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 Ca2RuO4 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. Searches for metastable states with properties not found in thermal equilibrium have been restricted to either ultrafast or slow timescales. A metastable state in an intermediate time window has now been identified in a photo-doped Mott insulator.

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 Sr2IrO4 and Sr3Ir2O7, we show using time-resolved THz spectroscopy that excitons exist only 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.

Coherent manipulation of magnetism through the lattice provides opportunities for controlling spintronic functionalities on the ultrafast timescale. Such nonthermal control typically involves nonlinear excitation of Raman-active phonons which are coupled to the magnetic order. Linear excitation, in contrast, holds potential for more efficient and selective modulation of magnetic properties. However, since the linear excitation of Raman-active phonons is conventionally considered forbidden in inversion symmetric quantum materials, the simultaneous linear and nonlinear excitation of a collective mode involving lattice component has remained elusive. Here, we harness strong coupling between magnons and Raman-active phonons to achieve both linear and quadratic excitation regimes of magnon-polarons, magnon-phonon hybrid quasiparticles. We demonstrate this by driving magnon-polarons with an intense terahertz pulse in the van der Waals antiferromagnet FePS3. Such excitation behavior enables a unique way to coherently control the amplitude of magnon-polaron oscillations by tuning the terahertz field strength and its polarization. The polarimetry of the resulting coherent oscillation amplitude breaks the crystallographic C2 symmetry due to strong interference between different excitation channels. Our findings unlock a wide range of possibilities to manipulate material properties, including modulation of exchange interactions by phonon-Floquet engineering.

In 1964, Keldysh laid the groundwork for strong-field physics in atomic, molecular, and solid-state systems by delineating a ubiquitous transition from multiphoton absorption to classical field-driven electron tunneling under intense electromagnetic waves. While both processes in semiconductors can generate carriers and result in photon emission through electron-hole recombination, the low quantum yields in most materials have hindered direct observation of the Keldysh crossover. Leveraging the large quantum yields of photoluminescence in lead halide perovskites, we show that we can not only induce bright light emission from extreme subbandgap excitation but also distinguish between photon-induced and electric-field-induced processes. Our results span the transition between quantum-mechanical and classical field effects of the light and provide generalizable insights into the nonequilibrium dynamics that result from strong-field light-matter interactions. The findings also open avenues for light upconversion and subbandgap photon detection, highlighting the potential of lead halide perovskites in advanced optoelectronic applications.

Second-order superlattices emerge from the interference between moir & eacute; superlattices of comparable periodicities. Direct real-space visualization reveals their rich structural diversity and extreme sensitivity to external parameters such as strain and twist angle.

The kagome superconductor CsV3Sb5 hosts a variety of charge density wave (CDW) phases, which play a fundamental role in the formation of other exotic electronic instabilities. However, identifying the precise structure of these CDW phases and their intricate relationships remain the subject of intense debate, due to the lack of static probes that can distinguish the CDW phases with identical spatial periodicity. Here, we unveil the out-of-equilibrium competition between two coexisting 2 × 2 × 2 CDWs in CsV3Sb5 harnessing time-resolved X-ray diffraction. By analyzing the light-induced changes in the intensity of CDW superlattice peaks, we demonstrate the presence of both phases, each displaying a significantly different amount of melting upon excitation. The anomalous light-induced sharpening of peak width further shows that the phase that is more resistant to photo-excitation exhibits an increase in domain size at the expense of the other, thereby showcasing a hallmark of phase competition. Our results not only shed light on the interplay between the multiple CDW phases in CsV3Sb5, but also establish a non-equilibrium framework for comprehending complex phase relationships that are challenging to disentangle using static techniques. The interplay between charge density wave states in emerging kagome superconductors is a topic of ongoing debate. Here, the authors unveil the out-of-equilibrium competition between two coexisting charge density waves in CsV3Sb5 by harnessing time-resolved X-ray diffraction.

