Photoinduced phase transitions in two-dimensional charge-density-wave 1T-TaS_2

Charge-density-wave(CDW) materials with strongly correlated electrons have broadband light absorption and ultrafast response to light irradiation, and hence hold great potential in photodetection. 1 T-TaS2 is a typical CDW material with various thermodynamically CDW ground states at different temperatures and fertile out-of-equilibrium intermediate/hidden states. In particular, the light pulses can trigger melting of CDW ordering and also forms hidden states, which exhibits strikingly different electrical conductivity compared to the ground phase. Here, we review the recent research on phase transitions in 1 T-TaS2 and their potential applications in photodetection. We also discuss the ultrafast melting of CDW ordering by ultrafast laser irradiation and the out-of-equilibrium intermediate/hidden states by optical/electrical pulse. For photodetection, demonstrations of photoconductors and bolometers are introduced. Finally, we discuss some of the challenges that remain.     

Tri-hexagonal charge order in kagome metal CsV3Sb5 revealed by 121Sb nuclear quadrupole resonance

We report ¹²¹Sb nuclear quadrupole resonance(NQR)measurements on kagome superconductor CsV₃Sb₅ with Tc=2.5 K.¹²¹Sb NQR spectra split after a charge density wave(CDW)transition at 94 K,which demonstrates a commensurate CDW state.The coexistence of the high temperature phase and the CDW phase between 91 K and 94 K manifests that it is a first order phase transition.The CDW order exhibits tri-hexagonal deformation with a lateral shift between the adjacent kagome layers,which is consistent with 2×2×2 superlattice modulation.The superconducting state coexists with CDW order and shows a conventional s-wave behavior in the bulk state.     

Direct observation of melted Mott state evidenced from Raman scattering in 1T-TaS_2 single crystal

The evolution of electron correlation and charge density wave(CDW)in 1T-TaS_2 single crystal has been investigated by temperature-dependent Raman scattering,which undergoes two obvious peaks of A_(1g) modes about 70.8 cm~(-1) and 78.7 cm~(-1) at 80 K,respectively.The former peak at 70.8 cm~(-1) is accordant with the lower Hubbard band,resulting in the electron-correlation-driven Mott transition.Strikingly,the latter peak at 78.7 cm~(-1) shifts toward low energy with increasing the temperature,demonstrating the occurrence of nearly commensurate CDW phase(melted Mott phase).In this case,phonon transmission could be strongly coupled to commensurate CDW lattice via Coulomb interaction,which likely induces appearance of hexagonal domains suspended in an interdomain phase,composing the melted Mott phase characterized by a shallow electron pocket.Combining electronic structure,atomic structure,transport properties with Raman scattering,these findings provide a novel dimension in understanding the relationship between electronic correlation,charge order,and phonon dynamics.     

S-Wave Superconductivity in Kagome Metal CsV_3Sb_5 Revealed by ~(121/123)Sb NQR and ~(51)V NMR Measurements

We report ~(121/123)Sb nuclear quadrupole resonance(NQR) and ~(51)V nuclear magnetic resonance(NMR) measurements on kagome metal CsV_3 Sb_5 with T_c=2.5 K.Both ~(51)V NMR spectra and ~(121/123)Sb NQR spectra split after a charge density wave(CDW) transition,which demonstrates a commensurate CDW state.The coexistence of the high temperature phase and the CDW phase between 91 K and 94 K manifests that it is a first-order phase transition.At low temperature,electric-field-gradient fluctuations diminish and magnetic fluctuations become dominant.Superconductivity emerges in the charge order state.Knight shift decreases and 1/T_1T shows a Hebel-Slichter coherence peak just below T_c,indicating that CSV_3 Sb_5 is an s-wave superconductor.     

