Perovskite solar cells are one of the most actively studied next-generation solar cells. This is mainly because high power conversion efficiencies can be achieved even with simple solution-based fabrication processes. In addition, wide bandgap perovskite solar cells can be used as top sub-cells in multi-junction solar cells due to their easily tunable bandgap properties. On the other hand, colloidal quantum dots (CQDs), whose band gap depends on the quantum dot size, are one of the few options that are compatible with solution processes and can be employed as lower sub-cells. Here, we show the potential of both types for the construction of multi-junction solar cells. To this end, we constructed a wide bandgap perovskite solar cell that is ideal for monolithic 2-junction perovskite/GaAs solar cells. We also developed a colloidal quantum dot solar cell with infrared absorbing PbS CQDs and constructed a spectral splitting multi-junction solar cell as a proof of concept.
The luminescent coupling (LC) effect is one of the strategies for further boosting the efficiency of multijunction solar cells by improving the current mismatch among subcells. This work examined the LC effect in III–V compound InGaP/GaAs/InGaAs inverted metamorphic triple-junction solar cell (IMM-3JSC) by the laser beam-induced current mapping characterization method. A strong LC effect in the bottom subcell of the IMM-3J sample was demonstrated with an LC yield of around 0.13 under 7 suns irradiance. In addition, by effectively homogenizing the LC effect, the bottom subcell of IMM-3JSCs may potentially gain a current density of ∼0.6 mA/cm2 at 10 suns irradiance.
The unique electronic features of highly mismatched alloys such as III-V GaNAs are suitable for the intermediate band solar cell (IBSC) application, in which an intermediate band (IB) acts as a stepping stone to generate additional photocarriers across the host semiconductor bandgap through sequential two-step below-bandgap photon absorption (TSPA). However, the collection of photocarriers in a realistic GaNAs IBSC is much lower and often accompanies S-shape kink features in the current–voltage (J–V) curves under illumination for which a coherent picture is lacking. Based on the solar cell characterization of GaNAs IBSC devices grown with and without barriers, with and without antimony, and with and without indium using molecular beam epitaxy, and also with the photocarrier collection analysis using equivalent circuit models, it was identified that the TSPA and the S-shape J–V of this system depend on two critical factors: (1) high carrier recombination currents (I0CI) across the GaNAs sub-gap between the conduction- and intermediate bands (EgCI) and (2) the counterdiode effect of the AlGaAs IB electron barrier. Dramatic improvements in the S-shape J–V feature of the solar cell characteristics were achieved when lattice-strain was compensated in GaInNAsSb epitaxial layers.
Epitaxially grown quantum well and quantum dot solar cells suffer from weak light absorption, strongly limiting their performance. Light trapping based on optical resonances is particularly relevant for such devices to increase light absorption and thereby current generation. Compared to homogeneous media, the position of the quantum layers within the device is an additional parameter that can strongly influence resonant absorption. However, this effect has so far received little attention from the photovoltaic community. We develop a theoretical framework to evaluate and optimize resonant light absorption in a thin slab with multiple quantum layers. Using numerical simulations, we show that the position of the layers can make the difference between strong absorption enhancement and completely suppressed absorption, and that an optimal position leads to a resonant absorption enhancement two times larger than average. We confirm these results experimentally by measuring the absorption enhancement from photoluminescence spectra in InAs/GaAs quantum dot samples. Overall, this work provides an additional degree of freedom to substantially improve absorption, encouraging the development of quantum wells and quantum dots-based devices such as intermediate-band solar cells.
Quantum-dot solar cells are a promising high-efficiency concept, but suffer from low absorption. Resonant light trapping can enable to absorb most of the incident light while maintaining good device quality. In this paradigm, the absorption depends critically on the vertical position of the quantum dot layers, but this has been largely ignored so far (this also applies to quantum wells). Here, we show the importance of the position of 10 InAs layers in a GaAs Fabry-Perot cavity. We then extend this approach to multi-resonant absorption, showing the potential absorption gain from optimizing the position of quantum dots in full devices.