Chirality, the breaking of improper rotational symmetry, is a fundamental concept spanning diverse scientific domains. In condensed matter physics, chiral phonons, originating from circular atomic motions that carry angular momentum, have sparked intense interest due to their coupling to magnetic degrees of freedom, enabling potential phonon-controlled spintronics. However, modes and their counter-rotating counterparts are typically degenerate at the Brillouin zone center. Selective excitation of a single-handed circulating phonon requires external stimuli that break the degeneracy. Whether energetically nondegenerate circularly polarized phonons can appear spontaneously without structural or external symmetry breaking remains an open question. Here, we demonstrate that nondegenerate elliptically polarized phonon pairs can be induced by coupling to magnons with same helicity in the van der Waals antiferromagnet FePSe_3. We confirm the presence of magnon-phonon hybrids, also known as magnon polarons, which exhibit inherent elliptical polarization with opposite helicities and distinct energies. This nondegeneracy enables their coherent excitation with linearly polarized terahertz pulses, which also endows these rotating modes with chirality. By tuning the polarization of the terahertz drive and measuring phase-resolved polarimetry of the resulting coherent oscillations, we determine the ellipticity and map the trajectory of these hybrid quasiparticles. Our findings establish a general approach to search for intrinsically nondegenerate phonons with angular momentum at the center of the Brillouin zone and introduce a new methodology for characterizing their ellipticity, outlining a roadmap towards chiral-phonon-controlled spintronic functionalities.

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 experimentally detected. 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 intraexcitonic 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 the Mott gap size, implying extremely strong coupling to magnon modes.

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.

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-fs pump pulse duration. By sweeping the electric field amplitude, we demonstrate continuous bandwidth tuning and a Keldysh crossover from a multiphoton 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.

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.

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 Letter expands the field of ultrafast order parameter control beyond spin and charge ordered materials.

The bands are formed by the quasi-one-dimensional lattice and i, k are the corresponding lattice sites and momentum. Each operator and parameter is defined in the main text. We also set ~ = 1 for simplicity. The equations of motion for the complex exciton order parameter Φi = 〈civi〉 and the real lattice displacement Xi = 〈bi + bi〉 can be obtain by expressing Eq. (1) in terms of a nonequilibrium path integral (i.e. in the Keldysh framework) and introducing Φ as a dynamic, bosonic Hubbard-Stratonovich field. This allows one to integrate out the fermionic modes and derive the equations of motion for Φ, X via saddle point equations. In a path integral approach, the partition function Z corresponding to the Hamiltonian in Eq. (1) is formally obtained from a field integral of the form

We theoretically predict and experimentally demonstrate a nonthermal pathway to optically enhance superexchange interaction energies in a material based on exciting ligand-to-metal charge-transfer transitions, which introduces lower-order virtual hopping contributions that are absent in the ground state. We demonstrate this effect in the layered ferromagnetic insulator CrSiTe_{3} by exciting Te-to-Cr charge-transfer transitions using ultrashort laser pulses and detecting coherent phonon oscillations that are impulsively generated by superexchange enhancement via magneto-elastic coupling. This mechanism kicks in below the temperature scale where short-range in-plane spin correlations begin to develop and disappears when the excitation energy is tuned away from the charge-transfer resonance, consistent with our predictions.

Background The prognostic significance of misfolded alpha-synuclein (alpha-Syn) aggregates in Parkinson's disease (PD) has not been well investigated. The aim of this study was to reveal the relationship between misfolded alpha-Syn aggregate concentration in cerebrospinal fluid (CSF) and cognitive decline risk in PD. Methods A total of 278 patients with PD were retrospectively included. They were diagnosed between 2011 and 2013. The end-point was 2016, and the follow-up period was 54.3 +/- 10.0 months. Cognitive decline was defined as a 4-point decrease in the Mini-Mental State Examination score during follow-up. Misfolded alpha-Syn aggregate concentration in baseline CSF was measured using the protein misfolding cyclic amplification (PMCA) technique. Time to reach 50% of the maximum fluorescence value was recorded. Results The PMCA technique successfully detected the level of misfolded alpha-Syn aggregates in CSF with a sensitivity of 85.3% and a specificity of 91.4%. The time to reach 50% of the maximum fluorescence value was shorter in the patients with cognitive decline than in the patients without cognitive decline (190.7 +/- 40.1 h vs. 240.8 +/- 45.6 h, P < 0.001). Multifactorial Cox regression analysis revealed that reaching 50% of the maximum fluorescence value in <= 219 h at baseline was associated with increased risk of cognitive decline during the follow-up (HR: 4.90, 95% CI: 2.75-8.74, P < 0.001). Conclusion Baseline concentration of misfolded alpha-Syn aggregates in CSF measured by the PMCA technique predicts risk of cognitive decline in PD.

