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    Arraysof quantum dots promise improved

    performancefor semiconductor lasersandhavethe

    added advantage that theycanassem ble themselves

    Quantum-dot lasers

    KARLEBERL

    bulk semiconductor material

    SEMICONDUCTOR lasers

    are key

    components

    in

    many

    of

    the appliances that wetakefor granted in everyday life.

    Fibre-optic communications and compact-disc players

    are

    perhaps the two best known examples. There is alsoa

    world-wide research

    and

    development effort

    to

    improve

    the performance of these devices by making them smaller,

    brighter, more efficient

    or

    capable

    of

    lasing

    at

    new wave-

    lengths. A new class

    of

    semicond uctor laser

    - a

    quantum-

    dot laser that self assembles

    -

    is showing great promise

    in

    many

    of

    these areas.

    Semicon ductor lasers emit light when

    an

    electron

    in the

    conduction band recombines with an empty electron

    state

    or

    hole

    in

    the valence b and. The wavelength

    of

    the

    lightisusually determined by thebandgap ofthe semi-

    conductor

    - the

    energy difference between

    the top of

    the

    valence band

    and the

    bottom

    of the

    conduction band.

    Gallium indium phosphide,

    for

    example,

    has a

    band

    gap

    of about

    1.9

    eV, which leads

    to the

    emission

    of

    red light.

    The band gap, whichisresponsibleformostofthe use-

    ful properties

    of

    sem iconductors,

    is due to the

    quantum

    nature of the electron waves as they travel throughthe

    crystal. Quantum mechanics

    forbids the electrons from

    having energies inside

    the

    band gap.

    In

    a

    bulk semiconductor,

    such as silicon or gallium

    arsenide,

    an

    electron

    in the

    conduction band behaves like

    a free electron and can occupy

    states with continuous values

    of momentum and energy.

    This picture changes dramat-

    ically, however, when the

    motion

    of the

    electron

    is

    restricted in one or more

    dimensions (figure la

    and

    b .

    Iftheelectrons are confinedin

    a small enough region, their

    energy levels will be quantized,

    similar

    to the

    energy levels

    in

    an atom.

    One way to

    make

    such

    an

    artificial atom

    or

    quantum dot

    is to

    surround

    a small regionofsemiconduc-

    tor with another semiconduc-

    tor thathas alarger bandgap

    (figure lc).

    The

    electrons

    are

    effectively confined

    in the

    region with

    the

    smaller band

    gap as they seek to reduce

    their energy.

    Ina simplified modeltheconfinement potentialcan be

    considered

    as a

    square well (figure Id .

    In

    this model

    the

    separationof the discrete energy levels depends inversely

    on the size ofthequantumdot.Th e dot must be 10

    nm or

    smaller

    for the

    energy levels

    of

    the quan tum well

    to be

    separated

    by

    more than

    the

    thermal energy

    at

    room

    tem-

    perature. Such quantum dots contain only a few thousand

    atoms

    and

    should

    be

    able

    to

    emit light

    at

    wavelengths

    determine d by the energy levels

    in

    die do t, rather tha n

    the

    band-gap energy.

    However, various processes conspiretostopasemicon-

    ductor emitting light. Impurity atoms

    can, for

    example,

    trap the charge carriers and prevent recombination.

    Electrons

    and

    holes

    can

    also emit phonons

    (i.e.

    lattice

    vibrations) rather than photon s when diey recombine. To

    overcome these problems, the surface

    of

    the qu antum

    dot

    mustbe passivated :inother words,thesmall-band-gap

    material must

    be

    completely embedded

    in the

    barrier

    material without any crystal defects

    and

    impu rities.

