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The excitonic insulator is an electronically driven phase of matter that emerges upon the spontaneous formation and Bose condensation of excitons. Detecting this exotic order in candidate materials is a subject of paramount importance, as the size of the excitonic gap in the band structure establishes the potential of this collective state for superfluid energy transport. However, the identification of this phase in real solids is hindered by the coexistence of a structural order parameter with the same symmetry as the excitonic order. Only a few materials are currently believed to host a dominant excitonic phase, Ta 2 NiSe 5 being the most promising. Here, we test this scenario by using an ultrashort laser pulse to quench the broken-symmetry phase of this transition metal chalcogenide. Tracking the dynamics of the material’s electronic and crystal structure after light excitation reveals spectroscopic fingerprints that are compatible only with a primary order parameter of phononic nature. We rationalize our findings through state-of-the-art calculations, confirming that the structural order accounts for most of the gap opening. Our results suggest that the spontaneous symmetry breaking in Ta 2 NiSe 5 is mostly of structural character, hampering the possibility to realize quasi-dissipationless energy transport.

Continuous and concerted development of colloidal quantum-dot light-emitting diodes over the past two decades has established them as a bedrock technology for the next generation of displays. However, a fundamental issue that limits the performance of these devices is the quenching of photoluminescence due to excess charges from conductive charge transport layers. Although device designs have leveraged various workarounds, doing so often comes at the cost of limiting efficient charge injection. Here we demonstrate that high-field terahertz (THz) pulses can dramatically brighten quenched QDs on metallic surfaces, an effect which persists for minutes after THz irradiation. This phenomenon is attributed to the ability of the THz field to remove excess charges, thereby reducing trion and non-radiative Auger recombination. Our findings show that THz technologies can be used to suppress and control such undesired non-radiative decay, potentially in a variety of luminescent materials for future device applications., 28 pages, 4 figures

arXiv:2006.04786v1, The interaction between off-resonant laser pulses and excitons in monolayer transition metal dichalcogenides is attracting increasing interest as a route for the valley-selective coherent control of the exciton properties. Here, we extend the classification of the known off-resonant phenomena by unveiling the impact of a strong THz field on the excitonic resonances of monolayer MoS2. We observe that the THz pump pulse causes a selective modification of the coherence lifetime of the excitons, while keeping their oscillator strength and peak energy unchanged. We rationalize these results theoretically by invoking a hitherto unobserved manifestation of the Franz–Keldysh effect on an exciton resonance. As the modulation depth of the optical absorption reaches values as large as 0.05 dB/nm at room temperature, our findings open the way to the use of semiconducting transition metal dichalcogenides as compact and efficient platforms for high-speed electroabsorption devices., This manuscript is based upon work by J.S. and K.A.N. supported in part by the U.S. Army Research Laboratory (ARL) and the U.S. Army Research Office through the Institute for Soldier Nanotechnologies, under Cooperative Agreement number W911-NF-18-2-0048. J.S. and K.A.N. acknowledge additional support from the Samsung Global Outreach Program. E.B. acknowledges additional support from the Swiss National Science Foundation under fellowships P2ELP2-172290 and P400P2-183842. N.G. and E.B. acknowledge support from DOE, BES DMSE. S.L. acknowledges support from the Alexander von Humboldt foundation. S.A.S. acknowledges JST-CREST under Grant No. JP-MJCR16N5. This work was supported by the European Research Council (ERC-2015-AdG694097), the Cluster of Excellence (AIM), Grupos Consolidados (IT1249-19), and SFB925. The Flatiron Institute is a division of the Simons Foundation. P.C.S. and J.K. acknowledge the financial support from the Center for Energy Efficient Electronics Science (NSF Award No. 0939514).

The observation of chirality is ubiquitous in nature. Contrary to intuition, the population of opposite chiralities is surprisingly asymmetric at fundamental levels. Examples range from parity violation in the subatomic weak force to the homochirality in essential biomolecules. The ability to achieve chirality-selective synthesis (chiral induction) is of great importance in stereochemistry, molecular biology and pharmacology. In condensed matter physics, a crystalline electronic system is geometrically chiral when it lacks any mirror plane, space inversion center or roto-inversion axis. Typically, the geometrical chirality is predefined by a material's chiral lattice structure, which is fixed upon the formation of the crystal. By contrast, a particularly unconventional scenario is the gyrotropic order, where chirality spontaneously emerges across a phase transition as the electron system breaks the relevant symmetries of an originally achiral lattice. Such a gyrotropic order, proposed as the quantum analogue of the cholesteric liquid crystals, has attracted significant interest. However, to date, a clear observation and manipulation of the gyrotropic order remain challenging. We report the realization of optical chiral induction and the observation of a gyrotropically ordered phase in the transition-metal dichalcogenide semimetal $1T$-TiSe$_2$. We show that shining mid-infrared circularly polarized light near the critical temperature leads to the preferential formation of one chiral domain. As a result, we are able to observe an out-of-plane circular photogalvanic current, whose direction depends on the optical induction. Our study provides compelling evidence for the spontaneous emergence of chirality in the correlated semimetal TiSe$_2$. Such chiral induction provides a new way of optical control over novel orders in quantum materials.

