Coherent Longitudinal Optical Phonons Research Articles

Coherent-Phonon-Driven Hot-Carrier Effect in a Superlattice Solar Cell

Carrier thermalization in a superlattice solar cell made of polar semiconductors is studied theoretically by considering a minimal model where electron-phonon scattering is the principal channel of carrier energy loss. Importantly, the effect of an intrinsic quantum mechanical property; the phonon coherence, on carrier thermalization is investigated, within semiclassical picture in terms of phonon wave packet. It turns out that coherent longitudinal optical (LO) phonons weaken the effective electron-phonon coupling, thus supposedly lowering the carrier energy loss rate in solar cell. The resulting thermalization power is indeed significantly reduced by the coherent phonons, resulting in enhanced hot carrier effect, particularly for thin enough well layer where carrier confinement is also strong. A recent experiment on superlattice solar cell prototype is shown to manifest the coherent phonons-driven phenomenon. Our results demonstrate the practical implications of the fundamental quantum coherence property of phonons in semiconductors for improving superlattice solar cell performance, via hot carrier effect.

Decay time extension of terahertz electromagnetic waves emitted from coherent longitudinal optical phonons in GaAs epitaxial layers with the use of fast atom bombardment

We succeeded in extending the decay time of terahertz electromagnetic waves from coherent longitudinal optical (LO) phonons in GaAs epitaxial layers with the use of fast atom bombardment, a treatment method for introducing defects and/or disorders at the surface. The decay time becomes long, up to 4.81 ± 0.15 ps, with the bombardment time of 4.0 min. This value is 2.4-times larger than the decay time of 2.04 ± 0.04 ps of the reference sample (untreated sample). We attribute the origin of the present phenomenon to the fact that the reduction of the photogenerated carrier scattering effect on the coherent LO phonon, which is caused by the presence of the surface defects and disorders formed by the fast atom bombardment, results in the extending of the decay time of the terahertz wave from the coherent LO phonon.

Coherent surface-to-bulk vibrational coupling in the 2D topologically trivial insulator Bi2Se3 monitored by ultrafast transient absorption spectroscopy

Ultrafast carrier relaxation in the 2D topological insulator (TI) Bi2Se3 [gapped Dirac surface states (SS)] and how it inherits ultrafast relaxation in the 3D TI Bi2Se3 (gapless Dirac SS) remains a challenge for developing new optoelectronic devices based on these materials. Here ultrashort (~ 100 fs) pumping pulses of ~ 340 nm wavelength (~ 3.65 eV photon energy) were applied to study ultrafast electron relaxation in the 2D TI Bi2Se3 films with a thickness of 2 and 5 quintuple layers (~ 2 and ~ 5 nm, respectively) using transient absorption (TA) spectroscopy in the ultraviolet–visible spectral region (1.65–3.9 eV). The negative and positive contributions of TA spectra were attributed to absorption bleaching that mostly occurs in the bulk states and to the inverse bremsstrahlung type free carrier absorption in the gapped Dirac SS, respectively. Owing to this direct and selective access to the bulk and surface carrier dynamics, we were able to monitor coherent longitudinal optical (LO) phonon oscillations, which were successively launched in the bulk and surface states by the front of the relaxing electron population within the LO-phonon cascade emission. We have also recognized the coherent surface-to-bulk vibrational coupling that appears through the phase-dependent amplitude variations of coherent LO-phonon oscillations. This unique behavior manifests itself predominantly for the topologically trivial insulator phase of the 2D TI Bi2Se3 (2 nm thick film) in the photon energy range (~ 2.0–2.25 eV) where efficient energy exchange between the bulk and surface states occurs. We also found that the coherent surface-to-bulk vibrational coupling significantly weakens with increasing both the Bi2Se3 film thickness and pumping power.

