Carrier-phonon Interaction Research Articles

Polarization and bandgap characteristics of monolayer black phosphoene in magnetic field

The effect of magnetic field on the polarization effect of black phosphorene is studied. The ground state energy and the relevant energy bandgap formula of carrier and carrier–phonon interaction system is derived in turn, and the effect of applied magnetic field on ground state energy and bandgap is also investigated, by the method of variational method, LLP unitary transformation method and linear combination operator method. When the substrate is given, the ground state energy and the relevant bandgap of the carrier–phonon interaction system changes with the magnetic induction intensity, phonon energy and cutoff wave vector. It can be shown by numerical calculation: The ground state energy and the relevant bandgap of the Hole and the Hole–phonon interaction system in black phosphorene increases with increase in magnetic induction intensity [Formula: see text]. The ground state energy of the Hole, Hole–phonon system and the relevant bandgap are different when the substrate is different. Under the action of a magnetic field, the ground state energy of the Hole and Hole–phonon system and bandgap decreases with increase in phonon energy and increases with increase in cutoff wave vector when the substrate is fixed.

Role of Exciton Binding Energy on LO Phonon Broadening and Polaron Formation in (BA)2PbI4 Ruddlesden–Popper Films

The effect of carrier-carrier and carrier-phonon interactions are presented in n = 1 (2D) (BA)2PbI4 Ruddlesden-Popper thin films and their effect compared to that of conventional MAPbI3. While temp...

Hot Phonon and Auger Heating Mediated Slow Intraband Carrier Relaxation in Mixed Halide Perovskite

A clear understanding of excited carrier relaxation to their equilibrium state via carrier-phonon, carrier-carrier interaction etc. is always required for the advancement of perovskite based device performance. Organic/inorganic lead halide perovskite have shown remarkable slow hot carrier cooling properties. Herein, we investigate the effect of hot phonon and Auger heating on hot carrier relaxation dynamics in Methyl-ammonium lead iodide-chloride (CH3NH3PbI3-XClX or mixed halide) perovskite using transient absorption spectroscopy. The reduced energy-loss rate on sub-picosecond time scale clearly shows the non-equilibrium build-up of longitudinal optical and acoustic phonon modes (carrier-phonon interaction) at low pump excitation (1018 cm-3). However at high pump excitation (1019 cm-3), dominating Auger heating process (carrier-carrier interaction) further reduces the energy-loss rate by more than two order of magnitude and delays the carrier relaxation process to tens of picoseconds which makes perovskite as a promising candidates in hot carrier photovoltaic.

Lead-free cesium tin halide nanocrystals for light-emitting diodes and color down conversion.

Organometal halide perovskites are attracting a great deal of attention because of their long carrier diffusion lengths, wide wavelength tunability, and narrow-band emission. However, the toxicity of lead has caused considerable environmental and health concerns. In this work, lead-free cesium tin halide nanocrystals are synthesized and investigated. CsSnBr3 and CsSnI3 nanocrystals, 25 and 7 nm in size, are synthesized by a facile hot injection method. Absorption spectroscopy, photoluminescence spectroscopy, and X-ray diffraction were used to understand their structural and optical properties. CsSnBr3 and CsSnI3 nanocrystals show emission peaks at 683 and 938 nm, respectively. These nanocrystals show shelf stability for a few months. Temperature-dependent photoluminescence is utilized to know more about fundamental physical parameters, such as exciton binding energy, charge carrier–phonon interactions and band gap. Light-emitting diodes and color down-conversion films are also demonstrated using these lead free perovskite nanocrystals.

Possible Fröhlich surface polaron formation in graphene on a polar substrate

Abstract We theoretically study the formation of Frohlich polaron in monolayer graphene on a substrate made of polar materials. In this calculation, the Rayleigh-Schrodinger perturbation theory is used to obtain analytical expression of polaron energy. The decrease (increase) in the electron (hole) energy due to interaction with surface optical phonons indicates that the formation of a surface polaron is preferred. The charge carrier-phonon interaction in monolayer graphene on a polar substrate does not lead to the formation of a gap between the valence and the conduction bands, as there exist the same energy shifts for both electron and hole at k = 0 . The expression for the renormalized Fermi velocity due to carrier-phonon coupling for small values of k is obtained. Our results show that the influence of the screening effect on polaron energies is significant for k ≤ k F .

Non-Markovian stochastic Schrödinger equation in k-space toward the calculation of carrier dynamics in organic semiconductors.