Hot-carrier solar cells could overcome the Shockley-Queisser limit by having electrons and holes at a higher temperature than the lattice. To generate these hot carriers under concentrated sunlight, the thermalization rate should be as low as possible. Our objective in this presentation is to quantify the influence of different thermalization mechanisms. We determine the carrier temperature in ultrathin GaAs absorbers using continuous-wave photoluminescence and identify distinct surface and volume thermalization contributions. We explain the origin of these contributions using theoretical models involving non-equilibrium LO phonon populations and thermionic emission. We implement these mechanisms in detailed balance calculations for further understanding.
The luminescent coupling effect in a multijunction solar cell is known to help achieve current matching among subcells through carrier redistribution. We demonstrate the carrier redistribution in III-V multijunction solar cell devices using a moisture-resistant, all-inorganic perovskite quantum dot (PQD) film. This hydrophobic PQD film was applied on a full III-V multijunction solar cell device. This successfully demonstrated current redistribution vertically, shown by the increased current collection in the lower bandgap subcells, and laterally, as observed from improved current collection homogeneity in the lower bandgap subcell adjacent to the higher bandgap subcell where the luminescence originated.
In intermediate band solar cells (IBSCs), voltage preservation is a key issue to overcome efficiency limit in singlejunction solar cells. To achieve this, quasi-Fermi level splitting of respective transitions should be investigated because equivalent circuit model of an IBSC is series-parallel connected diodes. In this study, we have quantitatively investigated quasi-Fermi level splitting, Δμ in InAs quantum dot solar cells (QDSCs) by performing absolute intensity calibrated photoluminescence (PL) spectroscopy. Multi-stacked InAs/GaAs QDs were fabricated in the i-region of a GaAs p-i-n single-junction solar cell. QD ground states and GaAs band edge emissions were observed simultaneously by using a near-infrared sensitive CCD spectrometer. Excitation density dependence and temperature dependence were investigated in detail to clarify photo-carrier kinetics in QDSCs and tackle the voltage preservation issue on IBSCs. At room temperature, nonlinear increase in PL intensity was clearly observed at high excitation density above 1000 suns. Absolute PL spectra was analyzed at respective transitions by using generalized Plank’s law. As the result of detail analysis, increase in Δμ was confirmed at high excitation density and at room temperature, which suggested voltage recovering via photo-filling effect. It would be desirable to implement voltage preservation in IBSCs.
A hot-carrier solar cell (HCSC) is a high-efficiency photovoltaic concept where electrons and holes are at a higher temperature than the lattice, allowing an additional thermoelectric energy conversion. There are two requirements for a HCSC: establishing a hot-carrier population and converting the temperature into extra voltage through energy-selective contacts. We focus on the generation of hot carriers, and the design of absorbers that can make this generation easier. Fundamentally, this requires to increase the power density absorbed per volume unit, so the photocarriers cannot fully thermalize (phonon bottleneck). Beyond simply increasing the light intensity, the main control knobs to favor hot carriers include reducing the thickness of the absorber, increasing its absorptivity, and reducing its bandgap. In this proceeding, we report the fabrication of structures that aim at measuring the influence of these different parameters. We justify our choices for sample structure and fabrication method from the need for high thermal conductivity, in order to prevent lattice heating. We characterize our structures in order to determine precisely the final thickness of all layers, and the absorptivity of the absorber layer. These samples are to be used for an analysis of the temperature with many variable parameters, in order to better understand the thermalization mechanisms and design better absorbers. Ultimately, our objective is to implement all solutions together in order to evidence a hot carrier population under concentrated sunlight illumination.
Photoluminescence spectroscopy is a powerful technique to investigate the properties of photo-generated hot carriers in materials in steady state conditions. Hot carrier temperature can be determined via fitting the emitted PL spectrum with the generalized Planck’s law. However, this analysis is not trivial, especially for nanostructured materials, such as quantum wells, with a modified density of states due to quantum confinement effects. Here, we present comprehensively different methods to determine carrier temperature via fitting the emitted PL spectrum with the generalized Planck’s law and discuss under what conditions it is possible to simplify the analysis.
