Florian Hudert

Ultrafast time-domain spectroscopy based on high-speed asynchronous optical sampling

High-speed asynchronous optical sampling (ASOPS) is a novel technique for ultrafast time-domain spectroscopy (TDS). It employs two mode-locked femtosecond oscillators operating at a fixed repetition frequency difference as sources of pump and probe pulses. We present a system where the 1 GHz pulse repetition frequencies of two Ti:sapphire oscillators are linked at an offset of Deltaf(R)=10 kHz. As a result, their relative time delay is repetitively ramped from zero to 1 ns within a scan time of 100 micros. Mechanical delay scanners common to conventional TDS systems are eliminated, thus systematic errors due to beam pointing instabilities and spot size variations are avoided when long time delays are scanned. Owing to the multikilohertz scan-rate, high-speed ASOPS permits data acquisition speeds impossible with conventional schemes. Within only 1 s of data acquisition time, a signal resolution of 6 x 10(-7) is achieved for optical pump-probe spectroscopy over a time-delay window of 1 ns. When applied to terahertz TDS, the same acquisition time yields high-resolution terahertz spectra with 37 dB signal-to-noise ratio under nitrogen purging of the spectrometer. Spectra with 57 dB are obtained within 2 min. A new approach to perform the offset lock between the two femtosecond oscillators in a master-slave configuration using a frequency shifter at the third harmonic of the pulse repetition frequency is employed. This approach permits an unprecedented time-delay resolution of better than 160 fs. High-speed ASOPS provides the functionality of an all-optical oscilloscope with a bandwidth in excess of 3000 GHz and with 1 GHz frequency resolution.

Femtosecond time-resolved optical pump-probe spectroscopy at kilohertz-scan-rates over nanosecond-time-delays without mechanical delay line

We demonstrate a technique for femtosecond time-resolved optical pump-probe spectroscopy that allows to scan over a nanosecond time delay at a kilohertz scan rate without mechanical delay line. Two mode-locked femtosecond lasers with approximately 1 GHz repetition rate are linked at a fixed difference frequency of ΔfR=11kHz. One laser delivers the pump pulses, the other provides the probe pulses. The relative time delay is linearly ramped between zero and the inverse laser repetition frequency at a rate ΔfR, enabling high-speed scanning over a 1 ns time delay. The advantages of this method for all-optical pump-probe experiments become evident in an observation of coherent acoustic phonons in a semiconductor superlattice via transient reflectivity changes. A detection shot-noise limited signal resolution of 7×10−8 is obtained with a total measurement time of 250 s. The time resolution is 230 fs.

Subharmonic Resonant Optical Excitation of Confined Acoustic Modes in a Free-Standing Semiconductor Membrane at GHz Frequencies with a High-Repetition-Rate Femtosecond Laser

We propose subharmonic resonant optical excitation with femtosecond lasers as a new method for the characterization of phononic and nanomechanical systems in the gigahertz to terahertz frequency range. This method is applied for the investigation of confined acoustic modes in a free-standing semiconductor membrane. By tuning the repetition rate of a femtosecond laser through a subharmonic of a mechanical resonance we amplify the mechanical amplitude, directly measure the linewidth with megahertz resolution, infer the lifetime of the coherently excited vibrational states, accurately determine the systems quality factor, and determine the amplitude of the mechanical motion with femtometer resolution.

Coherent acoustic oscillations of nanoscale Au triangles and pyramids: influence of size and substrate

We investigate the impulsively excited acoustic dynamics of nanoscale Au triangles of different sizes and thicknesses on silicon and glass substrates. We employ high-speed asynchronous optical sampling in order to study the damping of the acoustic vibrations with high sensitivity in the time domain. From the observed damping dynamics we deduce the reflection coefficient of acoustic energy from the gold?substrate interface. The observed damping times of coherent acoustic vibrations are found to be significantly longer than expected from the acoustic impedance mismatch for an ideal gold?substrate interface, hence pointing towards a reduced coupling strength. The strength of the coupling can be determined quantitatively. For Au triangles with large lateral size-to-thickness ratio, i.e. a small aspect ratio, the acoustic dynamics is dominated by a thickness oscillation similar to that of a closed film. For triangles with large aspect ratio the coherent acoustic excitation consists of a superposition of different three-dimensional modes which exhibit different damping times.