Engineering novel states of matter with light is at the forefront of materials research. An intensely studied direction is to realize broken-symmetry phases that are "hidden" under equilibrium conditions but can be unleashed by an ultrashort laser pulse. Despite a plethora of experimental discoveries, the nature of these orders and how they transiently appear remain unclear. To this end, we investigate a nonequilibrium charge density wave (CDW) in rare-earth tritellurides, which is suppressed in equilibrium but emerges after photoexcitation. Using a pump-pump-probe protocol implemented in ultrafast electron diffraction, we demonstrate that the light-induced CDW consists solely of order parameter fluctuations, which bear striking similarities to critical fluctuations in equilibrium despite differences in the length scale. By calculating the dynamics of CDW fluctuations in a nonperturbative model, we further show that the strength of the light-induced order is governed by the amplitude of equilibrium fluctuations. These findings highlight photoinduced fluctuations as an important ingredient for the emergence of transient orders out of equilibrium. Our results further suggest that materials with strong fluctuations in equilibrium are promising platforms to host "hidden" orders after laser excitation.

Collective excitations of bound electron-hole pairs -- known as excitons -- are ubiquitous in condensed matter, emerging in systems as diverse as band semiconductors, molecular crystals, and proteins. Recently, their existence in strongly correlated electron materials has attracted increasing interest due to the excitons' unique coupling to spin and orbital degrees of freedom. The non-equilibrium driving of such dressed quasiparticles offers a promising platform for realizing unconventional many-body phenomena and phases beyond thermodynamic equilibrium. Here, we achieve this in the van der Waals correlated insulator NiPS$_3$ by photoexciting its newly discovered spin-orbit-entangled excitons that arise from Zhang-Rice states. By monitoring the time evolution of the terahertz conductivity, we observe the coexistence of itinerant carriers produced by exciton dissociation and the long-wavelength antiferromagnetic magnon that coherently precesses in time. These results demonstrate the emergence of a transient metallic state that preserves long-range antiferromagnetism, a phase that cannot be reached by simply tuning the temperature. More broadly, our findings open an avenue toward the exciton-mediated optical manipulation of magnetism., 24 pages, 23 figures

Exciting electrons in solids with intense light pulses offers the possibility of generating new states of matter through nonthermal means and controlling their macroscopic properties on femto- to picosecond timescales. One way to manipulate a solid is by altering its lattice structure, which often underlies the electronic, magnetic and other phases. Here, we review how structures of solids are affected by photoexcitation and how their ultrafast dynamics are captured with time-resolved electron diffraction and microscopy. Specifically, we survey how a strong light pulse has been used to tailor the nonequilibrium characteristics to yield on-demand properties in various material classes. In the existing literature, four main routes have been exploited to control material structures: (i) phase competition, (ii) electronic correlations, (iii) excitation of coherent modes, and (iv) defect generation. In this review, we discuss experiments relevant to all four schemes and finish by speculating about future directions.

Hysteresis underlies a large number of phase transitions in solids, giving rise to exotic metastable states that are otherwise inaccessible. Here, we report an unconventional hysteretic transition in a quasi-2D material, EuTe_{4}. By combining transport, photoemission, diffraction, and x-ray absorption measurements, we observe that the hysteresis loop has a temperature width of more than 400 K, setting a record among crystalline solids. The transition has an origin distinct from known mechanisms, lying entirely within the incommensurate charge density wave (CDW) phase of EuTe_{4} with no change in the CDW modulation periodicity. We interpret the hysteresis as an unusual switching of the relative CDW phases in different layers, a phenomenon unique to quasi-2D compounds that is not present in either purely 2D or strongly coupled 3D systems. Our findings challenge the established theories on metastable states in density wave systems, pushing the boundary of understanding hysteretic transitions in a broken-symmetry state.