Separation of interface and substrate carrier dynamics at a heterointerface based on coherent phonons

Transient reflectivity spectroscopy is widely used to study ultrafast carrier- and phonon-dynamics in semiconductors. In their heterostructures, it is often not straightforward to distinguish contributions to the signal from the various layers. In this work, we perform transient reflectivity measurements on lattice-matched GaP/Si(001) using a near infrared pulse, to which GaP is transparent. The pump laser pulse can generate coherent longitudinal optical (LO) phonons both in the GaP overlayer as well as in the Si substrate which have distinct frequencies. This enables us to track the amplitude of the respective signal contributions as a function of GaP layer thickness $d$. The Si phonon amplitude in the signal exhibits an oscillatory behavior with increasing $d$. This can be quantitatively explained by the interference of the probe light reflected at the air/GaP/Si heterointerface. Based on this knowledge, we can then separate the interface- and the substrate-contributions in the carrier-induced non-oscillatory transient reflectivity signal. The obtained interface signal provides evidence for ultrafast carrier injection from the Si substrate into the GaP overlayer. This is also corroborated by examining the deviation of the polarization-dependence of the GaP coherent optical phonon signal from that of the bulk semiconductor.

Complex energies of the coherent longitudinal optical phonon–plasmon coupled mode according to dynamic mode decomposition analysis

In a dissipative quantum system, we report the dynamic mode decomposition (DMD) analysis of damped oscillation signals. We used a reflection-type pump-probe method to observe time-domain signals, including the coupled modes of long-lived longitudinal optical phonons and quickly damped plasmons (LOPC) at various pump powers. The Fourier transformed spectra of the observed damped oscillation signals show broad and asymmetric modes, making it difficult to evaluate their frequencies and damping rates. We then used DMD to analyze the damped oscillation signals by precisely determining their frequencies and damping rates. We successfully identified the LOPC modes. The obtained frequencies and damping rates were shown to depend on the pump power, which implies photoexcited carrier density. We compared the pump-power dependence of the frequencies and damping rates of the LOPC modes with the carrier density dependence of the complex eigen-energies of the coupled modes by using the non-Hermitian phenomenological effective Hamiltonian. Good agreement was obtained between the observed and calculated dependences, demonstrating that DMD is an effective alternative to Fourier analysis which often fails to estimate effective damping rates.

Coherent control of optical phonons in GaAs by relative-phase-locked optical pulses under perpendicularly polarized conditions

Coherent control of the optical phonons in GaAs is realized via paired femtosecond pulses that are relative phase-locked and have perpendicular polarizations. To investigate polarization effects, only phonon interference occurs, which contrasts previous experiments with parallel-polarized pulses, which produced as well electronic interference. The results suggest that for an n-GaAs(001) sample the diagonal components of the Raman tensor determinate in the generation of coherent longitudinal optical phonons.

The effect of ion irradiation on dephasing of coherent optical phonons in GaP

The dephasing of coherent longitudinal optical (LO) phonons in ion-irradiated GaP has been investigated with a femtosecond pump-probe technique based on electro-optic sampling. The dephasing time of the coherent LO phonon is found to be dramatically prolonged by the introduction of a small amount of defects by means of Ga-ion irradiation. The maximum dephasing time observed at room temperature is 9.1 ps at a Ga+ ion dose of 1013/cm2, which is significantly longer than the value of 8.3 ps for GaP before ion irradiation. The longer dephasing time is explained in terms of the suppression of electron-LO-phonon scattering by the presence of defect-induced deep levels.

Atomic fluctuations in electronic materials revealed by dephasing

The microscopic origin and timescale of the fluctuations of the energies of electronic states has a significant impact on the properties of interest of electronic materials, with implication in fields ranging from photovoltaic devices to quantum information processing. Spectroscopic investigations of coherent dynamics provide a direct measurement of electronic fluctuations. Modern multidimensional spectroscopy techniques allow the mapping of coherent processes along multiple time or frequency axes and thus allow unprecedented discrimination between different sources of electronic dephasing. Exploiting modern abilities in coherence mapping in both amplitude and phase, we unravel dissipative processes of electronic coherences in the model system of CdSe quantum dots (QDs). The method allows the assignment of the nature of the observed coherence as vibrational or electronic. The expected coherence maps are obtained for the coherent longitudinal optical (LO) phonon, which serves as an internal standard and confirms the sensitivity of the technique. Fast dephasing is observed between the first two exciton states, despite their shared electron state and common environment. This result is contrary to predictions of the standard effective mass model for these materials, in which the exciton levels are strongly correlated through a common size dependence. In contrast, the experiment is in agreement with ab initio molecular dynamics of a single QD. Electronic dephasing in these materials is thus dominated by the realistic electronic structure arising from fluctuations at the atomic level rather than static size distribution. The analysis of electronic dephasing thereby uniquely enables the study of electronic fluctuations in complex materials.