Influence of doping profiles on coherent acoustic phonon detection and generation in semiconductors

The doping profile in different n-doped GaAs homoepitaxial structures grown by molecular beam epitaxy is investigated in the time domain by employing a laser based picosecond ultrasound technique in a contactless and noninvasive way. Experiments based on asynchronous optical sampling employ two femtosecond lasers, which allow us to detect changes in the optical reflectivity over a 1 ns time delay with a signal-to-noise ratio of 107 and 100 fs time resolution in <1 min of acquisition time. We show that the doping profile with doping densities of the order of 1018 cm−3 can be detected with picosecond ultrasound, although there is no difference in the acoustic properties of the doped and undoped region. The detection mechanism is based on a different sensitivity function for a coherent strain pulse in the doped and undoped regions. These results are corroborated by experiments at room temperature and 10 K.

Coherent acoustic phonons in phonon cavities investigated by asynchronous optical sampling

Using a recently introduced measurement technique, called asynchronous optical sampling (ASOPS), we have investigated the dynamics of coherent acoustic phonons in a semiconductor heterostructure composed of a GaAs film between two GaAs/AlAs superlattices, serving as a cavity for acoustic phonons. Measurements were performed at liquid helium temperatures. The possibility to perform two-color pump-probe spectroscopy allowed us to tune the probe pulse energy to the cavity band gap, while sweeping the pump pulse energy over the superlattice resonance. The large measurement window of 1 ns in combination with a resolution of about 150 fs made a detailed analysis of the observed phonon dynamics possible. We observed a long lived oscillation in the gap of the phonon dispersion at 466 GHz, which we attribute to a cavity mode.

High-speed asynchronous optical sampling for high-sensitivity detection of coherent phonons

A new optical pump-probe technique is implemented for the investigation of coherent acoustic phonon dynamics in the GHz to THz frequency range which is based on two asynchronously linked femtosecond lasers. Asynchronous optical sampling (ASOPS) provides the performance of on all-optical oscilloscope and allows us to record optically induced lattice dynamics over nanosecond times with femtosecond resolution at scan rates of 10 kHz without any moving part in the set-up. Within 1 minute of data acquisition time signal-to-noise ratios better than 107 are achieved. We present examples of the high-sensitivity detection of coherent phonons in superlattices and of the coherent acoustic vibration of metallic nanoparticles.

Femtosecond time-resolved investigation of coherent acoustic modes of free-standing Si membranes

We present a time-resolved investigation of the acoustic vibrarional dynamics in thin freestanding Silicon membranes. The confinement of the longitudinal acoustic modes caused by the small thickness of the membranes leads to a discretization of the vibrational acoustic spectrum [1]. Within the time domain, this behaviour is evidenced by the superposition of oscillations of a fundamental mode and the different higher odd harmonics. In this work we report the first time-resolved experimental observation of these oscillations. The femtosecond time resolved pump-probe experiments are performed using the newly developed high-speed asynchronous optical sampling (ASOPS) method [2]. This method is based on two asynchronously linked femtosecond unidirectional ring lasers of ∼1GHz repetition rate. The time delay between the pump and the probe beams is realized through an off-set in the repetition rates of the two lasers, which lies in the kHz frequency range. The absence of mechanical moving parts in the set-up allows a very fast scanning time and a high signal-to-noise ratio, impossible to archive with the usual pump-probe set-ups [3].

Femtosecond pump-probe spectroscopy without mechanical delay line

Femtosecond optical pump-probe spectroscopy is performed over 1 ns time-delay at 11 kHz scan-rate without mechanical delay-line and with 230 fs resolution. Coherent phonons in a semiconductor sample are detected at the shot-noise limit with 1 GHz spectral resolution.