Strong luminescent coupling (LC) effect reduces current mismatch in III-V-based multijunction solar cells and consequently improves their power conversion efficiency. The LC current production in the Si bottom cell of InGaP/AlGaAs//Si triple junction solar cells having different sizes was investigated to determine the cell area dependence of LC effect. This was probed through laser beam-induced current (LBIC) mapping. The areal mapping was then assessed by obtaining the absolute difference between the quantum efficiencies calculated from the fitted LBIC map and simulated LC current considering uniform distribution using a quasi-two-dimensional electro-optical prediction model. At 9.17 suns concentration difference between the AlGaAs middle cell and the current-limiting Si bottom cell, the absolute LC quantum efficiency differences ranged between 0.16% and 1.68% in various cell sizes, which indicate potential current production increase if the LC current is made uniform.
Strong luminescent coupling (LC) effect in a multijunction solar cell (MJSC) allows better current balance among its subcells. The temperature dependence of wafer-bonded III-V on silicon (Si) MJSCs with LC effect was investigated. Experimentally, this was explored through light current density–voltage (J – V) characteristic measurements, external quantum efficiency measurements, and laser beam-induced current mapping of InGaP/AlGaAs//Si triple junction solar cells at different cell temperatures. Measurement results were analyzed using a quasi-two-dimensional electro-optical prediction model for LC current production and bandgap temperature dependence models of various semiconductors. It was revealed that at lower temperatures, LC current production in the limiting Si bottom cell resulted in a larger absolute LC quantum efficiency difference. At 15°C, the absolute LC quantum efficiency difference calculated was 0.17%, which indicates potential current production improvement if vertical LC current is made uniform.
Hot-carrier solar cells (HCSC) can potentially overcome the Shockley-Queisser limit, by having carriers at a higher temperature than the lattice. To this end, the carriers need to thermalize slower than power is generated by absorbing photons. In thin films, a hot-carrier distribution can only be achieved with very high incident power, by saturating the thermalization channels. Ultra-thin absorbers have a smaller thermalization rate, due to fewer channels. However, they typically absorb only a limited amount of light, which prevents them from reaching high efficiencies. Light trapping is an excellent way to increase significantly the amount of light absorbed in an ultra-thin material. Yet, studies on the coupling between light trapping and hot carriers are still lacking, due to the complexity of the whole system. We analyze numerically and experimentally how light trapping can enable high-efficiency HCSC. This manuscript presents the progress towards the experimental demonstration of the enhancement of the hot-carrier effect with light trapping. 280 nm-thick devices have successfully been reported on a gold mirror using epitaxial lift-off (ELO) and gold-gold bonding. These devices have been characterized by photoluminescence spectroscopy. Hot carriers with a temperature 37 K above lattice temperature were measured, in accordance with theoretical predictions. We are now working towards the ELO of absorbers 10 times thinner, on which we will implement light trapping to increase the carrier temperature.
Optimizing the luminescence coupling (LC) effect can reduce the current mismatch in multijunction solar cells (MJSCs), thereby enhancing their performance. In a previous work, the LC current collection was measured at room temperature. The temperature dependence of LC effect in InGaP/GaAs/Ge triple junction solar cells was observed by light J–V characteristics measurements and by laser beam-induced current mapping at operating temperatures between 18°C and 72°C. Results were analyzed using quasi-two-dimensional electro-optical model. At low operating temperatures, the photocurrent collection by LC effect has been found to be more dominant than the current collection due to bandgap reduction and thermal excitation of carriers. At 18°C and 72°C, when Ge bottom cell was made current limiting, the conversion efficiencies calculated were 6.68% and 0.01%, respectively. These findings show that the LC effect can contribute best to the MJSC performance when operated at the lowest temperature possible.
The Intermediate Band Solar Cell is an advanced concept, which has been predicted to overcome the Shockley-Queisser limit, despite efficiencies remaining below the best single junctions so far. Practical realizations with nanostructures suffer from two intrinsic deficiencies: narrow absorption widths and low radiative efficiencies. We evaluate in this paper the theoretical efficiency expectations with respect to those two properties, and consider in addition the possibility of including an electronic ratchet. We observe that an intermediate band solar cell using a ratchet becomes highly tolerant to non-ideal nanostructures, so that any combination of low absorption and low radiative efficiency becomes compatible with optimized performances above the Shockley-Queisser limit. We conclude that future practical realization may take advantage of quantum wells, which have been less considered so far than quantum dots, due to relatively higher nonradiative recombination rates. Such realizations would take advantage of the higher absorption properties of quantum wells.