    Quantum dots are widely used for experiments that

    semiconductor quantum dot

    10

    nm

    band gap

    light

    emission

    1 a) The periodic crystal potential in a piece of bulk

    semiconductor material allows almost free motion for

    electrons, which results in energetic bands separated by a

    forbidden band gap. Within the conduction band, electrons

    have continuous kinetic energy and momentum, o) The

    situation is totally different for an electron confined in a very

    small ~ 10 nm in diameter) semiconductor cluster and the energy spectrum becomes discrete like that for atoms.

    c) A schematic illustration of a passivated quantum dot with the charge carriers purple) confined in the small-

    band-gap material red), which is completely embedded in a large-band-gap material blue) without any crystal

    defects and impurities present. The charge carriers are confined in all directions. The location of the electron is

    indicated schematically and is similar to the orbitals in atoms, d) A model square-well confinement potential

    showing the quantized energy states red lines).

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    4 8 Physics World September 1997

    elastic strain relaxation

    wetting layer

    2(a) Cluster formation during epitaxial growth of a semiconductor

    material (red) on top of another se miconductor with a smaller (by a few

    per cent) lattice constant (blue). For example, indium phosphide has a

    4%

    larger lattice constant than gallium indium phosphide, so InP forms

    clusters as shown in figure 3. The cluster formation is energetically

    favourable, because the lattice can elastically relax compressive strain

    and thus reduce strain energy, (>) In an alternative growth mode the

    epilayer is laterally com pressed to match the substrate lattice. This so

    called "pseudomorphic growth" is observed for heterostructures that

    have only a small lattice mismatch.

    probe the fundamental quantum behaviour of semicon-

    ductors. They also have many potential device appli-

    cations. Th e most promising of these are single-electron

    transistors (see Harmans in further reading) and quan-

    tum-dot lasers. The latter offer the possibility of improved

    device performance and increased flexibility to adjust the

    laser wavelength.

    Early days

    Semiconductor lasers have developed rapidly since their

    invention in

    1962.

    Th e first semicondu ctor laser consisted

    ofagallium arsenide p -n junction that was forward biased

    such that electron-hole recombination took place in the

    depletion region between the positively doped (p) and

    negatively doped (n) regions. Polished surfaces (called

    facets) perpendicular to the junction were used to form

    the reso nant cavity needed for laser action. The se facets

    fill the role played by mirrors in conventional lasers.

    The performance of the early semiconductor lasers was

    greatly improved by sandwiching the gallium arsenide

    (GaAs) active layer between aluminium gallium arsenide

    (AlGaAs) layers in a hetero structure device. This

    improved laser performance for two reasons. First, the

    AlGaAs layers have a larger

    band gap than the GaAs

    layers, which helps to confine

    the charge carriers in the

    active layer. Second, AlGaAs

    has a lower refractive index

    than GaAs, which confines the

    light within the active layer

    and thus acts as a waveguide.

    In 1970 this concept lead to

    the continuous room-tem-

    perature operation of GaAs/

    AlGaAs heterostructure lasers.

    A key figure-of-merit for a

    semiconductor laser is the

    current density needed for lasing to start. This figure

    should be as low as possible and by 1975 threshold cur-

    rent densities of about 50 0Acm

    2

    had been achieved with

    active layers abou t 0.1 |0.m thick. The practical use of

    semiconductor lasers in real applications such as fibre-

    optic data transmission began around this time.

    In 1974 Raymond Dingle ofBellLaboratories in the US

    demonstrated quantum confinement of charge carriers for

    the first time. And in 1979 Won -Tien Tsan g, also of Bell

    Labs, built the first semiconductor laser based on quan-

    tum confinement. The active region in Tsang's laser was

    only about 0.01 um (10 nm) thick, so the charge carriers

    (i.e. electrons and holes) were only free to move in just

    two dimensions. The se qua ntum-w ell lasers had three

    advantages over previous devices: considerably higher

    light amplification or optical gain ; m uch lower thresho ld

    current densities (less than 50A cm

    2

    ) and significantly

    improved tem perature stability. The se advantages are all

    linked to the redu ced energy spread of occupied states for

    electrons and holes in quantum-well devices compared

    with bulk semiconductors.

    The next step - from quantum-well lasers to quantum-

    wire lasers - came in the late 1980s. In quantum-wire

    lasers the charge carriers are free to move in only one

    direction, which further increases optical gain, reduces

    threshold current densities (to less than 10A

    cm

    2

    ),

    and

    improves temperature stability.

