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Complete Report - University of New South Wales

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to re-heat the carrier population, thus slowingfurther carrier cooling. Therefore the criticalfactor is the mechanism by which these opticalphonons decay into acoustic phonons, or heat inthe lattice. The principal mechanism by which thiscan occur is the Klemens mechanism, in which theoptical phonon decays into two acoustic phonons<strong>of</strong> half its energy and <strong>of</strong> equal and oppositemomenta [4.5.59].The build up <strong>of</strong> emitted optical phonons isstrongly peaked at zone centre both for compoundsemiconductor due to the Frölich interactionand for elemental semiconducotrs due to thedeformation potential interaction. The strongcoupling <strong>of</strong> the Frölich interaction also means thathigh energy optical phonons are also constrainedto near zone centre even if parabolicty <strong>of</strong> the bandsis no longer valid [4.5.60]. This zone centre opticalphonon population determines that the dominantoptical phonon decay mechanism is this pureKlemens decay.4.5.3.3.1 Suppression <strong>of</strong> phonon decay inbulk materialsIn some bulk semiconductors, with a largedifference in their anion and cation masses, therecan be a large gap between the highest acousticphonon energy and the lowest optical phononenergy, possibly large enough to block operation<strong>of</strong> this Klemens mechanism, which can be termeda ‘phononic band gap’. Work previously presented[4.5.61] using a simple 1D force constant model andcomplemented by high accuracy DFT computation[4.5.62] indicated that GaN, InN and InP all havelarge phononic band gaps, which are close to thosefound experimentally [4.5.63]. We are using timeresolved photoluminescence (tr-PL) to investigatethe carrier cooling rates in these materials.4.5.3.3.2 Time resolvedphotoluminescence measurements <strong>of</strong>bulk phononic band gap materialsResearchersPasquale Aliberti, Dirk König, SantoshShrestha, Gavin Conibeer, Martin GreenCollaboration with:Raphael Clady, Murad Tayebjee, Tim Schmidt(<strong>University</strong> <strong>of</strong> Sydney), Nicholas Ekins-Daukes(Imperial College)The potential efficiency boost, which can beachieved by Hot Carrier solar cells, is directlyrelated to the possibility <strong>of</strong> extracting highenergy carriers from the absorber layer beforethermalisation, increasing the voltage and hencethe conversion efficiency. The poor conversionefficiency <strong>of</strong> photons with energies above the bandgap <strong>of</strong> the absorber is the main loss mechanismin conventional single junction solar cells. Theinvestigation <strong>of</strong> thermalisation time constants <strong>of</strong>hot carriers is a crucial step towards the engineering<strong>of</strong> Hot Carrier cells. The efficiency <strong>of</strong> an InN basedhot carrier solar cell has been calculated using acomplex theoretical model, see Section 4.5.3.1. Iwas found that the limiting efficiency is stronglyrelated to hot carriers relaxation velocity in theabsorber [4.5.57].A comparison <strong>of</strong> femtosecond time resolvedphotoluminescence (tr-PL) spectroscopy betweenInP and GaAs was reported in last year’s annualreport and is also now published [4.5.64]. Thisshowed a distinctly longer carrier cooling timeconstant for the wide phononic gap InP ascompared to almost zero phononic gap <strong>of</strong> GaAs.It also showed further evidence for excitationinto higher side valleys for both GaAs and InP forappropriate excitation wavelengths. In 2010 thehot carrier cooling in InN has been investigatedusing tr-PL. The wide gap between optical andacoustic branches in the InN phononic dispersionrelation (wider than that for InP) prevents theKlemens decay <strong>of</strong> optical phonon into acousticphonons. This can lead to slower carrier cooling dueto “Hot Phonon Effect” [4.5.65]. The decay <strong>of</strong> hotcarriers for different excitation wavelengths InN hasbeen investigated.Tr-PL experiments have been performedon InN samples using the measurementconfiguration shown in Fig. 4.5.53. In thistechnique a laser pulse acts as a switchinggate relating the photoluminescencesignal to the time domain. The PL signalis collected from the sample, after afemtosecond laser excitation, and focusedin a non linear crystal. The gate signalis generated from the same laser and isfocused on the same crystal after passingthrough an optical delay stage. The signalis detected using a monochromator anda PMT. Our system configuration provides150 fs pulses with tunable wavelengthover a range <strong>of</strong> 256 nm (4.84 eV) to 2.6 µm (0.48 eV).Figure 4.5.54 is a three dimensional representation<strong>of</strong> PL as a function <strong>of</strong> time for all the probedwavelengths. It can be observed that the PL sharplyrises when the carriers are photo-excited by thelaser pulse. The fast decay <strong>of</strong> the PL shows thethermalisation <strong>of</strong> carriers towards respective bandedges. The decay is faster for highly energeticcarriers compared to carriers closer to the bandgap.Thus the carrier population quickly degeneratestowards the band edges during the thermalisationprocess. In InN the thermalisation is most probablydue to interaction <strong>of</strong> highly energetic electrons andholes with LO phonons [4.5.66].To investigate the rate <strong>of</strong> the carrier coolingprocess, the effective temperature <strong>of</strong> the carrierpopulation has been calculated fitting the highenergy tail <strong>of</strong> the PL spectrum for every singletime during the cooling transient. The PL has beenfitted assuming that carriers form a Boltzmann-likedistribution in a femtosecond time scale using thefollowing equation.L(ε) represents the measured PL intensity atenergy ε, α(ε) is the measured sample absorptioncoefficient, E Gis the InN energy gap, 0.7 eV in thisARCPHOTOVOLTAICSCENTRE OFEXCELLENCE2010/11ANNUAL REPORT3D representation <strong>of</strong> InN timeresolved PL data.Figure 4.5.5487

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