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Materials with switchable absorption properties have been widely used for smart window applications to reduce energy consumption and enhance occupant comfort in buildings. In this work, we combine the benefits of smart windows with energy conversion by producing a photovoltaic device with a switchable absorber layer that dynamically responds to sunlight.
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Upon illumination, photothermal heating switches the absorber layer—composed of a metal halide perovskite-methylamine complex—from a transparent state (68% visible transmittance) to an absorbing, photovoltaic colored state (less than 3% visible transmittance) due to dissociation of methylamine. After cooling, the methylamine complex is re-formed, returning the absorber layer to the transparent state in which the device acts as a window to visible light. The thermodynamics of switching and performance of the device are described. This work validates a photovoltaic window technology that circumvents the fundamental tradeoff between efficient solar conversion and high visible light transmittance that limits conventional semitransparent PV window designs. Myriad materials that adopt the oxide and halide forms of the perovskite crystal structure are known to readily accommodate intercalating species to form a rich array of unique compounds. The intercalated compounds are stabilized by the formation of ionic, charge-transfer complex, van der Waals, and π-stacked fluorylaryl-aryl bonds. The weaker of these bonds are reversibly formed and dissociated with small energy input.
Lead halide perovskites (APbX 3, where A is an organic or alkali metal cation and X is a halide) have demonstrated unprecedented potential as a photovoltaic (PV) absorber and have also shown to reversibly form hydrates, and other compounds stabilized by charge-transfer complex bonds with nitrogen-, and oxygen-donor molecules. In this work, we leverage the low formation/dissociation energy of the methylammonium lead iodide-methylamine complex (CH 3NH 3PbI 3. xCH 3NH 2) to demonstrate a cohesive switchable PV window that adapts its absorption properties to solar conditions without pairing separate electrochromic and PV devices. The PV window device utilizes solar photothermal heating to dissociate CH 3NH 2 from the CH 3NH 3PbI 3 layer, thereby switching from its complexed, bleached (visibly transparent) state to its dissociated, colored (visibly opaque) state. The device is sealed in a closed atmosphere of dilute (2%) CH 3NH 2 gas in argon and thus returns to its complexed, bleached state upon removing the solar irradiation and cooling to re-form CH 3NH 3PbI 3. xCH 3NH 2. This phenomenon circumvents the fundamental tradeoff observed in conventional semitransparent PV window designs, which sacrifice solar-to-electricity power conversion efficiency (PCE) for the high visible light transmittance critical for window performance.
Coupled with the cost-effective, scalable solution-phase processing of lead halide perovskites, this technology widely expands the opportunity for energy-efficient PV deployment beyond solar farms and rooftops to glass building facades and vehicles. Switchable PV window design and performance The switchable PV window device design and reversible switching mechanism is shown in Fig. 1a, and fabrication details are outlined in the Methods section. Briefly, CH 3NH 3PbI 3 was deposited using established methods 26 on titanium dioxide (TiO 2) as the electron transport layer and fluorine-doped tin oxide (FTO) as the transparent bottom contact.
In order to demonstate switching in a PV device, a number of hole transport and top contact layers were explored. Four complementary layers were required in order to provide the necessary combination of high electrical conductivity, favorable energetic alignment with the CH 3NH 3PbI 3 layer, significant transparency in the visible portion of the solar spectrum, and permeability to CH 3NH 2 gas (Supplementary Table and Supplementary Fig. ). We first coated the CH 3NH 3PbI 3 with a bilayer of single-walled carbon nanotubes (SWCNTs). SWCNTs wrapped in poly(3-hexylthiophene) (SWCNT/P3HT) provide favorable energetic alignment to the CH 3NH 3PbI 3 for hole extraction, and a second layer of electronically sorted SWCNTs doped with 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (SWCNT F4TCNQ) was spray-coated to improve lateral electrical transport to the top contact.
