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Near-infrared (NIR) pump-terahertz (THz) probe spectroscopy is used to investigate the charge and spin exciations in a strongly correlated electron compound Na0.5CoO2. This compound exhibits a coexistence of various charge and spin orders arising from intricate interactions among charge, spin, and orbital degrees of freedom. NIR pulses create significantly diverse effects on the charge and spin orders; while the charge order is easily melted,coherent magnon excitations are present in all fluences examined. Furthermore, a novel {\pi} phase shift of the coherent magnon oscillations is observed in the pump-induced change of the terahertz electric field between regions of increasing and decreasing field change. These results unequivocally illustrate that ultrashort laser pulses enable the disentanglement of different interactions within complex systems characterized by multiple orders, providing a fresh perspective on the interplay between itinerant and localized electrons within the Co 3d t2g multiplets.

Ultrafast light-matter interaction has emerged as a powerful tool to control and probe the macroscopic properties of functional materials, especially two-dimensional transition metal dichalcogenides which can form different structural phases with distinct physical properties. However, it is often difficult to accurately determine the transient optical constants. In this work, we developed a near-infrared pump - terahertz to midinfrared (12-22 THz) probe system in transmission geometry to measure the transient optical conductivity in 2H-MoTe2 layered material. By performing separate measurements on bulk and thin-film samples, we are able to overcome issues related to nonuniform substrate thickness and penetration depth mismatch and to extract the transient optical constants reliably. Our results show that photoexcitation at 690 nm induces a transient insulator-metal transition, while photoexcitation at 2 um has a much smaller effect due to the photon energy being smaller than the band gap of the material. Combining this with a single-color pump-probe measurement, we show that the transient response evolves towards 1T' phase at higher flunece. Our work provides a comprehensive understanding of the photoinduced phase transition in the 2H-MoTe2 system., Comment: 9 pages, 11 figures

The ultrafast manipulation of quantum material has led to many novel and significant discoveries. Among them, the light-induced transient superconductivity in cuprates achieved by melting competing stripe orders represents a highly appealing accomplishment. However, recent investigations have shown that the notion of photoinduced superconductivity remains a topic of controversy, and its elucidation solely through c-axis time-resolved terahertz spectroscopy remains an arduous task. Here, we measure the in-plane and out-of-plane transient terahertz responses simultaneously in the stripe-ordered non-superconducting La$_{2-x}$Ba$_{x}$CuO$_4$ after near-infrared excitations. We find that although a pump-induced reflectivity edge appears in the c-axis reflectance spectrum, the reflectivity along the CuO$_2$ planes decreases simultaneously, indicating an enhancement in the scattering rate of quasiparticles. This in-plane transient response is clearly distinct from the features associated with superconducting condensation. Therefore, we conclude the out-of-plane transient responses cannot be explained by an equivalent of Josephson tunneling. Notably, those pump-induced terahertz responses remain consistent even when we vary the near-infrared optical pump wavelengths and hole concentrations. Our results provide a critical evidence that transient three-dimensional superconductivity cannot be induced by melting the competing stripe orders with pump pulses whose photon energy is much higher than the superconducting gap of cuprates., Comment: 11 pages, 6 figures

The study of interaction between different degrees of freedom in solids is of fundamental importance to understand the functionalities of materials. One striking example of such interaction is the intertwined coupling or competition between superconductivity (SC), charge density wave (CDW), pseudogap state (PG), and other exotic phases in cuprate superconductors. Recent emergence of nonlinear Terahertz (THz) third harmonic generation (THG) spectroscopy provides a powerful tool for exploring the collective (Higgs) modes of superconductivity order parameters, and its interaction with intertwined/competing phases. In this study, we report on nonlinear THz THG spectroscopy of the YBa$_2$Cu$_3$O$_{6+x}$ (YBCO) thin films with different doping. We identify a characteristic temperature $T_{THG}$, below which third order suscepetility $\chi^{(3)}$ emerges. Notably, the $T_{THG}$ is coincident with the crossover temperature $T^*$ of pseudogap in a wide range doping of phase diagram. Upon entering the superconducting state, THG increases sharply but exhibits an abnormal dip feature near $T_c$ which is more clearly seen in optimally doped sample. Strikingly, we observe a beating structure directly in the measured real time waveform of THG signal. Fourier transformation of the time domain waveform gives two separate modes below and above original THG frequency. The observation strongly indicates that an additional mode, presumably Higgs mode, appears at $T_c$ and couples to the mode already developed below $T^*$. The strong coupling effect offers new insight into the interplay between superconductivity and pseudogap. The result unambiguously suggests that the pseudogap phase is not a precursor of superconductivity but represents a distinct order.

