Local real-space view of the achiral 1T\text{\ensuremath{-}}{\mathrm{TiSe}}_{2} 2×2×22\times2\times2 charge density wave

The transition metal dichalcogenide 1T−TiSe2-two-dimensional layered material undergoing a commensurate 2×2×2 charge density wave (CDW) transition with a weak periodic lattice distortion (PLD) below ≈200 K. Scanning tunneling microscopy (STM) combined with intentionally introduced interstitial Ti atoms allows us to go beyond the usual spatial resolution of STM and to intimately probe the three- dimensional character of the PLD. Furthermore, the inversion-symmetric achiral nature of the CDW in the z direction is revealed, contradicting the claimed existence of helical CDW stacking and associated chiral order. This study paves the way to a simultaneous real-space probing of both charge and structural reconstructions in CDW compounds

Robustness of the charge-ordered phases in IrTe2{\mathrm{IrTe}}_{2} against photoexcitation

We present a time-resolved angle-resolved photoelectron spectroscopy study of IrTe2, which undergoes two first-order structural and charge-ordered phase transitions on cooling below 270 K and below 180 K. The possibility of inducing a phase transition by photoexcitation with near-infrared femtosecond pulses is investigated in the charge-ordered phases. We observe changes of the spectral function occurring within a few hundreds of femtoseconds and persisting up to several picoseconds, which we interpret as a partial photoinduced phase transition (PIPT). The necessary time for photoinducing these spectral changes increases with increasing photoexcitation density and reaches time scales longer than the rise time of the transient electronic temperature. We conclude that the PIPT is driven by a transient increase of the lattice temperature following the energy transfer from the electrons. However, the photoinduced changes of the spectral function are small, which indicates that the low- temperature phase is particularly robust against photoexcitation. We suggest that the system might be trapped in an out-of-equilibrium state, for which only a partial structural transition is achieved

Short-range phase coherence and origin of the 1T−TiSe21T-{\mathrm{TiSe}}_{2} charge density wave

The impact of variable Ti self-doping on the 1T−TiSe2 charge density wave (CDW) is studied by scanning tunneling microscopy. Supported by density functional theory, we show that agglomeration of intercalated-Ti atoms acts as preferential nucleation centers for the CDW that breaks up in phase-shifted CDW domains whose size directly depends on the intercalated-Ti concentration and which are separated by atomically sharp phase boundaries. The close relationship between the diminution of the CDW domain size and the disappearance of the anomalous peak in the temperature-dependent resistivity allows to draw a coherent picture of the 1T−TiSe2 CDW phase transition and its relation to excitons

Local resilience of the 1T\text{\ensuremath{-}}{\mathrm{TiSe}}_{2} charge density wave to Ti self-doping

In Ti-intercalated self-doped 1T−TiSe2 crystals, the charge density wave (CDW) superstructure induces two nonequivalent sites for Ti dopants. Recently, it has been shown that increasing Ti doping dramatically influences the CDW by breaking it into phase-shifted domains. Here, we report scanning tunneling microscopy and spectroscopy experiments that reveal a dopant-site dependence of the CDW gap. Supported by density functional theory, we demonstrate that the loss of the long-range phase coherence introduces an imbalance in the intercalated-Ti site distribution and restrains the CDW gap closure. This local resilient behavior of the 1T−TiSe2 CDW reveals an entangled mechanism between CDW, periodic lattice distortion, and induced nonequivalent defects