Integral to the exploration of nonequilibrium phenomena in solid-state systems is the study of lattice motion after photoexcitation by a femtosecond laser pulse. For the past two decades, ultrafast electron diffraction (UED) has played a critical role in this regard. Despite remarkable progress in instrumental development, this technique is still bottlenecked by a demanding sample preparation process, where ultrathin single crystals of large lateral size are typically required. In this work, we describe an efficient, versatile method that yields high-quality, laterally extended (≥ 100 µm), and thin (≤ 50 nm) single crystals on amorphous films of Si3N4 windows. It applies to most exfoliable materials, including those reactive in ambient conditions, and promises clean, flat surfaces. Besides the natural extension to fabricating van der Waals heterostructures, our method can also be applied to future-generation UED that enables additional control of sample parameters, such as electrostatic gating and excitation by a locally enhanced terahertz field. Our work significantly expands the type of samples for UED studies and also finds application in other time-resolved techniques such as attosecond extreme-ultraviolet absorption spectroscopy. This method hence provides further opportunities to explore photoinduced transitions and to discover novel states of matter out of equilibrium.

[EN] A phonoriton is an elementary excitation that is predicted to emerge from hybridization between exciton, phonon, and photon. Besides the intriguing many-particle structure, phonoritons are of interest as they could serve as functional nodes in devices that utilize electronic, phononic, and photonic elements for energy conversion and thermal transport applications. Although phonoritons are predicted to emerge in an excitonic medium under intense electromagnetic wave irradiation, the stringent condition for their existence has eluded direct observation in solids. In particular, on-resonance, intense pumping schemes have been proposed, but excessive photoexcitation of carriers prevents optical detection. Here, we theoretically predict the appearance of phonoritonic features in monolayer hexagonal boron nitride (h-BN) embedded in an optical cavity. The coherent superposition nature of phonoriton states is evidenced by the hybridization of exciton-polariton branches with phonon replicas that is tunable by the cavity-matter coupling strength. This finding simultaneously provides an experimental pathway for observing the predicted phonoritons and opens a new avenue for tuning materials properties. We thank Emre Ergecen for constructive discussions. We acknowledge financial support from the European Research Council (Grant No. ERC-2015-AdG-694097). Grupos Consolidados (Grant No. IT1249-19), and the Cluster of Excellence “CUI: Advanced Imaging of Matter” of the Deutsche Forschungsgemeinschaft (DFG)—EXC 2056— Project ID No. 390715994. The Flatiron Institute is a division of the Simons Foundation. S. L. acknowledges support from the Alexander von Humboldt foundation. Work at MIT was supported by the US Department of Energy, BES DMSE and by the Gordon and Betty Moore Foundations EPiQS Initiative Grant No. GBMF9459.

High harmonic generation of ultrafast laser pulses can be used to perform angle-resolved photoemission spectroscopy (ARPES) to map the electronic band structure of materials with femtosecond time resolution. However, currently it is difficult to reach high momenta with narrow energy resolution. Here, we combine a gas phase extreme ultraviolet (XUV) femtosecond light source, an XUV monochromator, and a time-of-flight electron analyzer to develop XUV-based time-resolved ARPES. Our technique can produce tunable photon energy between 24–33 eV with an unprecedented energy resolution of 30 meV and time resolution of 200 fs. This technique enables time-, energy- and momentum-resolved investigation of the nonequilibrium dynamics of electrons in materials with a full access to their first Brillouin zone. We evaluate the performance of this setup through exemplary measurements on various quantum materials, including WTe2, WSe2, TiSe2, and Bi2Sr2CaCu2O8+δ., Currently, it is difficult to reach high momenta with narrow energy resolution via laser-based angle-resolved photoemission spectroscopy (ARPES). Here, Sie et al. develop a time-resolved XUV based ARPES setup which can access the first Brillouin zone of all materials with narrow energy resolution.

Significance We uncover the presence of a new topological crystalline insulator (TCI) state in bismuth, which is protected by a twofold rotational symmetry. In contrast to the recently discovered higher-order topological phase in bismuth, the present TCI phase hosts unpinned Dirac cone surface states that could be accessed directly through photoemission experiments. Our study provides a comprehensive understanding of the rich topological electronic structure of bismuth., Bismuth-based materials have been instrumental in the development of topological physics, even though bulk bismuth itself has been long thought to be topologically trivial. A recent study has, however, shown that bismuth is in fact a higher-order topological insulator featuring one-dimensional (1D) topological hinge states protected by threefold rotational and inversion symmetries. In this paper, we uncover another hidden facet of the band topology of bismuth by showing that bismuth is also a first-order topological crystalline insulator protected by a twofold rotational symmetry. As a result, its (11¯0) surface exhibits a pair of gapless Dirac surface states. Remarkably, these surface Dirac cones are “unpinned” in the sense that they are not restricted to locate at specific k points in the (11¯0) surface Brillouin zone. These unpinned 2D Dirac surface states could be probed directly via various spectroscopic techniques. Our analysis also reveals the presence of a distinct, previously uncharacterized set of 1D topological hinge states protected by the twofold rotational symmetry. Our study thus provides a comprehensive understanding of the topological band structure of bismuth.

