arXiv subjects

Mark J. Stern

Publications and source records attributed to Mark J. Stern.

4 recordsLinked to original sources

arXiv2020

Mechanisms of electron-phonon coupling unraveled in momentum and time: The case of soft-phonons in TiSe$_2$

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-TiSe$_2$ in both momentum and time. We are able to distinguish effects due to the real part of the many-body bare electronic susceptibility, $\Re\left[χ_0(\mathbf{q})\right]$, from those due to the electron-phonon coupling vertex, $g_{\mathbf{q}}$, by following the response of semi-metallic (normal phase) 1T-TiSe$_2$ to the selective photo-doping of carriers into the electron pocket at the Fermi level. Quasi-impulsive and wavevector-specific renormalization of soft zone-boundary phonon frequencies (stiffening) is observed, followed by wavevector-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.

cond-mat.str-el↗

arXiv2019

Time- and momentum-resolved phonon population dynamics with ultrafast electron diffuse scattering

Interactions between the lattice and charge carriers can drive the formation of phases and ordering phenomena that give rise to conventional superconductivity, insulator-to-metal transitions, and charge-density waves. These couplings also play a determining role in properties that include electric and thermal conductivity. Ultrafast electron diffuse scattering (UEDS) has recently become a viable laboratory-scale tool to track energy flow into and within the lattice system across the entire Brillouin zone, and deconvolves interactions in the time domain. Here, we present a detailed quantitative framework for the interpretation of UEDS signals, ultimately extracting the phonon mode occupancies across the entire Brillouin zone. These transient populations are then used to extract momentum- and mode-dependent electron-phonon and phonon-phonon coupling constants. Results of this analysis are presented for graphite, which provides complete information on the phonon-branch occupations and a determination of the $A_1'$ phonon mode-projected electron-phonon coupling strength $\langle g_{e,A_1'}^2 \rangle = 0.035 \pm 0.001$ eV$^2$ that is in agreement with other measurement techniques and simulations.

cond-mat.mtrl-sci↗

arXiv2017

Mapping momentum-dependent electron-phonon coupling and non-equilibrium phonon dynamics with ultrafast electron diffuse scattering

Despite their fundamental role in determining material properties, detailed momentum-dependent information on the strength of electron-phonon and phonon-phonon coupling (EPC and PPC, respectively) across the entire Brillouin zone (BZ) has proved difficult to obtain. Here we demonstrate that ultrafast electron diffuse scattering (UEDS) directly provides such information. By exploiting symmetry-based selection rules and time-resolution, scattering from different phonon branches can be distinguished even without energy resolution. Using graphite as a model system, we show that UEDS patterns map the relative EPC and PPC strength through their profound sensitivity to photoinduced changes in phonon populations. We measure strong EPC to the $K$-point transverse optical phonon of $A_1'$ symmetry ($K-A_1'$) and along the entire longitudinal optical branch between $Γ-K$, not only to the $Γ-E_{2g}$ phonon as previously emphasized. We also determine that the subsequent phonon relaxation pathway involves three stages; decay via several identifiable channels to transverse acoustic (TA) and longitudinal acoustic (LA) phonons (1-2 ps), intraband thermalization of the non-equilibrium TA/LA phonon populations (30-40 ps) and interband relaxation of the LA/TA modes (115 ps). Combining UEDS with ultrafast angle-resolved photoelectron spectroscopy will yield a complete picture of the dynamics within and between electron and phonon subsystems, helping to unravel complex phases in which the intertwined nature of these systems have a strong influence on emergent properties.

cond-mat.mtrl-sci↗

arXiv2017

Solving the Jitter Problem in Microwave Compressed Ultrafast Electron Diffraction Instruments: Robust Sub-50 fs Cavity-Laser Phase Stabilization

We demonstrate the compression of electron pulses in a high-brightness ultrafast electron diffraction (UED) instrument using phase-locked microwave signals directly generated from a mode-locked femtosecond oscillator. Additionally, a continuous-wave phase stabilization system that accurately corrects for phase fluctuations arising in the compression cavity from both power amplification and thermal drift induced detuning was designed and implemented. An improvement in the microwave timing stability from 100 fs to 5 fs RMS is measured electronically and the long-term arrival time stability ($>$10 hours) of the electron pulses improves to below our measurement resolution of 50 fs. These results demonstrate sub-relativistic ultrafast electron diffraction with compressed pulses that is no longer limited by laser-microwave synchronization.

physics.plasm-ph↗