scholarly journals Ultrafast electron calorimetry uncovers a new long-lived metastable state in 1T-TaSe2 mediated by mode-selective electron-phonon coupling

2019 ◽  
Vol 5 (3) ◽  
pp. eaav4449 ◽  
Author(s):  
Xun Shi ◽  
Wenjing You ◽  
Yingchao Zhang ◽  
Zhensheng Tao ◽  
Peter M. Oppeneer ◽  
...  

Quantum materials represent one of the most promising frontiers in the quest for faster, lightweight, energy-efficient technologies. However, their inherent complexity and rich phase landscape make them challenging to understand or manipulate. Here, we present a new ultrafast electron calorimetry technique that can systematically uncover new phases of quantum matter. Using time- and angle-resolved photoemission spectroscopy, we measure the dynamic electron temperature, band structure, and heat capacity. This approach allows us to uncover a new long-lived metastable state in the charge density wave material 1T-TaSe2, which is distinct from all the known equilibrium phases: It is characterized by a substantially reduced effective total heat capacity that is only 30% of the normal value, because of selective electron-phonon coupling to a subset of phonon modes. As a result, less energy is required to melt the charge order and transform the state of the material than under thermal equilibrium conditions.

2021 ◽  
Vol 11 (1) ◽  
Author(s):  
M. Osiekowicz ◽  
D. Staszczuk ◽  
K. Olkowska-Pucko ◽  
Ł. Kipczak ◽  
M. Grzeszczyk ◽  
...  

AbstractThe temperature effect on the Raman scattering efficiency is investigated in $$\varepsilon$$ ε -GaSe and $$\gamma$$ γ -InSe crystals. We found that varying the temperature over a broad range from 5 to 350 K permits to achieve both the resonant conditions and the antiresonance behaviour in Raman scattering of the studied materials. The resonant conditions of Raman scattering are observed at about 270 K under the 1.96 eV excitation for GaSe due to the energy proximity of the optical band gap. In the case of InSe, the resonant Raman spectra are apparent at about 50 and 270 K under correspondingly the 2.41 eV and 2.54 eV excitations as a result of the energy proximity of the so-called B transition. Interestingly, the observed resonances for both materials are followed by an antiresonance behaviour noticeable at higher temperatures than the detected resonances. The significant variations of phonon-modes intensities can be explained in terms of electron-phonon coupling and quantum interference of contributions from different points of the Brillouin zone.


2021 ◽  
Vol 7 (20) ◽  
pp. eabf2810
Author(s):  
Martin R. Otto ◽  
Jan-Hendrik Pöhls ◽  
Laurent P. René de Cotret ◽  
Mark J. Stern ◽  
Mark Sutton ◽  
...  

The complex coupling between charge carriers and phonons is responsible for diverse phenomena in condensed matter. We apply ultrafast electron diffuse scattering to unravel electron-phonon coupling phenomena in 1T-TiSe2 in both momentum and time. We are able to distinguish effects due to the real part of the many-body bare electronic susceptibility, R[χ0(q)], from those due to the electron-phonon coupling vertex, gq, by following the response of semimetallic (normal-phase) 1T-TiSe2 to the selective photo-doping of carriers into the electron pocket at the Fermi level. Quasi-impulsive and wave vector–specific renormalization of soft zone-boundary phonon frequencies (stiffening) is observed, followed by wave vector–independent electron-phonon equilibration. These results unravel the underlying mechanisms driving the phonon softening that is associated with the charge density wave transition at lower temperatures.


2018 ◽  
Vol 115 (47) ◽  
pp. 11905-11910 ◽  
Author(s):  
Aryeh Gold-Parker ◽  
Peter M. Gehring ◽  
Jonathan M. Skelton ◽  
Ian C. Smith ◽  
Dan Parshall ◽  
...  

Hybrid organic–inorganic perovskites (HOIPs) have become an important class of semiconductors for solar cells and other optoelectronic applications. Electron–phonon coupling plays a critical role in all optoelectronic devices, and although the lattice dynamics and phonon frequencies of HOIPs have been well studied, little attention has been given to phonon lifetimes. We report high-precision momentum-resolved measurements of acoustic phonon lifetimes in the hybrid perovskite methylammonium lead iodide (MAPI), using inelastic neutron spectroscopy to provide high-energy resolution and fully deuterated single crystals to reduce incoherent scattering from hydrogen. Our measurements reveal extremely short lifetimes on the order of picoseconds, corresponding to nanometer mean free paths and demonstrating that acoustic phonons are unable to dissipate heat efficiently. Lattice-dynamics calculations using ab initio third-order perturbation theory indicate that the short lifetimes stem from strong three-phonon interactions and a high density of low-energy optical phonon modes related to the degrees of freedom of the organic cation. Such short lifetimes have significant implications for electron–phonon coupling in MAPI and other HOIPs, with direct impacts on optoelectronic devices both in the cooling of hot carriers and in the transport and recombination of band edge carriers. These findings illustrate a fundamental difference between HOIPs and conventional photovoltaic semiconductors and demonstrate the importance of understanding lattice dynamics in the effort to develop metal halide perovskite optoelectronic devices.