In0.227GaAs/GaAsN0.011 was introduced as a 1.2-eV multiple quantum well (MQW) with a flat conduction band (FCB) in which a conduction band edge of GaAsN was adjusted to be equal to that of InGaAs. This MQW was established as a candidate material for a middle absorption layer of three-junction solar cell since electron confinement was eliminated and a short electron lifetime in GaNAs was compensated by InGaAs layer. The band alignment of MQW was characterized by the power-dependent photoluminescence (PL) measurement under low temperature. According to the band-anti crossing model, the FCB is possibly constructed since a small amount of incorporated N can drastically reduce the energy of the conduction band edge of GaAsN. The PL results demonstrated that In0.227GaAs/GaAsN MQW was a type-I structure when N content was below 1.1%, and became a type-II structure when N content was above 1.1%. The type-II MQW was characterized by the observation of blueshift of PL peak when increasing excitation power. This blueshift is a result of band-bending effect due to the accumulation of excited carriers at the interface between two materials, which is unique for the type-II MQW. In addition, it was observed that the activation energy estimated from the Arrhenius plot provided a minimum value in the structure with 1.1%N; the lowest activation energy indicated the weakest confinement energy of carriers in the structure. These results approved that a transition from type-I to type-II occurred when N content surpassed 1.1%, and our designed In0.227GaAs/GaAsN0.011 MQW was potentially the FCB structure.
We have quantitatively investigated the two-step photon absorption in quantum dot solar cells (QDSCs) by using absolute intensity calibrated photoluminescence (PL) spectroscopy. Multi-stacked InAs/AlGaAs QDs were fabricated in the i-region of p-i-n single-junction solar cells by molecular beam epitaxy. Hyperspectral imaging, which combines both the spatial and spectral dimensions of the luminescence, was used to investigate QD ground state PL at room temperature. Two lasers simultaneously excited the QDSCs to characterize two-step photon absorption. An excitation laser caused interband transition to generate photo-carriers in QDs, and the other infrared (IR) laser excited intraband transition from the QD states. As the result of two-step photon absorption, reduction in PL intensity was clearly observed under IR bias excitation. We compared absolute PL intensity with and without IR illumination, and obtain quasi-Fermi level splitting and two-step photon absorption efficiency in QDSCs under study. Compared with the photocurrent measurements, PL spectroscopy performed under open-circuit conditions, so that higher carrier filling ratio can be realized in QDs. Furthermore, PL can characterize fundamental transition on two-step photon absorption because photocurrent production needs carrier extraction to the external circuit. Quantitative analysis of two-step photon absorption by PL spectroscopy could clarify physical insights, and it would be beneficial to realize high efficiency intermediate band solar cells.
The impact of nonuniform spatial distribution of the luminescence coupling (LC) effect to the limiting cell conversion efficiency of multijunction solar cells (MJSCs) has been investigated. For this purpose, the laser beam induced current distribution maps of the limiting bottom cell have been acquired experimentally under varying middle-to-bottom cell LC efficiencies. The minimum and the maximum LC efficiencies demonstrated were 8.5% and 69%, respectively. To further analyze the measurement results, a quasi-two-dimensional simulation model considering the spatially nonuniform nature of the LC effect has been developed. A good agreement between the simulation and the measurement results suggests that the nonuniform LC current distribution is induced by optical phenomena such as photon escape and internal reflection. This nonuniformity then causes the absolute conversion efficiency of the limiting cell to be reduced by 1.35% at maximum LC efficiency. This reduction, when suppressed, can yield higher limiting cell conversion efficiency, which in turn may improve the overall MJSC conversion efficiency.
For intermediate band solar cells, the control of the carrier filling ratio in intermediate band is important to achieve high efficiency. We have investigated the effect of carrier doping of InAs/GaAs quantum dots (QDs) with Si and sunlight concentration on the quantum dots solar cell (QDSC) characteristics. The prefilling by Si doping of InAs/GaAs QDs was performed using two methods: modulation or δ-doping and direct doping. A gradual recovery in the open-circuit voltage with increasing Si doping concentration was observed, and it suggested a decrease of recombination via Si-doped QD states. Under high-concentrated sunlight illumination, QD states were additionally filled with photocarriers, and the open-circuit voltage increased nonlinearly with concentration ratio in both the nondoped and Si-doped QDSCs.