A non-Markovian stochastic Schrödinger equation developed in our former work [Y. Ke and Y. Zhao, J. Chem. Phys. 147, 184103 (2017)] is extended to the reciprocal (k-) space to calculate the carrier dynamics in organic semiconductors with both local and nonlocal carrier-phonon interactions taken into account. The validity of this approach is examined by comparing with numerically exact benchmark results. As an application, the carrier mobilities are calculated within a one-dimensional periodic lattice model. The results reveal an inversion in the magnitude of the mobility as the nonlocal carrier-phonon interaction varies from weak to strong strengths, indicating a transition of the transport mechanism. This is also demonstrated by a variation in the temperature dependence of the mobility. In addition, a transient localization diffusive behavior caused by intramolecular vibrations is also found.

Collaborative effect of plasmon-induced resonance energy and electron transfer on the interfacial electron injection dynamics of dye-sensitized solar cell.

It has been widely recognized that plasmonic metal nanoparticles (MNPs) can enhance the power convention efficiency (PCE) of dye-sensitized solar cells (DSSCs). This enhancement is ascribed to the combined effects of plasmon decay, scattering, near-field enhancement, and exciting charge carriers in semiconductors through plasmon-induced resonance energy transfer (PIRET) and hot electron injection (HEI). PIRET and HEI processes appeared between MNPs, and semiconductors have been intensively investigated; however, it is not clear how the collaborative effect of PIRET and photon-induced direct and indirect electron transfer (PICT) occurred between plasmonic metals and dyes, and the interference of different charge separation channels (CSCs) starting from PIRET and PICT affects the PCE of DSSCs. This work aims to address these issues. We apply a model Hamiltonian method, which obviously includes both PIRET and PICT processes from Au MNP to dye molecules and incorporates the dye's electron-phonon interaction, to investigate the carrier dynamics. It is found that PIRET deforms the wavepacket dynamics of the molecular excited state and results in ten-fold enhancement of dye absorption. MNPs augment light absorption and increase the electron density in empty molecular orbitals of the dye molecule. Consequently, this enhances the interfacial charge separation. Furthermore, we observed the interference behavior of two CSCs and gave a full-scale insight into the correlation between the constructive/destructive interference and the electronic-state properties as well as carrier-phonon interactions. This work provides a theoretical guidance to optimize DSSCs.

Optical Properties of Single-Crystal Germanium in the THz Range

The transmission of intrinsic, antimony-doped, and gallium-doped Ge single crystals in the THz spectral range have been experimentally investigated. It is shown that the attenuation coefficient of intrinsic germanium in the range of 160‒220 μm is at a level of ~0.5 cm‒1, a value comparable with that for silicon. The free-carrier absorption cross sections of silicon and germanium are significantly different, which may be caused by the difference in the mechanisms of carrier–phonon interaction in these materials.

Оптические свойства монокристаллического германия в терагерцовой области спектра

AbstractThe transmission of intrinsic, antimony-doped, and gallium-doped Ge single crystals in the THz spectral range have been experimentally investigated. It is shown that the attenuation coefficient of intrinsic germanium in the range of 160‒220 μm is at a level of ~0.5 cm^‒1, a value comparable with that for silicon. The free-carrier absorption cross sections of silicon and germanium are significantly different, which may be caused by the difference in the mechanisms of carrier–phonon interaction in these materials.

Acceleration of Photocarrier Relaxation in Graphene Achieved by Epitaxial Growth: Ultrafast Photoluminescence Decay of Monolayer Graphene on SiC

Acceleration of photocarrier relaxation in graphene results in the enhancement of its properties for graphene-based ultrafast optical devices. The acceleration can be achieved by utilizing the relaxation paths outside the graphene to avoid bottlenecks in the graphene for photocarrier relaxation. In this study, we investigate photocarrier relaxation in epitaxial and transferred monolayer graphene on SiC with a buffer layer at room temperature by means of time-resolved photoluminescence spectroscopy. The photoluminescence decay at 0.7 eV in the epitaxial monolayer graphene is faster than that in the transferred monolayer graphene. On the basis of the three-temperature model calculation, it is found that the carrier–phonon interaction with phonons of the buffer layer for the epitaxial monolayer graphene is 3 times stronger than that for the transferred monolayer graphene. This study demonstrates that ultrafast photocarrier relaxation can be achieved in graphene by epitaxial growth.

Probing Phonon Dynamics in Individual Single-Walled Carbon Nanotubes.