Terahertz electromagnetic waves radiated from coherent longitudinal optical (LO) phonons and LO-phonon plasmon coupled modes in (001)-, (110)-, and (111)-oriented semi-insulating GaAs single crystals

We report on terahertz electromagnetic waves from coherent longitudinal optical (LO) phonons and coherent LO-phonon plasmon coupled (LOPC) modes in (001)-, (110)-, and (111)-oriented semi-insulating GaAs single crystals. The coherent LO phonons and coherent LOPC modes are observed in the three samples. In contrast, coherent transverse optical (TO) phonons are not observed in the (110)- and (111)-oriented samples in spite of that the TO phonon is the Raman active mode. We conclude that only the coherent longitudinal oscillating polarization such as coherent LO phonons and coherent LOPC modes radiate the terahertz wave and that the Raman selection rule does not contribute to the terahertz-wave-radiation process. The photogenerated electron-density dependence of the frequencies of the coherent LOPC mode is almost the same in the three samples. This finding indicates that the coupling of the LO phonon with the plasmon is not influenced by the surface orientations of the three samples.

Terahertz Driven Amplification of Coherent Optical Phonons in GaAs Coupled to a Metasurface.

We demonstrate amplification of longitudinal optical (LO) phonons by polar-optical interaction with an electron plasma in a GaAs structure coupled to a metallic metasurface using two-color two-dimensional spectroscopy. In a novel scheme, the metamaterial resonator enhances broadband terahertz fields, which generate coherent LO phonons and drive free electrons in the conduction band of GaAs. The time evolution of the LO phonon amplitude is monitored with midinfrared pulses via the LO-phonon-induced Kerr nonlinearity of the sample, showing an amplification of the LO phonon amplitude by up to a factor of 10, in agreement with a theoretical estimate.

Coherent optical and acoustic phonons generated at lattice-matched GaP/Si(0 0 1) heterointerfaces

Thin GaP films can be grown on an exact Si(0 0 1) substrate with nearly perfect lattice match. We perform all-optical pump–probe measurements to investigate the ultrafast electron–phonon coupling at the buried interface of GaP/Si. Above-bandgap excitation with a femtosecond laser pulse can induce coherent longitudinal optical (LO) phonons both in the GaP overlayer and in the Si substrate. The coupling of the GaP LO phonons with photoexcited plasma is reduced significantly with decreasing GaP layer thickness from 56 to 16 nm due to the quasi-two-dimensional confinement of the plasma. The same laser pulse can also generate coherent longitudinal acoustic phonons in the form of a strain pulse. The strain pulse induces not only a periodic modulation in the optical reflectivity as it propagates in the semiconductor, but also a sharp spike when it arrives at the GaP layer boundary. The acoustic pulse induced at the GaP/Si interface is remarkably stronger than that at the Si surface, suggesting a possible application of the GaP/Si heterostructure as an opto-acoustic transducer. The amplitude and the phase of the reflectivity modulation varies with the GaP layer thickness, which can be understood in terms of the interference caused by the multiple acoustic pulses generated at the top surface and at the buried interface.

Temperature effect on the coupling between coherent longitudinal phonons and plasmons in n -type and p -type GaAs

The coupling between longitudinal optical (LO) phonons and plasmons plays a fundamental role in determining the performance of doped semiconductor devices. In this work, we report a comparative investigation into the dependence of the coupling on temperature and doping in $n$- and $p$-type GaAs by using ultrafast coherent phonon spectroscopy. A suppression of coherent oscillations has been observed in $p$-type GaAs at lower temperature, strikingly different from $n$-type GaAs and other materials in which coherent oscillations are strongly enhanced by cooling. We attribute this unexpected observation to a cooling-induced elongation of the depth of the depletion layer which effectively increases the screening time of the surface field due to a slow diffusion of photoexcited carriers in $p$-type GaAs. Such an increase breaks the requirement for the generation of coherent LO phonons and, in turn, LO phonon-plasmon coupled modes because of their delayed formation in time.

