Kevin L. Silverman

Multidimensional coherent photocurrent spectroscopy of a semiconductor nanostructure

Multidimensional Coherent Optical Photocurrent Spectroscopy (MD-COPS) is implemented using unstabilized interferometers. Photocurrent from a semiconductor sample is generated using a sequence of four excitation pulses in a collinear geometry. Each pulse is frequency shifted by a unique radio frequency through acousto-optical modulation; the Four-Wave Mixing (FWM) signal is then selected in the frequency domain. The interference of an auxiliary continuous wave laser, which is sent through the same interferometers as the excitation pulses, is used to synthesize reference frequencies for lock-in detection of the photocurrent FWM signal. This scheme enables the partial compensation of mechanical fluctuations in the setup, achieving sufficient phase stability without the need for active stabilization. The method intrinsically provides both the real and imaginary parts of the FWM signal as a function of inter-pulse delays. This signal is subsequently Fourier transformed to create a multi-dimensional spectrum. Measurements made on the excitonic resonance in a double InGaAs quantum well embedded in a p-i-n diode demonstrate the technique.

Dark pulse quantum dot diode laser

We describe an operating regime for passively mode-locked quantum dot diode laser where the output consists of a train of dark pulses, i.e., intensity dips on a continuous background. We show that a dark pulse train is a solution to the master equation for mode-locked lasers. Using simulations, we study stability of the dark pulses and show they are consistent with the experimental results.

Direct measurement of polarization resolved transition dipole moment in InGaAs/GaAs quantum dots

The propagation of optical pulses resonant with the ground-to-excited state transition of InGaAs quantum dots is investigated. An analysis of low intensity excitation yields a dipole moment of 8.8×10−29 to 10.9×10−29 C m, depending on the quantum dot growth conditions. We observe polarization of the dipole moment exclusively in the plane perpendicular to the growth direction.

Laser plasma x-ray source for ultrafast time-resolved x-ray absorption spectroscopy.

We describe a laser-driven x-ray plasma source designed for ultrafast x-ray absorption spectroscopy. The source is comprised of a 1 kHz, 20 W, femtosecond pulsed infrared laser and a water target. We present the x-ray spectra as a function of laser energy and pulse duration. Additionally, we investigate the plasma temperature and photon flux as we vary the laser energy. We obtain a 75 μm FWHM x-ray spot size, containing ∼106 photons/s, by focusing the produced x-rays with a polycapillary optic. Since the acquisition of x-ray absorption spectra requires the averaging of measurements from >107 laser pulses, we also present data on the source stability, including single pulse measurements of the x-ray yield and the x-ray spectral shape. In single pulse measurements, the x-ray flux has a measured standard deviation of 8%, where the laser pointing is the main cause of variability. Further, we show that the variability in x-ray spectral shape from single pulses is low, thus justifying the combining of x-rays obtained from different laser pulses into a single spectrum. Finally, we show a static x-ray absorption spectrum of a ferrioxalate solution as detected by a microcalorimeter array. Altogether, our results demonstrate that this water-jet based plasma source is a suitable candidate for laboratory-based time-resolved x-ray absorption spectroscopy experiments.

Wavelength Bistability and Switching in Two-Section Quantum-Dot Diode Lasers

We report lasing wavelength bistability with respect to applied bias on the saturable absorbers in two-section mode-locked quantum dot lasers. We show data from three different devices exhibiting wavelength bistability. All lasers display wavelength bistability. Only one lasing wavelength is present at a time, with all other wavelengths totally quenched. The switchable ranges (the wavelength difference between two bistable lasing branches) are different for all three lasers and in one device can be manipulated by changing the current injection. All lasers show the remarkable property of switching only in integer multiples of about 8 nm. The bistable operation can be explained by the interplay of the cross-saturation and self-saturation properties in gain and absorber, and the quantum-confined Stark effect in absorber. The measured switching time between bistable wavelengths is 150 ps.

