of critical behavior near inversion symmetry breaking transitions in metals. △ Less

Submitted 1 August, 2020; originally announced August 2020.

Comments: 6 pages main text, 4 figures, 10 pages supplementary information

Journal ref: Phys. Rev. Research 2, 033174 (2020)

Linear magneto-electric phase in ultrathin MnPS$_{3}$ probed by optical second harmonic generation

Authors: H. Chu, C. J. Roh, J. O. Island, C. Li, S. Lee, J. Chen, J. G. Park, A. F. Young, J. S. Lee, D. Hsieh

Abstract: The transition metal thiophosphates $M$PS$_3$ ($M$ = Mn, Fe, Ni) are a class of van der Waals stacked insulating antiferromagnets that can be exfoliated down to the ultrathin limit. MnPS$_3$ is particularly interesting because its N$\acute{\textrm{e}}$el ordered state breaks both spatial-inversion and time-reversal symmetries, allowing for a linear magneto-electric phase that is rare among van der… ▽ More The transition metal thiophosphates $M$PS$_3$ ($M$ = Mn, Fe, Ni) are a class of van der Waals stacked insulating antiferromagnets that can be exfoliated down to the ultrathin limit. MnPS$_3$ is particularly interesting because its N$\acute{\textrm{e}}$el ordered state breaks both spatial-inversion and time-reversal symmetries, allowing for a linear magneto-electric phase that is rare among van der Waals materials. However, it is unknown whether this unique magnetic structure of bulk MnPS$_3$ remains stable in the ultrathin limit. Using optical second harmonic generation rotational anisotropy, we show that long-range linear magneto-electric type N$\acute{\textrm{e}}$el order in MnPS$_3$ persists down to at least 5.3 nm thickness. However an unusual mirror symmetry breaking develops in ultrathin samples on SiO$_2$ substrates that is absent in bulk materials, which is likely related to substrate induced strain. △ Less

Submitted 20 January, 2020; originally announced January 2020.

Comments: 6 pages, 4 figures

Journal ref: Phys. Rev. Lett. 124, 027601 (2020)

Valence bond phases of herbertsmithite and related copper kagome materials

Authors: M. R. Norman, N. J. Laurita, D. Hsieh

Abstract: Recent evidence from magnetic torque, electron spin resonance, and second harmonic generation indicate that the prototypical quantum spin liquid candidate, herbertsmithite, has a symmetry lower than its x-ray refined trigonal space group. Here, we consider known and possible distortions of this mineral class, along with related copper kagome oxides and fluorides, relate these to possible valence b… ▽ More Recent evidence from magnetic torque, electron spin resonance, and second harmonic generation indicate that the prototypical quantum spin liquid candidate, herbertsmithite, has a symmetry lower than its x-ray refined trigonal space group. Here, we consider known and possible distortions of this mineral class, along with related copper kagome oxides and fluorides, relate these to possible valence bond patterns, and comment on their relevance to the physics of these interesting materials. △ Less

Submitted 16 January, 2020; v1 submitted 30 October, 2019; originally announced October 2019.

Journal ref: Phys. Rev. Research 2, 013055 (2020)

Evidence for a Parity Broken Monoclinic Ground State in the S = 1/2 Kagomé Antiferromagnet Herbertsmithite

Authors: N. J. Laurita, A. Ron, J. W. Han, A. Scheie, J. P. Sheckelton, R. W. Smaha, W. He, J. -J. Wen, J. S. Lee, Y. S. Lee, M. R. Norman, D. Hsieh

Abstract: Nearest-neighbor interacting S = 1/2 spins on the ideal Kagomé lattice are predicted to form a variety of novel quantum entangled states, including quantum spin-liquid (SL) and valence bond solid (VBS) phases. In real materials, the presence of additional perturbative spin interactions may further expand the variety of entangled states, which recent theoretical analyses show are identifiable throu… ▽ More Nearest-neighbor interacting S = 1/2 spins on the ideal Kagomé lattice are predicted to form a variety of novel quantum entangled states, including quantum spin-liquid (SL) and valence bond solid (VBS) phases. In real materials, the presence of additional perturbative spin interactions may further expand the variety of entangled states, which recent theoretical analyses show are identifiable through the spontaneous loss of particular discrete point group symmetries. Here we comprehensively resolve the ground state point group symmetries of the prototypical Kagomé SL candidate ZnCu$_3$(OH)$_6$Cl$_2$ (Herbertsmithite) using a combination of optical ellipsometry and wavelength-dependent multi-harmonic optical polarimetry. We uncover a subtle parity breaking monoclinic structural distortion at a temperature above the nearest-neighbor exchange energy scale. Surprisingly, the parity-breaking order parameter is dramatically enhanced upon cooling and closely tracks the build-up of nearest-neighbor spin correlations, suggesting that it is energetically favored by the SL state. The refined low temperature symmetry group greatly restricts the number of viable ground states, and, in the perturbative limit, points toward the formation of a nematic $Z_2$ striped SL ground state - a SL analogue of a liquid crystal. △ Less

Submitted 29 October, 2019; originally announced October 2019.