    In 1986 Masahiro Asada of the Tokyo Institute of

    Technology and co-workers, building on earlier work by

    Yasuhito Arakawa from Tokyo University, predicted that

    quantum-dot lasers - lasers in which the active region

    contains a large number of equally sized quantum dots -

    would have even better characteristics. A quantum dot

    confines the motion of the electrons in all three of the

    spatial directions.

    The discrete energy spectrum of the quantum dots

    prom ises highly efficient lasing at a distinct energy. Two

    key requirements in any laser are a population inversion

    (i.e. there should be more electrons in the excited state

    than in the ground state) and that the optical gain is

    greater than the losses. Lasers also rely on stimulated

    emission: in this process a photon of a given frequency

    causes another photon of the same frequency to be emit-

    ted. In a laser diode, only those electrons in the conduc-

    tion-band minimum that recombine with holes in the

    valence-band maximum contribute to stimulated emis-

    sion. Since the electronic states in a quantum dot are

    squeezed into discrete transition energies, fewer charge

    carriers will be needed to create a population inversion,

    which should lead to lower threshold currents than found

    in existing laser diodes.

    Temperature stability should also be improved in quan-

    tum-dot lasers. In a conventional semiconductor laser the

    3 A cross-sectional transmission electron m icrograph of an InP cluster on GalnP. The cluster was formed

    during epitaxial growth of nominally three atomic layers of InP. Since the islands are extremely small and

    appear spontaneously during growth , they are called self-assembling quantum dots.

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    PhytkaWo rid Septembar 1997 4 9

    GaAs substrate

    laser output

    GalnP waveguide

    ^^

    with one layer of InP

    4 An optically pumped InP quantum-dot laser. The electron-hole pairs are excited by a ^ - i . * ^ ^ quantum d ots

    focused stripe of green light incident from the left. The stimulated red -light emission (laser

    output) originating from the dots is observed perpendicular to the excitation light. The experiment was performed at low temperature (8 K) under

    continuous excitation , with the sample mounted in a cryostat. The layer of InP dots is in the middle of a GalnP film, wh ich is surrounded by AllnP

    layers that have a smaller refractive index and thus keep the light close to the active layer.

    spread of energy states usually causes the threshold cur-

    rent to chang e significantly w ith tem perature. F or a q uan-

    tum-dot laser, however, the discrete energy spectrum and

    large separation between the energy levels almost elim-

    inates any temperature d ependence.

    Making quantum dots

    Th e exp erimental challenge is to make 10 nm semicon-

    ductor structures in an efficient and reproducible way. A

    large number of dots are needed and they must be equal

    in size and optically active. However, conventional semi-

    conductor-processing techniques that are based on litho-

    graphy and etching face inherent problems such as

    limited resolution and the introduction of surface defects

    during production.

    Over the past few years several research groups have

    started working on the direct synthesis of various semi-

    conductor nanostrucrures, including quantum dots, by

    combining epitaxial growth tech-

    niques, such as molecular beam

    epitaxy or chemical vapour de-

    position, with lithography. Con-

    ventional lithographic techniques

    are used to create a pattern on

    the surface before the quantum-

    dot material is deposited. Epi-

    taxial growth on patterned

    substrates leads to the formation

    of sharp edges or V-grooves on

    the surface. Quantum dots and

    wires can then be formed in a

    self-adjusting way.

    A much simpler idea is based

    on the islands that form when a

    semiconductor is deposited on a

    substrate that is made from a

    material with a significantly

    smaller lattice constant. This

    process is known as the Stranski-

    Krastanov growth mode, and

    quantum dots that have dimen-

    sions of only a few atomic dis-

    tances across have been grown

    this way (figure 2a . An import-

    ant point is that the size of the

    S S pectrum of the laser output (a) and photoluminescence

    spectrum (b) from the InP quantum-dot laser shown In figure

    4. The laser-output intensity19about a factor of 200 times

    more intensive than the lower spectrum.

    quantum structure is controlled within the epitaxial de-

    position in a self-adjusting process. For the first few

    atomic layers, the atoms arrange themselves in a planar

    layer called the wetting layer. As epitaxial growth pro-

    ceeds, the atoms tend to bunch up and form clusters.

