Size Dependence of Ultrafast Electron Transfer from Didodecyl Dimethylammonium Bromide-Modified CsPbBr3 Nanocrystals to Electron Acceptors

ABSTRACT

Charge transfer efficiencies in all-inorganic lead halide perovskite nanocrystals (NCs) are crucial for applications in photovoltaics and photocatalysis. Herein, CsPbBr₃ NCs with different sizes are synthesized by varying the ligand contents of didodecyl dimethylammonium bromide at room temperature. Adding benzoquinone (BQ) molecules leads to a decrease in the PL intensities and PL decay times in NCs. The electron transfer (ET) efficiency (ηET) increases with NC size in complexes of CsPbBr₃ NCs and BQ molecules (NC-BQ complexes), when the same concentration of BQ is maintained, as investigated by transient photobleaching and photoluminescence spectroscopies. Controlling the same number of attached BQ acceptor molecules per NC induces the same ηET in NC-BQ complexes even though with different NC sizes. Our findings provide new insights into ultrafast charge transfer behaviors in perovskite NCs, which is important for designing efficient light energy conversion devices.

CsPbBr3 NCs with different concentrations of DDAB ligands were synthesized on the basis of the reported literature at room temperature under an air atmosphere.17 Adding the DDAB ligands in amounts of 0.05, 0.1, 0.3, and 0.5 mmol can significantly affect the absorption and PL emission peaks of DDAB-modified CsPbBr3 NCs. The first exciton absorption peaks of as-grown CsPbBr3 NCs are blue-shifted from 509 to 477 nm with an increase in DDAB ligand concentration, and the corresponding PL emission peaks are blue-shifted from 512 to 480 nm, as shown in panels a and b, respectively, of Figure 1. In comparison, an only ∼6 nm PL peak shift happened upon addition of different contents of conventional OAm ligands (see Figure S1). It is known that the shifted emission peak is correlated with the NC size and bandgap of CsPbBr3 NCs,15,32 indicating that DDAB ligands have better size control for CsPbBr3 NCs compared to conventional OAm ligands when using room-temperature methods. The detailed synthesis procedures can be found in the experimental section in the Supporting Information.

Figure 2. PL spectra of as-grown CsPbBr3 NCs (normalized solid lines) and NC-BQ complexes (dashed lines) for different BQ concentration of (a) 0.46 mM and (b) 4.63 mM (b).

Figure 3. PL decay curves of as-grown CsPbBr3 NCs and NC-BQ complexes with different sizes of NCs. The BQ concentrations are 0.46 and 4.63 mM in the NC-BQ complexes. The initial PL intensities are normalized to the same values.

Figure 4. BQ concentration-dependent PL intensity for CsPbBr3 NC sizes of (a) 13.3 nm and (b) 6.3 nm. Integrated PL intensities (black lines) and the m values (red lines) as a function of BQ concentrations for CsPbBr3 NC sizes of (c) 13.3 nm and (d) 6.3 nm.

Figure 5. (a) PL spectra of as-grown CsPbBr3 NCs with NCs sizes of 6.3 and 13.3 nm and the corresponding NC-BQ complexes with different m values. Time-resolved PL spectra of as-grown CsPbBr3 NCs and NC-BQ complexes with different m values with NC sizes of (b) 13.3 nm and (c) 6.3 nm. (d) ηET as a function of m value.

To further demonstrate the interfacial ET mechanism, the relationship between BQ concentrations and PL intensities of CsPbBr₃ NCs with different sizes is investigated. The PL spectra of 13.3 and 6.3 nm as-grown CsPbBr₃ NCs and their corresponding NC-BQ complexes with different concentrations of BQ are shown in panels a and b of Figure 4. For 13.3 and 6.3 nm NCs, increasing the BQ concentration decreases the PL intensity. The adsorption of BQ molecules onto NCs surfaces is governed by the Langmuir adsorption isotherm and follows a Poissonian distribution. The integrated PL intensities and the formation of m values for 13.3 and 6.3 nm NCs as a function of BQ concentrations are plotted in panels c and d of Figure 4 (detailed calculation information can be found in the Supporting Information). As shown in panels c and d of Figure 4, with an increase in the BQ concentration (thus the m value), the integrated PL intensities decrease for both large and small NC-BQ complexes. Note that, when the NC size is decreased along with an increased E_g, the driving force increases in NC-BQ complexes, which accelerates the ET process. However, at the same BQ concentrations, the m value is smaller in 6.3 nm NCs than in 13.3 nm NCs, which plays the dominant role in the ET processes, resulting in longer ET times and thus longer decay times in 6.3 nm NCs as shown in Figure 3.

