arXiv subjects

Lena Yadgarov

Publications and source records attributed to Lena Yadgarov.

4 recordsLinked to original sources

arXiv2020

The tetragonal phase of CH$_{3}$NH$_{3}$PbI$_{3}$ is strongly anharmonic

Halide perovskite (HP) semiconductors exhibit unique strong coupling between the electronic and structural dynamics. The high-temperature cubic phase of HPs is known to be entropically stabilized, with imaginary frequencies in the calculated phonon dispersion relation. Similar calculations, based on the static average crystal structure, predict a stable tetragonal phase with no imaginary modes. This work shows that in contrast to standard theory predictions, the room-temperature tetragonal phase of CH$_{3} $NH$_{3} $PbI$_{3}$ is strongly anharmonic. We use Raman polarization-orientation (PO) measurements and \textit{ab initio} molecular dynamics (AIMD) to investigate the origin and temperature evolution of the strong structural anharmonicity throughout the tetragonal phase. Raman PO measurements reveal a new spectral feature that resembles a soft mode. This mode shows an unusual continuous increase in damping with temperature which is indicative of an anharmonic potential surface. The analysis of AIMD trajectories identifies two major sources of anharmonicity: the orientational unlocking of the [CH$_{3} $NH$_{3}$]$^+$ ions and large amplitude octahedral tilting that continuously increases with temperature. Our work suggests that the standard phonon picture cannot describe the structural dynamics of tetragonal CH$_{3} $NH$_{3} $PbI$_{3}$.

cond-mat.mtrl-sci↗

arXiv2019

Halide perovskites under polarized light: Vibrational symmetry analysis using polarized Raman

In the last decade, hybrid organic-inorganic halide perovskites have emerged as a new type of semiconductor for photovoltaics and other optoelectronic applications. Unlike standard, tetrahedrally bonded semiconductors (e.g. Si and GaAs), the ionic thermal fluctuations in the halide perovskites (i.e. structural dynamics) are strongly coupled to the electronic dynamics. Therefore, it is crucial to obtain accurate and detailed knowledge about the nature of atomic motions within the crystal. This has proved to be challenging due to low thermal stability and the complex, temperature dependent structural phase sequence of the halide perovskites. Here, these challenges are overcome and a detailed analysis of the mode symmetries is provided in the low-temperature orthorhombic phase of methylammonium-lead iodide. Raman measurements using linearly- and circularly- polarized light at 1.16 eV excitation are combined with density functional perturbation theory (DFPT). By performing an iterative analysis of Raman polarization-orientation dependence and DFPT mode analysis, the crystal orientation is determined. Subsequently, accounting for birefringence effects detected using circularly polarized light excitation, the symmetries of all the observed Raman-active modes at 10 K are assigned.

cond-mat.mtrl-sci↗

arXiv2017

Ultrafast near-field imaging of exciton-polariton dynamics in WSe_2 waveguides at room temperature

Van der Waals (vdW) materials, weakly bound layered compounds, have received enormous interest as they offer a malleable playground for a wide range of physical properties in thermal, electronic and optical devices. In particular, owing to their inherent deep subwavelength light confinement, they support a variety of light-matter interactions phenomena such as plasmons, excitons and phonons conveyed as polaritonic modes. Specifically, semiconductor vdW materials such as WSe_2 are particularly attractive for photonic and quantum integrated technologies since they sustain VIS-NIR exciton-polariton modes at room temperature. In the quest to unravel the underlying physics of these intriguing phenomena, advanced subdiffraction imaging techniques such as SNOM has provided valuable insights on the nature of the EP coupling mechanism to the waveguide modes sustained in vdW materials. While most of these works focused on the steady state of the EP, the spatio-temporal dynamics of EP formation, happening in the sub-picosecond regime, remains largely unexplored. Hence, a direct imaging at the femtosecond-nanoscale of the EP evolution is critical to the understanding of these coupled light-matter states. Here we report for the first time the ultrafast and deep-subwavelength imaging of EP formation and propagation in WSe2 waveguides. Our method, based on a novel ultrafast pump-probe near-field imaging, allows to directly visualize the EP time evolution at room temperature. More specifically, and in agreement with our time dependent model, we directly observe a significantly slow EP wave packet group velocity of v_g~0.017c which is attributed to the bandgap renormalization originating in the light coupling near the exciton transition. These findings suggest that vdW materials could be used for slow light with applications in light storage for memory, enhanced optical nonlinearity, sensing and more.

cond-mat.mes-hall↗

arXiv2011

New route for stabilization of 1T-WS2 and MoS2 phases

The phenomenon of a partial 2H\rightarrow1T phase transition within multiwalled WS2 nanotubes under substitutional Rhenium doping is discovered by means of high-resolution transmission electron microscopy. Using density-functional calculations for the related MoS2 compound we consider a possible origin of this phase transition, which was known formerly only for WS2 and MoS2 intercalated by alkali metals. An interplay between the stability of layered or nanotubular forms of 2H and 1T allotropes is found to be intimately related with their electronic structures and electro-donating ability of an impurity.

cond-mat.mtrl-sci↗