Multiferroic materials have garnered wide interest for their exceptional static and dynamical magnetoelectric properties. In particular, type-II multiferroics exhibit an inversion-symmetry-breaking magnetic order which directly induces a ferroelectric polarization through various mechanisms, such as the spin-current or the inverse Dzyaloshinskii-Moriya effect. This intrinsic coupling between the magnetic and dipolar order parameters results in record-strength magnetoelectric effects. Two dimensional materials possessing such intrinsic multiferroic properties have been long sought for harnessing magnetoelectric coupling in nanoelectronic devices. Here, we report the discovery of type-II multiferroic order in a single atomic layer of the transition metal-based van der Waals material NiI2. The multiferroic state of NiI2 is characterized by a proper-screw spin helix with given handedness, which couples to the charge degrees of freedom to produce a chirality-controlled electrical polarization. We use circular dichroic Raman measurements to directly probe the magneto-chiral ground state and its electromagnon modes originating from dynamic magnetoelectric coupling. Using birefringence and second-harmonic generation measurements, we detect a highly anisotropic electronic state simultaneously breaking three-fold rotational and inversion symmetry, and supporting polar order. The evolution of the optical signatures as a function of temperature and layer number surprisingly reveals an ordered magnetic, polar state that persists down to the ultrathin limit of monolayer NiI2. These observations establish NiI2 and transition metal dihalides as a new platform for studying emergent multiferroic phenomena, chiral magnetic textures and ferroelectricity in the two-dimensional limit.

Photoexcitation by an intense laser pulse can alter the free energy landscape of a solid so that it can access states of matter that do not normally exist in thermal equilibrium. Discoveries of such light-induced states are often found in materials that host phase competition, where one state of matter lies in close proximity to another and photoexcitation provides sufficient energy to overcome the barrier between the neighboring phases. Here, we study the rare-earth tritelluride family (RTe3): It possesses two nearly-equivalent and competing charge density waves (CDWs) in equilibrium, out of which one dominates over the other due to a small lattice anisotropy. When both CDWs are present, such as in ErTe3, an optical pulse transiently weakens both orders. If only the dominant CDW exists, such as in LaTe3, this order is suppressed by photoexcitation while the subdominant density wave emerges. The light-induced subdominant CDW is distinct from its equilibrium counterpart. Nonetheless, this light-induced CDW relaxes at the same time when the original CDW is re-established, indicating a strong phase competition between the two in the out-of-equilibrium regime. Our results provide a framework for understanding the interplay between competing orders and for unleashing novel states of matter that are "trapped" under equilibrium conditions.

Using density functional theory, we study the lattice dynamical properties of magnetite (Fe$_3$O$_4$) in the high-temperature cubic and low-temperature monoclinic phases. The calculated phonon dispersion curves and phonon density of states are compared with the available experimental data obtained by inelastic neutron, inelastic x-ray, and nuclear inelastic scattering. We find a very good agreement between the theoretical and experimental results for the monoclinic $Cc$ structure revealing the strong coupling between charge-orbital (trimeron) order and specific phonon modes. For the cubic phase, clear discrepancies arise which, remarkably, can be understood assuming that the strong trimeron-phonon coupling can be extended above the Verwey transition, with lattice dynamics influenced by the short-range trimeron order instead of the average cubic structure. Our results establish the validity of trimerons (and trimeron-phonon coupling) in explaining the physics of magnetite much beyond their original formulation., Comment: 11 pages, 9 figures, 1 table

The constituent particles of matter can arrange themselves in various ways, giving rise to emergent phenomena that can be surprisingly rich and often cannot be understood by studying only the individual constituents. Discovering and understanding the emergence of such phenomena in quantum materials-especially those in which multiple degrees of freedom or energy scales are delicately balanced-is of fundamental interest to condensed-matter research1,2. Here we report on the surprising observation of emergent ferroelectricity in graphene-based moire heterostructures. Ferroelectric materials show electrically switchable electric dipoles, which are usually formed by spatial separation between the average centres of positive and negative charge within the unit cell. On this basis, it is difficult to imagine graphene-a material composed of only carbon atoms-exhibiting ferroelectricity3. However, in this work we realize switchable ferroelectricity in Bernal-stacked bilayer graphene sandwiched between two hexagonal boron nitride layers. By introducing a moire superlattice potential (via aligning bilayer graphene with the top and/or bottom boron nitride crystals), we observe prominent and robust hysteretic behaviour of the graphene resistance with an externally applied out-of-plane displacement field. Our systematic transport measurements reveal a rich and striking response as a function of displacement field and electron filling, and beyond the framework of conventional ferroelectrics. We further directly probe the ferroelectric polarization through a non-local monolayer graphene sensor. Our results suggest an unconventional, odd-parity electronic ordering in the bilayer graphene/boron nitride moire system. This emergent moire ferroelectricity may enable ultrafast, programmable and atomically thin carbon-based memory devices.