The subband features E‒ and E+ for the conduction band of III-V dilute nitride alloys make them promising for intermediate band solar cell application. However, presence of bandgap states can limit the two-step photon absorption activity, a necessary requirement for IBSC functionality. A model analysis is performed to characterize the density of states. The sub-band tails states are characterized using a temperature-dependent map of photo-modulated reflectance spectroscopy for GaNAs thin films grown on GaAs substrates using molecular beam epitaxy. The effect of indium and antimony incorporation on the subband features were investigated. Marked improvements in the thin films were observed both for the lower (E‒) and the upper (E+) conduction bands (CB) when In was introduced with marginal enhancement by Sb. These improvements are associated with suppression of tail states below both the E‒ and E+ bands. Sb rather mainly plays a surfactant role improving the abruptness of the GaNAs/GaAs hetero-interface.
Double resonant tunneling barriers are considered for an application as energy selective contacts in hot carrier solar cells. Experimental symmetric and asymmetric double resonant tunneling barriers are realized by molecular beam epitaxy and characterized by temperature dependent current-voltage measurements. The negative differential resistance signal is enhanced for asymmetric heterostructures, and remains unchanged between low- and room-temperatures. Within Tsu-Esaki description of the tunnel current, this observation can be explained by the voltage dependence of the tunnel transmission amplitude, which presents a resonance under finite bias for asymmetric structures. This effect is notably discussed with respect to series resistance. Different parameters related to the electronic transmission of the structure and the influence of these parameters on the current voltage characteristic are investigated, bringing insights on critical processes to optimize in double resonant tunneling barriers applied to hot carrier solar cells.
Multi-stacked quantum dot solar cell (QDSC) is a promising candidate for intermediate band solar cell, which can exceed thermodynamic efficiency limit of single-junction solar cells. In recent years, lots of effort has been made to evaluate and understand the photo-carrier response of two-step photon absorption in QDSCs. One crucial issue is to suppress thermal excitation of photo-carriers out of QDs, which obscures the QD filling under quasi-equilibrium at operation conditions. We have investigated infrared photocurrent spectra of the QD states to conduction band (CB) transition by using Fourier transform infrared (FTIR) spectroscopy. Multi-stacked In(Ga)As QDSCs with different barrier materials, such as GaAs, GaNAs, GaAsSb, and AlGaAs, were investigated. The IR absorption edge of the QD to CB transition was evaluated at low temperature by analyzing the low energy tail of the FTIR spectra. The threshold temperature of the two-step photon absorption in In(Ga)As QDSCs was determined by observing temperature dependence of the IR photo-response. A universal linear relationship between the threshold temperature and the IR absorption edge was obtained in In(Ga)As QDSCs with varied barrier materials. The threshold temperature of 295 K was predicted for the absorption edge at 0.459 eV by extrapolating the linear relationship. It reveals strategy for cell optimization to achieve efficient two-step photon absorption at ambient conditions.
Having shown some demonstration of two photon absorption and multiband emission processes in quantum dots (QD), multiquantum wells (MQW), and highly mismatched alloys, intermediate band solar cells are currently the subject of numerous studies. To better understand the underlying mechanisms, our objective is to experimentally probe the multiband operation of this device. We used photoluminescence recorded with a calibrated hyperspectral imager which provides spectrally resolved images with a spatial resolution of 2 μm and spectral resolution of 2 nm on proof of concept QD and MQW solar cells samples. Device emission can be described with the generalized Planck’s law from which the quasi-Fermi level splitting of the three bands can be determined. The advantage of the technique is that it can be used to investigate the intermediate band material without the need to make contacts or a full device structure. We also discuss the usefulness of a dual-beam method.
