Nonequilibrium electron and lattice dynamics of strongly correlated Bi2Sr2CaCu2O8+? single crystals.
ABSTRACT: The interplay between the electronic and lattice degrees of freedom in nonequilibrium states of strongly correlated systems has been debated for decades. Although progress has been made in establishing a hierarchy of electronic interactions with the use of time-resolved techniques, the role of the phonons often remains in dispute, a situation highlighting the need for tools that directly probe the lattice. We present the first combined megaelectron volt ultrafast electron diffraction and time- and angle-resolved photoemission spectroscopy study of optimally doped Bi2Sr2CaCu2O8+?. Quantitative analysis of the lattice and electron subsystems' dynamics provides a unified picture of nonequilibrium electron-phonon interactions in the cuprates beyond the N-temperature model. The work provides new insights on the specific phonon branches involved in the nonequilibrium heat dissipation from the high-energy Cu-O bond stretching "hot" phonons to the lowest-energy acoustic phonons with correlated atomic motion along the <110> crystal directions and their characteristic time scales. It reveals a highly nonthermal phonon population during the first several picoseconds after the photoexcitation. The approach, taking advantage of the distinct nature of electrons and photons as probes, is applicable for studying energy relaxation in other strongly correlated electron systems.
Project description:The manipulation of coherent phonons in condensed systems has attracted fundamental interest, particularly for its applications to future devices. We demonstrate that a coherent phonon in Co/Pt nano-multilayer can be quantitatively controlled via electron-lattice coupling, specifically by changing the multilayer repeat number. To that end, systematic measurement of the time-resolved reflectivity and magneto-optical Kerr effect in Co/Pt multilayers was performed. The coherent phonon frequency was observed to be shifted with the change of the multilayer repeat number. This shift could be clearly explained based on the two-temperature model. Detailed analysis indicated that the lattice heat capacity and electron-lattice coupling strength are linearly dependent on the repeat number of the periodic multilayer structures. Accessing the control of coherent phonons using nanostructures opens a new avenue for advanced phonon-engineering applications.
Project description:A rapidly-growing interest in WTe2 has been triggered by the giant magnetoresistance effect discovered in this unique system. While many efforts have been made towards uncovering the electron- and spin-relevant mechanisms, the role of lattice vibration remains poorly understood. Here, we study the coherent vibrational dynamics in WTe2 crystals by using ultrafast pump-probe spectroscopy. The oscillation signal in time domain in WTe2 has been ascribed as due to the coherent dynamics of the lowest energy A1 optical phonons with polarization- and wavelength-dependent measurements. With increasing temperature, the phonon energy decreases due to anharmonic decay of the optical phonons into acoustic phonons. Moreover, a significant drop (15%) of the phonon energy with increasing pump power is observed which is possibly caused by the lattice anharmonicity induced by electronic excitation and phonon-phonon interaction.
Project description: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.
Project description:Electron-phonon coupling (EPC) plays an important role in solid state physics. Here, we demonstrate an experimental method that enables investigation of the elemental processes of the indirect transition, in which EPC participates in photoexcitation in solids, by resolving the energy and momentum of phonons and electrons simultaneously. For graphite, we used angle-resolved photoelectron spectroscopy to observe electron emission at the Γ-point being scattered from the K-point by a phonon. Energy conservation during phonon emission implies that the step-like structure in the spectrum is near the Fermi level, and angle-resolved measurements revealed phonon dispersions that contribute to EPC because of parallel momentum conservation. The observed phonon branch depends on the photon energy, i.e., the final photoexcitation state; this dependency is partly explained by the selection rule, which is determined by the electron state symmetry for the initial, intermediate, and final states and the phonon.
Project description:Hybrid organic-inorganic halide perovskites have shown remarkable optoelectronic properties, exhibiting an impressive tolerance to defects believed to originate from correlated motion of charge carriers and the polar lattice forming large polarons. Few experimental techniques are capable of directly probing these correlations, requiring simultaneous sub-millielectron volt energy and femtosecond temporal resolution after absorption of a photon. Here, we use time-resolved multi-THz spectroscopy, sensitive to the internal excitations of the polaron, to temporally and energetically resolve the coherent coupling of charges to longitudinal optical phonons in single-crystal CH<sub>3</sub>NH<sub>3</sub>PbI<sub>3</sub> (MAPI). We observe room temperature intraband quantum beats arising from the coherent displacement of charge from the coupled phonon cloud. Our measurements provide strong evidence for the existence of polarons in MAPI at room temperature, suggesting that electron/hole-phonon coupling is a defining aspect of the hybrid metal-halide perovskites contributing to the protection from scattering and enhanced carrier lifetimes that define their usefulness in devices.