This layer was then chemically treated with trifluoroacetic acid after deposition to de-polymerize and remove the wrapping polymer to enhance electrical conductivity between the SWCNTs. The device was completed by laminating Ni micromesh coated with poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS), an electrically conductive polymer and effective hole transport layer (Supplementary Fig. ), doped with d-sorbitol that serves as an “electric glue”. Optical and scanning electron microscopy characterization of the device stack is shown in Supplementary Fig. Composition and performance of switchable photovoltaic window devices. A Schematic of PV window device architecture and switching process. B Transmittance of PV devices in the bleached (red) and colored (blue) states as a function of wavelength. C Current density as a function of voltage of the champion switchable PV device in the dark (dashed) and under illumination (solid).
The inset table shows PV performance metrics of the device before being bleached. D Short-circuit current as a function of time for 20 cycles of 3 min of illumination followed by 5 min of cooling in the dark. E Short-circuit current as a function of time for the first illumination cycle. The optical images were extracted from Supplementary Movie 1 to show the transition from bleached to colored and back to bleached at the indicated times during the cycling process. Figure shows the transmittance of the full device stack spanning the UV to IR portions of the electromagnetic spectrum.
The visible portion is highlighted to illustrate reversible switching in this region of the spectrum. The device is highly absorbing in the visible portion in its colored state with an average visible light transmittance of 3%. The visible light transmittance increases to 68% when in the bleached state. The observed decrease in transmittance for both colored and bleached states of the device in the infrared region is due to thin film interference and FTO absorption. Reduced transmittance in this range is desirable for the thermal performance of windows and is the primary function of low-emissivity films used in current high-performance window technology. Figure shows the current density–voltage curve scanned from high to low positive voltage of the switchable PV device in the dark (dashed) and under 1-sun illumination (solid).
The champion device exhibits a PCE of 11.3% with an average of 10.3 ± 0.9% in five devices. A table with the performance metrics of the champion device are inset to Fig.
For comparison, control devices were fabricated with Li-doped 2,2′,7,7′-tetrakis( N,N-di- p-methoxyphenylamine)-9,9′-spirobifluorene (spiro-OMeTAD) as the hole transport layer and gold as the top contact to mimic conventional CH 3NH 3PbI 3-based PV devices. The control devices, which do not exhibit dynamic switching behavior since gold is not permeable to CH 3NH 2 gas, exhibit an average PCE of 16.3 ± 0.1%. The short-circuit current density ( J SC) of 21.2 mA cm −2 for the champion switchable device is identical to the control device, whereas the open-circuit voltage ( V OC) and fill factor (FF) are moderately reduced in the switchable PV window device.
Additional characterization of the switchable device (forward and reverse voltage sweeps, stabilized power output, and external quantum efficiency) is included in Supplementary Figs. –. We next demonstrate dynamic photothermal modulation of the PV window device while generating photocurrent under illumination.
Figure is a plot of short-circuit current output as a function of time for a device enclosed in an atmosphere of 2% CH 3NH 2 gas balanced with argon to atmospheric pressure. The initial complexed, bleached device was held at ambient temperature from time zero until the device was exposed to solar-simulated illumination at 30 s, indicated by gray boxes in Fig. Current was immediately observed from the device after illumination, which increased and began to plateau after 1 min.
The current dropped to zero when the lamp was turned off after 3 min. The lamp was turned back on after 5 min, and this cycle was repeated 20 times in the closed atmosphere (no additional CH 3NH 2 gas was introduced) to demonstrate repeated cycling.
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Optical images extracted from Supplementary Movie 1 in Fig. Show reversible color changes correlate with current during the cycling process. The exception to this correlation occurred during the initial stages of each illumination cycle, when the device produced current but did not exhibit visible color. After illumination, the current increased at a near-linear rate until 40 s of illumination when the current increased at a higher rate. This sharp rise in current was sustained for another 40 s and was accompanied by a visible color change. After 3 min, the color gradually changed from yellow-orange to dark red, corresponding to complete switching after 3 min. When the lamp was turned off, the device cooled in the chamber, which caused CH 3NH 2 gas to intercalate back into the CH 3NH 3PbI 3 layer to re-form the CH 3NH 3PbI 3.