We formulate a dynamical model to describe a photo-induced charge density wave (CDW) quench transition and apply it to recent multi-probe experiments on LaTe$_3$ [A. Zong et al., Nat. Phys. 15, 27 (2019)]. Our approach relies on coupled time-dependent Ginzburg-Landau equations tracking two order parameters that represent the modulations of the electronic density and the ionic positions. We aim at describing the amplitude of the order parameters under the assumption that they are homogeneous in space. This description is supplemented by a three-temperature model, which treats separately the electronic temperature, temperature of the lattice phonons with stronger couplings to the electronic subsystem, and temperature of all other phonons. The broad scope of available data for LaTe$_3$ and similar materials as well as the synergy between different time-resolved spectroscopies allow us to extract model parameters. The resulting calculations are in good agreement with ultra-fast electron diffraction experiments, reproducing qualitative and quantitative features of the CDW amplitude evolution during the initial few picoseconds after photoexcitation., Comment: 21 pages, 14 figures; this version is almost identical to the published version; comparing to the earlier arXiv submission, current version contains a new figure (Fig.10), and a broader discussion of theoretical results and approximations

When electrons in a solid are excited by light, they can alter the free energy landscape and access phases of matter that are out of reach in thermal equilibrium. This accessibility becomes important in the presence of phase competition, when one state of matter is preferred over another by only a small energy scale that, in principle, is surmountable by the excitation. Here, we study a layered compound, LaTe3, where a small lattice anisotropy in the a–c plane results in a unidirectional charge density wave (CDW) along the c axis1,2. Using ultrafast electron diffraction, we find that, after photoexcitation, the CDW along the c axis is weakened and a different competing CDW along the a axis subsequently emerges. The timescales characterizing the relaxation of this new CDW and the reestablishment of the original CDW are nearly identical, which points towards a strong competition between the two orders. The new density wave represents a transient non-equilibrium phase of matter with no equilibrium counterpart, and this study thus provides a framework for discovering similar states of matter that are ‘trapped’ under equilibrium conditions. Short pulses of light shift the balance between two competing charge density wave phases, allowing the weaker one to manifest transiently while suppressing the stronger one. This shows that competing phases can be tuned in a non-equilibrium setting.

The Verwey transition in magnetite (Fe$_3$O$_4$) is the first metal-insulator transition ever observed and involves a concomitant structural rearrangement and charge-orbital ordering. Due to the complex interplay of these intertwined degrees of freedom, a complete characterization of the low-temperature phase of magnetite and the mechanism driving the transition have long remained elusive. It was demonstrated in recent years that the fundamental building blocks of the charge-ordered structure are three-site small polarons called trimerons. However, electronic collective modes of this trimeron order have not been detected to date, and thus an understanding of the dynamics of the Verwey transition from an electronic point of view is still lacking. Here, we discover spectroscopic signatures of the low-energy electronic excitations of the trimeron network using terahertz light. By driving these modes coherently with an ultrashort laser pulse, we reveal their critical softening and hence demonstrate their direct involvement in the Verwey transition. These findings represent the first observation of soft modes in magnetite and shed new light on the cooperative mechanism at the origin of its exotic ground state., Comment: 20 pages, 18 figures

Upon excitation with an intense laser pulse, a symmetry-broken ground state can undergo a non-equilibrium phase transition through pathways different from those in thermal equilibrium. The mechanism underlying these photoinduced phase transitions has long been researched in the study of condensed matter systems1, but many details in this ultrafast, non-adiabatic regime still remain to be clarified. To this end, we investigate the light-induced melting of a unidirectional charge density wave (CDW) in LaTe3. Using a suite of time-resolved probes, we independently track the amplitude and phase dynamics of the CDW. We find that a fast (approximately 1 picosecond) recovery of the CDW amplitude is followed by a slower re-establishment of phase coherence. This longer timescale is dictated by the presence of topological defects: long-range order is inhibited and is only restored when the defects annihilate. Our results provide a framework for understanding other photoinduced phase transitions by identifying the generation of defects as a governing mechanism. Three different ultrafast probes investigate a non-adiabatic phase transition and find substantial evidence of topological defects inhibiting the reformation of the equilibrium phase.

The emergent phenomena that characterize quantum materials have received prominent exposure thanks to experimental techniques based on photoemission. In turn, the challenges and opportunities presented by quantum materials have driven improvements in the photoemission technology itself.