Electronic transport and specific heat of 1T-V Se2

The low-temperature thermoelectric power and the specific heat of 1T-V Se₂ (vanadium diselenide) have been reported along with the electrical resistivity and Hall coefficient of the compound. The charge density wave (CDW) transition is observed near 110 K in all these properties. The thermoelectric power has been measured from 15 K to 300 K, spanning the incommensurate and commensurate CDW regions. We observed a weak anomaly at the CDW transition for the first time in the specific heat of V Se₂. The linear temperature dependence of the resistivity and thermoelectric power at higher temperatures suggests a normal metallic behavior and electron–phonon scattering above the CDW transition. The positive thermoelectric power and negative Hall coefficient along with strongly temperature-dependent behavior in the CDW phase suggest a mixed conduction related to the strongly hybridized s–p–d bands in this compound.     

Suppression of the charge density waves in 1T-TaS2 by 70 MeV16O6+ bombardment

We report on the measurement of the nuclear quadrupole interaction by TDPAC on a single crystal of 1T-TaS₂ before and after bombardment with 70 MeV¹⁶O⁶⁺ ions. In 1T-TaS₂, two groups of inequivalent Ta-sites are observed at 298 K due to the presence of a nearly commensurate charge density wave (CDW) Upon¹⁶O⁶⁺ bombardment a single slightly broadened line is observed which resembles closely the incommensurate CDW state.     

Critical behavior of the one-dimensional commensurate-incommensurate transition

We study the low-temperature critical behavior of one-dimensional charge-density-waves coupled to an underlying lattice, using the McMillan free energy. For weak coupling, the incommensurate CDW orders at T = 0 as a lattice of phase slip solutions with XY critical behavior. For strong coupling, the commensurate CDW orders at T = 0 with Ising critical behavior. Analytic expressions for the low-temperature inverse correlation length and average phase change are obtained for all values of the coupling to the lattice.     

Charge-density waves and superlattices in the metallic layered transition metal dichalcogenides

The d1 layer metals TaS 2 , TaSe 2 , NbSe 2 , in all their various polytypic modifications, acquire, below some appropriate temperature, phase conditions that their electromagnetic properties have previously revealed as 'anomalous'. Our present electron-microscopic studies indicate that this anomalous behaviour usually included the adoption, at some stage, of a superlattice. The size of superlattice adopted often is forecast in the pattern of satellite spotting and strong diffuse scattering found above the transition. Our conclusions are that charge-density waves and their concomitant periodic structural distortions occur in all these 4d 1 /5d 1 dichalcogenides. We have related the observed periodicities of these CDW states to the theoretical form of the parent Fermi surfaces. Particularly for the 1T octahedrally coordinated polytypes the Fermi surface is very simple and markedly two-dimensional in character, with large near-parallel walls. Such a situation is known theoretically to favour the formation of charge and spin-density waves. When they first appear, the CDWs in the 1T (and 4Hb) polytypes are incommensurate with the lattice. This condition produes a fair amount of gapping in the density of states at the Fermi level. For the simplest case of 1T-TaSe 2 , the room temperature superlattice is realized when this existing CDW rotates into an orientation for which it then become commensurate. At this first-order transition the Fermi surface energy gapping increases beyond that generated by the incommensurate CDW, as is clearly evident in the electromagnetic properties. For the trigonal prismatically coordinated polytypes, CDW formation is withheld to low temperatures, probably because of the more complex band structures. This CDW state (in the cases measured) would seem at once commensurate, even though the transition is, from a wide variety of experiments, apparently second order. A wide range of doped and intercalated materials have been used to substantiate the presence of CDWs in these compounds, and to clarify the effect that their occurrence has on the physical properties. The observations further demonstrate the distinctiveness of the transition metal dichalcogenide layer compounds, and of the group VA metals in particular.     