Intermediate band solar cell (IBSC) is a promising concept to achieve next generation high-efficiency solar cells by producing the gain in photocurrent via two-step photon absorption while preserving the output voltage as of the host materials. Quantum dot (QD) superlattice is a widely studied candidate to implement the IB in real devices. In this paper, a missing transition from the IB to the conduction band (CB) has been investigated by applying extreme broadband photocurrent spectroscopy extended to mid-infrared (IR) region. In both direct and delta Si-doped InAs QDSCs, photocurrent signals were observed at the short-circuit condition at low temperature solely with sub-bandgap mid-IR photo-irradiation. On the other hand, in an undoped QDSC, no significant signal was obtained. Furthermore, the mid-IR signal was reduced by decreasing the modulation frequency and turned to be zero at DC detection. We ascribe this to the displacement photocurrent by the inter-subband transition of thermal equilibrium carriers in QDs.
Transmission-type concentrator photovoltaic (CPV) systems are a potential candidate to achieve high efficiency and low cost solar energy. The use of optical elements in these systems creates reflection losses of incoming solar energy that account for about 8% to 12% depending on the optical design. In order to reduce these losses, we have nanostructured the air/optical-elements’ interfaces by using plasma etching methods on the Fresnel lens made of poly(methyl methacrylate) (PMMA) and the homogenizer made of glass. On flat PMMA and glass substrates, transmittance enhancement measurements are in agreement with relative Jsc gains. The field test results using a CPV module with all textured optical-elements’ interfaces achieved 8.0% and 4.3% relative Jsc and efficiency gains, respectively, demonstrating the potential of this approach to tackle the reflection losses.
To realize high efficiency solar cells, new concepts beyond the Shockley-Queisser limit are widely investigated. The
intermediate band solar cell (IBSC) is one of the candidate concepts. From the importance of device physics, we have
developed a device simulator for IBSCs. For device simulation of IBSC, the Poisson equation, carrier continuity
equations of electrons in the conduction band (CB) and the valance band (VB) and balanced equation of IB state
electrons must be solved self-consistently. The simulation methods can clarify the intrinsic device behavior of IBSCs
which cannot be investigated by the detailed balance model. For example, by the existence of electrons trapped in IB
states, electrostatic potential along the depth direction of the solar cells is strongly modified from the equilibrium under
illumination of sunlight. This potential change is strongly related to its absorption property of sunlight. And the doping
to IB region can enhance short circuit current density via IB states. Under larger concentration, this doping effect is
decreased by the photofilling effects in the radiative limit. Absorption coefficients of each band-to-band transition are
decided by the semiconductor materials and fundamental physics. These limitations make the different spectra and
values from ideal treatments and decide the maximum efficiency of the IBSC. In this work, we present the fundamental
properties and suggestions to approach the high efficiency IBSC operations as a device.
Semiconductor quantum dots (QDs) grown using self-assembly techniques in the Stranski-
Krastanov (S-K) mode are expected to be useful for high-performance optical devices such as QD
lasers. A significant amount of research has been carried out on the development of highperformance
QD lasers because they offer the advantages of a low threshold current, temperature
stability, high modulation bandwidth, and low chirp. To realize these high-performance devices, the
surface QD density should be increased by fabricating a stacked structure. We have developed a
growth method based on a strain-compensation technique that enables the fabrication of a high
number of stacked InAs QD layers on an InP(311)B substrate. In this study, we employed the
proposed method to fabricate QD laser diodes consisting of highly stacked QD layers and
investigated the dependence of the diode parameters on the stacking layer number. We fabricated
QD laser diodes with 5, 10, 15, and 20 QD layers in the active region. All of the laser diodes
operated at around 1.55 μm at room temperature, and their threshold currents showed clear
dependence on the stacking layer number. Laser diodes with more than 10 QD layers showed
sufficient gain, i.e., the threshold currents decreased with a decrease in the cavity length. On the
other hand, for laser diodes with less than 10 QD layers, the threshold currents increased with a
decrease in the cavity length.
We review the properties of ordered InGaAs QDs arrays, which are formed by self-organization mechanism on GaAs (311)B substrate. We show that the QDs exhibit remarkably different characteristics compared to the more commonly studied InAs QDs grown on GaAs (00 1) substrate. In addition, some recent results of our strain-compensation growth of InAs QDs stack structures on InP (311)B substrate are presented. The stacked InAs QDs on InP (311)B substrate show strong photoluminescence emission at > 1.55µm at room temperature, which is thereby considered to be promising for the next generation fiber-optic communication devices.
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