We report a rare atom-like interaction between excitons in monolayer WS2, measured using ultrafast absorption spectroscopy. At increasing excitation density, the exciton resonance energy exhibits a pronounced redshift followed by an anomalous blueshift. Using both material-realistic computation and phenomenological modeling, we attribute this observation to plasma effects and an attraction-repulsion crossover of the exciton-exciton interaction that mimics the Lennard-Jones potential between atoms. Our experiment demonstrates a strong analogy between excitons and atoms with respect to inter-particle interaction, which holds promise to pursue the predicted liquid and crystalline phases of excitons in two-dimensional materials.

Coherent light-matter interaction can be used to manipulate the energy levels of atoms, molecules and solids. When light with frequency {\omega} is detuned away from a resonance {\omega}o, repulsion between the photon-dressed (Floquet) states can lead to a shift of energy resonance. The dominant effect is the optical Stark shift (1/({\omega}0-{\omega})), but there is an additional contribution from the so-called Bloch-Siegert shift (1/({\omega}o+{\omega})). Although it is common in atoms and molecules, the observation of Bloch-Siegert shift in solids has so far been limited only to artificial atoms since the shifts were small (

The notion of spontaneous symmetry breaking has been used to describe phase transitions in a variety of physical systems. In crystalline solids, the breaking of certain symmetries, such as mirror symmetry, is difficult to detect unambiguously. Using 1$T$-TaS$_2$, we demonstrate here that rotational-anisotropy second harmonic generation (RA-SHG) is not only a sensitive technique for the detection of broken mirror symmetry, but also that it can differentiate between mirror symmetry-broken structures of opposite planar chirality. We also show that our analysis is applicable to a wide class of different materials with mirror symmetry-breaking transitions. Lastly, we find evidence for bulk mirror symmetry-breaking in the incommensurate charge density wave phase of 1$T$-TaS$_2$. Our results pave the way for RA-SHG to probe candidate materials where broken mirror symmetry may play a pivotal role., 13 pages, 10 figures. Edited (v2) to include Bilal G\"okce in the authors list who was mistakenly excluded. Edited again (v3) to incorporate modifications recommended by referees. Replaced (v4) with version published in Physical Review B

Revealing the spin excitations of complex quantum magnets is key to developing a minimal model that explains the underlying magnetic correlations in the ground state. We investigate the low-energy magnons in $\alpha$-RuCl$_3$ by combining time-domain terahertz spectroscopy under an external magnetic field and model Hamiltonian calculations. We observe two absorption peaks around 2.0 and 2.4 meV, which we attribute to zone-center spin waves. Using linear spin-wave theory with only nearest-neighbor terms of the exchange couplings, we calculate the antiferromagnetic resonance frequencies and reveal their dependence on an external field applied parallel to the nearest-neighbor Ru-Ru bonds. We find that the magnon behavior in an applied magnetic field can be understood only by including an off-diagonal $\Gamma$ exchange term to the minimal Heisenberg-Kitaev model. Such an anisotropic exchange interaction that manifests itself as a result of strong spin-orbit coupling can naturally account for the observed mixing of the modes at higher fields strengths., Comment: 13 pages, 9 figures

Rotational-symmetry-protected topological crystalline insulators (TCIs) are expected to host unique boundary modes, in that the surface normal to the rotational axis can feature surface states with ‘unpinned’ Dirac points, which are not constrained to lie on high symmetry points or lines, but can lie at any general k point in the Brillouin zone. Also, as a higher order bulk boundary correspondence is involved here, a three-dimensional (3D) TCI can support one-dimensional (1D) helical edge states. Using first-principles band structure calculations, we identify the van der Waals material -Bi4Br4 as a purely rotation symmetry protected TCI. We show that the surface of Bi4Br4 exhibits a pair of unpinned topological Dirac fermions which are related to the presence of a two-fold rotation axis. These unpinned Dirac fermions possess an exotic spin texture which will be highly favorable for spin transport, and a band structure that consists of van Hove singularities due to a Lifshitz transition. We also identify 1D topological hinge states along the edges of an -Bi4Br4 rod. We comment on how the predicted topological features in -Bi4Br4 could be accessed experimentally.

Complex systems, which consist of a large number of interacting constituents, often exhibit universal behavior near a phase transition. A slowdown of certain dynamical observables is one such recurring feature found in a vast array of contexts. This phenomenon, known as critical slowing down, is well studied mostly in thermodynamic phase transitions. However, it is less understood in highly nonequilibrium settings, where the time it takes to traverse the phase boundary becomes comparable to the timescale of dynamical fluctuations. Using transient optical spectroscopy and femtosecond electron diffraction, we studied a photo-induced transition of a model charge-density-wave (CDW) compound, LaTe$_3$. We observed that it takes the longest time to suppress the order parameter at the threshold photoexcitation density, where the CDW transiently vanishes. This finding can be quantitatively captured by generalizing the time-dependent Landau theory to a system far from equilibrium. The experimental observation and theoretical understanding of dynamical slowing down may offer insight into other general principles behind nonequilibrium phase transitions in many-body systems.

