Quantum Cascade Lasers

Prachi Pande (2010PH10861)

General overview of lasers

Lasers (Light Amplification by Stimulated Emission of Radiation) are devices used to produce
beams of light that are monochromatic (having a narrow linewidth as compared to other sources
of light), coherent (the photons all have a fixed phase relationship to each other) and highly
collimated (having low divergence). The most common types of lasers are gas lasers (e.g. He-Ne
laser, CO2 laser, argon ion lasers, excimer lasers), solid state lasers (Nd:YAG laser, Ti:sapphire
laser), and semiconductor lasers (VCSELs, quantum cascade lasers).
In most materials, for photons propagating through the material, three kinds of processes take
place absorption, spontaneous emission and stimulated emission. Every emission is
associated with an electronic transition from a higher to a lower energy level, and every
absorption with a transition from a lower to a higher one. Given two energy levels, the
probability of spontaneous emission depends on the relative number of electrons in the two
levels at a particular temperature, which is given by Boltzmanns equation

In general, there are many more electrons in the lower energy levels than in the higher ones, so
there is more absorption than emission. In order to have a laser beam, population inversion is
required that is, there should be more electrons in the higher level. This is generally achieved
through a pumping mechanism in gas lasers, this is done using an electric discharge or
optically using other lasers, and for solid-state lasers the mechanism is optical pumping using
flash lamps or other lasers. Laser diodes are pumped electrically, but there are also other
semiconductor lasers that are optically pumped. The figure below shows a four-level pumping
system the actual laser transition takes place between the two middle levels, while the other
two levels are used to achieve population inversion between those levels.

However, the photons from spontaneous emission are out of phase and interfere destructively
with each other. In order to obtain a coherent beam, a resonator is used to create positive
feedback to prevent photons from escaping from the medium, so that they stimulate other
atoms, which oscillate in phase with the incoming photon and release another photon with that
phase (see figure below).

The characteristics of the resonator determine the modes that can travel within it. For parabolic
mirrors and optically homogeneous media, the modes are Hermite-Gaussian modes.
Theoretically, laser beams are usually analyzed as superpositions of modes.

Energy states, subbands and intersubband transitions in quantum wells

Quantum wells are potential wells formed from 2D semiconductor heterostructures. They have
applications in several kinds of devices, like LEDs, laser diodes, solar cells, HEMTs (High
Electron Mobility Transistors), infrared photodetectors and saturable absorbers (used for modelocking in lasers).
In bulk semiconductors there are energy bands, but in quantum-confined structures there are
further subbands within those energy bands. In a quantum well, due to the fact that quantum
confinement and hence discretization of energy levels only occurs in one direction, and
electrons and holes are still free to move in the other directions, subbands are created for each
confined state, starting at the energy of that state.

The parabolic curves represent the dispersion relations in the plane of the well. The energy of the
electron (hole) consists of the energy of the confined level plus the kinetic energy of the carrier.
The density of states for the subbands of a quantum well is given by

The optical absorption for a quantum well is a series of steps, one for each quantum number, that
smoothly transitions into the square-root dependence of the bulk DOS on energy.
Intersubband transitions (ISBTs) normally have linewidths around 6-20 MeV. They can reach
wavelengths of 0.2 mm, and are homogeneously broadened due to scattering processes. They are
also inhomogeneously broadened by subband non-parabolicity and sample growth variations.
Light polarized parallel to the plane of the quantum well is generally not absorbed in ISBTs.
The radiative emission of photons is not the dominant mechanism by which electrons in higher
subbands recombine to lower subbands. Spontaneous emission has very low efficiency, and other
mechanisms like phonon emission are more dominant. The figure below shows how an electron
transitions to another subband, thermalizes in that subband, transitions to a different point on the
lower subband (due to conservation of energy and momentum) and then again thermalizes.

Quantum cascade lasers

Two limitations of interband semiconductor lasers are

that the emission wavelength is determined by the band gap and is only tunable insofar as

the band gap can be altered, and

that because of the broad distribution of the population inversion, the gain spectrum of
the laser is broadened.