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xCH 3NH 2 complex and return the device to the bleached state after 3 min. The maximum current decreased monotonically from nearly 1 to 0.18 mA after 20 cycles. Supplementary Fig. Provides the same analysis as Fig. For the 15th cycle, which exhibits a similar kinetic profile but at a lower current output. Whereas decreased current output may be due to delamination or degradation of transport layers, optical images show inconsistent coloration across the device compared to that following the first cycle, which suggests degradation or morphological changes to the CH 3NH 3PbI 3 layer. The source of decreased current after cycling is discussed at length in a following section.
Thermodynamics of complex formation and dissociation We explain the observed reversible complex formation and dissociation process that drives photothermal switching of the PV window device using a simple thermodynamic model. The complexed state is stabilized by weak hydrogen bonds between CH 3NH 2 and the organic sublattice of CH 3NH 3PbI 3, and its conversion to the dissociated state is dependant on the partial pressure ( P) of CH 3NH 2 gas ( g) and temperature ( T) of the solid ( s) phase described. (1) The methylamine complex CH 3NH 3PbI 3. xCH 3NH 2 has been shown to form a solid at lower x values ( x ≈ 1, 2 based on prior work on hydrates ) and a second glassy solvate (liquid) phase at higher values of x.
Here we will focus on the solid complex observed at low CH 3NH 2 pressures that keeps x low and the complex in the solid regime. As demonstrated in previous work on thermochemical energy storage, the thermodynamics of Eq. are described by the Clausius–Clapeyron relation where the volume is constant and assumed to be equal to the volume of gas. (2) where R is the ideal gas constant (8.31 mol –1 K –1), Δ G i, Δ H i, and Δ S i are the Gibb’s energy change, enthalpy change, and entropy change, respectively. The subscript (i ) corresponds to the formation of the complexed bleached state or dissociated colored state. Contributions to Δ G i thus include complex formation and dissociation, ionic bond formation or destruction in the CH 3NH 3PbI 3 lattice, sublimation or condensation, and mixing. Lines of constant Δ G Colored and Δ G Bleached are shown in the Clausius–Clapeyron diagram, which plots CH 3NH 2 gas pressure vs.
Reciprocal temperature (Fig. ). The lines are separated by a regime of pseudo-equilibrium, which depends on the rates of the forward and reverse reactions. If one of the free parameters (e.g., P) is fixed, the variance is zero and phase transition occurs at a certain temperature T. The line from point A to point B shows the isothermal transition from the colored state (CH 3NH 3PbI 3( s)+ xCH 3NH 2( g)) to the bleached state (CH 3NH 3PbI 3. xCH 3NH 2( s)) at room temperature ( T 0). P Min is the minimum pressure of CH 3NH 2 gas needed for full transition to the bleached state.
The line from B to C shows an isobaric transition back to the phase-segregated state, which requires a minimum temperature T Min. For window applications, the transition temperature must be below what can be practically attained by solar photothermal heating. This is typically less than 75 °C for most climates, so this temperature defines T Solar (shaded region in Fig. ). The switching temperature of conventional vanadium dioxide thermochromic window technology is thus engineered closer to 45 °C for practical application. Thermodynamic model of complex formation and dissociation.
The Clausius–Clapeyron diagram describes the pressure–temperature ( P–T) dependence of CH 3NH 3PbI 3. xCH 3NH 2( s) formation and dissociation into CH 3NH 3PbI 3(s) + CH 3NH 2(g). Points labeled A—E are described in the text.
P Min indicates the minimum pressure needed for CH 3NH 3PbI 3. xCH 3NH 2 formation at room temperature ( T 0). T Min is the minimum temperature needed for phase transition at P Min. The shaded region indicates temperatures attainable by solar photothermal heating up to the maximum temperature, T Solar. The yellow region indicates the necessary phase space for achieving switchable PV with solar photothermal heating.