Richard M. Williams

Quantum cascade lasers: ultrahigh-speed operation, optical wireless communication, narrow linewidth, and far-infrared emission

Following an introduction to the history of the invention of the quantum cascade (QC) laser and of the band-structure engineering advances that have led to laser action over most of the mid-infrared (IR) and part of the far-IR spectrum, the paper provides a comprehensive review of recent developments that will likely enable important advances in areas such as optical communications, ultrahigh resolution spectroscopy and applications to ultrahigh sensitivity gas-sensing systems. We discuss the experimental observation of the remarkably different frequency response of QC lasers compared to diode lasers, i.e., the absence of relaxation oscillations, their high-speed digital modulation, and results on mid-IR optical wireless communication links, which demonstrate the possibility of reliably transmitting complex multimedia data streams. Ultrashort pulse generation by gain switching and active and passive modelocking is subsequently discussed. Recent data on the linewidth of free-running QC lasers (/spl sim/150 kHz) and their frequency stabilization down to 10 kHz are presented. Experiments on the relative frequency stability (/spl sim/5 Hz) of two QC lasers locked to optical cavities are discussed. Finally, developments in metallic waveguides with surface plasmon modes, which have enabled extension of the operating wavelength to the far IR are reported.

Kilohertz linewidth from frequency-stabilized mid-infrared quantum cascade lasers

Frequency stabilization of mid-IR quantum cascade (QC) lasers to the kilohertz level has been accomplished by use of electronic servo techniques. With this active feedback, an 8.5-microm QC distributed-feedback laser is locked to the side of a rovibrational resonance of nitrous oxide (N(2) O) at 1176.61cm (-1) . A stabilized frequency-noise spectral density of 42Hz/ radicalHz has been measured at 100 kHz; the calculated laser linewidth is 12 kHz.

Free-running frequency stability of mid-infrared quantum cascade lasers

The intrinsic frequency fluctuations of two single-mode quantum cascade (QC) distributed-feedback lasers operating continuously at a wavelength of 8.5 mum are reported. A Doppler-limited rovibrational resonance of nitrous oxide is used to transform the frequency noise into measurable intensity fluctuations. The QC lasers, along with recently improved current controllers, exhibit a free-running frequency stability of 150 kHz over a 15-ms time interval.

Frequency stabilization of quantum-cascade lasers by use of optical cavities

We report a heterodyne beat with a linewidth of 5.6+/-0.6 Hz between two cavity-stabilized quantum-cascade lasers operating at 8.5 microm . We also present a technique for measuring this beat that avoids the need for extreme isolation of the optical cavities from the environment, that of employing a third servo loop with low bandwidth to force one cavity to track the slow drifts and low-frequency fluctuations of the other. Although it is not fully independent, this technique greatly facilitates heterodyne beat measurements for evaluating the performance of cavity-locked lasers above the bandwidth of the third loop.

Compositional control of rovibrational wave packets in the E(1Σg+) “shelf” state of Li2 via quantum-state-resolved intermediate state selection

Compositional control in the preparation of rovibrational wave packets is demonstrated in the E(1Σg+) state of gas-phase Li2 molecules using ultrafast pump–probe laser spectroscopy combined with quantum-state-resolved intermediate state selection. The intermediate state, from which subsequent ultrafast excitation occurs, is a stationary rovibrational level in the A(1Σu+) state of Li2, produced by cw laser excitation from the ground X(1Σg+) state. The effect that the intermediate state has on the final composition of the wave packet is investigated by comparing the transients resulting from ultrafast pump–probe excitation of two different intermediate states (vA=14, JA=18 versus vA=13, JA=18). In these experiments the pump wavelength is compensated so that in each case the same E-state eigenstates (vE=13–18, JE=JA±1) make up the wave packet, but with different amplitudes. Theory predicts, and experiments confirm, that the relative amplitudes of the rovibrational eigenstates are strongly dependent upon the ...

Rapid-scan Doppler-limited absorption spectroscopy using mid-infrared quantum cascade lasers

Laser characteristics have been evaluated for mid-infrared quantum-cascade (QC) lasers operating in a continuous mode at cryogenic temperatures. These tests were performed to determine the suitability of QC lasers for use in various spectroscopic applications, including Doppler-limited molecular absorption spectroscopy and pressure-limited LIDAR instrumentation. Using rapid-scanning techniques, direct absorbance measurements of nitric oxide, ammonia and nitrous oxide have been performed with QC lasers, operating at either 5.2 or 8.5 micrometers . Measured Doppler-limited absorption profiles show no distortion with increased averaging (up to 103 - 104 samples averaged), thereby minimizing the need for sophisticated data acquisition systems which re- register successive data streams to accommodate for laser frequency jitter and drift. Additionally, the high tuning rates (2.5 cm-1 in 0.6 milliseconds; 5 - 10 kHz sweep repetition rate) achieved with the QC lasers allow for the measure of relatively rapid transient phenomena or a high degree of signal averaging in a short time. Noise- equivalent absorbances of 3 X 10-6 have also been obtained without optimizing the optical arrangement.

A new shallow underground gas-proportional counting lab—First results and Ar-37 sensitivity

A new ultra-low-background proportional counter was recently developed with an internal volume of 100 cm(3) and has been characterized at pressures from 1-10 atm with P-10 (90% Ar, 10% methane) gas. This design, along with a counting system providing event digitization and passive and active shielding, has been developed to complement a new shallow underground laboratory (30 m water-equivalent). Backgrounds and low-level reference materials have been measured, and system sensitivity for (37)Ar has been calculated.

Development of an absolute gas-counting capability for low to medium activities.

Pacific Northwest National Laboratory (PNNL) is developing a capability to measure the absolute activity concentration of gaseous radionuclides using length-compensated proportional-counting. This capability will enable the validation of low-level calibration standards for use in PNNLs new shallow underground laboratory. Two sets of unequal length proportional counters have been fabricated; one set has been fabricated using ultra-low background (ULB) electroformed copper and a second set fabricated from Oxygen-Free High-Conductivity Copper (OFHC).

Development of a Low-Level Ar-37 Calibration Standard

Argon-37 is an environmental signature of an underground nuclear explosion. Producing and quantifying low-level (37)Ar standards is an important step in the development of sensitive field measurement instruments. This paper describes progress at Pacific Northwest National Laboratory in developing a process to generate and quantify low-level (37)Ar standards, which can be used to calibrate sensitive field systems at activities consistent with soil background levels. This paper presents a discussion of the measurement analysis, along with assumptions and uncertainty estimates.

Development of a low-level (37)Ar calibration standard.

Argon-37 is an environmental signature of an underground nuclear explosion. Producing and quantifying low-level (37)Ar standards is an important step in the development of sensitive field measurement instruments. This paper describes progress at Pacific Northwest National Laboratory in developing a process to generate and quantify low-level (37)Ar standards, which can be used to calibrate sensitive field systems at activities consistent with soil background levels. This paper presents a discussion of the measurement analysis, along with assumptions and uncertainty estimates.