Wide-bandgap mixed-halide perovskite solar cells(WBG-PSCs)are promising top cells for efficient tandem photovoltaics to achieve high power conversion efficiency(PCE)at low cost.However,the open-circuit voltage(V_(OC))...Wide-bandgap mixed-halide perovskite solar cells(WBG-PSCs)are promising top cells for efficient tandem photovoltaics to achieve high power conversion efficiency(PCE)at low cost.However,the open-circuit voltage(V_(OC))of WBG-PSCs is still unsatisfactory as the V_(OC)-deficit is generally larger than 0.45 V.Herein,we report a buried interface engineering strategy that substantially improves the V_(OC)of WBG-PSCs by inserting amphiphilic molecular hole-selective materials featuring with a cyanovinyl phosphonic acid(CPA)anchoring group between the perovskite and substrate.The assembly and redistribution of CPA-based amphiphilic molecules at the perovskite-substrate buried interface not only promotes the growth of a low-defect crystalline perovskite thin film,but also suppresses the photo-induced halide phase separation.The energy level alignment between wide-bandgap perovskite and the hole-selective layer is further improved by modulating the substituents on the triphenylamine donor moiety(methoxyls for MPA-CPA,methyls for Me PA-CPA,and bare TPA-CPA).Using a 1.68 e V bandgap perovskite,the Me PA-CPA-based devices achieved an unprecedentedly high V_(OC)of 1.29 V and PCE of 22.3%under standard AM 1.5 sunlight.The V_(OC)-deficit(<0.40 V)is the lowest value reported for WBG-PSCs.This work not only provides an effective approach to decreasing the V_(OC)-deficit of WBG-PSCs,but also confirms the importance of energy level alignment at the charge-selective layers in PSCs.展开更多
We present here a systematically theoretical study on the nonlinearities and their structure-property relationship of cyanovinyl-substituted donor-acceptor molecules by virtue of semiempirical PM3/AM1-FF approach. Goo...We present here a systematically theoretical study on the nonlinearities and their structure-property relationship of cyanovinyl-substituted donor-acceptor molecules by virtue of semiempirical PM3/AM1-FF approach. Good consistency between measured and calculated hyperpolarizabilities is obtained. Results show that conformation has a significant effect on hyperpolarizabilities. The torsion angle change between two conjugated parts of the molecular systems can substantially alter the nonlinearities. The total amount of charge transfer difference from donor to acceptor has been introduced to understand the microscopic nature of the nonlinear optical properties for the title molecules. General guidelines may be sought out in the search of molecules with large values of beta. Some molecules with large molecular hyperpolarizabilities can be predicted by the optimization for the longer pi-electron systems with both acceptor and donor groups.展开更多
基金supported by the National Natural Science Foundation of China(22179037)Shanghai pilot program for Basic Research(22TQ1400100-1)+3 种基金Shanghai Municipal Science and Technology Major Project(2018SHZDZX03,21JC1401700)the Programmer of Introducing Talents of Discipline to Universities(B16017)the Fundamental Research Funds for the Central Universitiessupport from Royal Society of Chemistry(R23-0749928359)。
文摘Wide-bandgap mixed-halide perovskite solar cells(WBG-PSCs)are promising top cells for efficient tandem photovoltaics to achieve high power conversion efficiency(PCE)at low cost.However,the open-circuit voltage(V_(OC))of WBG-PSCs is still unsatisfactory as the V_(OC)-deficit is generally larger than 0.45 V.Herein,we report a buried interface engineering strategy that substantially improves the V_(OC)of WBG-PSCs by inserting amphiphilic molecular hole-selective materials featuring with a cyanovinyl phosphonic acid(CPA)anchoring group between the perovskite and substrate.The assembly and redistribution of CPA-based amphiphilic molecules at the perovskite-substrate buried interface not only promotes the growth of a low-defect crystalline perovskite thin film,but also suppresses the photo-induced halide phase separation.The energy level alignment between wide-bandgap perovskite and the hole-selective layer is further improved by modulating the substituents on the triphenylamine donor moiety(methoxyls for MPA-CPA,methyls for Me PA-CPA,and bare TPA-CPA).Using a 1.68 e V bandgap perovskite,the Me PA-CPA-based devices achieved an unprecedentedly high V_(OC)of 1.29 V and PCE of 22.3%under standard AM 1.5 sunlight.The V_(OC)-deficit(<0.40 V)is the lowest value reported for WBG-PSCs.This work not only provides an effective approach to decreasing the V_(OC)-deficit of WBG-PSCs,but also confirms the importance of energy level alignment at the charge-selective layers in PSCs.
基金Project supported by the State Science and Technology Commission and the National Natural Science Foundation of China.
文摘We present here a systematically theoretical study on the nonlinearities and their structure-property relationship of cyanovinyl-substituted donor-acceptor molecules by virtue of semiempirical PM3/AM1-FF approach. Good consistency between measured and calculated hyperpolarizabilities is obtained. Results show that conformation has a significant effect on hyperpolarizabilities. The torsion angle change between two conjugated parts of the molecular systems can substantially alter the nonlinearities. The total amount of charge transfer difference from donor to acceptor has been introduced to understand the microscopic nature of the nonlinear optical properties for the title molecules. General guidelines may be sought out in the search of molecules with large values of beta. Some molecules with large molecular hyperpolarizabilities can be predicted by the optimization for the longer pi-electron systems with both acceptor and donor groups.