In the 1970s, Kasarinov and Suris analyzed how a superlattice would behave optically if a strong
electric field were applied to it, such that for two adjacent quantum wells, the ground state of one
would be just below the second excited state of the other.

This would achieve population inversion and optical gain using only intersubband transitions
involving only one type of carrier. An electron in the ground state of one well would tunnel
through the barrier and make a radiative transition to the first excited state of the next quantum
well, after which it would relax to the ground state of the same well, which would function as the
upper laser level for the next transition. Thus, a four-level laser system would be set up in which
population inversion would always be ensured.
However, this was not easy to demonstrate experimentally because it was not electrically stable.
A doped superlattice of the type described would break into different field domains with aligned
energy states i.e. in one part of the superlattice, the ground state would be aligned with the
second excited state of the next well, while in another part it would be aligned with the first
excited state. Thus, a periodic arrangement of quantum wells was not enough.

The improved design had a more complex structure a periodic arrangement of unit cells
consisting of multiple wells and a barrier. This cell could be divided into a gain region and an
injection/relaxation region (see figure below).

The laser transition takes place in the active region, and then the energy of the electron is raised
in the injection/relaxation region to a level where resonant tunneling through the next barrier can
take place. This region functions as an electron reservoir to inject electrons into the next unit
cell, and is doped in order to prevent space-charge domains from being formed. The active
region is not doped since this would cause broadening of the laser line due to impurity states.
Increasing the size of the active region (to about 10-100 periods) enables a phenomenon called
cascading. A single electron is recycled in transitions down the structure, and is thus able to
cause the emission of a number of photons. The increase in the size of the active region also
means that the population density required in each period for population inversion is decreased.
These things lead to a decrease in the threshold current density and an increase in the slope
efficiency of the device. However, it also means that a much larger bias has to be applied in order
to flatten out all the injection regions. In effect, this leads to a reduction in energy losses
through ohmic heating.

In a QCL, the lifetimes of the energy levels must be engineered to achieve population inversion.
This can be done through several mechanisms. For instance, if the transition is diagonal, i.e. the
initial and final states belong to adjacent quantum wells, then the scattering rate can be decreased
by increasing the barrier thickness. To decrease the lifetime, resonant optical phonon emission
can be used, since optical phonon emission is the process that ultimately limits the lifetime for
mid-infrared lasers.
One of the popular designs for the active region was the three quantum well active structure. In
this, two quantum wells of different widths were designed with their ground states in resonance.
Then an electric field was applied such that the energy splitting was equal to the optical phonon
resonance. Then a third thinner quantum well was added upstream. This could either have a state
resonant with the n=3 state of the first quantum well, which would lead to a diagonal transition
with a longer lifetime, or slightly above it, which would lead to a vertical transition with better
injection efficiency due to the penetration of the wavefunction into the barrier.
The first working QCL followed this design, and was demonstrated in 1994 by Faist, Capasso et
al. It was made of heterostructures grown by molecular beam epitaxy and operated at a
wavelength of 4.2 m with peak power around 8 mW during pulsed operation. In this laser, the
tunneling rate through the barrier was (~0.2 ps)-1, the intersubband relaxation time between the
laser levels was ~4.3 ps at 105 V/cm, and the relaxation time of the lower state was ~0.6 ps.
One limitation of this was that the relatively long lifetime for the diagonal transition made the
population inversion difficult to achieve. To address this, the two-phonon resonance design was
developed. Here, the extraction is achieved using a 3-state ladder where the states are separated
by optical phonons, which greatly decreases the population of the lower state (see figure below).

