Enhancement of carrier lifetime by spin-orbit coupling in a topological insulator of an Sb2Te3 thin film.

Electrons and phonons in chalcogenide-based materials are important factors in the performance of optical data-storage media and thermoelectric devices. However, the fundamental kinetics of carriers in chalcogenide materials remains controversial, and active debate continues over the mechanism responsible for carrier relaxation. In this study, we used optical-pump terahertz-probe spectroscopy, which permits the relationship between structural phase transition and optical property transitions to be examined, to investigate the ultrafast carrier dynamics in a multilayered [Sb(3 Å)/Te(9 Å)]n thin film during the transition from the disordered to crystalline phase. Using terahertz time-domain spectroscopy and a contact-free optical technique, we demonstrated that the optical conductance and carrier concentration vary as functions of annealing temperature. Moreover, we observed that the topological surface state (TSS) affects the enhancement of the carrier lifetime, which is closely related to the degree of spin-orbit coupling (SOC). The combination of the optical technique and proposed carrier relaxation mechanism provides a powerful tool for monitoring TSS and SOC. Consequently, it was determined that the response of the disordered phase is dominated by an electron-phonon coupling effect, while that of the crystalline structure is controlled by a Dirac surface state and SOC effects. These results are important for understanding the fundamental physics of phase change materials and for optimizing and designing materials with better performance in optoelectronic devices.

Electron transport mechanism of bathocuproine exciton blocking layer in organic photovoltaics.

Efficient exciton management is a key issue to improve the power conversion efficiency of organic photovoltaics (OPVs). It is well known that the insertion of an exciton blocking layer (ExBL) having a large band gap promotes the efficient dissociation of photogenerated excitons at the donor-acceptor interface. However, the large band gap induces an energy barrier which disrupts the charge transport. Therefore, building an adequate strategy based on the knowledge of the true charge transport mechanism is necessary. In this study, the true electron transport mechanism of a bathocuproine (BCP) ExBL in OPVs is comprehensively investigated by in situ ultraviolet photoemission spectroscopy, inverse photoemission spectroscopy, density functional theory calculation, and impedance spectroscopy. The chemical interaction between deposited Al and BCP induces new states within the band gap of BCP, so that electrons can transport through these new energy levels. Localized trap states are also formed upon the Al-BCP interaction. The activation energy of these traps is estimated with temperature-dependent conductance measurements to be 0.20 eV. The Al-BCP interaction induces both transport and trap levels in the energy gap of BCP and their interplay results in the electron transport observed.

Tuning the Fermi level with topological phase transition by internal strain in a topological insulator Bi2Se3 thin film.

In a three-dimensional topological insulator Bi2Se3, a stress control for band gap manipulation was predicted but no systematic investigation has been performed yet due to the requirement of large external stress. We report herein on the strain-dependent results for Bi2Se3 films of various thicknesses that are grown via a self-organized ordering process. Using small angle X-ray scattering and Raman spectroscopy, the changes of d-spacings in the crystal structure and phonon vibration shifts resulted from stress are clearly observed when the film thickness is below ten quintuple layers. From the UV photoemission/inverse photoemission spectroscopy (UPS/IPES) results and ab initio calculations, significant changes of the Fermi level and band gap were observed. The deformed band structure also exhibits a Van Hove singularity at specific energies in the UV absorption experiment and ab initio calculations. Our results, including the synthesis of a strained ultrathin topological insulator, suggest a new direction for electronic and spintronic applications for the future.

Evolution of the surface state in Bi2Se2Te thin films during phase transition.

Topological insulators, a new quantum state of matter, have created exciting opportunities for studies in topological quantum physics and for exploring spintronics applications due to their gapless helical metallic surface states. In this study, thin films composed of alternate layers of Bi and Se (Te) ({Bi(3 Å)Te(9 Å)}n/{Bi(3 Å)Se(9 Å)}n) were fabricated by controlling the layer thickness within the atomic scale using thermal evaporation techniques. The high-purity growth of uniform Bi2Se2Te1 thin films has not yet been achieved using a thermal evaporation method. However, as a result of a self-ordering process during annealing, an as-grown amorphous film with p-type polarity could transform into single crystalline Bi2Se2Te1 with n-type polarity. Using THz-time domain spectroscopy (THz-TDS) and ultraviolet photoemission spectroscopy (UPS), we concluded that the conductivity is dominated by the Drude contribution, suggesting the presence of a quantum well state and surface states. Moreover we demonstrated that the emission of terahertz waves from the (001) surface of the single crystalline Bi2Se2Te1 thin film would be possible under the excitation of 790 nm femtosecond optical pulses, indicating the presence of a Dirac-fermion, a photo-Dember effect at the surface state and the transient current within the surface depletion region. The results reported herein provide useful information regarding a valuable deposition method that can be useful in studies of the evolution of surface state electrons in topological insulators.