Screening effects of photogenerated carriers on terahertz radiation from coherent GaAs-like longitudinal optical phonons in (11n)-oriented GaAs/In0.1Al0.9As strained multiple quantum wells

We investigated terahertz radiation from coherent GaAs-like longitudinal optical (LO) phonons in (11n)-oriented GaAs/In0.1Al0.9As strained multiple quantum wells for clarifying the screening effects of photogenerated carriers. We observed the intense quasi-monochromatic terahertz wave from the coherent GaAs-like LO phonon, which originates from the initial polarization enhanced by the strong piezoelectric field. The intensity of the coherent GaAs-like LO-phonon band exhibited a saturation behavior as the pump power was increased. We evaluated the saturation behavior in terms of excitation efficiency of the terahertz wave from the coherent GaAs-like LO phonon using the parameter of unit-power intensity. From the pump-power dependence of the unit-power intensity, we conclude that the screening effect of high density photogenerated carriers on the piezoelectric field causes saturation of the terahertz-wave intensity from the coherent GaAs-like LO phonon.

Effects of photogenerated carrier scattering on the decay process of coherent longitudinal optical phonons in an undoped GaAs/n-type GaAs epitaxial structure investigated by terahertz time-domain spectroscopy

The authors investigated the scattering effect of photogenerated carriers on the decay of the coherent longitudinal optical (LO) phonons in an undoped GaAs/n-type GaAs epitaxial structure using a terahertz time-domain spectroscopic technique. The terahertz wave from the coherent LO phonon was observed together with those emitted both by the ultrafast photocurrent and by the coherent LO-phonon-plasmon coupled (LOPC) mode. The simultaneous observation of the coherent LO phonon and coherent LOPC mode originates from the fact that the photogenerated carrier density laterally distributes around the surface of the undoped GaAs layer owing the Gaussian profile of the pump beam. The authors found that the terahertz wave from the coherent LO phonon lives up to 5.0 ps, whereas those from the coherent LOPC mode and ultrafast photocurrent disappear within 1.0 ps. The decay time of the coherent LO phonon monotonically decreases with an increase in the pump power. This finding indicates that the dephasing of the terahertz wave from the coherent LO phonon is dominated by the photogenerated carrier scattering in the time range shorter than 1.0 ps in which photogenerated carriers remain.

Dynamical Fano-Like Interference between Rabi Oscillations and Coherent Phonons in a Semiconductor Microcavity System.

We report on dynamical interference between short-lived Rabi oscillations and long-lived coherent phonons in CuCl semiconductor microcavities resulting from the coupling between the two oscillations. The Fourier-transformed spectra of the time-domain signals obtained from semiconductor microcavities by using a pump-probe technique show that the intensity of the coherent longitudinal optical phonon of CuCl is enhanced by increasing that of the Rabi oscillation, which indicates that the coherent phonon is driven by the Rabi oscillation through the Fröhlich interaction. Moreover, as the Rabi oscillation frequency decreases upon crossing the phonon frequency, the spectral profile of the coherent phonon changes from a peak to a dip with an asymmetric structure. The continuous wavelet transformation reveals that these peak and dip structures originate from constructive and destructive interference between Rabi oscillations and coherent phonons, respectively. We demonstrate that the asymmetric spectral structures in relation to the frequency detuning are well reproduced by using a classical coupled oscillator model on the basis of dynamical Fano-like interference.

Voltage-controllable terahertz radiation from coherent longitudinal optical phonons in a p-i-n diode structure of GaAs

We propose and demonstrate the voltage-controllable terahertz radiation from coherent longitudinal optical (LO) phonons in a p-i-n diode of GaAs at room temperature under illumination of a femtosecond pulse laser. It was found that the intensity of the terahertz radiation is continuously and drastically enhanced by an increase in reverse bias voltage (electric field strength) from 0 (22) to 8.0 V (140 kV/cm). The analysis of the electric-field-strength dependence of the intensity indicates that the initial polarization of the LO phonon induced by the electric field dominates the enhancement and that the second-order electric susceptibility is considerable.