High-resolution spectral hole burning in InGaAs-GaAs quantum dots

We report the use of continuous wave spectral hole burning to perform high-resolution spectroscopy of the homogeneous linewidth of self-assembled InGaAs-GaAs quantum dots at low temperature. We use this technique to examine the power broadening behavior of the homogeneous InGaAs-GaAs quantum dot line. We find that at a temperature of 9.8 K and over the majority of the pump powers considered, the spectral hole signal is well fit by a single Lorentizian line shape. Analysis of the power broadening yields a full width at half maximum of 0.74μeV for the homogeneous linewidth and a corresponding coherence time T2 of 1.76 ns.

Ultrafast time-resolved X-ray absorption spectroscopy of ferrioxalate photolysis with a laser plasma X-ray source and microcalorimeter array

The detailed pathways of photoactivity on ultrafast time scales are a topic of contemporary interest. Using a tabletop apparatus based on a laser plasma X-ray source and an array of cryogenic microcalorimeter X-ray detectors, we measured a transient X-ray absorption spectrum during the ferrioxalate photoreduction reaction. With these high-efficiency detectors, we observe the Fe K edge move to lower energies and the amplitude of the extended X-ray absorption fine structure reduce, consistent with a photoreduction mechanism in which electron transfer precedes disassociation. These results are compared to previously published transient X-ray absorption measurements on the same reaction and found to be consistent with the results from Ogi et al. and inconsistent with the results of Chen et al. ( Ogi , Y. ; et al. Struct. Dyn. 2015 , 2 , 034901 ; Chen , J. ; Zhang , H. ; Tomov , I. V. ; Ding , X. ; Rentzepis , P. M. Chem. Phys. Lett. 2007 , 437 , 50 - 55 ). We provide quantitative limits on the Fe-O bond length change. Finally, we review potential improvements to our measurement technique, highlighting the future potential of tabletop X-ray science using microcalorimeter sensors.

Wavelength Bistability in Two-Section Mode-Locked Quantum-Dot Diode Lasers

We report a two-section mode-locked quantum-dot laser with an emission wavelength that is bistable with respect to applied bias on the saturable absorber region. The two stable lasing wavelengths for this device are about 1173 and 1166 nm with a power contrast ratio of over 30 dB. The largest switchable wavelength range is 7.7 nm. The optical power and pulsewidth (6.5ps) are almost identical in the two lasing modes under optimized conditions. The operation of this laser can be explained by the interplay of the spectral-hole burning and the quantum-confined Stark effect

Photon antibunching from a single lithographically defined InGaAs/GaAs quantum dot

We demonstrate photon antibunching from a single lithographically defined quantum dot. Measurement of the second order autocorrelation function indicates g(2)(0) = 0.395 ± 0.030, below the 0.5 limit necessary for classification as a single photon source.

Observation of iron spin-states using tabletop x-ray emission spectroscopy and microcalorimeter sensors

X-ray emission spectroscopy (XES) is a powerful probe of the electronic and chemical state of elemental species embedded within complex compounds. X-ray sensors that combine high resolving power and high collecting efficiency are desirable for photon-starved XES experiments such as measurements of dilute, gaseous, and radiation-sensitive samples, time-resolved measurements, and in-laboratory XES. To assess whether arrays of cryogenic microcalorimeters will be useful in photon-starved XES scenarios, we demonstrate that these emerging energy-dispersive sensors can detect the spin-state of 3d electrons of iron in two different compounds, Fe2O3 and FeS2. The measurements were conducted with a picosecond pulsed laser-driven plasma as the exciting x-ray source. The use of this tabletop source suggests that time-resolved in-laboratory XES will be possible in the future. We also present simulations of and spectra that reveal the spin-state sensitivity of different combinations of sensor resolution and accumulated counts. These simulations predict that our current experimental apparatus can perform time-resolved XES measurements on some samples with a measurement time of a few 10 s of hours per time delay.