Current trends
External cavity quantum cascade lasers
One gain mechanism often used in semiconductor lasers is DFB (distributed feedback) where the
active region is designed as a diffraction grating that selects a narrow band of wavelengths and
provides optical feedback. The disadvantage of DFB lasers is their limited tuneability. They can
be tuned thermally, but only to about 10-20 cm-1. To overcome this, the EC-QCL can be used.
Here, the sides of the laser have antireflection coatings, and the mirrors that form the resonator
are arranged in an external configuration.
The EC-QCL comes in different kinds of designs. One is the bound-to-continuum design where
the radiative transitions take place between a single initial state and a quasiminiband of final
states delocalized over the coupled quantum wells of a chirped superlattice. Another design uses
heterogeneous active regions it stacks dissimilar bound-to-continuum gain stages to create a
structure that has a low gain variation over a much larger wavelength range than a normal singlewavelength laser, and therefore is much more broadly tunable. However, if too many substacks
are used, it becomes difficult to make their electrical properties similar and to ensure that they
remain transparent to all the other emission frequencies.
EC-QCLs are used for absorption spectroscopy in, for e.g., trace gas sensing, environmental
monitoring, industrial process control, and in heterodyne detection.
Other applications of QCLs
Terahertz imaging
The high power, sub-200-micron wavelengths and narrow linewidths of THz QCLs have
facilitated the development of THz imaging systems with fast acquisition rates, high dynamic
range, long-range capability and high transverse resolution. Apart from this, the phenomenon of
self-mixing (SM) has also been studied for coherent imaging applications. In SM, the radiation
emitted by a laser is partially reinjected into the laser cavity from an external target. This
radiation then interferes with the intra-cavity field and measurably alters the optical and
electrical properties of the laser that depend on phase as well as amplitude of the returning field.
Thus a single laser device can act as a radiation source as well as a coherent detector. The

potential of SM in QCLs for high resolution imaging over extended distances, for 2D and 3D
imaging, and for ISAR imaging has been explored.
Plasma diagnostics
QCL absorption spectroscopy is one of the most versatile techniques for studying molecular
plasmas. QCLAS allows the determination of absolute concentrations of the ground states of
stable as well as transient molecular species at time resolutions below a microsecond.
Information about population densities and gas temperature can also be derived from QCLAS
measurements.
Chemical physics
QCLs have been used for various spectroscopic applications in chemical physics: for instance,
photoacoustic spectroscopy, quartz-enhanced photoacoustic spectroscopy and Faraday rotation
spectroscopy (FRS). FRS is based on the magnetic circular birefringence exhibited by
paramagnetic molecular species in the presence of an external magnetic field. The suppression of
laser amplitude noise is important for FRS, and QCLs find an important application in this as
they have much less amplitude noise than color center laser sources.

References
1. Materials for Optoelectronics and Photonics, Mark Fox and Radu Ispasoiu
2. The Design of Anti-Reflective Coatings for a Quantum Cascade Laser Emitting
Light in the Mid-Infrared Range, Agatha Karan Bennett, M.A. thesis, University of
Texas, Austin, 2013
3. New Frontiers in Quantum Cascade Lasers and Applications, Capasso et al., IEEE
Journal on Selected Topics in Quantum Electronics, Nov-Dec 2000
4. Saturation of intersubband transitions in p-type and n-type III-V quantum wells,
Robert John Steed, PhD thesis, Imperial College, University of London, 2008
5. Quantum Cascade Laser, Faist et al., Science, vol. 264, 1994.
6. Intersubband Optoelectronics, lecture notes by Jerome Faist, ETH Zurich, 2009
7. Broadband all-electrically tunable MEMS terahertz quantum cascade lasers, Han et
al., Optics Letters 39(12), 2014

8. Quantum cascade lasers in chemical physics, Curl et al., Chemical Physics Letters
487, 2010.
9. Applications of quantum cascade lasers in plasma diagnostics: a review, Ropcke et
al., J Phys D: Appl Phys 45, 2012.
10. Terahertz imaging using quantum cascade lasers: a review of systems and
applications, Dean et al., J Phys D: Appl Phys 47, 2014
11. External cavity quantum cascade laser, Hugi et al., Semicond. Sci. Technol. 25,

2010.