2021 ◽  
Vol 7 (27) ◽  
pp. eabg7394
Author(s):  
Qisi Wang ◽  
Karin von Arx ◽  
Masafumi Horio ◽  
Deepak John Mukkattukavil ◽  
Julia Küspert ◽  
...  

Charge order is universal to all hole-doped cuprates. Yet, the driving interactions remain an unsolved problem. Electron-electron interaction is widely believed to be essential, whereas the role of electron-phonon interaction is unclear. We report an ultrahigh-resolution resonant inelastic x-ray scattering (RIXS) study of the in-plane bond-stretching phonon mode in stripe-ordered cuprate La1.675Eu0.2Sr0.125CuO4. Phonon softening and lifetime shortening are found around the charge ordering wave vector. In addition to these self-energy effects, the electron-phonon coupling is probed by its proportionality to the RIXS cross section. We find an enhancement of the electron-phonon coupling around the charge-stripe ordering wave vector upon cooling into the low-temperature tetragonal structure phase. These results suggest that, in addition to electronic correlations, electron-phonon coupling contributes substantially to the emergence of long-range charge-stripe order in cuprates.


2010 ◽  
Vol 132 (12) ◽  
Author(s):  
Patrick E. Hopkins

This work examines the effects of photonically induced interband excitations from the d-band to states at the Fermi energy on the electron temperature decay in noble metals. The change in the electron population in the d-band and the conduction band causes a change in electron heat capacity and electron-phonon coupling factor. In noble metals, due to the large d-band to Fermi energy separation, the contributions to electron heat capacity and electron-phonon coupling factor of intra- and interband transitions can be separated. The two temperature model describing electron-phonon heat transfer after short-pulsed laser heating is solved using the expressions for heat capacity and electron-phonon coupling factor after intra- and interband excitations, and the predicted electron temperature change of the intra- and interband excited electrons are examined. A critical fluence value is defined that represents the absorbed fluence needed to fill all available states at a given photon energy above the Fermi level. At high absorbed laser fluences and pulse energies greater than the interband transition threshold, the interband and intraband contributions to thermophysical properties differ and are shown to affect temporal electron temperature profiles.


2013 ◽  
Vol 2013 ◽  
pp. 1-4
Author(s):  
Anu Singh ◽  
Hempal Singh ◽  
Vinod Ashokan ◽  
B. D. Indu

The defect-induced anharmonic phonon-electron problem in high-temperature superconductors has been investigated with the help of double time thermodynamic electron and phonon Green’s function theory using a comprehensive Hamiltonian which includes the contribution due to unperturbed electrons and phonons, anharmonic phonons, impurities, and interactions of electrons and phonons. This formulation enables one to resolve the problem of electronic heat transport and equilibrium phenomenon in high-temperature superconductors in an amicable way. The problem of electronic heat capacity and electron-phonon problem has been taken up with special reference to the anharmonicity, defect concentration electron-phonon coupling, and temperature dependence.


2019 ◽  
Vol 97 (5) ◽  
pp. 472-476
Author(s):  
Samin Tajik ◽  
Božidar Mitrović ◽  
Frank Marsiglio

Using the Eliashberg theory of superconductivity we have examined several properties of a model in which electrons are coupled only to rattling phonon modes represented by a sharp peak in the electron–phonon coupling function. Our choice of parameters was guided by experiments on β-pyrochlore oxide superconductor KOs2Os6. We have calculated the temperature dependence of the superconducting gap edge; the quasi-particle decay rate; the NMR relaxation rate assuming that the coupling between the nuclear spins and the conduction electrons is via a contact hyperfine interaction, which would be appropriate for the O-site in KOs2Os6; and the microwave conductivity. We examined the limit of very strong coupling by considering three values of the electron–phonon coupling parameter λ = 2.38, 3, and 5 and did not assume that the rattler frequency Ω0 is temperature dependent in the superconducting state. We obtained a very unusual temperature dependence of the superconducting gap edge Δ(T), very much like the one extracted from photoemission experiments on KOs2O6.


2014 ◽  
Vol 597 ◽  
pp. 113-116
Author(s):  
Yue Qin Wang ◽  
Juan Gao ◽  
Shao Ping Yan

We investigated the lattice dynamics and electron-phonon coupling (EPC) of superhard material OsB2by first-principles linear response calculations. The calculated EPC parameters for the optical phonon modes at Г indicate that the heavy Os atoms play the most important role in deciding the superconducting behavior, and there are sizeable contributions from lighter B atoms to EPC. Our calculated EPC constant is 0.42, and the estimated superconducting transition temperatureTcis 2.1 K using the Coulomb pseudopotentialμ*=0.125, in excellent agreement with the experimental ones.


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