Comments: 13 pages main text, 4 figures, 10 pages supplementary information

Ultrafast enhancement of ferromagnetic spin exchange induced by ligand-to-metal charge transfer

Authors: A. Ron, S. Chaudhary, G. Zhang, H. Ning, E. Zoghlin, S. D. Wilson, R. D. Averitt, G. Refael, D. Hsieh

Abstract: Directly modifying spin exchange energies in a magnetic material with light can enable ultrafast control of its magnetic states. Current approaches rely on tuning charge hopping amplitudes that mediate exchange by optically exciting either virtual or real charge-transfer transitions (CT) between magnetic sites. Here we show that when exchange is mediated by a non-magnetic ligand, it can be substan… ▽ More Directly modifying spin exchange energies in a magnetic material with light can enable ultrafast control of its magnetic states. Current approaches rely on tuning charge hopping amplitudes that mediate exchange by optically exciting either virtual or real charge-transfer transitions (CT) between magnetic sites. Here we show that when exchange is mediated by a non-magnetic ligand, it can be substantially enhanced by optically exciting a real CT transition from the ligand to magnetic site, introducing lower order virtual hopping contributions. We demonstrate sub-picosecond enhancement in a superexchange dominated ferromagnet CrSiTe3 through this mechanism using phase-resolved coherent phonon spectroscopy. This technique can also be applied in the paramagnetic phase to disentangle light induced exchange modification from other ultrafast effects that alter the magnetization. This protocol can potentially be broadly applied to engineer thermally inaccessible spin Hamiltonians in superexchange dominated magnets. △ Less

Submitted 14 October, 2019; originally announced October 2019.

Comments: 13 pages main text, 4 figures, 14 pages supplementary information

Journal ref: Phys. Rev. Lett. 125, 197203 (2020)

Evidence for the weakly coupled electron mechanism in an Anderson-Blount polar metal

Authors: N. J. Laurita, A. Ron, J. Shan, D. Puggioni, N. Z. Koocher, K. Yamaura, Y. Shi, J. M. Rondinelli, D. Hsieh

Abstract: Over 50 years ago, Anderson and Blount proposed that ferroelectric-like structural phase transitions may occur in metals, despite the expected screening of the Coulomb interactions that often drive polar transitions. Recently, theoretical treatments have suggested that such transitions require the itinerant electrons be decoupled from the soft transverse optical phonons responsible for polar order… ▽ More Over 50 years ago, Anderson and Blount proposed that ferroelectric-like structural phase transitions may occur in metals, despite the expected screening of the Coulomb interactions that often drive polar transitions. Recently, theoretical treatments have suggested that such transitions require the itinerant electrons be decoupled from the soft transverse optical phonons responsible for polar order. However, this decoupled electron mechanism (DEM) has yet to be experimentally observed. Here we utilize ultrafast spectroscopy to uncover evidence of the DEM in LiOsO$_3$, the first known band metal to undergo a thermally driven polar phase transition ($T_c$ =140 K). We demonstrate that intra-band photo-carriers relax by selectively coupling to only a subset of the phonon spectrum, leaving as much as 60 % of the lattice heat capacity decoupled. This decoupled heat capacity is shown to be consistent with a previously undetected and partially displacive TO polar mode, indicating the DEM in LiOsO$_3$. △ Less

Submitted 23 July, 2019; originally announced July 2019.

Comments: 15 pages main text, 4 figures, 12 pages supplementary information

Journal ref: Nature Communications 10, 3217 (2019)

Orbital Floquet Engineering of Exchange Interactions in Magnetic Materials

Authors: Swati Chaudhary, David Hsieh, Gil Refael

Abstract: 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… ▽ More 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. △ Less

Submitted 9 May, 2019; originally announced May 2019.

Journal ref: Phys. Rev. B 100, 220403 (2019)

Dimensional crossover in a layered ferromagnet detected by spin correlation driven distortions

Authors: A. Ron, E. Zoghlin, L. Balents, S. D. Wilson, D. Hsieh

Abstract: Magneto-elastic distortions are commonly detected across magnetic long-range ordering (LRO) transitions. In principle, they are also induced by the magnetic short-range ordering (SRO) that precedes a LRO transition, which contains information about short-range correlations and energetics that are essential for understanding how LRO is established. However these distortions are difficult to resolve… ▽ More Magneto-elastic distortions are commonly detected across magnetic long-range ordering (LRO) transitions. In principle, they are also induced by the magnetic short-range ordering (SRO) that precedes a LRO transition, which contains information about short-range correlations and energetics that are essential for understanding how LRO is established. However these distortions are difficult to resolve because the associated atomic displacements are exceedingly small and do not break symmetry. Here we demonstrate high-multipole nonlinear optical polarimetry as a sensitive and mode selective probe of SRO induced distortions using CrSiTe$_3$ as a testbed. This compound is composed of weakly bonded sheets of nearly isotropic ferromagnetically interacting spins that, in the Heisenberg limit, would individually be impeded from LRO by the Mermin-Wagner theorem. Our results show that CrSiTe$_3$ evades this law via a two-step crossover from two- to three-dimensional magnetic SRO, manifested through two successive and previously undetected totally symmetric distortions above its Curie temperature. △ Less

Submitted 23 April, 2019; originally announced April 2019.