The combination of EUV based time-resolved Angle-Resolved-Photo-Electron-Spectroscopy (trARPES), Ultrafast-Electron-Diffraction (UED) and Transient-Optical-Spectroscopy (TOS) facilitates a comprehensive study and all-embracing analysis of correlated dynamics, exemplified on the system of Charge-Density-Waves (CDW’s) in rare earth tritellurides (RTe3).

Topological semimetals with different types of band crossings provide a rich platform to realize novel fermionic excitations, known as topological fermions. In particular, some fermionic excitations can be direct analogues of elementary particles in quantum field theory when both obey the same laws of physics in the low-energy limit. Examples include Dirac and Weyl fermions, whose solid-state realizations have provided new insights into long-sought phenomena in high-energy physics. Recently, theorists predicted new types of fermionic excitations in condensed-matter systems without any high-energy counterpart, and their existence is protected by crystalline symmetries. By studying the topology of the electronic structure in PdBiSe using density functional theory calculations and bulk-sensitive soft X-ray angle-resolved photoemission spectroscopy, we demonstrate a coexistence of four different types of topological fermions: Weyl, Rarita-Schwinger-Weyl, double class-II three-component, and charge-2 fourfold fermions. Our discovery provides a remarkable platform to realize multiple novel fermions in a single solid, charting the way forward to studies of their potentially exotic properties as well as their interplay.

Upon excitation by a laser pulse, broken-symmetry phases of a wide variety of solids demonstrate similar order parameter dynamics characterized by a dramatic slowing down of relaxation for stronger pump fluences. Motivated by this recurrent phenomenology, we develop a simple non-perturbative effective model of dynamics of collective bosonic excitations in pump-probe experiments. We find that as the system recovers after photoexcitation, it shows universal prethermalized dynamics manifesting a power-law, as opposed to exponential, relaxation, explaining the slowing down of the recovery process. For strong quenches, long-wavelength over-populated transverse modes dominate the long-time dynamics; their distribution function exhibits universal scaling in time and space, whose universal exponents can be computed analytically. Our model offers a unifying description of order parameter fluctuations in a regime far from equilibrium, and our predictions can be tested with available time-resolved techniques.

Coherent optical dressing of quantum materials offers technological advantages to control their electronic properties, such as the electronic valley degree of freedom in monolayer transition metal dichalcogenides (TMDs). Here, we observe a new type of optical Stark effect in monolayer WS2, one that is mediated by intervalley biexcitons under the blue-detuned driving with circularly polarized light. We found that such helical optical driving not only induces an exciton energy downshift at the excitation valley, but also causes an anomalous energy upshift at the opposite valley, which is normally forbidden by the exciton selection rules but now made accessible through the intervalley biexcitons. These findings reveal the critical, but hitherto neglected, role of biexcitons to couple the two seemingly independent valleys, and to enhance the optical control in valleytronics.

Ultrafast electron thermalization—the process leading to carrier multiplication via impact ionization and hot-carrier luminescence —occurs when optically excited electrons in a material undergo rapid electron–electron scattering to redistribute excess energy and reach electronic thermal equilibrium. Owing to extremely short time and length scales, the measurement and manipulation of electron thermalization in nanoscale devices remains challenging even with the most advanced ultrafast laser techniques. Here, we overcome this challenge by leveraging the atomic thinness of two-dimensional van der Waals (vdW) materials to introduce a highly tunable electron transfer pathway that directly competes with electron thermalization. We realize this scheme in a graphene–boron nitride–graphene (G–BN–G) vdW heterostructure through which optically excited carriers are transported from one graphene layer to the other. By applying an interlayer bias voltage or varying the excitation photon energy, interlayer carrier transport can be controlled to occur faster or slower than the intralayer scattering events, thus effectively tuning the electron thermalization pathways in graphene. Our findings, which demonstrate a means to probe and directly modulate electron energy transport in nanoscale materials, represent a step towards designing and implementing optoelectronic and energy-harvesting devices with tailored microscopic properties., United States. Air Force Office of Scientific Research (FA9550-11-1-0225), National Science Foundation (U.S.) (DMR-1231319)

Topological defects, potential information carriers, were written into and erased from a solid with femtosecond light pulses., Domain walls (DWs) are singularities in an ordered medium that often host exotic phenomena such as charge ordering, insulator-metal transition, or superconductivity. The ability to locally write and erase DWs is highly desirable, as it allows one to design material functionality by patterning DWs in specific configurations. We demonstrate such capability at room temperature in a charge density wave (CDW), a macroscopic condensate of electrons and phonons, in ultrathin 1T-TaS2. A single femtosecond light pulse is shown to locally inject or remove mirror DWs in the CDW condensate, with probabilities tunable by pulse energy and temperature. Using time-resolved electron diffraction, we are able to simultaneously track anti-synchronized CDW amplitude oscillations from both the lattice and the condensate, where photoinjected DWs lead to a red-shifted frequency. Our demonstration of reversible DW manipulation may pave new ways for engineering correlated material systems with light.