Kagome magnet TbMn$_6$Sn$_6$ is a new type of topological material that is known to support exotic quantum magnetic states. Experimental work has identified that TbMn$_6$Sn$_6$ hosts Dirac electronic states that could lead to topological and Chern quantum phases, but the optical response of the Dirac fermions of TbMn$_6$Sn$_6$ and its properties remain to be explored. Here, we perform optical spectroscopy measurement combined with first-principles calculations on single-crystal sample of TbMn$_6$Sn$_6$ to investigate the associated exotic phenomena. TbMn$_6$Sn$_6$ exhibits frequency-independent optical conductivity spectra in a broad range from 1800 to 3000 cm$^{-1}$ (220-370 meV) in experiments. The theoretical band structures and optical conductivity spectra are calculated with several shifted Fermi energy to compare with the experiment. The theoretical spectra with 0.56 eV shift for Fermi energy are well consistent with our experimental results. Besides, the massive quasi-two-dimensional (quasi-2D) Dirac bands, which have linear band dispersion in $k_x$-$k_y$ plane and no band dispersion along the $k_z$ direction, exist close to the shifted Fermi energy. According to tight-binding model analysis, the quasi-2D Dirac bands give rise to a flat optical conductivity, while its value is smaller than, about one tenth of, that from the calculations and experiments. It indicates that the other trivial bands also contribute to the flat optical conductivity.

1T'-TaTe2 exhibits an intriguing first-order structural phase transition at around 170 K. Understanding the electronic structural properties is a crucial way to comprehend the origin of the structural phase transition. We performed a combined optical and ultrafast pump-probe study on the compound across the transition temperature. The phase transition leads to abrupt changes of both optical spectra and ultrafast electronic relaxation dynamics. The measurements revealed a sudden reconstruction of band structure. We elaborate that the phase transition is of the first order and can not be attributed to the conventional density-wave type instability. Our work is illuminating for understanding the origin of the structural phase transition.

We report the observation of two-fold rotation symmetry in charge density wave (CDW) state in the newly discovered Kagome superconductor CsV$_3$Sb$_5$. Below its CDW transition temperature ($T_{CDW}$), the polarization rotation of the reflected laser beam promptly emerges and increases close to about 1 mrad, and the rotation angle shows two-fold rotation symmetry. With femtosecond laser pulse pumping, the rotation angle can be easily suppressed and then recovers in several picoseconds accompanied with coherent oscillations. Significantly, the oscillations in the signal also experience a 180 degree periodic change. Our investigation provides clear optical evidence for the formation of nematic order with two-fold rotation symmetry just below $T_{CDW}$. The results imply a immediate development of nematicity and possible time-reversal symmetry breaking in CDW state of CsV$_3$Sb$_5$., Comment: 6 pages, 3 figures

CuTe is a two-dimensional (2D) layered material, yet forming a quasi-one-dimensional (quasi-1D) charge-density-wave (CDW) along the a-axis in the ab-plane at high transition temperature $T_{CDW}=335$ K. However, the anisotropic properties of CuTe remain to be explored. Here we performed combined transport, polarized infrared reflectivity, and ultrafast pump-probe spectroscopy to investigate the underlying CDW physics of CuTe. Polarized optical measurement clearly revealed that an energy gap gradually forms along the a-axis upon cooling, while optical evidence of gap signature is absent along the b-axis, suggesting pronounced electronic anisotropy in this quasi-2D material. Time-resolved optical reflectivity measurement revealed that the amplitude and relaxation time of photo-excited quasiparticles change dramatically across the CDW phase transition. Taking fast Fourier transformation of the oscillation signals arising from collective excitations, we identify the 1.65-THz mode as the CDW amplitude mode, whose energy softens gradually at elevated temperatures. Consequently, we provide further evidence for the formation of completely anisotropic CDW order in CuTe, which is quite rare in quasi-2D materials., Comment: 6 pages, 4 figures

We present both static and time-resolved second harmonic generation (SHG) measurements on polar antiferromagnet Fe$_2$Mo$_3$O$_8$ to monitor the evolution of the electric polarization change and its coupling to magnetic order. We find that only one of the second order tensor elements, $\chi_{ccc}^{(2)}$ ,shows a prominent change below the Neel temperature $T_N = 60$ K, indicating a magnetic order induced electric polarization change along the c-axis. Time-resolved SHG measurement reveals an ultrafast recovery of the second order tensor element upon the ultrashort laser excitation with fluence above 0.3 $mJ/cm^2$, yielding evidence for a photoinduced ultrafast phase transition from the AFM ordered state to the paramagnetic state. Our work will help understand the spin induced polarization and the ultrafast optical tuning effect in Fe$_{2}$Mo$_{3}$O$_{8}$., Comment: 6 pages. 5 figures