Comments: 17 pages main text, 4 figures, 12 pages supplementary information

Journal ref: Nature Communications 10, 1654 (2019)

Floquet Engineering in Quantum Chains

Authors: D. M. Kennes, A. de la Torre, A. Ron, D. Hsieh, A. J. Millis

Abstract: We consider a one-dimensional interacting spinless fermion model, which displays the well-known Luttinger liquid (LL) to charge density wave (CDW) transition as a function of the ratio between the strength of the interaction, $U$, and the hopping, $J$. We subject this system to a spatially uniform drive which is ramped up over a finite time interval and becomes time-periodic in the long time limit… ▽ More We consider a one-dimensional interacting spinless fermion model, which displays the well-known Luttinger liquid (LL) to charge density wave (CDW) transition as a function of the ratio between the strength of the interaction, $U$, and the hopping, $J$. We subject this system to a spatially uniform drive which is ramped up over a finite time interval and becomes time-periodic in the long time limit. We show that by using a density matrix renormalization group (DMRG) approach formulated for infinite system sizes, we can access the large-time limit even when the drive induces finite heating. When both the initial and long-time states are in the gapless (LL) phase, the final state has power law correlations for all ramp speeds. However, when the initial and final state are gapped (CDW phase), we find a pseudothermal state with an effective temperature that depends on the ramp rate, both for the Magnus regime in which the drive frequency is very large compared to other scales in the system and in the opposite limit where the drive frequency is less than the gap. Remarkably, quantum defects (instantons) appear when the drive tunes the system through the quantum critical point, in a realization of the Kibble-Zurek mechanism. △ Less

Submitted 25 March, 2018; v1 submitted 21 January, 2018; originally announced January 2018.

Comments: 4.5 + 5 pages, 5 figures, version as published

Journal ref: Phys. Rev. Lett. 120, 127601 (2018)

Evidence of an improper displacive phase transition in Cd$_2$Re$_2$O$_7$ via time-resolved coherent phonon spectroscopy

Authors: J. W. Harter, D. M. Kennes, H. Chu, A. de la Torre, Z. Y. Zhao, J. -Q. Yan, D. G. Mandrus, A. J. Millis, D. Hsieh

Abstract: We have used a combination of ultrafast coherent phonon spectroscopy, ultrafast thermometry, and time-dependent Landau theory to study the inversion symmetry breaking phase transition at $T_c = 200$ K in the strongly spin-orbit coupled correlated metal Cd$_2$Re$_2$O$_7$. We establish that the structural distortion at $T_c$ is a secondary effect through the absence of any softening of its associate… ▽ More We have used a combination of ultrafast coherent phonon spectroscopy, ultrafast thermometry, and time-dependent Landau theory to study the inversion symmetry breaking phase transition at $T_c = 200$ K in the strongly spin-orbit coupled correlated metal Cd$_2$Re$_2$O$_7$. We establish that the structural distortion at $T_c$ is a secondary effect through the absence of any softening of its associated phonon mode, which supports a purely electronically driven mechanism. However, the phonon lifetime exhibits an anomalously strong temperature dependence that decreases linearly to zero near $T_c$. We show that this behavior naturally explains the spurious appearance of phonon softening in previous Raman spectroscopy experiments and should be a prevalent feature of correlated electron systems with linearly coupled order parameters. △ Less

Submitted 16 January, 2018; originally announced January 2018.

Comments: 5 pages main text, 5 figures, 7 pages supplementary information

Journal ref: Phys. Rev. Lett. 120, 047601 (2018)

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

Authors: Tom Hogan, Xiaoping Wang, H. Chu, David Hsieh, Stephen D. Wilson

Abstract: 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 appear… ▽ More 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. △ Less

Submitted 12 May, 2017; originally announced May 2017.

Comments: 8 pages, 4 figures

A parity-breaking electronic nematic phase transition in the spin-orbit coupled metal Cd$_2$Re$_2$O$_7$

Authors: J. W. Harter, Z. Y. Zhao, J. -Q. Yan, D. G. Mandrus, D. Hsieh

Abstract: Strong electron interactions can drive metallic systems toward a variety of well-known symmetry-broken phases, but the instabilities of correlated metals with strong spin-orbit coupling have only recently begun to be explored. We uncovered a multipolar nematic phase of matter in the metallic pyrochlore Cd$_2$Re$_2$O$_7$ using spatially resolved second-harmonic optical anisotropy measurements. Like… ▽ More Strong electron interactions can drive metallic systems toward a variety of well-known symmetry-broken phases, but the instabilities of correlated metals with strong spin-orbit coupling have only recently begun to be explored. We uncovered a multipolar nematic phase of matter in the metallic pyrochlore Cd$_2$Re$_2$O$_7$ using spatially resolved second-harmonic optical anisotropy measurements. Like previously discovered electronic nematic phases, this multipolar phase spontaneously breaks rotational symmetry while preserving translational invariance. However, it has the distinguishing property of being odd under spatial inversion, which is allowed only in the presence of spin-orbit coupling. By examining the critical behavior of the multipolar nematic order parameter, we show that it drives the thermal phase transition near 200 kelvin in Cd$_2$Re$_2$O$_7$ and induces a parity-breaking lattice distortion as a secondary order. △ Less

Submitted 24 April, 2017; originally announced April 2017.