Uniaxial strain-induced phase transition in the 2D topological semimetal IrTe2

Strain is ubiquitous in solid-state materials, but despite its fundamental importance and technological relevance, leveraging externally applied strain to gain control over material properties is still in its infancy. In particular, strain control over the diverse phase transitions and topological states in two-dimensional transition metal dichalcogenides remains an open challenge. Here, we exploit uniaxial strain to stabilize the long-debated structural ground state of the 2D topological semimetal IrTe$_{2}$, which is hidden in unstrained samples. Combined angle-resolved photoemission spectroscopy and scanning tunneling microscopy data reveal the strain-stabilized phase has a 6 × 1 periodicity and undergoes a Lifshitz transition, granting unprecedented spectroscopic access to previously inaccessible type-II topological Dirac states that dominate the modified inter-layer hopping. Supported by density functional theory calculations, we show that strain induces an Ir to Te charge transfer resulting in strongly weakened inter-layer Te bonds and a reshaped energetic landscape favoring the 6×1 phase. Our results highlight the potential to exploit strain-engineered properties in layered materials, particularly in the context of tuning inter-layer behavior

Selective probing of hidden spin-polarized states in inversion-symmetric bulk MoS2{\mathrm{MoS}}_{2}

Spin- and angle-resolved photoemission spectroscopy is used to reveal that a large spin polarization is observable in the bulk centrosymmetric transition metal dichalcogenide MoS2. It is found that the measured spin polarization can be reversed by changing the handedness of incident circularly polarized light. Calculations based on a three-step model of photoemission show that the valley and layer-locked spin- polarized electronic states can be selectively addressed by circularly polarized light, therefore providing a novel route to probe these hidden spin-polarized states in inversion-symmetric systems as predicted by Zhang et al. [Nat. Phys. 10, 387 (2014).]

Phase separation in the vicinity of Fermi surface hot spots

Spatially inhomogeneous electronic states are expected to be key ingredients for the emergence of superconducting phases in quantum materials hosting charge-density waves (CDWs). Prototypical materials are transitionmetal dichalcogenides (TMDCs) and among them, 1T-TiSe2 exhibiting intertwined CDW and superconducting states under Cu intercalation, pressure, or electrical gating. Although it has been recently proposed that the emergence of superconductivity relates to CDW fluctuations and the development of spatial inhomogeneities in the CDW order, the fundamental mechanism underlying such a phase separation (PS) is still missing. Using angle- resolved photoemission spectroscopy and variable-temperature scanning tunneling microscopy, we report on the phase diagram of the CDW in 1T-TiSe2 as a function of Ti self-doping, an overlooked degree of freedom inducing CDW texturing. We find an intrinsic tendency towards electronic PS in the vicinity of Fermi surface (FS) “hot spots,” i.e., locations with band crossigs close to, but not at the Fermi level.We therefore demonstrate an intimate relationship between the FS topology and the emergence of spatially textured electronic phases which is expected to be generalizable to many doped CDW compound

Carrier-Density Control of the Quantum-Confined 1T-TiSe2 Charge Density Wave

International audienceUsing angle-resolved photoemission spectroscopy, combined with first principle and coupled selfconsistent Poisson-Schrödinger calculations, we demonstrate that potassium (K) atoms adsorbed on the low-temperature phase of 1T-TiSe 2 induce the creation of a two-dimensional electron gas (2DEG) and quantum confinement of its charge-density wave (CDW) at the surface. By further changing the K coverage, we tune the carrier density within the 2DEG that allows us to nullify, at the surface, the electronic energy gain due to exciton condensation in the CDW phase while preserving a long-range structural order. Our Letter constitutes a prime example of a controlled exciton-related many-body quantum state in reduced dimensionality by alkali-metal dosing

Unveiling the Semimetallic Nature of 1TT-TiSe2_2 by Doping its Charge Density Wave

The semimetallic or semiconducting nature of the transition metal dichalcogenide 1$T$-TiSe$_2$ remains under debate after many decades mainly due to the fluctuating nature of its 2 x 2 x 2 charge-density-wave (CDW) phase at room- temperature. In this letter, using angle-resolved photoemission spectroscopy, we unambiguously demonstrate that the 1$T$-TiSe$_2$ normal state is semimetallic with an electron-hole band overlap of ~110 meV by probing the low-energy electronic states of the perturbed CDWphase strongly doped by alkali atoms. Our study not only closes a long-standing debate but also supports the central role of the Fermi surface for driving the CDW and superconducting instabilities in 1$T$-TiSe$_2$