Project description:Electronic properties and lattice vibrations are expected to be strongly correlated in metal-halide perovskites, due to the soft fluctuating nature of their crystal lattice. Thus, unveiling electron-phonon coupling dynamics upon ultrafast photoexcitation is necessary for understanding the optoelectronic behavior of the semiconductor. Here, we use impulsive vibrational spectroscopy to reveal vibrational modes of methylammonium lead-bromide perovskite under electronically resonant and non-resonant conditions. We identify two excited state coherent phonons at 89 and 106?cm-1, whose phases reveal a shift of the potential energy minimum upon ultrafast photocarrier generation. This indicates the transition to a new geometry, reached after approximately 90?fs, and fully equilibrated within the phonons lifetime of about 1?ps. Our results unambiguously prove that these modes drive the crystalline distortion occurring upon photo-excitation, demonstrating the presence of polaronic effects.
Project description:Investigation of the non-equilibrium dynamics after an impulsive impact provides insights into couplings among various excitations. A two-temperature model (TTM) is often a starting point to understand the coupled dynamics of electrons and lattice vibrations: the optical pulse primarily raises the electronic temperature T(el) while leaving the lattice temperature T(l) low; subsequently the hot electrons heat up the lattice until T(el) = T(l) is reached. This temporal hierarchy owes to the assumption that the electron-electron scattering rate is much larger than the electron-phonon scattering rate. We report herein that the TTM scheme is seriously invalidated in semimetal graphite. Time-resolved photoemission spectroscopy (TrPES) of graphite reveals that fingerprints of coupled optical phonons (COPs) occur from the initial moments where T(el) is still not definable. Our study shows that ultrafast-and-efficient phonon generations occur beyond the TTM scheme, presumably associated to the long duration of the non-thermal electrons in graphite.
Project description:High harmonic generation of ultrafast laser pulses can be used to perform angle-resolved photoemission spectroscopy (ARPES) to map the electronic band structure of materials with femtosecond time resolution. However, currently it is difficult to reach high momenta with narrow energy resolution. Here, we combine a gas phase extreme ultraviolet (XUV) femtosecond light source, an XUV monochromator, and a time-of-flight electron analyzer to develop XUV-based time-resolved ARPES. Our technique can produce tunable photon energy between 24-33 eV with an unprecedented energy resolution of 30 meV and time resolution of 200 fs. This technique enables time-, energy- and momentum-resolved investigation of the nonequilibrium dynamics of electrons in materials with a full access to their first Brillouin zone. We evaluate the performance of this setup through exemplary measurements on various quantum materials, including WTe2, WSe2, TiSe2, and Bi2Sr2CaCu2O8+δ.
Project description:The low-energy electronic structure, including the Fermi surface topology, of the itinerant metamagnet [Formula: see text] is investigated for the first time by synchrotron-based angle-resolved photoemission. Well-defined quasiparticle band dispersions with matrix element dependencies on photon energy or photon polarization are presented. Four bands crossing the Fermi-level, giving rise to four Fermi surface sheets are resolved; and their complete topography, effective mass as well as their electron and hole character are determined. These data reveal the presence of kink structures in the near-Fermi-level band dispersion, with energies ranging from 30 to 69 meV. Together with previously reported Raman spectroscopy and lattice dynamic calculation studies, the data suggest that these kinks originate from strong electron-phonon coupling present in [Formula: see text]. Considering that the kink structures of [Formula: see text] are similar to those of the other three members of the Ruddlesden Popper structured ruthenates, the possible universality of strong coupling of electrons to oxygen-related phonons in [Formula: see text] compounds is proposed.
Project description:The role of the crystal lattice for the electronic properties of cuprates and other high-temperature superconductors remains controversial despite decades of theoretical and experimental efforts. While the paradigm of strong electronic correlations suggests a purely electronic mechanism behind the insulator-to-metal transition, recently the mutual enhancement of the electron-electron and the electron-phonon interaction and its relevance to the formation of the ordered phases have also been emphasized. Here, we combine polarization-resolved ultrafast optical spectroscopy and state-of-the-art dynamical mean-field theory to show the importance of the crystal lattice in the breakdown of the correlated insulating state in an archetypal undoped cuprate. We identify signatures of electron-phonon coupling to specific fully symmetric optical modes during the buildup of a three-dimensional (3D) metallic state that follows charge photodoping. Calculations for coherently displaced crystal structures along the relevant phonon coordinates indicate that the insulating state is remarkably unstable toward metallization despite the seemingly large charge-transfer energy scale. This hitherto unobserved insulator-to-metal transition mediated by fully symmetric lattice modes can find extensive application in a plethora of correlated solids.