Comments: 9 pages main text, 4 figures, 10 pages supplementary information

Journal ref: Science 356, 295-299 (2017)

A charge density wave-like instability in a doped spin-orbit-assisted weak Mott insulator

Authors: H. Chu, L. Zhao, A. de la Torre, T. Hogan, S. D. Wilson, D. Hsieh

Abstract: Layered perovskite iridates realize a rare class of Mott insulators that are predicted to be strongly spin-orbit coupled analogues of the parent state of cuprate high-temperature superconductors. Recent discoveries of pseudogap, magnetic multipolar ordered and possible $d$-wave superconducting phases in doped Sr$_2$IrO$_4$ have reinforced this analogy among the single layer variants. However, unli… ▽ More Layered perovskite iridates realize a rare class of Mott insulators that are predicted to be strongly spin-orbit coupled analogues of the parent state of cuprate high-temperature superconductors. Recent discoveries of pseudogap, magnetic multipolar ordered and possible $d$-wave superconducting phases in doped Sr$_2$IrO$_4$ have reinforced this analogy among the single layer variants. However, unlike the bilayer cuprates, no electronic instabilities have been reported in the doped bilayer iridate Sr$_3$Ir$_2$O$_7$. Here we show that Sr$_3$Ir$_2$O$_7$ realizes a weak Mott state with no cuprate analogue by using ultrafast time-resolved optical reflectivity to uncover an intimate connection between its insulating gap and antiferromagnetism. However, we detect a subtle charge density wave-like Fermi surface instability in metallic electron doped Sr$_3$Ir$_2$O$_7$ at temperatures ($T_{DW}$) close to 200 K via the coherent oscillations of its collective modes, which is reminiscent of that observed in cuprates. The absence of any signatures of a new spatial periodicity below $T_{DW}$ from diffraction, scanning tunneling and photoemission based probes suggests an unconventional and possibly short-ranged nature of this density wave order. △ Less

Submitted 18 January, 2017; originally announced January 2017.

Comments: 13 pages main text, 4 figures, 10 pages supplementary information, in Nature Materials (2017)

Journal ref: Nature Materials 16, 200-203 (2017)

A global inversion-symmetry-broken phase inside the pseudogap region of YBa$_2$Cu$_3$O$_y$

Authors: L. Zhao, C. A. Belvin, R. Liang, D. A. Bonn, W. N. Hardy, N. P. Armitage, D. Hsieh

Abstract: The phase diagram of cuprate high-temperature superconductors features an enigmatic pseudogap region that is characterized by a partial suppression of low energy electronic excitations. Polarized neutron diffraction, Nernst effect, THz polarimetery and ultrasound measurements on YBa$_2$Cu$_3$O$_y$ suggest that the pseudogap onset below a temperature T* coincides with a bona fide thermodynamic phas… ▽ More The phase diagram of cuprate high-temperature superconductors features an enigmatic pseudogap region that is characterized by a partial suppression of low energy electronic excitations. Polarized neutron diffraction, Nernst effect, THz polarimetery and ultrasound measurements on YBa$_2$Cu$_3$O$_y$ suggest that the pseudogap onset below a temperature T* coincides with a bona fide thermodynamic phase transition that breaks time-reversal, four-fold rotation and mirror symmetries respectively. However, the full point group above and below T* has not been resolved and the fate of this transition as T* approaches the superconducting critical temperature T$_c$ is poorly understood. Here we reveal the point group of YBa$_2$Cu$_3$O$_y$ inside its pseudogap and neighboring regions using high sensitivity linear and second harmonic optical anisotropy measurements. We show that spatial inversion and two-fold rotational symmetries are broken below T* while mirror symmetries perpendicular to the Cu-O plane are absent at all temperatures. This transition occurs over a wide doping range and persists inside the superconducting dome, with no detectable coupling to either charge ordering or superconductivity. These results suggest that the pseudogap region coincides with an odd-parity order that does not arise from a competing Fermi surface instability and exhibits a quantum phase transition inside the superconducting dome. △ Less

Submitted 25 November, 2016; originally announced November 2016.

Comments: 14 pages main text, 4 figures, 11 pages supplementary information, Nature Physics (2016)

Journal ref: Nature Physics 13, 250-254 (2017)

Structural investigation of the bilayer iridate Sr3Ir2O7

Authors: Tom Hogan, Lars Bjaalie, Liuyan Zhao, Carina Belvin, Xiaoping Wang, Chris G. Van de Walle, David Hsieh, Stephen D. Wilson

Abstract: 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 rotationa… ▽ More 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. △ Less

Submitted 23 March, 2016; originally announced March 2016.