Interactions between elementary excitations, such as carriers, phonons, and plasmons, are critical for understanding the optical and electronic properties of materials. The significance of these interactions is more prominent in low-dimensional materials and can dominate their physical properties due to the enhanced interactions between these excitations. One-dimensional single-walled carbon nanotubes provide an ideal system for studying such interactions due to their perfect physical structures and rich electronic properties. Here we investigated G-mode phonon dynamics in individual suspended chirality-resolved single-walled carbon nanotubes by time-resolved anti-Stokes Raman spectroscopy. The improved technique allowed us to probe the intrinsic phonon information on a single-tube level and exclude the influences of tube-tube and tube-substrate interactions. We found that the G-mode phonon lifetime ranges from 0.75-2.25 ps and critically depends on whether the tube is metallic or semiconducting. In comparison with the phonon lifetimes in graphene and graphite, we revealed structure-dependent carrier-phonon and phonon-phonon interactions in nanotubes. Our results provide new information for optimizing the design of nanotube electronic/optoelectronic devices by better understanding and utilizing their phonon decay channels.

Controllable population dynamics in Landau-quantized graphene

In this paper, we carry out a theoretical investigation on the population dynamics of graphene system under continuous-wave (cw) laser and chirped pulse excitation. Results of our numerical simulations reveal that complete population transfer from an initially occupied ground state to the initially unoccupied excited states can be achieved by choosing appropriate values of the chirp rate, the laser field intensity and frequency, as well as other system parameters. Also, we observe coherent Rabi-like population oscillations between the initial ground state and the excited final state. It is induced by the combined effect of cw and chirped-pulse laser fields. These results will contribute to the understanding of carrier-carrier and carrier-phonon interactions in graphene system, and may find applications in graphene-based high-speed electronic and optoelectronic devices.

Carrier transport in layered nanolaminated carbides

This paper summarizes the ab-initio electronic and phonon band structures and the temperature-dependent carrier transport in layered Ti2AlC. It is found that the cylindrical Fermi surface is the origin of the anisotropic carrier effective mass (infinite effective mass along the c axis), which leads to a strong anisotropic (insulator along the c axis and metallic along the layer) carrier transport in these films. Using electronic and phonon band structure calculations, we have developed an analytical model for the carrier-phonon interaction and the in-plane carrier conductivity originating from the strong inter-valley (s → d) scattering in Ti2AlC. The density functional theory is used to calculate the average deformation potential corresponding to the acoustic phonon vibrations. The calculated deformation potential is in good agreement with the extracted deformation potential from the transport data available in the literature. The extracted deformation potential will be useful for predicting the transport quantities of these metals at elevated temperatures.

Identification of Ultrafast Photophysical Pathways in Photoexcited Organic Heterojunctions

The exciton dissociation and charge separation occurring on subpicosecond time scales following the photoexcitation are studied in a model donor/acceptor heterojunction using a fully quantum approach. Higher-than-LUMO acceptor orbitals which are energetically aligned with the donor LUMO orbital participate in the ultrafast interfacial dynamics by creating photon-absorbing charge-bridging states in which charges are spatially separated and which can be directly photoexcited. Along with the states brought about by single-particle resonances, the two-particle (exciton) mixing gives rise to bridge states in which charges are delocalized. Bridge states open up a number of photophysical pathways that indirectly connect the initial donor states with states of spatially separated charges and compete with the efficient progressive deexcitation within the manifold of donor states. The diversity and efficiency of these photophysical pathways depend on a number of factors, such as the precise energy alignment of exciton states, the central frequency of the excitation, and the strength of carrier–phonon interaction.

Midinfrared Photoluminescence up to 290 K Reveals Radiative Mechanisms and Substrate Doping-Type Effects of InAs Nanowires.

Photoluminescence (PL) as a conventional yet powerful optical spectroscopy may provide crucial insight into the mechanism of carrier recombination and bandedge structure in semiconductors. In this study, mid-infrared PL measurements on vertically aligned InAs nanowires (NWs) are realized for the first time in a wide temperature range of up to 290 K, by which the radiative recombinations are clarified in the NWs grown on n- and p-type Si substrates, respectively. A dominant PL feature is identified to be from the type-II optical transition across the interfaces between the zinc-blend (ZB) and the wurtzite (WZ) InAs, a lower-energy feature at low temperatures is ascribed to impurity-related transition, and a higher-energy feature at high temperatures originates in the interband transition of the WZ InAs being activated by thermal-induced electron transfer. The optical properties of the ZB-on-WZ and WZ-on-ZB interfaces are asymmetric, and stronger nonradiative recombination and weaker carrier-phonon interaction show up in the NWs on p-type substrate in which built-in electric field forms and leads to carrier assembling around the WZ-on-ZB interface. The results indicate that wide temperature-range infrared PL analysis can serve as efficient vehicle for clarifying optical properties and bandedge processes of the crystal-phase interfaces in vertically aligned InAs NWs.