Searching for Kitaev quantum spin liquid (QSL) is a fascinating and challenging problem. Much effort has been devoted to honeycomb lattice candidates with strong spin-orbit coupling in 5d-electron iridates and 4delectron RuCl3. Recently, theoretical studies suggested that the 3d7 Co-based honeycomb materials with high spin state S=3/2 and effective orbital angular momentum L=1 could also be promising candidates of Kitaev QSL. One of the candidates, BaCo2(AsO4)2, was revisited recently. The long range magnetic order in BaCo2(AsO4)2 can be suppressed by very weak in-plane magnetic field, suggesting its proximity to Kitaev QSL. Here we perform time domain terahertz spectroscopy measurement to study the magnetic excitations on BaCo2(AsO4)2. We observe different magnon excitations upon increasing external magnetic field. In particular, the system is easily driven to a field-polarized paramagnetic phase, after the long range magnetic order is suppressed by a weak field Hc 2. The spectra beyond Hc2 are dominated by single magnon and two magnon excitations without showing signature of QSL. We discuss the similarity and difference of the excitation spectra between BaCo2(AsO4)2 and the widely studied Kitaev QSL candidate RuCl3., Comment: 6 pages, 4 figures

Recently, kagome lattice metal AV$_3$Sb$_5$ (A = K, Rb, Cs) family has received wide attention due to its presence of superconductivity, charge density wave (CDW) and peculiar properties from topological nontrivial electronic structure. With time-resolved pump-probe spectroscopy, we show that the excited quasiparticle relaxation dynamics can be explained by formation of energy gap below the phase transition being similar to a usual second-order CDW condensate, by contrast, the structure change is predominantly first order phase transition. Furthermore, no CDW amplitude mode is identified in the ordered phase. The results suggest that the CDW order is very different from the traditional CDW condensate. We also find that weak pump pulse can non-thermally melt the CDW order and drive the sample into its high temperature phase, revealing the fact that the difference in lattice potential between those phases is small., Comment: 3 figures, 6 pages

Utrafast control of material physical properties represents a rapid developing field in condensed matter physics. Yet, accessing to the long-lived photoinduced electronic states is still in its early stage, especially with respect to an insulator to metal phase transition. Here, by combing transport measurement with ultrashort photoexcitation and coherent phonon spectroscopy, we report on photoinduced multistage phase transitions in Ta2NiSe5. Upon excitation by weak pulse intensity, the system is triggered to a short-lived state accompanied by a structural change. Further increasing the excitation intensity beyond a threshold, a photoinduced steady new state is achieved where the resistivity drops by more than four orders at temperature 50 K. This new state is thermally stable up to at least 350 K and exhibits the lattice structure different from any of the thermally accessible equilibrium states. Transmission electron microscopy reveals an in-chain Ta atom displacement in the photoinduced new structure phase. We also found that nano-sheet samples with the thickness less than the optical penetration depth are required for attaining a complete transition., Comment: 10 pages, 4 figures, accepted by Nature Communications

The parkerite-type ternary chalcogenide Bi$_2$Rh$_3$Se$_2$ was discovered to be a charge density wave (CDW) superconductor. However, there was a debate on whether the observed phase transition at 240 K could be attributed to the formation of CDW order. To address the issue, we performed optical spectroscopy and ultrafast pump-probe measurements on single crystal samples of Bi$_2$Rh$_3$Se$_2$. Our optical conductivity measurement reveals clearly the formation of an energy gap with associated spectral change only at low energies, yielding strong evidence for a CDW phase transition at 240 K. Time resolved pump-probe measurement provides further support for the CDW phase transition. The amplitude and relaxation time of quasiparticles extracted from the photoinduced reflectivity show strong enhancement near transition temperature, yielding further evidence for the CDW energy gap formation. Additionally, a collective mode is identified from the oscillations in the pump-probe time delay at low temperature. This mode, whose frequency decreases gradually at elevated temperature, could be naturally attributed to the amplitude mode of CDW state., Comment: 6 pages, 6 figures, to be published in Phys. Rev. B

The dynamical properties of single crystal 1T-TaS$_{2}$ are investigated both in commensurate charge density wave state (CCDW state) and hidden charge density wave state (HCDW state). We develop a useful criterion in time-domain transmission terahertz measurement to judge whether the compound is driven into a metastable state or still in its virgin state. An increase of terahertz conductivity by two orders of magnitude from CCDW state to HCDW state is obtained by taking account of the penetration depth mismatch, which is in agreement with reported \emph{dc} transport measurement. Upon weak pumping, only transient processes with rapid decay dynamics are triggered in both CCDW and HCDW states. We compare the conductivity increases in terahertz frequency range between transient and HCDW states and suggest that fluctuated metallic domain walls may develop in the transient states., Comment: 11 pages, 6 figures

