skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.
Attention:The NSF Public Access Repository (NSF-PAR) system and access will be unavailable from 7:00 AM ET to 7:30 AM ET on Friday, April 24 due to maintenance. We apologize for the inconvenience.

Explore Research Products in the PAR
It may take a few hours for recently added research products to appear in PAR search results.


Title: Electronic coherence evolution at the nearly commensurate-incommensurate CDW boundary of 1T-TaS2
Transition-metal dichalcogenides host a variety of charge-density-wave phases that couple lattice, charge, and correlation effects. In 1T -TaS2, the commensurate and nearly commensurate states are well characterized, yet the transition near 350 K into the incommensurate phase has lacked direct momentum-resolved insight. Here, we use temperature-dependent angle-resolved photoemission spectroscopy to track the electronic structure across this transition. We observe a suppression of quasiparticle spectral weight at the Brillouin-zone center, coincident with the transport anomaly, but without clear evidence of a full band-gap opening. The transition appears to involve momentum-dependent redistribution of spectral weight, consistent with a loss of coherence that reshapes the Fermi surface while leaving conduction dispersions largely intact. These results suggest that the nearly commensurate–incommensurate transition may not align with a conventional metal-insulator transition picture, but rather as an electronic reconstruction driven by loss of coherence. Our work provides new microscopic insight into the resistivity anomaly near room temperature and may guide design principles for collective electronic switching in transition-metal dichalcogenides  more » « less
Award ID(s):
2233149
PAR ID:
10678149
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ;
Publisher / Repository:
Nature portfolio
Date Published:
Journal Name:
PHYSICAL REVIEW MATERIALS
Volume:
7
Issue:
1
ISSN:
2399-3650
Page Range / eLocation ID:
034007
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ; (, Nanoscale)
    null (Ed.)
    Group IVB transition metal dichalcogenides (TMDCs) have attracted significant attention due to their predicted high charge carrier mobility, large sheet current density, and enhanced thermoelectric power. Here, we investigate the electrical and optoelectronic properties of few-layer titanium diselenide (TiSe 2 )-metal junctions through spatial-, wavelength-, temperature-, power- and temporal-dependent scanning photocurrent measurements. Strong photocurrent responses have been detected at TiSe 2 -metal junctions, which is likely attributed to both photovoltaic and photothermoelectric effects. A fast response time of 31 μs has been achieved, which is two orders of magnitude better than HfSe 2 based devices. More importantly, our experimental results reveal a significant enhancement in the response speed upon cooling to the charge-density-wave (CDW) phase transition temperature ( T CDW = 206 K), which may result from dramatic reduction in carrier scattering that occurs as a result of the switching between the normal and CDW phases of TiSe 2 . Additionally, the photoresponsivity at 145 K is up to an order of magnitude higher than that obtained at room temperature. These fundamental studies not only offer insight for the photocurrent generation mechanisms of group IVB TMDC materials, but also provide a route to engineering future temperature-dependent, two-dimensional, fast electronic and optoelectronic devices. 
    more » « less
  2. ; ; ; ; ; ; ; ; ; ; et al (, 2411.14746)
    A charge density wave (CDW) is a phase of matter characterized by a periodic modulation of the valence electron density accompanied by a distortion of the lattice structure. The microscopic details of CDW formation are closely tied to the dynamic charge susceptibility, χ(q, ω), which describes the behavior of electronic collective modes. Despite decades of extensive study, the behavior of χ(q, ω) in the vicinity of a CDWtransition has never been measured with high energy resolution (∼meV). Here, we investigate the canonical CDW transition in ErTe3 using momentum-resolved electron energy loss spectroscopy (M-EELS), a technique uniquely sensitive to valence band charge excitations. Unlike phonons in these materials, which undergo conventional softening due to the Kohn anomaly at the CDW wavevector, the electronic excitations display purely relaxational dynamics that are well described by a diffusive model. The diffusivity peaks around 250 K, just below the critical temperature. Additionally, we report, for the first time, a divergence in the real part of χ(q, ω) in the static limit (ω → 0), a phenomenon predicted to characterize CDWs since the 1970s. These results highlight the importance of energy- and momentum-resolved measurements of electronic susceptibility and demonstrate the power of M-EELS as a versatile probe of charge dynamics in materials. 