Nanoshell-mediated robust entanglement between coupled quantum dots

The exact entanglement dynamics in a hybrid structure consisting of two quantum dots (QDs) in the proximity of a metal nanoshell is investigated. Nanoshells can enhance the local density of states, leading to a strong-coupling regime where the excitation energy can coherently be transferred between the QDs and the nanoshell in the form of Rabi oscillations. The long-lived entangled states can be created deterministically by optimizing the shell thickness as well as the ratio of the distances between the QDs and the surface of the shell. The loss of the system is greatly reduced even when the QDs are ultraclose to the shell, which signifies a slow decay rate of the coherence information and longtime entanglement preservation. Our protocol allows for an on-demand, fast, and almost perfect entanglement even at strong carrier-phonon interaction where other systems fail.

Impact of doping on the carrier dynamics in graphene.

We present a microscopic study on the impact of doping on the carrier dynamics in graphene, in particular focusing on its influence on the technologically relevant carrier multiplication in realistic, doped graphene samples. Treating the time- and momentum-resolved carrier-light, carrier-carrier, and carrier-phonon interactions on the same microscopic footing, the appearance of Auger-induced carrier multiplication up to a Fermi level of 300 meV is revealed. Furthermore, we show that doping favors the so-called hot carrier multiplication occurring within one band. Our results are directly compared to recent time-resolved ARPES measurements and exhibit an excellent agreement on the temporal evolution of the hot carrier multiplication for n- and p-doped graphene. The gained insights shed light on the ultrafast carrier dynamics in realistic, doped graphene samples.

Carrier-carrier and carrier-phonon interactions in the dynamics of photoexcited electrons in graphene

In this work we use the Monte Carlo method to simulate the photoexcited carrier relaxation dynamics in suspended monolayer graphene to unveil the role of the different scattering mechanisms involved. The results show a strong activity of carrier-carrier and carrier-optical phonon interactions in the very early stages of the relaxation process driving the thermalization and cooling dynamics. The consideration of the coupling between the electron and phonon population reveals an intense damping in the cooling rates that is dependent on the pumped carrier concentration.

The new metal–insulator transitions and nanoscale phase separation in doped cuprates

We use the theory of extrinsic and intrinsic polarons to examine the new mechanisms of metal-insulating transitions (MITs) and nanoscale phase separation in hole-doped cuprates and propose a unified description of these interrelated phenomena. We argue that the relevant charge carriers in these polar materials are extrinsic (impurity-bound) and intrinsic large polarons. We show that the strong carrier-defect-phonon and carrier-phonon interactions together with the charge inhomogeneities are responsible for the carrier localization, the ordering of polaronic carriers and formation of their superlattices, the new MITs and nanoscale phase separation, which are accompanied by the stripe formation in the lightly to the slightly underdoped cuprates. We demonstrate that in doped cuprates La2-xSrxCuO4 and YBa2Cu3O7-δ the static (insulating) and dynamic (metallic) stripes coexist in the doping range x≃0.03–0.13. Our results are in quantitative agreement with experimental findings in these high-Tc materials.

Excitonic polarons in low-dimensional transition metal dichalcogenides

We examine the excitonic polaron properties of common monolayer transition metal dichalcogenides (MoS2, MoSe2, WS2 and WSe2). The excitonic polaron is formed when excitons interact with acoustic or optical phonons via coupling to the deformation potentials associated with the conduction and valence bands. A unitary transformation which performs an approximate diagonalization of the exciton–phonon operator is used to evaluate the ground state energy of the excitonic polaron. We derive analytical expressions of the changes in the excitonic polaron energy and mass at small exciton wavevectors involving the deformation potential due to optical phonons. The polaronic effect of the monolayer transition metal dichalcogenides is examined by comparing changes in the energy gap shift and effective masses based on known deformation potential constants for carrier–phonon interactions. Our results indicate the occurrence of comparable energy shifts when the ground state exciton interacts with optical or acoustic phonons. We extend our calculations to explore the influence of exciton–lattice interactions on the binding energies and the self-trapping of excitons in two-dimensional layers of transition metal dichalcogenides.