Terahertz single conductance quantum and topological phase transitions in topological insulator Bi2Se3 ultrathin films.

Strong spin-orbit interaction and time-reversal symmetry in topological insulators generate novel quantum states called topological surface states. Their study provides unique opportunities to explore exotic phenomena such as spin Hall effects and topological phase transitions, relevant to the development of quantum devices for spintronics and quantum computation. Although ultrahigh-vacuum surface probes can identify individual topological surface states, standard electrical and optical experiments have so far been hampered by the interference of bulk and quantum well states. Here, with terahertz time-domain spectroscopy of ultrathin Bi2Se3 films, we give evidence for topological phase transitions, a single conductance quantum per topological surface state, and a quantized terahertz absorbance of 2.9% (four times the fine structure constant). Our experiment demonstrates the feasibility to isolate, detect and manipulate topological surface states in the ambient at room temperature for future fundamental research on the novel physics of topological insulators and their practical applications.

Theoretical study on the effects of nitrogen and methyl substitution on tris-(8-hydroxyquinoline) aluminum: an efficient exciton blocking layer for organic photovoltaic cells.

We studied the effect of nitrogen and methyl substitution on tris-(8-hydroxyquinoline) aluminum (Alq(3)) with density functional theory, which has been adopted as an exciton blocking layer (EBL) in organic photovoltaic cells (OPVCs). The substitution of electron withdrawing nitrogen on the phenoxide moiety of Alq(3) lowers the highest molecular orbital (HOMO) level, thus photogenerated excitons can be effectively blocked in OPVC. Additional substitution of methyl on the pyridine moiety makes that Alq(3) has a smaller electron reorganization energy, which results in higher electron mobility with keeping HOMO level almost intact. Therefore, nitrogen and methyl simultaneous substitution shows high performance both in exciton blocking and electron mobility. This is the origins of the short circuit current enhancement in OPVC with 4-hydroxy-8-methyl-1,5-naphthyridine aluminum chelate (Alq(3) with the substitution of both nitrogen and methyl group) EBL.

Electronic structure of Te/Sb/Ge and Sb/Te/Ge multi layer films using photoelectron spectroscopy.

Te/Sb/Ge and Sb/Te/Ge multilayer films with an atomically controlled interface were synthesized using effusion cell and e-beam techniques. The layers interacted during the deposition, resulting in films composed of Sb-Te+Sb-Sb/Ge and Sb/Sb-Te/Ge-Te/Ge respectively. Atomic diffusion and chemical reactions in films during the annealing process were investigated by photoemission spectroscopy. In the case of Te/Sb/Ge, Ge diffused into the Sb-Te region released Sb in Sb-Te bonds and interacted with residual Te, resulting in a change in valence band line shape, which was similar to that of a Ge(1)Sb(2)Te(4) crystalline phase. The Ge-Sb-Te alloy underwent a stoichiometric change during the process, resulting in a 1.2:2:4 ratio, consistent with the most stable stoichiometry value calculated by ab initio density-functional theory. The experimental results strongly suggest that the most stable structure is generated through a reaction process involving the minimization of total energy. In addition, Ge in the Sb/Te/Ge film diffused into Sb-Te region by thermal energy. However, Ge was not able to diffuse to the near surface because Sb atoms of the high concentration at the surface were easily segregated and hindered the diffusion of other elements.

The interface state assisted charge transport at the MoO(3)/metal interface.

The interface formation between a metal and MoO(3) was examined. We carried out in situ ultraviolet and x-ray photoemission spectroscopy with step-by-step deposition of MoO(3) on clean Au and Al substrates. The MoO(3) induces huge interface dipoles, which significantly increase the work functions of Au and Al surfaces. This is the main origin of the carrier injection improvement in organic devices. In addition, interface states are observed at the initial stages of MoO(3) deposition on both Au and Al. The interface states are very close to the Fermi level, assisting the charge transport from the metal electrode. This explains that thick MoO(3) layers provide good charge transport when adopted in organic devices.