Contribution of inter- and intraband transitions into electron–phonon coupling in metals

We recently developed an approach for calculation of the electron–phonon (electron–ion in a more general case) coupling in materials based on tight-binding molecular dynamics simulations. In the present work, we utilize this approach to study partial contributions of inter- and intraband electron scattering events into total electron–phonon coupling in Al, Au, and Cu elemental metals and in AlCu alloy. We demonstrate that the interband scattering plays an important role in the electron–ion energy exchange process in Al and AlCu, whereas intraband d–d transitions are dominant in Au and Cu. Moreover, inter- and intraband transitions exhibit qualitatively different dependencies on the electron temperature. Our findings should be taken into account for the interpretation of experimental results on the electron–phonon coupling parameter. Graphic abstract

When band convergence is not beneficial for thermoelectrics

Band convergence is considered a clear benefit to thermoelectric performance because it increases the charge carrier concentration for a given Fermi level, which typically enhances charge conductivity while preserving the Seebeck coefficient. However, this advantage hinges on the assumption that interband scattering of carriers is weak or insignificant. With first-principles treatment of electron-phonon scattering in the CaMg2Sb2-CaZn2Sb2 Zintl system and full Heusler Sr2SbAu, we demonstrate that the benefit of band convergence can be intrinsically negated by interband scattering depending on the manner in which bands converge. In the Zintl alloy, band convergence does not improve weighted mobility or the density-of-states effective mass. We trace the underlying reason to the fact that the bands converge at a one k-point, which induces strong interband scattering of both the deformation-potential and the polar-optical kinds. The case contrasts with band convergence at distant k-points (as in the full Heusler), which better preserves the single-band scattering behavior thereby successfully leading to improved performance. Therefore, we suggest that band convergence as thermoelectric design principle is best suited to cases in which it occurs at distant k-points.

Optimal band structure for thermoelectrics with realistic scattering and bands

Understanding how to optimize electronic band structures for thermoelectrics is a topic of long-standing interest in the community. Prior models have been limited to simplified bands and/or scattering models. In this study, we apply more rigorous scattering treatments to more realistic model band structures—upward-parabolic bands that inflect to an inverted-parabolic behavior—including cases of multiple bands. In contrast to common descriptors (e.g., quality factor and complexity factor), the degree to which multiple pockets improve thermoelectric performance is bounded by interband scattering and the relative shapes of the bands. We establish that extremely anisotropic “flat-and-dispersive” bands, although best-performing in theory, may not represent a promising design strategy in practice. Critically, we determine optimum bandwidth, dependent on temperature and lattice thermal conductivity, from perfect transport cutoffs that can in theory significantly boost zT beyond the values attainable through intrinsic band structures alone. Our analysis should be widely useful as the thermoelectric research community eyes zT > 3.

Ultrafast evolution of bulk, surface and surface resonance states in photoexcited $$\hbox {Bi}_{2}\hbox {Te}_{3}$$

We use circular dichroism (CD) in time- and angle-resolved photoemission spectroscopy (trARPES) to measure the femtosecond charge dynamics in the topological insulator (TI) $$\hbox {Bi}_{2}\hbox {Te}_{3}$$ Bi 2 Te 3 . We detect clear CD signatures from topological surface states (TSS) and surface resonance (SR) states. In time-resolved measurements, independently from the pump polarization or intensity, the CD shows a dynamics which provides access to the unexplored electronic evolution in unoccupied states of $$\hbox {Bi}_{2}\hbox {Te}_{3}$$ Bi 2 Te 3 . In particular, we are able to disentangle the unpolarized electron dynamics in the bulk states from the spin-textured TSS and SR states on the femtosecond timescale. Our study demonstrates that photoexcitation mainly involves the bulk states and is followed by sub-picosecond transport to the surface. This provides essential details on intra- and interband scattering in the relaxation process of TSS and SR states. Our results reveal the significant role of SRs in the subtle ultrafast interaction between bulk and surface states of TIs.

XXIV Международный симпозиум Нанофизика и наноэлектроника", Нижний Новгород, 10-13 марта 2020 г. Анализ фононных мод и электрон-фононного взаимодействия в квантово-каскадных лазерных гетероструктурах

The phonon modes of quantum cascade heterostructures based on binary and ternary semiconductor compounds are modeled. The dependences of the frequencies of the interface phonon modes of the structure on the wave vector in the plane of the layers and on the phase shift in the period of the superlattice are calculated. It was found that the range of variation of the quantum energy of the phonon modes of the GaAs/Al0.25Ga0.75As structure does not exceed 2 meV. The calculated resulting interband scattering rate in the structure, taking into account the interface and confined modes, practically does not differ from the calculations in the approximation of bulk phonons of the structure.