Growth and Properties of Topological Insulator Thin Films Based on the Bi2Se3 Compound

This dissertation summarizes the growth, structural and electrical transport properties of topological insulators based on Bi2Se3 compound grown by molecular beam epitaxy. In the first three chapters, I review the theoretical background and experimental procedures necessary to understand the properties of topological insulators. The next three chapters cover the results of the structural characterization and electrical transport measurements. The final chapter summarizes the overall results and suggests future directions for research on Bi2Se3 compounds. Topological insulators (TIs) are a new class of quantum matter with a bulk band gap and gapless metallic surface states. The spin and momentum degrees of freedom are locked and are robust against non-magnetic perturbations. Here, I study the growth, structural and electronic properties of Bi2Se3 and Mn doped Bi 2Se3 thin films. Bi2Se3/Bi2-x MnxSe3 thin films were grown on single crystal Al2O3 (0001) substrate by molecular beam epitaxy (MBE). Epitaxy was confirmed by reflection high energy electron diffraction (RHEED). Crystal orientation and lattice parameters were extracted from x-ray diffraction (XRD) measurements. The thin film thickness and roughness values were determined by fitting the x-ray reflectivity data (XRR) to a model based on optical scattering theory. To determine the Mn impurity site in Bi2-xMnxSe 3, extended x-ray absorption fine structure (EXAFS) measurements were performed at the Mn k-edge Finally, resistivity and Hall effect measurements were performed as functions of magnetic field and temperature. I focus on the weak antilocalization (WAL) and 2D magnetoconductance in the electrical transport measurements

Plasmon-enhanced electron-phonon coupling in Dirac surface states of the thin-film topological insulator Bi2Se3

Raman measurements of a Fano-type surface phonon mode associated with Dirac surface states (SS) in Bi2Se3 topological insulator thin films allowed an unambiguous determination of the electron-phonon coupling strength in Dirac SS as a function of film thickness ranging from 2 to 40 nm. A non-monotonic enhancement of the electron-phonon coupling strength with maximum for the 8 - 10 nm thick films was observed. The non-monotonicity is suggested to originate from plasmon-phonon coupling which enhances electron-phonon coupling when free carrier density in Dirac SS increases with decreasing film thickness and becomes suppressed for thinnest films when anharmonic coupling between in-plane and out-of-plane phonon modes occurs. The observed about four-fold enhancement of electron-phonon coupling in Dirac SS of the 8 - 10 nm thick Bi2Se3 films with respect to the bulk samples may provide new insights into the origin of superconductivity in this-type materials and their applications

Effect of Mn doping on ultrafast carrier dynamics in thin films of the topological insulator Bi2Se3

Transient reflectivity (TR) measured at laser photon energy 1.51 eV from the indirectly intersurface coupled topological insulator Bi2-xMnxSe3 films (12 nm thick) revealed a strong dependence of the rise-time and initial decay-time constants on photoexcited carrier density and Mn content. In undoped samples (x = 0), these time constants are exclusively governed by electron-electron and electron-phonon scattering, respectively, whereas in films with x = 0.013 - 0.27 ultrafast carrier dynamics are completely controlled by photoexcited electron trapping by ionized Mn2+ acceptors and their dimers. The shortest decay-time (~0.75 ps) measured for the film with x = 0.27 suggests a great potential of Mn-doped Bi2Se3 films for applications in high-speed optoelectronic devices. Using Raman spectroscopy exploiting similar laser photon energy (1.58 eV), we demonstrate that due to indirect intersurface coupling in the films, the photoexcited electron trapping in the bulk enhances the electron-phonon interaction strength in Dirac surface states