Comments: 7 pages, 3 figures

Journal ref: Physical Review B 93, 134110 (2016)

Nonlinear and time-resolved optical study of the 112-type iron-based superconductor parent Ca$_{1-x}$La$_{x}$FeAs$_{2}$ across its structural phase transition

Authors: J. W. Harter, H. Chu, S. Jiang, N. Ni, D. Hsieh

Abstract: The newly discovered 112-type ferropnictide superconductors contain chains of As atoms that break the tetragonal symmetry between the $a$ and $b$ axes. This feature eliminates the need for uniaxial strain that is usually required to stabilize large single domains in the electronic nematic state that exists in the vicinity of magnetic order in the iron-based superconductors. We report detailed stru… ▽ More The newly discovered 112-type ferropnictide superconductors contain chains of As atoms that break the tetragonal symmetry between the $a$ and $b$ axes. This feature eliminates the need for uniaxial strain that is usually required to stabilize large single domains in the electronic nematic state that exists in the vicinity of magnetic order in the iron-based superconductors. We report detailed structural symmetry measurements of 112-type Ca$_{0.73}$La$_{0.27}$FeAs$_{2}$ using rotational anisotropy optical second harmonic generation. This technique is complementary to diffraction experiments and enables a precise determination of the point group symmetry of a crystal. By combining our measurements with density functional theory calculations, we uncover a strong optical second harmonic response of bulk electric dipole origin from the Fe and Ca $3d$-derived states that enables us to assign $C_2$ as the crystallographic point group. This makes the 112-type materials high-temperature superconductors without a center of inversion, allowing for the possible mixing of singlet and triplet Cooper pairs in the superconducting state. We also perform pump-probe transient reflectivity experiments that reveal a 4.6 THz phonon mode associated with the out-of-plane motion of As atoms in the FeAs layers. We do not observe any suppression of the optical second harmonic response or shift in the phonon frequency upon cooling through the reported monoclinic-to-triclinic transition at 58 K. This allows us to identify $C_1$ as the low-temperature crystallographic point group but suggests that structural changes induced by long-range magnetic order are subtle and do not significantly affect electronic states near the Fermi level. △ Less

Submitted 11 March, 2016; originally announced March 2016.

Journal ref: Phys. Rev. B 93, 104506 (2016); Editors' Suggestion

Evidence of an odd-parity hidden order in a spin-orbit coupled correlated iridate

Authors: L. Zhao, D. H. Torchinsky, H. Chu, V. Ivanov, R. Lifshitz, R. Flint, T. Qi, G. Cao, D. Hsieh

Abstract: A rare combination of strong spin-orbit coupling and electron-electron correlations makes the iridate Mott insulator Sr$_2$IrO$_4$ a promising host for novel electronic phases of matter. The resemblance of its crystallographic, magnetic and electronic structures to La$_2$CuO$_4$, as well as the emergence upon doping of a pseudogap region and a low temperature $d$-wave gap, has particularly strengt… ▽ More A rare combination of strong spin-orbit coupling and electron-electron correlations makes the iridate Mott insulator Sr$_2$IrO$_4$ a promising host for novel electronic phases of matter. The resemblance of its crystallographic, magnetic and electronic structures to La$_2$CuO$_4$, as well as the emergence upon doping of a pseudogap region and a low temperature $d$-wave gap, has particularly strengthened analogies to cuprate high-$T_c$ superconductors. However, unlike the cuprate phase diagram that features a plethora of broken symmetry phases in a pseudogap region that include charge density wave, stripe, nematic and possibly intra-unit cell loop-current orders, no broken symmetry phases proximate to the parent antiferromagnetic Mott insulating phase in Sr$_2$IrO$_4$ have been observed to date, making the comparison of iridate to cuprate phenomenology incomplete. Using optical second harmonic generation, we report evidence of a hidden non-dipolar magnetic order in Sr$_2$IrO$_4$ that breaks both the spatial inversion and rotational symmetries of the underlying tetragonal lattice. Four distinct domain types corresponding to discrete 90$^{\circ}$ rotated orientations of a pseudovector order parameter are identified using nonlinear optical microscopy, which is expected from an electronic phase that possesses the symmetries of a magneto-electric loop-current order. The onset temperature of this phase is monotonically suppressed with bulk hole doping, albeit much more weakly than the Néel temperature, revealing an extended region of the phase diagram with purely hidden order. Driving this hidden phase to its quantum critical point may be a path to realizing superconductivity in Sr$_2$IrO$_4$. △ Less

Submitted 7 January, 2016; originally announced January 2016.

Comments: 13 pages main text, 4 figures, 21 pages supplementary information

Journal ref: Nature Physics 12, 32-36 (2016)

High-speed measurement of rotational anisotropy nonlinear optical harmonic generation using position sensitive detection

Authors: J. W. Harter, L. Niu, A. J. Woss, D. Hsieh

Abstract: We present a method of performing high-speed rotational anisotropy nonlinear optical harmonic generation experiments at rotational frequencies of several hertz by projecting the harmonic light reflected at different angles from a sample onto a stationary position sensitive detector. The high rotational speed of the technique, $10^3$ to $10^4$ times larger than existing methods, permits precise mea… ▽ More We present a method of performing high-speed rotational anisotropy nonlinear optical harmonic generation experiments at rotational frequencies of several hertz by projecting the harmonic light reflected at different angles from a sample onto a stationary position sensitive detector. The high rotational speed of the technique, $10^3$ to $10^4$ times larger than existing methods, permits precise measurements of the crystallographic and electronic symmetries of samples by averaging over low frequency laser power, beam pointing, and pulse width fluctuations. We demonstrate the sensitivity of our technique by resolving the bulk four-fold rotational symmetry of GaAs about its [001] axis using second harmonic generation. △ Less

Submitted 15 September, 2015; originally announced September 2015.

