Prof Henry Snaith FRS

Abstract:

The energy costs associated with separating tightly bound excitons (photoinduced electron-hole pairs) and extracting free charges from highly disordered low-mobility networks represent fundamental losses for many low-cost photovoltaic technologies. We report a low-cost, solution-processable solar cell, based on a highly crystalline perovskite absorber with intense visible to near-infrared absorptivity, that has a power conversion efficiency of 10.9% in a single-junction device under simulated full sunlight. This "meso- superstructured solar cell" exhibits exceptionally few fundamental energy losses; it can generate open-circuit photovoltages of more than 1.1 volts, despite the relatively narrow absorber band gap of 1.55 electron volts. The functionality arises from the use of mesoporous alumina as an inert scaffold that structures the absorber and forces electrons to reside in and be transported through the perovskite.

Abstract:

The energy costs associated with separating tightly bound excitons (photoinduced electron-hole pairs) and extracting free charges from highly disordered low-mobility networks represent fundamental losses for many low-cost photovoltaic technologies. We report a low-cost, solution-processable solar cell, based on a highly crystalline perovskite absorber with intense visible to near-infrared absorptivity, that has a power conversion efficiency of 10.9% in a single-junction device under simulated full sunlight. This "meso-superstructured solar cell" exhibits exceptionally few fundamental energy losses; it can generate open-circuit photovoltages of more than 1.1 volts, despite the relatively narrow absorber band gap of 1.55 electron volts. The functionality arises from the use of mesoporous alumina as an inert scaffold that structures the absorber and forces electrons to reside in and be transported through the perovskite.

Abstract:

We observe a strong "light-soaking" effect in SnO 2 based solid-state dye-sensitized solar cells (SDSCs). Both with and without the presence of UV light, the device's short-circuit photocurrent and efficiency increase significantly over 20-30 minutes, until steady-state is achieved. We demonstrate that this is not due to improved charge collection and investigate the charge generation dynamics employing optical-pump terahertz-probe spectroscopy. We observe a monotonic speeding-up of the generation of free-electrons in the SnO 2 conduction band as a function of the light-soaking time. This improved charge generation can be explained by a positive shift in the conduction band edge or, alternatively, an increase in the density of states (DoS) at the energy at which photoinduced electron transfer occurs. To verify this hypothesis, we perform capacitance and charge extraction measurements which indicate a shift in the surface potential of SnO 2 of up to 70 mV with light soaking. The increased availability of states into which electrons can be transferred justifies the increase in both the charge injection rate and ensuing photocurrent. The cause for the shift in surface potential is not clear, but we postulate that it is due to the photoinduced charging of the SnO 2 inducing a rearrangement of charged species or loss of surface oxygen at the dye-sensitized heterojunction. Understanding temporally evolving processes in DSCs is of critical importance for enabling this technology to operate optimally over a prolonged period of time. This work specifically highlights important changes that can occur at the dye-sensitized heterojunction, even without direct light absorption in the metal oxide. © 2012 The Royal Society of Chemistry.

Abstract:

The coating of n-type mesoporous metal oxides with nanometer thick dielectric shells is a route that has proven to be successful at enhancing the efficiency of some families of dye-sensitized solar cells. The primary intention is to introduce a "surface passivation layer" to inhibit recombination between photoinduced electrons and holes across the dye-sensitized interface. However, the precise function of these dielectric interlayers is often ambiguous. Here, the role of a thin MgO interlayer conformally deposited over mesoporous SnO 2 in liquid electrolyte and solid-state dye-sensitized solar cells is investigated. For both families of devices the open-circuit voltage is increased by over 200 mV; however, the short-circuit photocurrent is increased for the solid-state cells, but reduced for the electrolyte based devices. Through electronic and spectroscopic characterization we deduce that there are four distinct influences of the MgO interlayer: It increases dye-loading, slows down recombination, slows down photoinduced electron transfer, and results in a greater than 200 mV shift in the conduction band edge, with respect to the electrolyte redox potential. The compilation of these four factors have differing effects and magnitudes in the solid-state and electrolyte DSCs but quantitatively account for the difference in device performances observed for both systems with and without the MgO shells. To the best of our knowledge, this is the most comprehensive account of the role of dielectric shells in dye-sensitized solar cells and will enable much better interfacial design of photoelectrodes for DSCs. © 2012 American Chemical Society.