Further investigations of ultrafast charge dynamics in different-sized NCs with and without BQ but with the same m value are measured by using transient photobleaching spectra (or time-resolved differential transmission measure-ments).40 The wavelengths of pump and probe pulses are set at the first exciton transition for each sample of CsPbBr3 NCs and NC-BQ complexes. For as-grown CsPbBr3 NCs with sizes of 13.3 and 6.3 nm, a pump fluence (Fp) of 20 μJ/cm2 produces an average of 0.74 and 0.038 electron−hole pair per NC (termed ⟨N⟩ below), respectively41 (detailed calculation information can be found in the Supporting Information). Figure 6 shows the transient photobleaching dynamics of as-grown CsPbBr3 NCs with sizes of 13.3 and 6.3 nm and their corresponding NC-BQ complexes with the same m value. All of the transient photobleaching dynamics exhibit two decay components, fast and slow decay (τTA1 and τTA2, respectively). Figure 6a shows the transient photobleaching dynamics of as-grown NCs with an L of 13.3 nm, showing the fast and slow decay processes with a τTA1 of 300 ps and a τTA2 of 1130 ps. The fast decay component can be ascribed to the electron and/or hole trapping processes, while the slow decay component in photobleaching measurement is in accordance with the detected fast PL decay component and can be attributed to the nonradiative recombination processes.29 The photobleach-ing dynamic in 13.3 nm NC-BQ complexes also shows a fast decay component τTA1 of 185 ps and a slow decay component τTA2 of 1000 ps. The shortening of τTA1 and τTA2 after adding BQ molecules, compared with that of in as-grown NCs, can be attributed to ET from the conduction bands of CsPbBr3 NCs to LUMO of BQ electron acceptors. The transfer efficiencies of the fast and slow processes are 38% and 12%, respectively. As shown in Figure 6b, as-grown CsPbBr3 NCs and NC-BQ complexes with a size of 6.3 nm exhibit similar phenomena but with different decay time constants, compared with that in 13.3 nm NCs. The times of fast and slow decay processes are as follows: τTA1 = 120 ps and τTA2 = 800 ps in 6.3 nm as-grown NCs, which is faster than that in 13.3 nm NCs. For the 6.3 nm NC-BQ complexes, the lifetimes of fast and slow decay components change to a τTA1 of 71 ps and a τTA2 of 700 ps. The two processes show transfer efficiencies of 41% and 13%, respectively. The detailed parameters are listed in Table S3. Note that the ratios of time constants between NCs with and without BQ are nearly independent of pump fluence (or ⟨N⟩), as shown in Figure S6 and Table S4. According to the results presented above, we can conclude that controlling the same m value can obtain the same ET efficiencies in NC-BQ complexes even with different sizes.

In conclusion, CsPbBr3 NCs with various sizes have been synthesized by varying the contents of the DDAB ligand at room temperature under an air atmosphere. Electron acceptor BQ molecules are employed to investigate the ultrafast interfacial ET processes from CsPbBr3 NCs by using time-resolved PL and differential transmission spectra. The addition of BQ molecules can effectively quench the PL in all-sized CsPbBr3 NCs. Upon addition of the same concentration of BQ molecules, ηET increases with NC size, due to the fact that the number of BQ molecules per NC is larger in larger NCs. When the same number of BQ molecules per NC is maintained, both the degree of PL quenching and ηET in NC-BQ complexes are almost the same for different NC sizes. This reveals that the acceptor number per NC is the dominant factor for controlling the efficiency of interfacial ET processes, as compared with NC sizes.

This work is supported by the National Natural Science Foundation of China (Grants 12104311, 12174108, and 12004239), the Shanghai Chenguang Program (Grant 22CGA74), the National Key R&D Program of China (Grant 2021YFB3501700), the Shanghai Science and Technology Committee (STCSM) Science and Technology Innovation Program (Grants 22N21900400 and 23N21900100), the Key R&D Program of Jiangsu Province (Grant BE2023048), and the Key R&D Program of Zhejiang Province (Grant 2024C01193).

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