Sercan Babakiray

Ultrafast carrier dynamics in thin-films of the topological insulator Bi2Se3

Transient reflectivity measurements of thin films, ranging from 6 to 40 nm in thickness, of the topological insulator Bi2Se3 reveal a strong dependence of the carrier relaxation time on the film thickness. For thicker films, the relaxation dynamics are similar to those of bulk Bi2Se3, where the contribution of the bulk insulating phase dominates over that of the surface metallic phase. The carrier relaxation time shortens with decreasing film thickness, reaching values comparable to those of noble metals. This effect may result from the hybridization of Dirac cone states at the opposite surfaces for the thinnest films.

Thickness tunable quantum interference between surface phonon and Dirac plasmon states in thin films of the topological insulator Bi2Se3

We report on a >100-fold enhancement of Raman responses from Bi2Se3 thin films if laser photon energy switches from 2.33 eV (532 nm) to 1.58 eV (785 nm), which is due to direct optical coupling to Dirac surface states (SS) at the resonance energy of ∼1.5 eV (a thickness-independent enhancement) and due to nonlinearly excited Dirac plasmon (a thickness-dependent enhancement). Owing to the direct optical coupling, we observed an in-plane phonon mode of hexagonally arranged Se-atoms associated with a continuous network of Dirac SS. This mode revealed a Fano lineshape for films <15 nm thick, resulting from quantum interference between surface phonon and Dirac plasmon states.

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 revealed 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 insulatorBi2Se3

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.

Coherent control of injection currents in high-quality films of Bi2Se3

Films of the topological insulator Bi2Se3 are grown by molecular beam epitaxy with in-situ reflection high-energy electron diffraction. The films are shown to be high-quality by X-ray reflectivity and diffraction and atomic-force microscopy. Quantum interference control of photocurrents is observed by excitation with harmonically related pulses and detected by terahertz radiation. The injection current obeys the expected excitation irradiance dependence, showing linear dependence on the fundamental pulse irradiance and square-root irradiance dependence of the frequency-doubled optical pulses. The injection current also follows a sinusoidal relative-phase dependence between the two excitation pulses. These results confirm the third-order nonlinear optical origins of the coherently controlled injection current. Experiments are compared to a tight-binding band structure to illustrate the possible optical transitions that occur in creating the injection current.

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.

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

Transient reflectivity traces measured for nanometer-sized films (6–40 nm) of the topological insulator Bi2Se3 revealed GHz-range oscillations driven within the relaxation of hot carriers photoexcited with ultrashort (∼100 fs) 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 agr...

Identification of photocurrents in topological insulators

Optical injection and detection of charge currents can complement conventional transport and photoemission measurements without the necessity of invasive contact that may disturb the system being examined. This is a particular concern for the surface states of a topological insulator. In this work oneand two-color sources of photocurrents are examined in epitaxial, thin films of Bi2Se3. We demonstrate that optical excitation and terahertz detection simultaneously captures oneand twocolor photocurrent contributions, as previously not required in other material systems. A method is devised to isolate the two components, and in doing so each can be related to surface or bulk excitations through symmetry. This strategy allows surface states to be examined in a model system, where they have independently been verified with angle-resolved photoemission spectroscopy.Optical injection and detection of charge currents is an alternative to conventional transport and photoemission measurements, avoiding the necessity of invasive contact that may disturb the system being examined. This is a particular concern for analyzing the surface states of topological insulators. In this work one- and two-color sources of photocurrents are isolated and examined in epitaxial thin films of Bi2Se3. We demonstrate that optical excitation and terahertz detection simultaneously captures one- and two-color photocurrent contributions, which has not been required for other material systems. A method is devised to extract the two components, and in doing so each can be related to surface or bulk excitations through symmetry. The separation of such photocurrents in topological insulators opens a new avenue for studying these materials by all-optical methods.

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-x Mn x Se3 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 Mn(2+) 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.

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 second-harmonic 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 states.