Coexistence of gapless excitations and commensurate charge-density wave in the 2H transition metal dichalcogenides

An unexpected feature common to 2H transition metal dichalcogenides ( 2H TMDs) is revealed with a first-principles Wannier function analysis of the electronic structure of the prototype 2H TaSe2: The low-energy Ta "5d(z2)" bands governing the physics of a charge-density wave (CDW) is dominated by hopping between next-nearest neighbors. With this motivation we develop a minimal effective model for the CDW formation, in which the unusual form of the hopping leads to an approximate decoupling of the three sublattices. In the CDW phase one sublattice remains undistorted, leaving the bands associated with it ungapped everywhere in the Fermi surface, resolving the long-standing puzzle of the coexistence of gapless excitations and commensurate CDW in the 2H TMDs.     

Charge-density-wave transitions in the local-moment magnet Er5Ir4Si10

We report the observation of a new type of charge-density wave (CDW) in the large magnetic-moment rare-earth intermetallic compound, Er5Ir4Si10, which then orders magnetically at low temperatures. Single crystal x-ray diffraction shows the development of a 1D incommensurate CDW at 155 K, which then locks into a purely commensurate state below 55 K. The well-localized Er3+ moments are antiferromagnetically ordered below 2.8 K. We observe very sharp anomalies in the specific heat at 145 and 2.8 K, signifying the bulk nature of these transitions. Our data suggest the coexistence of strongly coupled CDW with local-moment antiferromagnetism in Er5Ir4Si10.     

Ultraviolet photoemission spectroscopy of (TaSe4)2I

The vacuum ultraviolet photoemission spectra of quasi-one-dimensional charge density wave ( CDW ) system, (TaSe₄)₂I, were measured for photon energies between 32 and 100 eV at room temperature ( in the normal phase ) and at about 100 K ( in the CDW phase ). The spectrum of Ta 4f core-levels has shown no additional splitting due to the two different Ta sites. The spectra of the valence and conduction bands have revealed the resonant enhancement for the excitation of the Ta 5p core states, which demonstrates the remarkable hybridization of Ta 5d orbitals with Se 4p orbitals with binding energies smaller than 4 eV. In the CDW phase, the partial cross section decreases for both Ta 5d bands and Se 4p bands with Ta 5d components.     

Novel charge density wave transition in crystals of R5Ir4Si10

We review the observation of novel charge density wave (CDW) transitions in ternary R₅Ir₄Si₁₀ compounds. A high quality single crystal of Lu₅Ir₄Si₁₀ shows the formation of a commensurate CDW along c-axis below 80 K in the (h, 0, l) plane that coexists with BCS type superconductivity below 3.9 K. However, in a single crystal of Er₅Ir₄Si₁₀, one observes the development of a 1D-incommensurate CDW at 155 K, which then locks into a purely commensurate state below 55 K. The well-localized Er³ moments are antiferromagnetically ordered below 2.8 K which results in the coexistence of strongly coupled CDW with local moment antiferromagnetism in Er₅Ir₄Si₁₀. Unlike conventional CDW systems, extremely sharp transition (width ∼ 1.5 K) in all bulk properties along with huge heat capacity anomalies in these compounds makes this CDW transition an interesting one.     

Collective quantum tunneling of strongly correlated electrons in commensurate mesoscopic rings

We present a new effect that is possible for strongly correlated electrons in commensurate mesoscopic rings: the collective tunneling of electrons between classically equivalent configurations, corresponding to ordered states possessing charge and spin density waves (CDW, SDW) and charge separation (CS). Within an extended Hubbard model at half filling studied by exact numerical diagonalization, we demonstrate that the ground state phase diagram comprises, besides conventional critical lines separating states characterized by different orderings (e.g. CDW, SDW, CS), critical lines separating phases with the same ordering (e.g. CDW-CDW) but with different symmetries. While the former also exist in infinite systems, the latter are specific for mesoscopic systems and directly related to a collective tunnel effect. We emphasize that, in order to construct correctly a phase diagram for mesoscopic rings, the examination of CDW, SDW and CS correlation functions alone is not sufficient, and one should also consider the symmetry of the wave function that cannot be broken. We present examples demonstrating that the jumps in relevant physical properties at the conventional and new critical lines are of comparable magnitude. These transitions could be studied experimentally e.g. by optical absorption in mesoscopic systems. Possible candidates are cyclic molecules and ring-like nanostructures of quantum dots. Received 27 November 2000     

