Abstract

Organic solar cells (OSCs) are promising alternatives to the conventional inorganic solar cells due to their low-cost processing and compatibility with flexible substrates. The development of low band-gap polymer, e.g., poly-[[4,8-bis[(2-ethylhexyl)oxy]benzo[1,2–b:4,5–b’]dithiophene-2,6-diyl] [3-fluoro-2-[(2-ethylhexyl)carbonyl]thieno[3]thiophenediyl]] (PTB7), increases the power conversion efficiency (PCE) in the last decade. Here, we investigated the interrelation between the instantaneous carrier density (n) per donor (D)/acceptor (A) interface area and the carrier density (ncollected) collected as photocurrent in PTB7/C70 heterojunction (HJ) device. By means of the time-resolved spectroscopy, we confirmed that the exciton—to—carrier conversion process takes place within ~1 ps at the D/A interface of the PTB7/C70 HJ device. We further determined the absolute magnitude of n by combination of the time-resolved and electrochemical spectroscopies. We found that the carrier recombination becomes dominant if n exceeds a critical concentration (nc = 0.003 carriers/nm−2). We confirmed that a similar behaviors is observed in the PTB7/[6,6]-phenyl C71-butyric acid methyl ester (PC71BM) bulk heterojunction (BHJ) device. Our quantitative investigation based on the HJ device demonstrates that the fast carrier escape from the D/A interface region is indispensable for high PCE, because the carrier accumulation nonlinearly accelerates the carrier recombination process.

Highlights

  • The time-resolved spectroscopy was performed in a pump-probe configuration

  • The pump pulse at 400 nm was generated as the second harmonics of a regenerative amplified Ti: sapphire laser in a β -BaB2O4 (BBO) crystal

  • The frequency of the pump pulse was decreased by half (500 Hz) to provide “pump-on” and “pump-off ” conditions

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Summary

Introduction

The time-resolved spectroscopy was performed in a pump-probe configuration. The pump pulse at 400 nm was generated as the second harmonics of a regenerative amplified Ti: sapphire laser in a β -BaB2O4 (BBO) crystal. The pulse width, repetition rate, and pulse energy were 100 fs, 1000 Hz, and 27 μ J/cm[2] respectively. The frequency of the pump pulse was decreased by half (500 Hz) to provide “pump-on” and “pump-off ” conditions. A white probe pulse, generated by self-phase modulation in a sapphire plate was focused on the sample with the pump pulse. The spot sizes of the pump and probe pulses were 4.0 and 2.1 mm in diameter, respectively. The differential absorption (Δ OD) spectrum is expressed as -log(Ion/Ioff) , where Ion and Ioff are the transmission spectra under the pump-on and pump-off conditions, respectivel

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