The broadband photothermoelectric effect has been studied on a graphene-2D semiconductor lateral heterojunction., The massless Dirac electron transport in graphene has led to a variety of unique light-matter interaction phenomena, which promise many novel optoelectronic applications. Most of the effects are only accessible by breaking the spatial symmetry, through introducing edges, p-n junctions, or heterogeneous interfaces. The recent development of direct synthesis of lateral heterostructures offers new opportunities to achieve the desired asymmetry. As a proof of concept, we study the photothermoelectric effect in an asymmetric lateral heterojunction between the Dirac semimetallic monolayer graphene and the parabolic semiconducting monolayer MoS2. Very different hot-carrier cooling mechanisms on the graphene and the MoS2 sides allow us to resolve the asymmetric thermalization pathways of photoinduced hot carriers spatially with electrostatic gate tunability. We also demonstrate the potential of graphene-2D semiconductor lateral heterojunctions as broadband infrared photodetectors. The proposed structure shows an extreme in-plane asymmetry and provides a new platform to study light-matter interactions in low-dimensional systems.

Heterostructures of topological insulators and ferromagnets offer new opportunities in spintronics and a route to novel anomalous Hall states. In one such structure, EuS/${\mathrm{Bi}}_{2}{\mathrm{Se}}_{3}$, a dramatic enhancement of the Curie temperature was recently observed. We performed Raman spectroscopy on a similar set of thin films to investigate the magnetic and lattice excitations. Interfacial strain was monitored through its effects on the ${\mathrm{Bi}}_{2}{\mathrm{Se}}_{3}$ phonon modes while the magnetic system was probed through the EuS Raman mode. Despite its appearance in bare EuS, the heterostructures lack the corresponding EuS Raman signal. Through numerical calculations we rule out the possibility of Fabry-Perot interference suppressing the mode. Direct measurements of the magnetic system also eliminate room temperature ordering from suppressing the mode. We therefore attribute the absence of a magnetic signal in EuS to a charge transfer with the ${\mathrm{Bi}}_{2}{\mathrm{Se}}_{3}$. This could provide an additional pathway for manipulating the magnetic, optical, or electronic response of topological heterostructures.

Coherent light-matter interaction can be used to manipulate the energy levels of atoms, molecules and solids. When light with frequency ω is detuned away from a resonance ω 0 , repulsion between the photon-dressed (Floquet) states can lead to a shift of energy resonance. The dominant effect is the optical Stark shift (∝ 1/( ω 0 − ω)), but there is an additional contribution from the so-called Bloch-Siegert shift (∝ 1/( ω 0 + ω)). Although it is common in atoms and molecules, the observation of Bloch-Siegert shift in solids has so far been limited only to artificial atoms since the shifts were small ( 2 under infrared optical driving by virtue of the strong light-matter interaction in this system. Moreover, we can disentangle the Bloch-Siegert shift entirely from the optical Stark shift, because the two effects are found to obey opposite selection rules at different valleys. By controlling the light helicity, we can confine the Bloch-Siegert shift to occur only at one valley, and the optical Stark shift at the other valley. Such a valley-exclusive Bloch-Siegert shift allows for enhanced control over the valleytronic properties in two-dimensional materials, and offers a new avenue to explore quantum optics in solids.

Topological crystalline insulators (TCI) are insulating electronic phases of matter with nontrivial topology originating from crystalline symmetries. Recent theoretical advances have provided powerful guidelines to search for TCIs in real materials. Using density functional theory, we identify a class of new TCI states in the tetragonal lattice of the Ca$_2$As material family. On both top and side surfaces, we observe topological surface states protected independently by rotational and mirror symmetries. We show that a particular lattice distortion can single out the newly proposed topological protection by the rotational symmetry. As a result, the Dirac points of the topological surface states are moved to generic locations in momentum space away from any high symmetry lines. Such topological surface states have not been seen before. Moreover, the other family members, including Ca$_2$Sb, Ca$_2$Bi and Sr$_2$Sb, feature different topological surface states due to their distinct topological invariants. We thus further propose topological phase transitions in the pseudo-binary systems such as (Ca$_{1-x}$Sr$_x$)$_2$As and Ca$_2$As$_x$Sb$_{1-x}$. Our work reveals rich and exotic TCI physics across the Ca$_2$As family of materials, and suggests the feasibility of materials database search methods to discover new TCIs., 5 pages, 4 figures