    more » « less
  3. ; ; ; ; ; ; (, Proceedings of the National Academy of Sciences)
    Incommensurate charge order in hole-doped oxides is intertwined with exotic phenomena such as colossal magnetoresistance, high-temperature superconductivity, and electronic nematicity. Here, we map, at atomic resolution, the nature of incommensurate charge–lattice order in a manganite using scanning transmission electron microscopy at room temperature and cryogenic temperature (∼93 K). In diffraction, the ordering wave vector changes upon cooling, a behavior typically associated with incommensurate order. However, using real space measurements, we discover that the ordered state forms lattice-locked regions over a few wavelengths interspersed with phase defects and changing periodicity. The cations undergo picometer-scale (∼6 pm to 11 pm) transverse displacements, suggesting that charge–lattice coupling is strong. We further unearth phase inhomogeneity in the periodic lattice displacements at room temperature, and emergent phase coherence at 93 K. Such local phase variations govern the long-range correlations of the charge-ordered state and locally change the periodicity of the modulations, resulting in wave vector shifts in reciprocal space. These atomically resolved observations underscore the importance of lattice coupling and phase inhomogeneity, and provide a microscopic explanation for putative “incommensurate” order in hole-doped oxides. 
    more » « less
  4. ; ; ; ; ; (, Nature Communications)
    Abstract The charge density wave material 1T-TaS2exhibits a pulse-induced insulator-to-metal transition, which shows promise for next-generation electronics such as memristive memory and neuromorphic hardware. However, the rational design of TaS2devices is hindered by a poor understanding of the switching mechanism, the pulse-induced phase, and the influence of material defects. Here, we operate a 2-terminal TaS2device within a scanning transmission electron microscope at cryogenic temperature, and directly visualize the changing charge density wave structure with nanoscale spatial resolution and down to 300 μs temporal resolution. We show that the pulse-induced transition is driven by Joule heating, and that the pulse-induced state corresponds to the nearly commensurate and incommensurate charge density wave phases, depending on the applied voltage amplitude. With our in operando cryogenic electron microscopy experiments, we directly correlate the charge density wave structure with the device resistance, and show that dislocations significantly impact device performance. This work resolves fundamental questions of resistive switching in TaS2devices, critical for engineering reliable and scalable TaS2electronics. 
    more » « less
  5. ; ; ; ; ; ; ; ; ; (, APL Materials)
    Here, we present comprehensive phononic and charge density wave properties (CDW) of rare-earth van der Waals tritellurides through temperature dependent angle-resolved Raman spectroscopy measurements. All the possible rare-earth tritellurides (RTe 3 ) ranging from R = La–Nd, Sm, Gd–Tm were synthesized through a chemical vapor transport technique to achieve high quality crystals with excellent CDW characteristics. Raman spectroscopy studies successfully identify the emergence of the CDW state and transition temperature (T CDW ), which offers a non-destructive method to identify their CDW response with micron spatial resolution. Temperature dependent Raman measurements further correlate how the atomic mass of metal cations and the resulting chemical pressure influence its CDW properties and offer detailed insight into the strength of CDW amplitude mode-phonon coupling during the CDW transition. Angle-resolved Raman measurements offer the first insights into the CDW-phonon symmetry interplay by monitoring the change in the symmetry of phonon mode across the CDW transition. Overall results introduce the library of RTe 3 CDW materials and establish their characteristics through the non-destructive angle-resolved Raman spectroscopy technique. 
    more » « less
  • Citation Formats
  • MLA
  • APA
  • Chicago
  • BibTeX
  • Text Encoded Conversion
  • XML
  • Save / Share this Record
  • Send to Email