Amplitude `Higgs' mode in 2H-NbSe2 Superconductor

We report experimental evidences for the observation of the superconducting amplitude mode, so-called `Higgs' mode in the charge density wave superconductor 2H-NbSe2 using Raman scattering. By comparing 2H-NbSe2 and its iso-structural partner 2H-NbS2 which shows superconductivity but lacks the charge density wave order, we demonstrate that the superconducting mode in 2H-NbSe2 owes its spectral weight to the presence of the coexisting charge density wave order. In addition, temperature dependent measurements in 2H-NbSe2 show a full spectral weight transfer from the charge density wave mode to the superconducting mode upon entering the superconducting phase. Both observations are fully consistent with a superconducting amplitude mode or Higgs mode.Comment: Accepted for publication in Phys. Rev. B Rapid Com. 5 pages with 3 figure

Anionic redox topochemistry for materials design: chalcogenides and beyond

Topochemistry refers to a generic category of solid-state reactions in which precursors and products display strong filiation in their crystal structures. Various low-dimensional materials are subject to this stepwise structure transformation by accommodating guest atoms or molecules in between their 2D slabs or 1D chains loosely bound by van der Waals (vdW) interactions. Those processes are driven by redox reactions between guests and the host framework, where transition metal cations have been widely exploited as the redox center. Topochemistry coupled with this cationic redox not only enables technological applications such as Li-ion secondary batteries but also serves as a powerful tool for structural or electronic fine-tuning of layered transition metal compounds. Over recent years, we have been pursuing materials design beyond this cationic redox topochemistry that was mostly limited to 2D or 1D vdW systems. For this, we proposed new topochemical reactions of non-vdW compounds built of 2D arrays of anionic chalcogen dimers alternating with redox-inert host cationic layers. These chalcogen dimers were found to undergo redox reaction with external metal elements, triggering either (1) insertion of these metals to construct 2D metal chalcogenides or (2) deintercalation of the constituent chalcogen anions. As a whole, this topochemistry works like a “zipper”, where reductive cleavage of anionic chalcogen–chalcogen bonds opens up spaces in non-vdW materials, allowing the formation of novel layered structures. This Perspective briefly summarizes seminal examples of unique structure transformations achieved by anionic redox topochemistry as well as challenges on their syntheses and characterizations

First-Order Insulator-to-Metal Mott Transition in the Paramagnetic 3D System GaTa4Se8

The nature of the Mott transition in the absence of any symmetry braking remains a matter of debate. We study the correlation-driven insulator-to-metal transition in the prototypical 3D Mott system GaTa4Se8, as a function of temperature and applied pressure. We report novel experiments on single crystals, which demonstrate that the transition is of first order and follows from the coexistence of two states, one insulating and one metallic, that we toggle with a small bias current. We provide support for our findings by contrasting the experimental data with calculations that combine local density approximation with dynamical mean-field theory, which are in very good agreement.Comment: 5 pages and 4 figures. Supplemental material: 2 pages, 2 figure

Scanning tunneling spectroscopy of layers of superconducting 2H-TaSe2_\textbf{2}: Evidence for a zero bias anomaly in single layers

We report a characterization of surfaces of the dichalcogenide TaSe$_2$ using scanning tunneling microscopy and spectroscopy (STM/S) at 150 mK. When the top layer has the 2H structure and the layer immediately below the 1T structure, we find a singular spatial dependence of the tunneling conductance below 1 K, changing from a zero bias peak on top of Se atoms to a gap in between Se atoms. The zero bias peak is additionally modulated by the commensurate $3a_0 \times 3a_0$ charge density wave of 2H-TaSe$_2$. Multilayers of 2H-TaSe$_2$ show a spatially homogeneous superconducting gap with a critical temperature also of 1 K. We discuss possible origins for the peculiar tunneling conductance in single layers.Comment: 10 pages, 10 figure

Domain size effects on the dynamics of a charge density wave in 1T-TaS2

Recent experiments have shown that the high temperature incommensurate (I) charge density wave (CDW) phase of 1T-TaS2 can be photoinduced from the lower temperature, nearly commensurate (NC) CDW state. Here we report a time-resolved x-ray diffraction study of the growth process of the photoinduced I-CDW domains. The layered nature of the material results in a marked anisotropy in the size of the photoinduced domains of the I-phase. These are found to grow self-similarly, their shape remaining unchanged throughout the growth process. The photoinduced dynamics of the newly formed I-CDW phase was probed at various stages of the growth process using a double pump scheme, where a first pump creates I-CDW domains and a second pump excites the newly formed I-CDW state. We observe larger magnitudes of the coherently excited I-CDW amplitude mode in smaller domains, which suggests that the incommensurate lattice distortion is less stable for smaller domain sizes.Comment: 8 pages, 8 figure

Superconducting density of states and vortex cores of 2H-NbS2

Scanning tunneling microscopy and spectroscopy (STM/S) measurements in the superconducting dichalcogenide 2H-NbS2 show a peculiar superconducting density of states with two well defined features at 0.97 meV and 0.53 meV, located respectively above and below the value for the superconducting gap expected from single band s-wave BCS model (D=1.76kBTc=0.9 meV). Both features have a continuous temperature evolution and disappear at Tc = 5.7 K. Moreover, we observe the hexagonal vortex lattice with radially symmetric vortices and a well developed localized state at the vortex cores. The sixfold star shape characteristic of the vortex lattice of the compound 2H-NbSe2 is, together with the charge density wave order (CDW), absent in 2H-NbS2.Comment: 5 pages, 4 figure

Ultrafast filling of an electronic pseudogap in an incommensurate crystal

We investigate the quasiperiodic crystal (LaS)1.196(VS2) by angle and time resolved photoemission spectroscopy. The dispersion of electronic states is in qualitative agreement with band structure calculated for the VS2 slab without the incommensurate distortion. Nonetheless, the spectra display a temperature dependent pseudogap instead of quasiparticles crossing. The sudden photoexcitation at 50 K induces a partial filling of the electronic pseudogap within less than 80 fs. The electronic energy flows into the lattice modes on a comparable timescale. We attribute this surprisingly short timescale to a very strong electron-phonon coupling to the incommensurate distortion. This result sheds light on the electronic localization arising in aperiodic structures and quasicrystals

Watching the birth of a charge density wave order: diffraction study on nanometer-and picosecond-scales

Femtosecond time-resolved X-ray diffraction is used to study a photo-induced phase transition between two charge density wave (CDW) states in 1T-TaS$_2$, namely the nearly commensurate (NC) and the incommensurate (I) CDW states. Structural modulations associated with the NC-CDW order are found to disappear within 400 fs. The photo-induced I-CDW phase then develops through a nucleation/growth process which ends 100 ps after laser excitation. We demonstrate that the newly formed I-CDW phase is fragmented into several nanometric domains that are growing through a coarsening process. The coarsening dynamics is found to follow the universal Lifshitz-Allen-Cahn growth law, which describes the ordering kinetics in systems exhibiting a non-conservative order parameter.Comment: 6 pages, 5 figure