    Cluster formation is energetically favourable, because the

    lattice can elastically relax the compressive strain and thus

    reduce the strain energy within the islands.

    In an alternative growth mode known as pseu dom or-

    phic grow th , the epilayer is laterally compressed to ma tch

    the substrate lattice (figure

    2b .

    The lateral strain is auto-

    matically introduced as the growth proceeds.

    To see how these techniques work, consider the growth

    of indium phosphide (InP) on gallium indium phosphide

    (GalnP). GagjInojP has the same lattice constant as

    gallium arsenide, so it is possible to grow good quality

    G aln P layers on gallium arsenide sub strates. Th e lattice

    constant of InP is about 4% larger. However, with opti-

    mized molecular-beam-epitaxy growth conditions, defect-

    free clusters or dots form after

    1.5 or more monolayers of InP

    have been deposited. For exam-

    ple,

    after three nominal layers

    have been deposited, clusters can

    be seen on top of the wetting

    layer. There are about 5 x l0

    1 0

    dots per square centimetre and

    they nucleate preferentially at the

    atomic step s that are always

    present on a surface. The dots

    have a truncated pyramid shape,

    and are about 15 nm in diameter

    and 3 nm high (figure 3). Sur-

    prisingly, the dot size varies by

    only about 10%, which is essen-

    tial for making a quantum-dot

    laser. After the InP dots have

    been grown, a thick layer of

    GalnP is deposited to passivate

    the dots.

    The dot size strongly depends

    on the amount of deposited dot

    material. And since the energy

    levels in the dot depend on its

    size, so does the wavelength of

    light emitted by the dot. Bulk

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    5 0 Ptiyttct Worid Septwntw S97

    indium phosphide has a band gap

    of 1.35 eV, which corresponds to a

    wavelength of

    1

    [im.The growth of

    two monolayers of InP on GalnP

    produces dots with diameters of

    abou t 12 nm , whereas for seven

    monolayers the diameter is about

    50 nm. The energy shift for 12 nm

    dots is 1.85 eV, which corresponds

    to red-light emission. The larger

    50 nm dots have lower energy shifts

    (1.65 eV) and emit in the infrared.

    The pronounced increases in

    energy are due to carrier confine-

    ment and strain in the dots.

    However, once more than seven

    monolayers of InP have been

    grown, various dislocations are

    introduced and these reduce the

    light output.

    The size of the dots can also be

    adjusted within a certain range by

    changing the growth conditions.

    For example, an extended interrup-

    tion between the deposition of the

    dot material and the growth of the capping layer leads to

    larger dots with a lower dot density - smaller dots disap-

    pear and larger dots grow higher during the interruption.

    The same happens for very slow deposition rates. Larger

    clusters are energetically favourable because there is less

    strain at the top of large dots. However, short-wavelength

    lasers (e.g. those working in the visible) require small dots,

    which can be made by keeping the growth interruption

    short. This also reduces the range of dot sizes.

    The ability of self assembly to make regular arrays of

    extremely small quantum dots without the need for litho-

    graphy and etching makes it a highly promising technique

    for the fabrication of quantum-dot lasers.

    Let there be light

    To make a quantum-dot laser we need a dense array of

    equal-sized dots within the active region, and a mirror at

    each end ofthe region to form the laser

    cavity.

    The energy

    of the radiation depe nds on the ba nd gap of the dot m ater-

    ial and the strain, and inversely on the size of the dots.

    Electrons an d holes can be created in the dot by optical or

    electrical excitation (figure 4).