Intense laser pulses have recently emerged as a tool to tune between different orders in complex quantum materials. Among different light-induced phenomena, transient superconductivity far above the equilibrium transition temperature in cuprates is particularly attractive. Key to those experiments was the resonant pumping of specific phonon modes, which was believed to induce superconducting phase coherence by suppressing the competing orders or modifying the structure slightly. Here, we present a comprehensive study of photo-induced nonequilibrium response in underdoped YBa$_2$Cu$_3$O$_{6+x}$. We find that upon photo-excitations, Josephson plasma edge in superconducting state is initially removed accompanied by quasiparticle excitations, and subsequently reappears at frequency lower than the static plasma edge within short time. In normal state, an enhancement or weaker edge-like shape is indeed induced by pump pulses in the reflectance spectrum accompanied by simultaneous rises in both real and imaginary parts of conductivity. We compare the pump-induced effects between near- and mid-infrared excitations and exclude phonon pumping as a scenario for the photo-induced effects above. We further elaborate the transient responses in normal state are unlikely to be explained by photo-induced superconductivity., Comment: 8 pages, 4 figures and supplementary

We report a novel quasi-two dimensional compound of EuTe4 hosting charge density waves (CDW) instability. The compound has a crystallographic structure in a orthorhombic space group Pmmn (No.59) with cell parameters a = 4.6347(2){\AA}, b = 4.5119(2){\AA}, c = 15.6747(10){\AA} at room temperature. The pristine structure contains consecutive near-square Te sheets separated by corrugated Eu-Te slabs. Upon cooling, the compound experiences a phase transition near 255 K. X-ray crystallographic analysis and transmission electron microscopy (TEM) measurements reveal strong structural distortions in the low temperature phase, showing a superstructure with a periodic formation of Te-trimers in the monolayer Te sheets, yielding evidence for the formation of CDW order. The charge transport properties show a semiconducting behavior in the CDW state. Density functional theory calculations reveals a Fermi surface nesting driven instability with a nesting vector in good agreement with the one observed experimentally. Our finding provides a promising system for the study of CDW driven 2D semiconducting mechanisms, which would shed a new light on exploring novel 2D semiconductors with collective electronic states., Comment: 8 pages,4 figs

Photoexcitations on a superconductor using ultrafast nir-infrared (NIR) pulses, whose energy is much higher than the superconducting energy gap, are expected to suppress/destroy superconductivity by breaking Cooper pairs and excite quasiparticles from occupied state to unoccupied state far above the Fermi level. This appears to be true only for small pumping fluence. Here we show that the intense NIR pumping has different effect. We perform an intense NIR pump, c-axis terahertz probe measurement on an electron-doped cuprate superconductor Pr$_{0.88}$LaCe$_{0.12}$CuO$_4$ with T$_c$=22 K. The measurement indicates that, instead of destroying superconductivity or exciting quasiparticles, the intense NIR pump drives the system from an equilibrium superconducting state with uniform Josephson coupling strength to a new metastable superconducting phase with modulated Josephson coupling strengths below T$_c$., Comment: 7 pages, 4 figures

Charge-density wave (CDW) is one of the most fundamental quantum phenomena in solids. Different from ordinary metals in which only single particle excitations exist, CDW also has collective excitations and can carry electric current in a collective fashion. Manipulating this collective condensation for applications has long been a goal in the condensed matter and materials community. Here we show that the CDW system of 1T-TaS2 is highly sensitive to light directly from visible down to terahertz, with current responsivities around the order of ~1 AW-1 at room temperature. Our findings open a new avenue for realizing uncooled, ultrabroadband and sensitive photoelectronics continuously down to terahertz spectral range., Comment: 21 pages, 13 figures. ( Accepted for publication in Science Advances)

Recent development of ultrashort laser pulses allows for optical control of structural and electronic properties of complex quantum materials. The layered transition metal dichalcogenide MoTe2, which can crystalize into several different structures with distinct topological and electronic properties, provides possibilities to control or switch between different phases. In this study we report a photo-induced sub-picosecond structural transition between the type-II Weyl semimetal phase and normal semimetal phase in bulk crystalline MoTe2 by using ultrafast pump-probe and time-resolved second harmonic generation spectroscopy. The phase transition is most clearly characterized by the dramatic change of the shear oscillation mode and the intensity loss of second harmonic generation. This work opens up new possibilities for ultrafast manipulation of the topological properties of solids, enabling potentially practical applications for topological switch device with ultrafast excitations., Comment: 8 pages,4 figures