Journal ref: Optics Letters 40, 4671-4674 (2015)

A structural distortion induced magneto-elastic locking in Sr$_2$IrO$_4$ revealed through nonlinear optical harmonic generation

Authors: D. H. Torchinsky, H. Chu, L. Zhao, N. B. Perkins, Y. Sizyuk, T. Qi, G. Cao, D. Hsieh

Abstract: We report a global structural distortion in Sr$_2$IrO$_4$ using spatially resolved optical second and third harmonic generation rotational anisotropy measurements. A symmetry lowering from an $I4_{1}/acd$ to $I4_{1}/a$ space group is observed both above and below the Néel temperature that arises from a staggered tetragonal distortion of the oxygen octahedra. By studying an effective super-exchange… ▽ More We report a global structural distortion in Sr$_2$IrO$_4$ using spatially resolved optical second and third harmonic generation rotational anisotropy measurements. A symmetry lowering from an $I4_{1}/acd$ to $I4_{1}/a$ space group is observed both above and below the Néel temperature that arises from a staggered tetragonal distortion of the oxygen octahedra. By studying an effective super-exchange Hamiltonian that accounts for this lowered symmetry, we find that perfect locking between the octahedral rotation and magnetic moment canting angles can persist even in the presence of large non-cubic local distortions. Our results explain the origin of the forbidden Bragg peaks recently observed in neutron diffraction experiments and reconcile the observations of strong tetragonal distortion and perfect magneto-elastic locking in Sr$_2$IrO$_4$. △ Less

Submitted 4 November, 2014; originally announced November 2014.

Comments: 6 pages, 4 figures

Journal ref: Phys. Rev. Lett. 114, 096404 (2015)

A Low Temperature Nonlinear Optical Rotational Anisotropy Spectrometer for the Determination of Crystallographic and Electronic Symmetries

Authors: D. H. Torchinsky, H. Chu, T. Qi, G. Cao, D. Hsieh

Abstract: Nonlinear optical generation from a crystalline material can reveal the symmetries of both its lattice structure and underlying ordered electronic phases and can therefore be exploited as a complementary technique to diffraction based scattering probes. Although this technique has been successfully used to study the lattice and magnetic structures of systems such as semiconductor surfaces, multife… ▽ More Nonlinear optical generation from a crystalline material can reveal the symmetries of both its lattice structure and underlying ordered electronic phases and can therefore be exploited as a complementary technique to diffraction based scattering probes. Although this technique has been successfully used to study the lattice and magnetic structures of systems such as semiconductor surfaces, multiferroic crystals, magnetic thin films and multilayers, challenging technical requirements have prevented its application to the plethora of complex electronic phases found in strongly correlated electron systems. These requirements include an ability to probe small bulk single crystals at the micron length scale, a need for sensitivity to the entire nonlinear optical susceptibility tensor, oblique light incidence reflection geometry and incident light frequency tunability among others. These measurements are further complicated by the need for extreme sample environments such as ultra low temperatures, high magnetic fields or high pressures. In this review we present a novel experimental construction using a rotating light scattering plane that meets all the aforementioned requirements. We demonstrate the efficacy of our scheme by making symmetry measurements on a micron scale facet of a small bulk single crystal of Sr$_2$IrO$_4$ using optical second and third harmonic generation. △ Less

Submitted 17 June, 2014; originally announced June 2014.

Comments: 8 pages, 5 figures

Journal ref: Rev. Sci. Instrum. 85, 083102 (2014)

A Neutron Scattering Study of the H-T Phase Diagram of the Bond Frustrated ZnCr2S4

Authors: D. Hsieh, Y. W. Li, S. Watauchi, Chang Liu, Q. Huang, R. J. Cava, J. W. Lynn, M. Z. Hasan

Abstract: Detailed neutron scattering measurements on the bond frustrated magnet ZnCr2S4 reveal a rich H-T phase diagram. The field dependence of the two subsequent antiferromagnetic transitions follows closely that of recently reported structural instabilities, providing further evidence for spin driven Jahn-Teller physics. The incommensurate helical ordered phase below TN1 = 15.5 K exhibits gapless spin w… ▽ More Detailed neutron scattering measurements on the bond frustrated magnet ZnCr2S4 reveal a rich H-T phase diagram. The field dependence of the two subsequent antiferromagnetic transitions follows closely that of recently reported structural instabilities, providing further evidence for spin driven Jahn-Teller physics. The incommensurate helical ordered phase below TN1 = 15.5 K exhibits gapless spin wave excitations, whereas a spin wave gap (about 2 meV) opens below TN2 = 8 K as the system undergoes a first-order transition to a commensurate collinear ordered phase. The spin wave gap is closed by a strong magnetic field. △ Less

Submitted 1 June, 2014; originally announced June 2014.