Enhancement mechanism of terahertz radiation from coherent longitudinal optical phonons in undoped GaAs/n-type GaAs epitaxial structures

We have investigated the characteristics of monochromatic terahertz electromagnetic waves emitted from coherent longitudinal optical (LO) phonons in undoped GaAs/n-type GaAs epitaxial structures with various thicknesses, which range from 200 nm to 1200 nm, of the undoped GaAs layer. The terahertz waves were measured at room temperature using an optical gating method with a photoconductive dipole antenna. It was found that the intensity of the terahertz waves markedly depends on the thickness of the undoped GaAs layer. The analysis of Franz-Keldysh oscillations observed with photoreflectance spectroscopy demonstrates that the built-in electric field strength in the undoped GaAs layer, which results from the Fermi-level pinning at the surface, increases from 6.1 kV/cm to 28.4 kV/cm with a decrease in the thickness. It was revealed that the amplitude of the terahertz wave is proportional to the electric field strength in the undoped GaAs layer. This fact indicates that the efficiency of the terahertz radiation is dominated by the initial polarization of the LO phonons induced by the built-in electric field, which provides us a simple strategy for the enhancement of the terahertz radiation from the coherent LO phonons.

Terahertz radiation from the coherent longitudinal optical phonon-plasmon coupled mode in an i-GaAs/n-GaAs epitaxial structure

We have investigated the time-domain terahertz radiation from an undoped GaAs/n-type GaAs (i-GaAs/n-GaAs) epitaxial structure using an optical gating method with a femtosecond pulse laser. We have found from the Fourier power spectra of the terahertz waveforms that two terahertz bands, the frequencies of which obviously depend on the pump power, appear in a high density excitation regime in addition to a broad band due to a surge current and a sharp band due to the coherent longitudinal optical (LO) phonon. Based on a model for the LO phonon-plasmon coupled (LOPC) mode, we reasonably explain the pump-power (photogenerated-carrier-density) dependence of the frequencies of the two bands peculiar to the high density excitation. This fact demonstrates that the two terahertz bands are assigned to the lower and upper branches of the LOPC mode. The frequencies of the LOPC mode are determined only by the pump power. Thus, the LOPC mode originates from the i-GaAs layer; namely, the plasmon component of the surge current flowing through the i-GaAs layer couples with the coherent LO phonon.

Delayed formation of coherent LO phonon-plasmon coupled modes inn- andp-type GaAs measured using a femtosecond coherent control technique

Coherent control experiments using a pair of collinear femtosecond laser pulses have been carried out to manipulate longitudinal optical (LO) phonon-plasmon coupled (LOPC) modes in both $p$- and $n$-type GaAs. By tuning the interpulse separation, remarkably distinct responses have been observed in the two samples. To understand the results obtained a phenomenological model taking the delayed formation of coherent LOPC modes into account is proposed. The model suggests that the lifetime of coherent LOPC modes plays a key role and the interference of the coherent LO phonons excited successively by two pump pulses strongly affects the manipulation of coherent LOPC modes.

Photogenerated‐carrier‐induced band bending effects on generation of a coherent longitudinal optical phonon in a GaAs buffer layer optically masked by a GaSb top epitaxial layer

AbstractWe demonstrate that, in a GaSb/GaAs epitaxial structure, the coherent longitudinal optical (LO) phonon in a GaAs buffer layer optically masked by a GaSb top layer is observed utilizing terahertz spectroscopy. It is confirmed from Raman scattering measurements that only the optical phonons in the GaSb layer is observable. In the terahertz‐wave measurement, the Fourier power spectrum of a terahertz waveform exhibits both the coherent GaAs and GaSb LO phonon bands; namely, the coherent LO phonon in the optically masked GaAs buffer layer is observed. This fact demonstrates that the instantaneous surface potential modulation, which originates from the impulsive carrier excitation by a pump beam, reaches the GaAs buffer layer. We perform a time‐partitioning Fourier transform analysis in order to investigate the decay dynamics of the coherent GaAs and GaSb LO phonons. (© 2012 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)