Acoustic phonon dynamics in thin-films of the topological insulator Bi2Se3

Transient reflectivity traces measured for nanometer-sized films of the topological insulator Bi2Se3 revealed GHz-range oscillations driven within the relaxation of hot carriers photoexcited with ultrashort laser pulses of 1.51 eV photon energy. These oscillations have been suggested to result from acoustic phonon dynamics, including coherent longitudinal acoustic phonons in the form of standing acoustic waves. An increase of oscillation frequency from ~35 to ~70 GHz with decreasing film thickness from 40 to 15 nm was attributed to the interplay between two different regimes employing traveling-acoustic-waves for films thicker than 40 nm and the film bulk acoustic wave resonator (FBAWR) modes for films thinner than 40 nm. The amplitude of oscillations decays rapidly for films below 15 nm thick when the indirect intersurface coupling in Bi2Se3 films switches the FBAWR regime to that of the Lamb wave excitation. The frequency range of coherent longitudinal acoustic phonons is in good agreement with elastic properties of Bi2Se3

Effect of carrier recombination on ultrafast carrier dynamics in thin films of the topological insulator Bi2Se3

Transient reflectivity (TR) from thin films (6 - 40 nm thick) of the topological insulator Bi2Se3 reveal ultrafast carrier dynamics, which suggest the existence of both radiative and non-radiative recombination between electrons residing in the upper cone of initially unoccupied high energy Dirac surface states (SS) and holes residing in the lower cone of occupied low energy Dirac SS. The modeling of measured TR traces allowed us to conclude that recombination is induced by the depletion of bulk electrons in films below ~20 nm thick due to the charge captured on the surface defects. We predict that such recombination processes can be observed using time-resolved photoluminescence techniques

Resonance-type thickness dependence of optical second harmonic generation in thin-films of the topological insulator Bi2Se3

Optical second harmonic generation (SHG) has been measured for the first time in reflection from the nanometer-thick films (6 to 40 nm) of the topological insulator Bi2Se3 using 1.51 eV (820 nm) Ti:Sapphire laser photons and revealed a strong dependence of the integral SHG intensity on the film thickness. The integral SHG intensity was determined by area integration of the SHG rotational anisotropy patterns measured for different input-output light polarization geometries. A ~100-fold enhancement of the integral SHG intensity with decreasing film thickness has been suggested to result from the DC-electric-field-induced SHG (EFISHG) effects. Two sources of dynamically created DC electric field were proposed: (i) the capacitor-type DC electric field that gradually increases with decreasing film thickness from 40 to 6 nm due to a dynamical imbalance of photoexcited long-lived carriers between the opposite-surface Dirac surface states and (ii) an DC electric field associated with a nonlinearly excited Dirac plasmon, which is responsible for the resonant enhancement of the integral SHG intensity for the 10 nm thick film with a Lorentz-shaped resonance of ~1.6 nm full width at half maximum. Additionally to the general SHG enhancement trends with decreasing film thickness, a relative decrease of the out-of-plane contribution with respect to the in-plane contribution was observed. Using a theoretical treatment of the measured SHG rotational anisotropy patterns, this effect has been suggested to result from the joint contributions of the linear and quadratic DC electric field effects to the EFISHG response

Nonlinear Optical Observation of Coherent Acoustic Dirac Plasmons in Thin-Film Topological Insulators

Low-energy collective electronic excitations exhibiting sound-like linear dispersion have been intensively studied both experimentally and theoretically for a long time. However, coherent acoustic plasmon modes appearing in time-domain measurements are rarely observed due to Landau damping by the single-particle continua. Here we report on the observation of coherent acoustic Dirac plasmon (CADP) modes excited in indirectly (electrostatically) opposite-surface coupled films of the topological insulator Bi2Se3. Using transient secondharmonic generation, a technique capable of independently monitoring the in-plane and out-of-plane electron dynamics in the films, the GHz-range oscillations were observed without corresponding oscillations in the transient reflectivity. These oscillations were assigned to the transverse magnetic and transverse electric guided CADP modes induced by the evanescent guided Lamb acoustic waves and remained Landau undamped due to fermion tunnelling between the opposite-surface Dirac state