Comments: 4 Pages, 4 Figures

Spin Order by Quantum Frustration in Triangular Lattice Mott Insulator NaCrO2 : A Neutron Scattering Study

Authors: D. Hsieh, D. Qian, R. F. Berger, C. Liu, B. Ueland, P. Schiffer, Q. Huang, R. J. Cava, J. W. Lynn, M. Z. Hasan

Abstract: We report high resolution neutron scattering measurements on the triangular lattice Mott insulator Na$_x$CrO$_2$ ($x$=1) which has recently been shown to exhibit an unusually broad fluctuating crossover regime extending far below the onset of spin freezing ($T_c\sim$41K). Our results show that below some crossover temperature ($T\sim0.75T_c$) a small incommensuration develops which helps resolve t… ▽ More We report high resolution neutron scattering measurements on the triangular lattice Mott insulator Na$_x$CrO$_2$ ($x$=1) which has recently been shown to exhibit an unusually broad fluctuating crossover regime extending far below the onset of spin freezing ($T_c\sim$41K). Our results show that below some crossover temperature ($T\sim0.75T_c$) a small incommensuration develops which helps resolve the spin frustration and drives three-dimensional magnetic order supporting coherent spin wave modes. This incommensuration assisted dimensional crossover suggests that inter-layer frustration is responsible for stabilizing the rare 2D correlated phase above 0.75$T_c$. In contrast to the host compound of 2D cobaltate superconductor such as Na$_x$CoO$_2$ ($ξ_c>50$Å), no magnetic long-range order is observed down to 1.5K ($ξ_c<16$Å). △ Less

Submitted 23 May, 2014; originally announced May 2014.

Comments: 5 pages, 4 figures

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

Authors: M. Zahid Hasan, Su-Yang Xu, David Hsieh, L. Andrew Wray, Yuqi Xia

Abstract: 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… ▽ More 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. △ Less

Submitted 4 January, 2014; originally announced January 2014.

Comments: 18 Figures, 23 pages; Invited Review, Accepted for publication, Related papers at http://arxiv.org/abs/1105.0396 and http://scholar.google.com/citations?user=G1Qpy6MAAAAJ&hl=en

Measurement of intrinsic Dirac fermion cooling on the surface of a topological insulator Bi$_2$Se$_3$ using time- and angle-resolved photoemission spectroscopy

Authors: Y. H. Wang, D. Hsieh, E. J. Sie, H. Steinberg, D. R. Gardner, Y. S. Lee, P. Jarillo-Herrero, N. Gedik

Abstract: We perform time- and angle-resolved photoemission spectroscopy of a prototypical topological insulator Bi$_2$Se$_3$ to study the ultrafast dynamics of surface and bulk electrons after photo-excitation. By analyzing the evolution of surface states and bulk band spectra, we obtain their electronic temperature and chemical potential relaxation dynamics separately. These dynamics reveal strong phonon-… ▽ More We perform time- and angle-resolved photoemission spectroscopy of a prototypical topological insulator Bi$_2$Se$_3$ to study the ultrafast dynamics of surface and bulk electrons after photo-excitation. By analyzing the evolution of surface states and bulk band spectra, we obtain their electronic temperature and chemical potential relaxation dynamics separately. These dynamics reveal strong phonon-assisted surface-bulk coupling at high lattice temperature and total suppression of inelastic scattering between the surface and the bulk at low lattice temperature. In this low temperature regime, the unique cooling of Dirac fermions in TI by acoustic phonons is manifested through a power law dependence of the surface temperature decay rate on carrier density. △ Less

Submitted 23 August, 2012; originally announced August 2012.

Comments: Accepted to Phys. Rev. Lett

Journal ref: Phys. Rev. Lett. 109, 127401 (2012)

Deviating band symmetries and many-body interactions in a model hole doped iron pnictide superconductor

Authors: L. A. Wray, R. Thomale, C. Platt, D. Hsieh, D. Qian, G. F. Chen, J. L. Luo, N. L. Wang, M. Z. Hasan

Abstract: We present a polarization resolved study of the low energy band structure in the optimally doped iron pnictide superconductor Ba$_{0.6}$K$_{0.4}$Fe$_2$As$_2$ (T$_c$=37K) using angle resolved photoemission spectroscopy. Polarization-contrasted measurements are used to identify and trace all three low energy hole-like bands predicted by local density approximation (LDA) calculations. The photoemitte… ▽ More We present a polarization resolved study of the low energy band structure in the optimally doped iron pnictide superconductor Ba$_{0.6}$K$_{0.4}$Fe$_2$As$_2$ (T$_c$=37K) using angle resolved photoemission spectroscopy. Polarization-contrasted measurements are used to identify and trace all three low energy hole-like bands predicted by local density approximation (LDA) calculations. The photoemitted electrons reveal an inconsistency with LDA-predicted symmetries along the $Γ$-X high symmetry momentum axis, due to unexpectedly strong rotational anisotropy in electron kinetics. We evaluate many-body effects such as Mott-Hubbard interactions that are likely to underlie the anomaly, and discuss how the observed deviations from LDA band structure affect the energetics of iron pnictide Cooper pairing in the hole doped regime. △ Less

Submitted 30 September, 2012; v1 submitted 10 July, 2012; originally announced July 2012.