    In 1995 my group at the Max Planck Institute in

    Stuttgart in collaboration with Andreas H angleiter's group

    at the University of Stuttgart observed room-temperature

    lasing in the visible range from an optically excited indium

    phosphide q uantum -dot laser. Th e electron-hole pairs

    were formed by focusing green light onto the active layer,

    and red laser emission was observed emerging from the

    mirrors of the laser structure (figure 5). Th e threshold

    current for lasing was comparable with that obtained for

    GalnP/AlGalnP quantum wells in a similar set-up.

    Also in 1995 Dieter Bimberg's group at the Technical

    University in Berlin, in collaboration with researchers

    from the A F Ioffe Physical Technical Institute in St

    Petersburg, demonstrated room-temperature operation

    of an electrically pumped quantum-dot laser. This

    device contained a closely packed stack of indium

    arsenide (InAs) quantum-dot layers and emitted in the

    infrared. Bimberg and co-workers also achieved thresh-

    old current densities comparable with quantum-well

    lasers (below 20

    A cm

    2

    )

    at liquid-nitrogen temperatures

    6 A cross-sectional transmission electron micrograph

    from a sample with three stacked layers of InP dots.

    Stacking individual do t layers helps to Increase the total

    amount of active material within the waveguide of a

    laser structure.

    and with better temperature sta-

    bility. However, they have not yet

    been able to match the perform-

    ance of quantum-well laser diodes

    at room temperature.

    Stacking layers of dots in the laser

    structure increases the amount of

    active material in devices (figure 6).

    In 1995 James Harris and co-

    workers at Stanford University in

    California reported a significant

    reduction in photoluminescence

    linewidth from stacked InAs dot

    layers. This reduction is thought to

    be due to the more uniform distri-

    bution of dot sizes caused by the

    correlated nucleation of the dots:

    atoms that arrive during the growth

    of the upper layer tend to accumu-

    late and form new dots just above

    those in the underlying layer. This

    correlation - which is caused by the

    strain field around the embedded

    dots - is observed if the separation

    between the layers is not too large.

    Recently Bimberg and co-workers and Hideaki Saito's

    group at NEC in Tsukuba have built laser diodes with a

    stack of ten layers of dots.

    Self-assembled futures

    Although the research is still at an early stage, experiments

    have already shown that self-assembled quantum dots do

    make good lasers. Th e next challenge is to ma tch and sur-

    pass the performance of quantum-well lasers. This would

    give quantum-dot lasers a chance to move into appli-

    cations such as ultrafast optical data transfer. A key aspect

    of this challenge will be to improve our control over the

    size distribution of the dots produced in the self-assembly

    process. But given the rapid progress m ade so far, experts

    in the field are confident that there will be significant per-

    formance improvements in the near future.

    Further reading

    1986 Gain and the

    box lasers

    IEEE J.

    M Asada, Y Miyamoto and Y Suematsu

    threshold of three-dimensional quantum

    Quantum

    Electron.

    QE-22 1915

    D Bimberget

    al.

    1997 InGaAs-GaAs quantum dot lasers IEEE

    J.QuantumElectron.

    3 1

    K Eberl, P M Petroff and P Demeester 1995 Low-dimensional

    structures prepared by epitaxial growth or regrowth on pat-

    terned substrates

    NATO ASI

    Series

    E:

    Applied Science VbL

    29 8

    (Kluwer, Dordrecht)

    K Harmans 1992 Next electron, please...Physics Wbrld March

    pp5O-53

    A M oritzet al 1996 Optical gain and lasing in self-assembling

    InP/GalnP quantum dotsA pp Phys.Lett.69 212

    P M Petroff and S P DenBaars 1994 MBE and MO CVD growth

    and properties of self-assembling quantum dot arrays in HI-V

    semiconductor structuresSuperlatticesan dMicrostructures 15 15

    H Saito et al. 1996 Room-temperature lasing operation of a

    quantum-dot vertical-cavity surface-emitting laser

    App. Phys.

    Lea.

    69 3140

    Karl Eberl is in the Max-Planck-lnstitut fur Festkorperfof

    schung,

    Heisenbergstr. 1, 70569 Stuttgart, Germany (email:

    [email protected])

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