Submitted for the MAR16 Meeting of The American Physical Society Negative to Positive Crossover of Magnetoresistance in WS2 nanoflakes with Ohmic Contact YANGWEI ZHANG, HONGLIE NING, YANAN LI, YANZHAO LIU, JIANWANG1, —We report studies on the transport measurements of WS2 nanoflakes including contact optimization and magnetoresistance measurement. We find that the platinum electrodes deposited by focused ion beam (FIB) technology on WS2 exhibit an ohmic contact, which provides a pathway to solve the dilemma of Shottky barrier for WS2 devices. A temperature-modulated negative-to-positive crossover of magnetoresistance (MR) is also observed, replenishing the existing data which mainly emphasizes field effect transistor (FET) related transport. Our work may stimulate further studies and potential electronic and optoelectronic applications on transition-metal dichalcogenides. 1

The discovery of graphene has ignited intensive investigation on two dimensional (2D) materials. Among them, transition metal dichalcogenide (TMDC), a typical representative, attracts much attention due to the excellent performance in field effect transistor (FET) related measurements and applications. Particularly, when TMDC eventually reaches few-layer dimension, a wide range of electronic and optical properties, in striking contrast to bulk samples, are detected. In this Letter, we synthesized single crystalline WS2 nanoflakes by physical vapor deposition (PVD) method and carried out a series of transport measurements of contact resistance and magnetoresistance. Focused ion beam (FIB) technology was applied to deposit Pt electrodes on WS2 flakes. Different from the electron beam lithography (EBL) fabricated electrodes, FIB-deposited leads exhibited ohmic contact, resolving the dilemma of Schottky barrier. Furthermore, a temperature-modulated negative-to-positive transition of magnetoresistance (MR) associated with a crossover of carrier type at similar temperature was demonstrated. Our work offers a pathway to optimize the contact for TMDC and reveals the magnetoresistance characteristics of WS2 flakes, which may stimulate further studies on TMDC and corresponding potential electronic and optoelectronic applications.

The telomeric protein TRF2, involving in telomeric and extratelomeric DNA damage response, has been previously reported to facilitate multidrug resistance (MDR) in gastric cancer cells by interfering ATM-dependent DNA damage response induced by anticancer drugs. Rap1 is the TRF2-interacting protein in the shelterin complex. Complex formation between Rap1 and TRF2 is essential for their function in telomere and end protection. Here we focus on the effects of Rap1 on TRF2 function in DNA damage response induced by anticancer drugs. Both Rap1 and TRF2 expression were upregulated in SGC7901 and its MDR variant SGC7901/VCR after etoposide treatment, which was more marked in SGC7901/VCR than in SGC7901. Rap1 silencing by siRNA in SGC7901/VCR partially reversed the etoposide resistance. And Rap1 silencing partially reversed the TRF2-mediated resistance to etoposide in SGC7901. Rap1 silencing did not affect the TRF2 upregulation induced by etoposide, but eliminated the inhibition effect of TRF2 on ATM expression and ATM phosphorylation at serine 1981 (ATM pS1981). Furthermore, phosphorylation of ATM targets, including γH2AX and serine 15 (S15) on p53, were increased in Rap1 silencing cells in response to etoposide. Thus, we confirm that Rap1, interacting with TRF2 in the shelterin complex, also has an important role in TRF2-mediated DNA damage response in gastric cancer cells treated by etoposide.