Comments: 7.1 pages, 5 figures. Symmetry analysis revised. Accepted for publication in Phys. Rev. B

Journal ref: PRB 86, 144515 (2012)

Observation of a Slater-type metal-to-insulator transition in Sr$_2$IrO$_4$ from time-resolved photo-carrier dynamics

Authors: D. Hsieh, F. Mahmood, D. H. Torchinsky, G. Cao, N. Gedik

Abstract: We perform a time-resolved optical study of Sr$_2$IrO$_4$ to understand the influence of magnetic ordering on the low energy electronic structure of a strongly spin-orbit coupled $J_{eff}$=1/2 Mott insulator. By studying the recovery dynamics of photo-carriers excited across the Mott gap, we find that upon cooling through the Néel temperature $T_N$ the system evolves continuously from a metal-like… ▽ More We perform a time-resolved optical study of Sr$_2$IrO$_4$ to understand the influence of magnetic ordering on the low energy electronic structure of a strongly spin-orbit coupled $J_{eff}$=1/2 Mott insulator. By studying the recovery dynamics of photo-carriers excited across the Mott gap, we find that upon cooling through the Néel temperature $T_N$ the system evolves continuously from a metal-like phase with fast ($\sim$50 fs) and excitation density independent relaxation dynamics to a gapped phase characterized by slower ($\sim$500 fs) excitation density dependent bimolecular recombination dynamics. The development of the insulating gap is accompanied by a transfer of in-gap spectral weight to energies far in excess of the gap and occurs over an unusually broad temperature window, which suggests Sr$_2$IrO$_4$ to be a Slater- rather than Mott-Hubbard type insulator and naturally explains the absence of anomalies at $T_N$ in transport and thermodynamic measurements. △ Less

Submitted 20 March, 2012; originally announced March 2012.

Control over topological insulator photocurrents with light polarization

Authors: J. W. McIver, D. Hsieh, H. Steinberg, P. Jarillo-Herrero, N. Gedik

Abstract: Three-dimensional topological insulators represent a new quantum phase of matter with spin-polarized surface states that are protected from backscattering. The static electronic properties of these surface states have been comprehensively imaged by both photoemission and tunneling spectroscopies. Theorists have proposed that topological surface states can also exhibit novel electronic responses to… ▽ More Three-dimensional topological insulators represent a new quantum phase of matter with spin-polarized surface states that are protected from backscattering. The static electronic properties of these surface states have been comprehensively imaged by both photoemission and tunneling spectroscopies. Theorists have proposed that topological surface states can also exhibit novel electronic responses to light, such as topological quantum phase transitions and spin-polarized electrical currents. However, the effects of optically driving a topological insulator out of equilibrium have remained largely unexplored experimentally, and no photocurrents have been measured. Here we show that illuminating the topological insulator Bi2Se3 with circularly polarized light generates a photocurrent that originates from topological helical Dirac fermions, and that reversing the helicity of the light reverses the direction of the photocurrent. We also observe a photocurrent that is controlled by the linear polarization of light, and argue that it may also have a topological surface state origin. This approach may allow the probing of dynamic properties of topological insulators and lead to novel opto-spintronic devices. △ Less

Submitted 15 November, 2011; originally announced November 2011.

Comments: Accepted in Nature Nanotechnology, November 2 2011

Selective probing of photo-induced charge and spin dynamics in the bulk and surface of a topological insulator

Authors: D. Hsieh, F. Mahmood, J. W. McIver, D. R. Gardner, Y. S. Lee, N. Gedik

Abstract: Topological insulators possess completely different spin-orbit coupled bulk and surface electronic spectra that are each predicted to exhibit exotic responses to light. Here we report time-resolved fundamental and second harmonic optical pump-probe measurements on the topological insulator Bi2Se3 to independently measure its photo-induced charge and spin dynamics with bulk and surface selectivity.… ▽ More Topological insulators possess completely different spin-orbit coupled bulk and surface electronic spectra that are each predicted to exhibit exotic responses to light. Here we report time-resolved fundamental and second harmonic optical pump-probe measurements on the topological insulator Bi2Se3 to independently measure its photo-induced charge and spin dynamics with bulk and surface selectivity. Our results show that a transient net spin density can be optically induced in both the bulk and surface, which may drive spin transport in topological insulators. By utilizing a novel rotational anisotropy analysis we are able to separately resolve the spin de-polarization, intraband cooling and interband recombination processes following photo-excitation, which reveal that spin and charge degrees of freedom relax on very different time scales owing to strong spin-orbit coupling. △ Less

Submitted 8 August, 2011; originally announced August 2011.

Comments: Accepted to Phys. Rev. Lett

Journal ref: Phys. Rev. Lett. 107, 077401 (2011)