Electron-lattice interaction and the CDW state of 1T-TiSe2

The electronic band structure in the CDW state (superlattice structure) of 1T-TiSe₂ is calculated on the basis of the band-type Jahn-Teller model by extending our theory of lattice instability in the normal phase. A strong coupling between the hole-band (Se p states) around the Λ point and the electron-bands (Ti d states) around the Λ points is caused by the electron-lattice interaction. Reflecting such a strong coupling remarkable changes appear in the dispersion curves near the Fermi energy and the largest CDW gap is obtained to be 0.2 eV. We have also calculated a change of the density of states near the Fermi energy due to the superlattice formation. The result is consistent with that observed by angle-integrated photoemmision by Margaritondo et al. It is also shown that the magnitude of the lattice distortion observed at low temperatures can be explained in a way consistent with the lattice dynamics in the normal phase.     

Anomalously large negative magnetoresistance of 1T-TaS2 at ultra low temperatures

The magnetoresistance of 1T-TaS₂ in the commensurate CDW phase was measured from 8 K down to 50 mK. Very large negative magnetoresistance was observed below 0.5 K for both transverse and longitudinal configurations of the magnetic field with respect to the current. This result is explained by Fukuyama and Yosida's theory based on the variable-range hopping in the Anderson localized states.     

The CDW transition with tripling of the period along the chains in quasi 1d crystals

It is shown that due to the influence of the interchain interaction the commensurate x3 CDW transition may be either I or II order. The possible types of 3d CDW ordering in this case are discussed. We point out also that for x3 transition the 2k_F and 4k_F anomalies coincide and add to increase the critical temperature and the gap or pseudogap. The results are discussed in connection with the properties of TTF-TCNQ under pressure.     

Polaronic conductivity in the photoinduced phase of 1T-TaS2

The transient optical conductivity of photoexcited 1T-TaS2 is determined over a three-order-of-magnitude frequency range. Prompt collapse and recovery of the Mott gap is observed. However, we find important differences between this transient metallic state and that seen across the thermally driven insulator-metal transition. Suppressed low-frequency conductivity, Fano phonon line shapes, and a midinfrared absorption band point to polaronic transport. This is explained by noting that the photoinduced metallic state of 1T-TaS2 is one in which the Mott gap is melted but the lattice retains its low-temperature symmetry, a regime only accessible by photodoping.     

Semimetal-to-semimetal charge density wave transition in 1T-TiSe(2)

We report an infrared study on 1T-TiSe(2), the parent compound of the newly discovered superconductor Cu(x)TiSe(2). Previous studies of this compound have not conclusively resolved whether it is a semimetal or a semiconductor-information that is important in determining the origin of its unconventional charge density wave (CDW) transition. Here we present optical spectroscopy results that clearly reveal that the compound is metallic in both the high-temperature normal phase and the low-temperature CDW phase. The carrier scattering rate is dramatically different in the normal and CDW phases and the carrier density is found to change with temperature. We conclude that the observed properties can be explained within the scenario of an Overhauser-type CDW mechanism.     

Incommensurate magnetic order in TbTe3

We report a neutron diffraction study of the magnetic phase transitions in the charge-density wave (CDW) TbTe(3) compound. We discover that in the paramagnetic phase there are strong 2D-like magnetic correlations, consistent with the pronounced anisotropy of the chemical structure. A long-range incommensurate magnetic order emerges in TbTe(3) at T(mag1) = 5.78 K as a result of continuous phase transitions. We observe that near the temperature T(mag1) the magnetic Bragg peaks appear around the position (0, 0, 0.24) (or its rational multiples), that is fairly close to the propagation vector (0,0,0.29) associated with the CDW phase transition in TbTe(3). This suggests that correlations leading to the long-range magnetic order in TbTe(3) are linked to the modulations that occur in the CDW state.